WorldWideScience

Sample records for high aerosol activity

  1. Development of unmanned aerial vehicle (UAV) based high altitude balloon (HAB) platform for active aerosol sampling

    Science.gov (United States)

    Lateran, S.; Sedan, M. F.; Harithuddin, A. S. M.; Azrad, S.

    2016-10-01

    The knowledge on the abundance and diversity of the minute particles or aerosols in the earth's stratosphere is still in its infancy as aerosol sampling at high-altitude still possess a lot of challenges. Thus far, high-altitude aerosol sampling has been conducted mostly using manned flights, which requires enormous financial and logistical resources. There had been researches for the utilisation of high altitude balloon (HAB) for active and passive aerosol samplings within the stratosphere. However, the gathered samples in the payload were either brought down by controlling the balloon air pressure or were just dropped with a parachute to slow the descend speed in order to reduce the impact upon landing. In most cases, the drop location of the sample are unfavorable such as in the middle of the sea, dense foliage, etc. Hence a system that can actively sample aerosols at high-altitude and improve the delivery method in terms of quality and reliability using unmanned aerial vehicle (UAV) is designed and tested in this study.

  2. Importance of aerosol composition and mixing state for cloud droplet activation in the high Arctic

    Directory of Open Access Journals (Sweden)

    C. Leck

    2014-08-01

    Full Text Available Concentrations of cloud condensation nuclei (CCN were measured throughout an expedition by icebreaker around the central Arctic Ocean, including a 3 week ice drift operation at 87° N, from 3 August to 9 September 2008. In agreement with previous observations in the area and season median daily CCN concentrations at 0.2% water vapor supersaturation were typically in the range of 15 to 30 cm−3, but concentrations varied by two to three orders of magnitude over the expedition and were occasionally below 1 cm−3. The CCN concentrations were highest near the ice edge and fell by a factor of three in the first 48 h of transport from the open sea into the pack ice region. For longer transport times they increased again indicating a local source over the pack ice, suggested to be polymer gels, via drops injected into the air by bubbles bursting on open leads. By assuming Köhler theory and simulating the cloud nucleation process using a Lagrangian adiabatic air parcel model that solves the kinetic formulation for condensation of water on size resolved aerosol particles we inferred the properties of the unexplained non-water soluble aerosol fraction that is necessary for reproducing the observed concentrations of CCN. We propose that the portion of the internally/externally mixed water insoluble particles was larger in the corresponding smaller aerosol sizes ranges. These particles were physically and chemically behaving as polymer gels: the interaction of the hydrophilic and hydrophobic entities on the structures of polymer gels during cloud droplet activation would at first only show a partial wetting character and only weak hygroscopic growth. Given time, a high CCN activation efficiency is achieved, which is promoted by the hydrophilicity or surface-active properties of the gels. Thus the result in this study argues for that the behavior of the high Arctic aerosol in CCN-counters operating at water vapor supersaturations > 0.4% (high relative

  3. Using Airborne High Spectral Resolution Lidar Data to Evaluate Combined Active Plus Passive Retrievals of Aerosol Extinction Profiles

    Science.gov (United States)

    Burton, S. P.; Ferrare, R. A.; Hostetler, C. A.; Hair, J. W.; Kittaka, C.; Vaughn, M. A.; Remer, L. A.

    2010-01-01

    We derive aerosol extinction profiles from airborne and space-based lidar backscatter signals by constraining the retrieval with column aerosol optical thickness (AOT), with no need to rely on assumptions about aerosol type or lidar ratio. The backscatter data were acquired by the NASA Langley Research Center airborne High Spectral Resolution Lidar (HSRL) and by the Cloud-Aerosol Lidar with Orthogonal Polarization (CALIOP) instrument on the Cloud-Aerosol Lidar and Infrared Pathfinder Satellite Observation (CALIPSO) satellite. The HSRL also simultaneously measures aerosol extinction coefficients independently using the high spectral resolution lidar technique, thereby providing an ideal data set for evaluating the retrieval. We retrieve aerosol extinction profiles from both HSRL and CALIOP attenuated backscatter data constrained with HSRL, Moderate-Resolution Imaging Spectroradiometer (MODIS), and Multiangle Imaging Spectroradiometer column AOT. The resulting profiles are compared with the aerosol extinction measured by HSRL. Retrievals are limited to cases where the column aerosol thickness is greater than 0.2 over land and 0.15 over water. In the case of large AOT, the results using the Aqua MODIS constraint over water are poorer than Aqua MODIS over land or Terra MODIS. The poorer results relate to an apparent bias in Aqua MODIS AOT over water observed in August 2007. This apparent bias is still under investigation. Finally, aerosol extinction coefficients are derived from CALIPSO backscatter data using AOT from Aqua MODIS for 28 profiles over land and 9 over water. They agree with coincident measurements by the airborne HSRL to within +/-0.016/km +/- 20% for at least two-thirds of land points and within +/-0.028/km +/- 20% for at least two-thirds of ocean points.

  4. Highly Resolved Paleoclimatic Aerosol Records

    DEFF Research Database (Denmark)

    Kettner, Ernesto

    experimentally. Over the last decades Continuous Flow Analysis (CFA) has become a well-established technique for aerosol quantification. In CFA, a piece of core is melted continuously and the melt water is analysed for an array of chemical impurities. When designing a CFA system, a trilemma between high sample...... with frequently changing signs are preserved. Therefore, these aerosol records can be used for dating by annual layer counting. However, with increasing depth the annual layer thicknesses decreases due to pressure and ice flow and accurate dating is possible only as long as the rapid variations can be resolved...... impossible to circumvent by employing a third detection technique - laser scattering. Reliable information on size changes, even relative ones, cannot be obtained using optical methods. It is therefore proposed to focus further efforts on electrical measurements, making use of the advancements made over...

  5. CCN activity of aliphatic amine secondary aerosol

    Directory of Open Access Journals (Sweden)

    X. Tang

    2014-01-01

    Full Text Available Aliphatic amines can form secondary aerosol via oxidation with atmospheric radicals (e.g. hydroxyl radical and nitrate radical. The particle composition can contain both secondary organic aerosol (SOA and inorganic salts. The fraction of organic to inorganic materials in the particulate phase influences aerosol hygroscopicity and cloud condensation nuclei (CCN activity. SOA formed from trimethylamine (TMA and butylamine (BA reactions with hydroxyl radical (OH is composed of organic material of low hygroscopicity (single hygroscopicity parameter, κ ≤ 0.25. Secondary aerosol formed from the tertiary aliphatic amine (TMA with N2O5 (source of nitrate radical, NO3, contains less volatile compounds than the primary aliphatic amine (BA aerosol. TMA + N2O5 form semi-volatile organics in low RH conditions that have κ ~ 0.20, indicative of slightly soluble organic material. As RH increases, several inorganic amine salts are formed as a result of acid-base reactions. The CCN activity of the humid TMA-N2O5 aerosol obeys Zdanovskii, Stokes, and Robinson (ZSR ideal mixing rules. Higher CCN activity (κ > 0.3 was also observed for humid BA+N2O5 aerosols compared with dry aerosol (κ ~ 0.2, as a result of the formation of inorganic salts such as NH4NO3 and butylamine nitrate (C4H11N · HNO3. Compared with TMA, BA+N2O5 reactions produce more volatile aerosols. The BA+N2O5 aerosol products under humid experiments were found to be very sensitive to the temperature within the stream-wise continuous flow thermal gradient CCN counter. The CCN counter, when set above a 21 °C temperature difference, evaporates BA+N2O5 aerosol formed at RH ≥ 30%; κ ranges from 0.4 to 0.7 and is dependent on the instrument supersaturation (ss settings. The aerosol behaves non-ideally, hence simple ZSR rules cannot be applied to the CCN results from the primary aliphatic amine system. Overall, aliphatic amine aerosol systems κ ranges from 0.2 < κ < 0.7. This work indicates that

  6. Total Lightning Flash Activity Response to Aerosol over China Area

    Directory of Open Access Journals (Sweden)

    Pengguo Zhao

    2017-01-01

    Full Text Available Twelve years of measurements of aerosol optical depth (AOD, cloud fraction, cloud top height, ice cloud optical thickness and lightning flash density from 2001 to 2012 have been analyzed to investigate the effect of aerosols on electrical activity over an area of China. The results show that increasing aerosol loading inspires the convective intensity, and then increases the lightning flash density. The spatial distribution of the correlation between aerosol loading and electrical activity shows a remarkable regional difference over China. The high-correlation regions embody the positive aerosol microphysical effect on the intensity of the electrical activity, while the large-scale processes may play the main role in convection development and producing lightning in low-correlation regions.

  7. CCN activity of aliphatic amine secondary aerosol

    Science.gov (United States)

    Tang, X.; Price, D.; Praske, E.; Vu, D.; Purvis-Roberts, K.; Silva, P. J.; Cocker, D. R., III; Asa-Awuku, A.

    2014-01-01

    Aliphatic amines can form secondary aerosol via oxidation with atmospheric radicals (e.g. hydroxyl radical and nitrate radical). The particle composition can contain both secondary organic aerosol (SOA) and inorganic salts. The fraction of organic to inorganic materials in the particulate phase influences aerosol hygroscopicity and cloud condensation nuclei (CCN) activity. SOA formed from trimethylamine (TMA) and butylamine (BA) reactions with hydroxyl radical (OH) is composed of organic material of low hygroscopicity (single hygroscopicity parameter, κ ≤ 0.25). Secondary aerosol formed from the tertiary aliphatic amine (TMA) with N2O5 (source of nitrate radical, NO3), contains less volatile compounds than the primary aliphatic amine (BA) aerosol. TMA + N2O5 form semi-volatile organics in low RH conditions that have κ ~ 0.20, indicative of slightly soluble organic material. As RH increases, several inorganic amine salts are formed as a result of acid-base reactions. The CCN activity of the humid TMA-N2O5 aerosol obeys Zdanovskii, Stokes, and Robinson (ZSR) ideal mixing rules. Higher CCN activity (κ > 0.3) was also observed for humid BA+N2O5 aerosols compared with dry aerosol (κ ~ 0.2), as a result of the formation of inorganic salts such as NH4NO3 and butylamine nitrate (C4H11N · HNO3). Compared with TMA, BA+N2O5 reactions produce more volatile aerosols. The BA+N2O5 aerosol products under humid experiments were found to be very sensitive to the temperature within the stream-wise continuous flow thermal gradient CCN counter. The CCN counter, when set above a 21 °C temperature difference, evaporates BA+N2O5 aerosol formed at RH ≥ 30%; κ ranges from 0.4 to 0.7 and is dependent on the instrument supersaturation (ss) settings. The aerosol behaves non-ideally, hence simple ZSR rules cannot be applied to the CCN results from the primary aliphatic amine system. Overall, aliphatic amine aerosol systems κ ranges from 0.2 systems.

  8. Highly Resolved Paleoclimatic Aerosol Records

    DEFF Research Database (Denmark)

    Kettner, Ernesto

    In ice cores a plethora of proxies for paleoclimatic conditions is archived. Air trapped in the ice during firnification allows for direct measurements of the concentrations and isotope ratios of paleoatmospheric gases while, the isotopic composition of the ice matrix itself is related...... to paleotemperatures. Impurities in the matrix are comprised of particulate and soluble aerosols, each carrying information on its source’s activitiy and|or proximity. Opposed to gases and water isotopes, the seasonality of many aerosols is not smoothed out in the firn column so that large concentration gradients...... with frequently changing signs are preserved. Therefore, these aerosol records can be used for dating by annual layer counting. However, with increasing depth the annual layer thicknesses decreases due to pressure and ice flow and accurate dating is possible only as long as the rapid variations can be resolved...

  9. Aerosol classification by airborne high spectral resolution lidar observations

    Directory of Open Access Journals (Sweden)

    S. Groß

    2012-10-01

    Full Text Available During four aircraft field experiments with the DLR research aircraft Falcon in 1998 (LACE, 2006 (SAMUM-1 and 2008 (SAMUM-2 and EUCAARI, airborne High Spectral Resolution Lidar (HSRL and in situ measurements of aerosol microphysical and optical properties were performed. Altogether, the properties of six different aerosol types and aerosol mixtures – Saharan mineral dust, Saharan dust mixtures, Canadian biomass burning aerosol, African biomass burning aerosol, anthropogenic pollution aerosol, and marine aerosol have been studied. On the basis of this extensive HSRL data set, we present an aerosol classification scheme which is also capable to identify mixtures of different aerosol types. We calculated mixing lines that allowed us to determine the contributing aerosol types. The aerosol classification scheme was validated with in-situ measurements and backward trajectory analyses. Our results demonstrate that the developed aerosol mask is capable to identify complex stratifications with different aerosol types throughout the atmosphere.

  10. Incorporation of advanced aerosol activation treatments into CESM/CAM5: model evaluation and impacts on aerosol indirect effects

    Science.gov (United States)

    Gantt, B.; He, J.; Zhang, X.; Zhang, Y.; Nenes, A.

    2014-07-01

    One of the greatest sources of uncertainty in the science of anthropogenic climate change is from aerosol-cloud interactions. The activation of aerosols into cloud droplets is a direct microphysical linkage between aerosols and clouds; parameterizations of this process link aerosol with cloud condensation nuclei (CCN) and the resulting indirect effects. Small differences between parameterizations can have a large impact on the spatiotemporal distributions of activated aerosols and the resulting cloud properties. In this work, we incorporate a series of aerosol activation schemes into the Community Atmosphere Model version 5.1.1 within the Community Earth System Model version 1.0.5 (CESM/CAM5) which include factors such as insoluble aerosol adsorption and giant cloud condensation nuclei (CCN) activation kinetics to understand their individual impacts on global-scale cloud droplet number concentration (CDNC). Compared to the existing activation scheme in CESM/CAM5, this series of activation schemes increase the computation time by ~10% but leads to predicted CDNC in better agreement with satellite-derived/in situ values in many regions with high CDNC but in worse agreement for some regions with low CDNC. Large percentage changes in predicted CDNC occur over desert and oceanic regions, owing to the enhanced activation of dust from insoluble aerosol adsorption and reduced activation of sea spray aerosol after accounting for giant CCN activation kinetics. Comparison of CESM/CAM5 predictions against satellite-derived cloud optical thickness and liquid water path shows that the updated activation schemes generally improve the low biases. Globally, the incorporation of all updated schemes leads to an average increase in column CDNC of 150% and an increase (more negative) in shortwave cloud forcing of 12%. With the improvement of model-predicted CDNCs and better agreement with most satellite-derived cloud properties in many regions, the inclusion of these aerosol activation

  11. High Concentration Standard Aerosol Generator.

    Science.gov (United States)

    1985-07-31

    materials. In addition to material problems, many liquids are extremely flammable or explosive when aerosolized. This can be checked by putting a small...Hochriner. D. (1975) Stub 3A 440-445. St6ber, W. Flachsbart, H. and Hochramn, D. (1970) Staub 3^, 277. Yoshida. H. Fujii, K. Yomimoto, Y. Masuda. H. and

  12. Aerosol classification by airborne high spectral resolution lidar observations

    Science.gov (United States)

    Groß, S.; Esselborn, M.; Weinzierl, B.; Wirth, M.; Fix, A.; Petzold, A.

    2013-03-01

    During four aircraft field experiments with the DLR research aircraft Falcon in 1998 (LACE), 2006 (SAMUM-1) and 2008 (SAMUM-2 and EUCAARI), airborne High Spectral Resolution Lidar (HSRL) and in situ measurements of aerosol microphysical and optical properties were performed. Altogether, the properties of six different aerosol types and aerosol mixtures - Saharan mineral dust, Saharan dust mixtures, Canadian biomass burning aerosol, African biomass burning mixture, anthropogenic pollution aerosol, and marine aerosol have been studied. On the basis of this extensive HSRL data set, we present an aerosol classification scheme which is also capable to identify mixtures of different aerosol types. We calculated mixing lines that allowed us to determine the contributing aerosol types. The aerosol classification scheme was supported by backward trajectory analysis and validated with in-situ measurements. Our results demonstrate that the developed aerosol mask is capable to identify complex stratifications with different aerosol types throughout the atmosphere.

  13. Coarse mode aerosols in the High Arctic

    Science.gov (United States)

    Baibakov, K.; O'Neill, N. T.; Chaubey, J. P.; Saha, A.; Duck, T. J.; Eloranta, E. W.

    2014-12-01

    Fine mode (submicron) aerosols in the Arctic have received a fair amount of scientific attention in terms of smoke intrusions during the polar summer and Arctic haze pollution during the polar winter. Relatively little is known about coarse mode (supermicron) aerosols, notably dust, volcanic ash and sea salt. Asian dust is a regular springtime event whose optical and radiative forcing effects have been fairly well documented at the lower latitudes over North America but rarely reported for the Arctic. Volcanic ash, whose socio-economic importance has grown dramatically since the fear of its effects on aircraft engines resulted in the virtual shutdown of European civil aviation in the spring of 2010 has rarely been reported in the Arctic in spite of the likely probability that ash from Iceland and the Aleutian Islands makes its way into the Arctic and possibly the high Arctic. Little is known about Arctic sea salt aerosols and we are not aware of any literature on the optical measurement of these aerosols. In this work we present preliminary results of the combined sunphotometry-lidar analysis at two High Arctic stations in North America: PEARL (80°N, 86°W) for 2007-2011 and Barrow (71°N,156°W) for 2011-2014. The multi-years datasets were analyzed to single out potential coarse mode incursions and study their optical characteristics. In particular, CIMEL sunphotometers provided coarse mode optical depths as well as information on particle size and refractive index. Lidar measurements from High Spectral Resolution lidars (AHSRL at PEARL and NSHSRL at Barrow) yielded vertically resolved aerosol profiles and gave an indication of particle shape and size from the depolarization ratio and color ratio profiles. Additionally, we employed supplementary analyses of HYSPLIT backtrajectories, OMI aerosol index, and NAAPS (Navy Aerosol Analysis and Prediction System) outputs to study the spatial context of given events.

  14. On the limits of Köhler activation theory: how do collision and coalescence affect the activation of aerosols?

    Science.gov (United States)

    Hoffmann, Fabian

    2017-07-01

    Activation is necessary to form a cloud droplet from an aerosol, and it is widely accepted that it occurs as soon as a wetted aerosol grows beyond its critical radius. Traditional Köhler theory assumes that this growth is driven by the diffusion of water vapor. However, if the wetted aerosols are large enough, the coalescence of two or more particles is an additional process for accumulating sufficient water for activation. This transition from diffusional to collectional growth marks the limit of traditional Köhler theory and it is studied using a Lagrangian cloud model in which aerosols and cloud droplets are represented by individually simulated particles within large-eddy simulations of shallow cumuli. It is shown that the activation of aerosols larger than 0. 1 µm in dry radius can be affected by collision and coalescence, and its contribution increases with a power-law relation toward larger radii and becomes the only process for the activation of aerosols larger than 0. 4-0. 8 µm depending on aerosol concentration. Due to the natural scarcity of the affected aerosols, the amount of aerosols that are activated by collection is small, with a maximum of 1 in 10 000 activations. The fraction increases as the aerosol concentration increases, but decreases again as the number of aerosols becomes too high and the particles too small to cause collections. Moreover, activation by collection is found to affect primarily aerosols that have been entrained above the cloud base.

  15. Constructing An Event Based Aerosol Product Under High Aerosol Loading Conditions

    Science.gov (United States)

    Levy, R. C.; Shi, Y.; Mattoo, S.; Remer, L. A.; Zhang, J.

    2016-12-01

    High aerosol loading events, such as the Indonesia's forest fire in Fall 2015 or the persistent wintertime haze near Beijing, gain tremendous interests due to their large impact on regional visibility and air quality. Understanding the optical properties of these events and further being able to simulate and predict these events are beneficial. However, it is a great challenge to consistently identify and then retrieve aerosol optical depth (AOD) from passive sensors during heavy aerosol events. Some reasons include:1). large differences between optical properties of high-loading aerosols and those under normal conditions, 2) spectral signals of optically thick aerosols can be mistaken with surface depending on aerosol types, and 3) Extremely optically thick aerosol plumes can also be misidentified as clouds due to its high optical thickness. Thus, even under clear-sky conditions, the global distribution of extreme aerosol events is not well captured in datasets such as the MODIS Dark-Target (DT) aerosol product. In this study, with the synthetic use of OMI Aerosol Index, MODIS cloud product, and operational DT product, the heavy smoke events over the seven sea region are identified and retrieved over the dry season. An event based aerosol product that would compensate the standard "global" aerosol retrieval will be created and evaluated. The impact of missing high AOD retrievals on the regional aerosol climatology will be studied using this newly developed research product.

  16. Aerosol effects on deep convective clouds: impact of changes in aerosol size distribution and aerosol activation parameterization

    Science.gov (United States)

    Ekman, A. M. L.; Engström, A.; Söderberg, A.

    2010-03-01

    A cloud-resolving model including explicit aerosol physics and chemistry is used to study the impact of aerosols on deep convective strength. More specifically, by conducting six sensitivity series we examine how the complexity of the aerosol model, the size of the aerosols and the aerosol activation parameterization influence the aerosol-induced deep convective cloud sensitivity. Only aerosol effects on liquid droplet formation are considered. We find that an increased aerosol concentration generally results in stronger convection, which for the simulated case is in agreement with the conceptual model presented by Rosenfeld et al. (2008). However, there are two sensitivity series that do not display a monotonic increase in updraft velocity with increasing aerosol concentration. These exceptions illustrate the need to: 1) account for changes in evaporation processes and subsequent cooling when assessing aerosol effects on deep convective strength, 2) better understand graupel impaction scavenging of aerosols which may limit the number of CCN at a critical stage of cloud development and thereby dampen the convection, 3) increase our knowledge of aerosol recycling due to evaporation of cloud droplets. Furthermore, we find a significant difference in the aerosol-induced deep convective cloud sensitivity when using different complexities of the aerosol model and different aerosol activation parameterizations. For the simulated case, a 100% increase in aerosol concentration results in a difference in average updraft between the various sensitivity series which is as large as the average updraft increase itself. The model simulations also show that the change in graupel and rain formation is not necessarily directly proportional to the change in updraft velocity. For example, several of the sensitivity series display a decrease of the rain amount at the lowest model level with increasing updraft velocity. Finally, an increased number of aerosols in the Aitken mode (here

  17. Aerosol effects on deep convective clouds: impact of changes in aerosol size distribution and aerosol activation parameterization

    Directory of Open Access Journals (Sweden)

    A. M. L. Ekman

    2010-03-01

    Full Text Available A cloud-resolving model including explicit aerosol physics and chemistry is used to study the impact of aerosols on deep convective strength. More specifically, by conducting six sensitivity series we examine how the complexity of the aerosol model, the size of the aerosols and the aerosol activation parameterization influence the aerosol-induced deep convective cloud sensitivity. Only aerosol effects on liquid droplet formation are considered. We find that an increased aerosol concentration generally results in stronger convection, which for the simulated case is in agreement with the conceptual model presented by Rosenfeld et al. (2008. However, there are two sensitivity series that do not display a monotonic increase in updraft velocity with increasing aerosol concentration. These exceptions illustrate the need to: 1 account for changes in evaporation processes and subsequent cooling when assessing aerosol effects on deep convective strength, 2 better understand graupel impaction scavenging of aerosols which may limit the number of CCN at a critical stage of cloud development and thereby dampen the convection, 3 increase our knowledge of aerosol recycling due to evaporation of cloud droplets. Furthermore, we find a significant difference in the aerosol-induced deep convective cloud sensitivity when using different complexities of the aerosol model and different aerosol activation parameterizations. For the simulated case, a 100% increase in aerosol concentration results in a difference in average updraft between the various sensitivity series which is as large as the average updraft increase itself. The model simulations also show that the change in graupel and rain formation is not necessarily directly proportional to the change in updraft velocity. For example, several of the sensitivity series display a decrease of the rain amount at the lowest model level with increasing updraft velocity. Finally, an increased number of aerosols in the

  18. High resolution aerosol optical thickness retrieval over the Pearl River Delta region with improved aerosol modelling

    Institute of Scientific and Technical Information of China (English)

    WONG; ManSing; NICHOL; Janet; LEE; Kwon; Ho

    2009-01-01

    Aerosol retrieval algorithms for the MODerate Resolution Imaging Spectroradiometer (MODIS) have been developed to estimate aerosol and microphysical properties of the atmosphere, which help to address aerosol climatic issues at global scale. However, higher spatial resolution aerosol products for urban areas have not been well researched mainly due to the difficulty of differentiating aerosols from bright surfaces in urban areas. Here, a new aerosol retrieval algorithm using the MODIS 500 m resolution images is described, to retrieve aerosol properties over Hong Kong and the Pearl River Delta region. The rationale of our technique is to first estimate the aerosol reflectance by decomposing the top-of-atmosphere reflectance from surface reflectance and Rayleigh path reflectance. For the determination of surface reflectance, a modified Minimum Reflectance Technique (MRT) is used, and MRT images are computed for different seasons. A strong correlation is shown between the surface reflectance of MRT images and MODIS land surface reflectance products (MOD09), with a value of 0.9. For conversion of aerosol reflectance to Aerosol Optical Thickness (AOT), comprehensive Look Up Tables (LUT) are constructed, in which aerosol properties and sun-viewing geometry in the radiative transfer calculations are taken into account. Four aerosol types, namely mixed urban, polluted urban, dust, and heavy pollution, were derived using cluster analysis on three years of AERONET measurements in Hong Kong. Their aerosol properties were input for LUT calculation. The resulting 500 m AOT images are highly correlated (r = 0.89) with AERONET sunphotometer observations in Hong Kong. This study demonstrates the applicability of aerosol retrieval at fine resolution scale in urban areas, which can assist the study of aerosol loading distribution and the impact of localized and transient pollution on urban air quality. In addition, the MODIS 500 m AOT images can be used to study cross

  19. High resolution aerosol optical thickness retrieval over the Pearl River Delta region with improved aerosol modelling

    Institute of Scientific and Technical Information of China (English)

    WONG ManSing; NICHOL Janet; LEE Kwon Ho; LI ZhanQing

    2009-01-01

    Aerosol retrieval algorithms for the MODerate Resolution Imaging Spectroradiometer (MODIS) have been developed to estimate aerosol and microphysical properties of the atmosphere, which help to address aerosol climatic issues at global scale. However, higher spatial resolution aerosol products for urban areas have not been well researched mainly due to the difficulty of differentiating aerosols from bright surfaces in urban areas. Here, a new aerosol retrieval algorithm using the MODIS 500 m resolu-tion images is described, to retrieve aerosol properties over Hong Kong and the Pearl River Delta re-gion. The rationale of our technique is to first estimate the aerosol reflectance by decomposing the top-of-atmosphere reflectance from surface reflectance and Rayleigh path reflectance. For the deter-mination of surface reflectance, a modified Minimum Reflectance Technique (MRT) is used, and MRT images are computed for different seasons. A strong correlation is shown between the surface reflec-tance of MRT images and MODIS land surface reflectance products (MOD09), with a value of 0.9. For conversion of aerosol reflectance to Aerosol Optical Thickness (AOT), comprehensive Look Up Tables (LUT) are constructed, in which aerosol properties and sun-viewing geometry in the radiative transfer calculations are taken into account. Four aerosol types, namely mixed urban, polluted urban, dust, and heavy pollution, were derived using cluster analysis on three years of AERONET measurements in Hong Kong. Their aerosol properties were input for LUT calculation. The resulting 500 m AOT images are highly correlated (r=0.89) with AERONET sunphotometer observations in Hong Kong. This study demonstrates the applicability of aerosol retrieval at fine resolution scale in urban areas, which can assist the study of aerosol loading distribution and the impact of localized and transient pollution on urban air quality. In addition, the MODIS 500 m AOT images can be used to study cross

  20. Ben Macdhui High Altitude Trace Gas and Aerosol Transport Experiment

    CSIR Research Space (South Africa)

    Piketh, SJ

    1999-01-01

    Full Text Available The Ben Macdhui High Altitude Aerosol and Trace Gas Transport Experiment (BHATTEX) was started to characterize the nature and magnitude of atmospheric, aerosol and trace gas transport paths recirculation over and exiting from southern Africa...

  1. Aerosols and lightning activity: The effect of vertical profile and aerosol type

    Science.gov (United States)

    Proestakis, E.; Kazadzis, S.; Lagouvardos, K.; Kotroni, V.; Amiridis, V.; Marinou, E.; Price, C.; Kazantzidis, A.

    2016-12-01

    The Cloud-Aerosol Lidar with Orthogonal Polarization (CALIOP) instrument on board the Cloud-Aerosol Lidar and Infrared Pathfinder Satellite Observations (CALIPSO) satellite has been utilized for the first time in a study regarding lightning activity modulation due to aerosols. Lightning activity observations, obtained by the ZEUS long range Lightning Detection Network, European Centre for Medium range Weather Forecasts (ECMWF) Convective Available Potential Energy (CAPE) data and Cloud Fraction (CF) retrieved by MODIS on board Aqua satellite have been combined with CALIPSO CALIOP data over the Mediterranean basin and for the period March to November, from 2007 to 2014. The results indicate that lightning activity is enhanced during days characterized by higher Aerosol Optical Depth (AOD) values, compared to days with no lightning. This study contributes to existing studies on the link between lightning activity and aerosols, which have been based just on columnar AOD satellite retrievals, by performing a deeper analysis into the effect of aerosol profiles and aerosol types. Correlation coefficients of R = 0.73 between the CALIPSO AOD and the number of lightning strikes detected by ZEUS and of R = 0.93 between ECMWF CAPE and lightning activity are obtained. The analysis of extinction coefficient values at 532 nm indicates that at an altitudinal range exists, between 1.1 km and 2.9 km, where the values for extinction coefficient of lightning-active and non-lightning-active cases are statistically significantly different. Finally, based on the CALIPSO aerosol subtype classification, we have investigated the aerosol conditions of lightning-active and non-lightning-active cases. According to the results polluted dust aerosols are more frequently observed during non-lightning-active days, while dust and smoke aerosols are more abundant in the atmosphere during the lightning-active days.

  2. CCN activation of ambient and "synthetic ambient" urban aerosol

    Science.gov (United States)

    Burkart, Julia; Reischl, Georg; Steiner, Gerhard; Bauer, Heidi; Leder, Klaus; Kistler, Magda; Puxbaum, Hans; Hitzenberger, R.

    2013-05-01

    In this study, the Cloud Condensation Nuclei (CCN) activation properties of the urban aerosol in Vienna, Austria, were investigated in a long term (11 month) field study. Filter samples of the aerosol below 100 nm were taken in parallel to these measurements, and later used to generate "synthetic ambient" aerosols. Activation parameters of this "synthetic ambient" aerosol were also obtained. Hygroscopicity parameters κ [1] were calculated both for the urban and the "synthetic ambient" aerosol and also from the chemical composition. Average κ for the "synthetic ambient" aerosol ranged from 0.20 to 0.30 with an average value of 0.24, while the κ from the chemical composition of this "synthetic ambient" aerosol was significantly higher (average 0.43). The full results of the study are given elsewhere [2,3].

  3. Ice Nucleation Activity of Various Agricultural Soil Dust Aerosol Particles

    Science.gov (United States)

    Schiebel, Thea; Höhler, Kristina; Funk, Roger; Hill, Thomas C. J.; Levin, Ezra J. T.; Nadolny, Jens; Steinke, Isabelle; Suski, Kaitlyn J.; Ullrich, Romy; Wagner, Robert; Weber, Ines; DeMott, Paul J.; Möhler, Ottmar

    2016-04-01

    Recent investigations at the cloud simulation chamber AIDA (Aerosol Interactions and Dynamics in the Atmosphere) suggest that agricultural soil dust has an ice nucleation ability that is enhanced up to a factor of 10 compared to desert dust, especially at temperatures above -26 °C (Steinke et al., in preparation for submission). This enhancement might be caused by the contribution of very ice-active biological particles. In addition, soil dust aerosol particles often contain a considerably higher amount of organic matter compared to desert dust particles. To test agricultural soil dust as a source of ice nucleating particles, especially for ice formation in warm clouds, we conducted a series of laboratory measurements with different soil dust samples to extend the existing AIDA dataset. The AIDA has a volume of 84 m3 and operates under atmospherically relevant conditions over wide ranges of temperature, pressure and humidity. By controlled adiabatic expansions, the ascent of an air parcel in the troposphere can be simulated. As a supplement to the AIDA facility, we use the INKA (Ice Nucleation Instrument of the KArlsruhe Institute of Technology) continuous flow diffusion chamber based on the design by Rogers (1988) to expose the sampled aerosol particles to a continuously increasing saturation ratio by keeping the aerosol temperature constant. For our experiments, soil dust was dry dispersed into the AIDA vessel. First, fast saturation ratio scans at different temperatures were performed with INKA, sampling soil dust aerosol particles directly from the AIDA vessel. Then, we conducted the AIDA expansion experiment starting at a preset temperature. The combination of these two different methods provides a robust data set on the temperature-dependent ice activity of various agriculture soil dust aerosol particles with a special focus on relatively high temperatures. In addition, to extend the data set, we investigated the role of biological and organic matter in more

  4. Biological aerosol detection with combined passive-active infrared measurements

    Science.gov (United States)

    Ifarraguerri, Agustin I.; Vanderbeek, Richard G.; Ben-David, Avishai

    2004-12-01

    A data collection experiment was performed in November of 2003 to measure aerosol signatures using multiple sensors, all operating in the long-wave infrared. The purpose of this data collection experiment was to determine whether combining passive hyperspectral and LIDAR measurements can substantially improve biological aerosol detection performance. Controlled releases of dry aerosols, including road dust, egg albumin and two strains of Bacillus Subtilis var. Niger (BG) spores were performed using the ECBC/ARTEMIS open-path aerosol test chamber located in the Edgewood Area of Aberdeen Proving Grounds, MD. The chamber provides a ~ 20' path without optical windows. Ground truth devices included 3 aerodynamic particle sizers, an optical particle size spectrometer, 6 nephelometers and a high-volume particle sampler. Two sensors were used to make measurements during the test: the AIRIS long-wave infrared imaging spectrometer and the FAL CO2 LIDAR. The AIRIS and FAL data sets were analyzed for detection performance relative to the ground truth. In this paper we present experimental results from the individual sensors as well as results from passive-active sensor fusion. The sensor performance is presented in the form of receiver operating characteristic curves.

  5. Impact of aerosol composition on cloud condensation nuclei activity

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    Q. Zhang

    2012-04-01

    Full Text Available The impact of aerosol composition on cloud condensation nuclei (CCN activity were analyzed in this study based on field experiments carried out at downtown Tianjin, China in September 2010. In the experiments, the CCN measurements were performed at supersaturation (SS of 0.1%, 0.2% and 0.4% using a thermal-gradient diffusion chamber (DMT CCNC, whereas the aerosol size distribution and composition were simultaneously measured with a TSI SMPS and an Aerodyne Aerosol Mass Spectrometer (AMS, respectively. The results show that the influence of aerosol composition on CCN activity is notable under low SS (0.1%, and their influence decreased with increasing SS. For example, under SS of 0.1%, the CCN activity increases from 4.5±2.6% to 12.8±6.1% when organics fraction decrease from 30–40% to 10–20%. The rate of increase reached up to 184%. While under SS of 0.4%, the CCN activity increases only from 35.7±19.0% to 46.5±12.3% correspondingly. The calculated NCCN based on the size-resolved activation ratio and aerosol number size distribution correlated well with observed NCCN at high SS (0.4%, but this consistence decreased with the falling of SS. The slopes of linear fitted lines between calculated and observed NCCN are 0.708, 0.947, and 0.995 at SS of 0.1%, 0.2% and 0.4% respectively. Moreover, the stand deviation (SD of calculated NCCN increased with the decreasing of SS. A case study of CCN closure analyses indicated that the calculated error of NCCN could reach up to 34% at SS of 0.1% if aerosol composition were not included, and the calculated error decreased with the raising of SS. It is decreased to 9% at SS of 0.2%, and further decreased to 4% at SS of 0.4%.

  6. Impact of aerosol composition on cloud condensation nuclei activity

    Directory of Open Access Journals (Sweden)

    Q. Zhang

    2012-01-01

    Full Text Available The impact of aerosol composition on cloud condensation nuclei (CCN activity was analyzed in this study based on field experiments carried out at downtown Tianjin, China, in September 2010. In the experiments, the CCN measurements were performed at supersaturation (SS of 0.1%, 0.2% and 0.4% using a thermal-gradient diffusion chamber (DMT CCNC, whereas the aerosol size distribution and composition were simultaneously measured with a TSI SMPS and an Aerodyne Aerosol Mass Spectrometer (AMS, respectively. The results show that the influence of aerosol composition on CCN activity is notable under low SS (0.1%, and their influence decreased with increasing SS. For example, under SS of 0.1%, the CCN activity increases from 4.5 ± 2.6% to 12.8 ± 6.1% when organics fraction decrease from 30–40% to 10–20%. The rate of increase reaches up to 184%. While under SS of 0.4%, the CCN activity increases only from 35.7 ± 19.0% to 46.5 ± 12.3%, correspondingly. The calculated NCCN based on the size-resolved activation ratio and aerosol number size distribution correlates well with observed NCCN at high SS (0.4%, but this correlation decreases with the falling of SS. The slopes of linear fitted lines between calculated and observed NCCN are 0.708, 0.947, and 0.995 at SS of 0.1%, 0.2% and 0.4%, respectively. Moreover, the standard deviation (SD of calculated NCCN increases with the decreasing of SS. A case study of CCN closure analyses indicates that the calculated error of NCCN can reach up to 34% at SS of 0.1% if aerosol composition is not included, and the calculated error decreases with the raising of SS. It decreases to 9% at SS of 0.2%, and further decreases to 4% at SS of 0.4%.

  7. Estimation of daily photosynthetically active radiation (PAR) in presence of low to high aerosol loads: application to OLCI-like satellite data.

    Science.gov (United States)

    Harmel, Tristan; Chami, Malik

    2016-10-31

    Estimation of daily photosynthetically active radiation (PAR) is of primary importance for monitoring the ocean primary production and the subsequent production of carbon by phytoplankton at global scale from remote sensing ocean color sensors. On the other hand, aerosol abundance and composition play a critical role in the modulation of PAR. In this study, an original algorithm, so-called OLCIPAR, is proposed for routinely determining the daily PAR from optical satellite sensors such as the OLCI sensor aboard Sentinel-3 (ESA). The OLCIPAR algorithm has been developed to overcome some of the limitations of the current existing methods. In particular, multiple scattering effects induced by the atmospheric layer are taken into account based on exact radiative transfer calculations. Another advantage of OLCIPAR method is to consider a great variety of aerosol models to better account for their optical variability as observed in real world conditions. The OLCIPAR algorithm was applied to the archive of MERIS data, whose sensor is similar to OLCI. The validation of the retrieved daily PAR was carried out based on comparison with the time series acquired by the BOUSSOLE oceanographic buoy moored in the Mediterranean Sea. Results show a regression slope of 1% and an accuracy within 10% which confirms the robustness of the algorithm. The comparison of OLCIPAR retrievals with the products routinely distributed by NASA shows that estimates of PAR differ by up to 20% in the subtropical Atlantic Ocean where important amounts of dust aerosols are present. The improvements brought by OLCIPAR method for deriving the daily PAR could thus permit to better assess the impact of aerosols on reduction of PAR with implications on the estimation of oceanic primary production.

  8. Cloud condensation nuclei (CCN) activity of aliphatic amine secondary aerosol

    Science.gov (United States)

    Tang, X.; Price, D.; Praske, E.; Vu, D. N.; Purvis-Roberts, K.; Silva, P. J.; Cocker, D. R., III; Asa-Awuku, A.

    2014-06-01

    Aliphatic amines can form secondary aerosol via oxidation with atmospheric radicals (e.g., hydroxyl radical and nitrate radical). The particle can contain both secondary organic aerosol (SOA) and inorganic salts. The ratio of organic to inorganic materials in the particulate phase influences aerosol hygroscopicity and cloud condensation nuclei (CCN) activity. SOA formed from trimethylamine (TMA) and butylamine (BA) reactions with hydroxyl radical (OH) is composed of organic material of low hygroscopicity (single hygroscopicity parameter, κ, ≤ 0.25). Secondary aerosol formed from the tertiary aliphatic amine (TMA) with N2O5 (source of nitrate radical, NO3) contains less volatile compounds than the primary aliphatic amine (BA) aerosol. As relative humidity (RH) increases, inorganic amine salts are formed as a result of acid-base reactions. The CCN activity of the humid TMA-N2O5 aerosol obeys Zdanovskii, Stokes, and Robinson (ZSR) ideal mixing rules. The humid BA + N2O5 aerosol products were found to be very sensitive to the temperature at which the measurements were made within the streamwise continuous-flow thermal gradient CCN counter; κ ranges from 0.4 to 0.7 dependent on the instrument supersaturation (ss) settings. The variance of the measured aerosol κ values indicates that simple ZSR rules cannot be applied to the CCN results from the primary aliphatic amine system. Overall, aliphatic amine aerosol systems' κ ranges within 0.2 systems.

  9. Unexpectedly high ultrafine aerosol concentrations above East Antarctic sea-ice

    Directory of Open Access Journals (Sweden)

    R. S. Humphries

    2015-10-01

    Full Text Available The effect of aerosols on clouds and their radiative properties is one of the largest uncertainties in our understanding of radiative forcing. A recent study has concluded that better characterisation of pristine, natural aerosol processes leads to the largest reduction in these uncertainties. Antarctica, being far from anthropogenic activities, is an ideal location for the study of natural aerosol processes. Aerosol measurements in Antarctica are often limited to boundary layer air-masses at spatially sparse coastal and continental research stations, with only a handful of studies in the sea ice region. In this paper, the first observational study of sub-micron aerosols in the East Antarctic sea ice region is presented. Measurements were conducted aboard the ice-breaker Aurora Australis in spring 2012 and found that boundary layer condensation nuclei (CN3 concentrations exhibited a five-fold increase moving across the Polar Front, with mean Polar Cell concentrations of 1130 cm−3 – higher than any observed elsewhere in the Antarctic and Southern Ocean region. The absence of evidence for aerosol growth suggested that nucleation was unlikely to be local. Air parcel trajectories indicated significant influence from the free troposphere above the Antarctic continent, implicating this as the likely nucleation region for surface aerosol, a similar conclusion to previous Antarctic aerosol studies. The highest aerosol concentrations were found to correlate with low pressure systems, suggesting that the passage of cyclones provided an accelerated pathway, delivering air-masses quickly from the free-troposphere to the surface. After descent from the Antarctic free troposphere, trajectories suggest that sea ice boundary layer air-masses travelled equator-ward into the low albedo Southern Ocean region, transporting with them emissions and these aerosol nuclei where, after growth, may potentially impact on the region's radiative balance. The high aerosol

  10. Cloud — Aerosol interaction during lightning activity over land and ocean: Precipitation pattern assessment

    Science.gov (United States)

    Pal, Jayanti; Chaudhuri, Sutapa; Chowdhury, Arumita Roy; Bandyopadhyay, Tanuka

    2016-06-01

    The present study attempts to identify the land - ocean contrast in cloud - aerosol relation during lightning and non-lightning days and its effect on subsequent precipitation pattern. The thermal hypothesis in view of Convective Available Potential Energy (CAPE) behind the land - ocean contrast is observed to be insignificant in the present study region. The result shows that the lightning activities are significantly and positively correlated with aerosols over both land and ocean in case of low aerosol loading whereas for high aerosol loading the correlation is significant but, only over land. The study attempts to comprehend the mechanism through which the aerosol and lightning interact using the concept of aerosol indirect effect that includes the study of cloud effective radius, cloud fraction and precipitation rate. The result shows that the increase in lightning activity over ocean might have been caused due to the first aerosol indirect effect, while over land the aerosol indirect effect might have been suppressed due to lightning. Thus, depending on the region and relation between cloud parameters it is observed that the precipitation rate decreases (increases) over ocean during lightning (non-lightning) days. On the other hand during non-lightning days, the precipitation rate decreases over land.

  11. Primary and Secondary Organic Marine Aerosol and Oceanic Biological Activity: Recent Results and New Perspectives for Future Studies

    Directory of Open Access Journals (Sweden)

    Matteo Rinaldi

    2010-01-01

    Full Text Available One of the most important natural aerosol systems at the global level is marine aerosol that comprises both organic and inorganic components of primary and secondary origin. The present paper reviews some new results on primary and secondary organic marine aerosol, achieved during the EU project MAP (Marine Aerosol Production, comparing them with those reported in the recent literature. Marine aerosol samples collected at the coastal site of Mace Head, Ireland, show a chemical composition trend that is influenced by the oceanic biological activity cycle, in agreement with other observations. Laboratory experiments show that sea-spray aerosol from biologically active sea water can be highly enriched in organics, and the authors highlight the need for further studies on the atmospheric fate of such primary organics. With regard to the secondary fraction of organic aerosol, the average chemical composition and molecular tracer (methanesulfonic-acid, amines distribution could be successfully characterized by adopting a multitechnique analytical approach.

  12. Aerosol hygroscopicity at high (99 to 100% relative humidities

    Directory of Open Access Journals (Sweden)

    C. R. Ruehl

    2009-07-01

    Full Text Available The hygroscopicity of an aerosol largely determines its influence on climate and, for smaller particles, atmospheric lifetime. While much aerosol hygroscopicity data is available at lower relative humidities (RH and under cloud formation conditions (RH>100%, relatively little data is available at high RH (99.2 to 99.9%. We measured the size of droplets at high RH that had formed on particles composed of one of seven compounds with dry diameters between 0.1 and 0.5 μm, and calculated the hygroscopicity of these compounds. We use a parameterization of the Kelvin term, in addition to a standard parameterization (κ of the Raoult term, to express the hygroscopicity of surface-active compounds.

    For inorganic compounds, hygroscopicity could reliably be predicted using water activity data and assuming a surface tension of pure water. In contrast, most organics exhibited a slight to mild increase in hygroscopicity with droplet diameter. This trend was strongest for sodium dodecyl sulfate (SDS, the most surface-active compound studied. The results suggest that partitioning of surface-active compounds away from the bulk solution, which reduces hygroscopicity, dominates any increases in hygroscopicity due to reduced surface tension. This is opposite to what is typically assumed for soluble surfactants. Furthermore, we saw no evidence that micellization limits SDS activity in micron-sized solution droplets, as observed in macroscopic solutions. These results suggest that while the high-RH hygroscopicity of inorganic compounds can be reliably predicted using readily available data, surface-activity parameters obtained from macroscopic solutions with organic solutes may be inappropriate for calculations of the hygroscopicity of micron-sized droplets.

  13. The ice nucleation activity of biological aerosols

    Science.gov (United States)

    Grothe, H.; Pummer, B.; Bauer, H.; Bernardi, J.

    2012-04-01

    Primary Biological Aerosol Particles (PBAPs), including bacteria, spores and pollen may be important for several atmospheric processes. Particularly, the ice nucleation caused by PBAPs is a topic of growing interest, since their impact on ice cloud formation and thus on radiative forcing, an important parameter in global climate is not yet fully understood. In laboratory model studies we investigated the ice nucleation activity of selected PBAPs. We studied the immersion mode freezing using water-oil emulsion, which we observed by optical microscopy. We particularly focused on pollen. We show that pollen of different species strongly differ in their ice nucleation behavior. The average freezing temperatures in laboratory experiments range from 240 K to 255 K. As the most efficient nuclei (silver birch, Scots pine and common juniper pollen) have a distribution area up to the Northern timberline, their ice nucleation activity might be a cryoprotective mechanism. For comparison the ice nucleation activity of Snomax, fungal spores, and mushrooms will be discussed as well. In the past, pollen have been rejected as important atmospheric IN, as they are not as abundant in the atmosphere as bacteria or mineral dust and are too heavy to reach higher altitudes. However, in our experiments (Pummer et al. 2011) it turned out that water, which had been in contact with pollen and then been separated from the bodies, nucleates as good as the pollen grains themselves. So the ice nuclei have to be easily-suspendable macromolecules (100-300 kDa) located on the pollen. Once extracted, they can be distributed further through the atmosphere than the heavy pollen grains and so augment the impact of pollen on ice cloud formation even in the upper troposphere. It is widely known, that material from the pollen, like allergens and sugars, can indeed leave the pollen body and be distributed independently. The most probable mechanism is the pollen grain bursting by rain, which releases

  14. Using High-Resolution Airborne Remote Sensing to Study Aerosol Near Clouds

    Science.gov (United States)

    Levy, Robert; Munchak, Leigh; Mattoo, Shana; Marshak, Alexander; Wilcox, Eric; Gao, Lan; Yorks, John; Platnick, Steven

    2016-01-01

    The horizontal space in between clear and cloudy air is very complex. This so-called twilight zone includes activated aerosols that are not quite clouds, thin cloud fragments that are not easily observable, and dying clouds that have not quite disappeared. This is a huge challenge for satellite remote sensing, specifically for retrieval of aerosol properties. Identifying what is cloud versus what is not cloud is critically important for attributing radiative effects and forcings to aerosols. At the same time, the radiative interactions between clouds and the surrounding media (molecules, surface and aerosols themselves) will contaminate retrieval of aerosol properties, even in clear skies. Most studies on aerosol cloud interactions are relevant to moderate resolution imagery (e.g. 500 m) from sensors such as MODIS. Since standard aerosol retrieval algorithms tend to keep a distance (e.g. 1 km) from the nearest detected cloud, it is impossible to evaluate what happens closer to the cloud. During Studies of Emissions, Atmospheric Composition, Clouds and Climate Coupling by Regional Surveys (SEAC4RS), the NASA ER-2 flew with the enhanced MODIS Airborne Simulator (eMAS), providing MODIS-like spectral observations at high (50 m) spatial resolution. We have applied MODIS-like aerosol retrieval for the eMAS data, providing new detail to characterization of aerosol near clouds. Interpretation and evaluation of these eMAS aerosol retrievals is aided by independent MODIS-like cloud retrievals, as well as profiles from the co-flying Cloud Physics Lidar (CPL). Understanding aerosolcloud retrieval at high resolution will lead to better characterization and interpretation of long-term, global products from lower resolution (e.g.MODIS) satellite retrievals.

  15. Aerosol activation and cloud processing in the global aerosol-climate model ECHAM5-HAM

    Directory of Open Access Journals (Sweden)

    G. J. Roelofs

    2006-01-01

    Full Text Available A parameterization for cloud processing is presented that calculates activation of aerosol particles to cloud drops, cloud drop size, and pH-dependent aqueous phase sulfur chemistry. The parameterization is implemented in the global aerosol-climate model ECHAM5-HAM. The cloud processing parameterization uses updraft speed, temperature, and aerosol size and chemical parameters simulated by ECHAM5-HAM to estimate the maximum supersaturation at the cloud base, and subsequently the cloud drop number concentration (CDNC due to activation. In-cloud sulfate production occurs through oxidation of dissolved SO2 by ozone and hydrogen peroxide. The model simulates realistic distributions for annually averaged CDNC although it is underestimated especially in remote marine regions. On average, CDNC is dominated by cloud droplets growing on particles from the accumulation mode, with smaller contributions from the Aitken and coarse modes. The simulations indicate that in-cloud sulfate production is a potentially important source of accumulation mode sized cloud condensation nuclei, due to chemical growth of activated Aitken particles and to enhanced coalescence of processed particles. The strength of this source depends on the distribution of produced sulfate over the activated modes. This distribution is affected by uncertainties in many parameters that play a direct role in particle activation, such as the updraft velocity, the aerosol chemical composition and the organic solubility, and the simulated CDNC is found to be relatively sensitive to these uncertainties.

  16. Aerosol activation and cloud processing in the global aerosol-climate model ECHAM5-HAM

    Directory of Open Access Journals (Sweden)

    G. J. Roelofs

    2006-01-01

    Full Text Available A parameterization for cloud processing is presented that calculates activation of aerosol particles to cloud drops, cloud drop size, and pH-dependent aqueous phase sulfur chemistry. The parameterization is implemented in the global aerosol-climate model ECHAM5-HAM. The cloud processing parameterization uses updraft speed, temperature, and aerosol size and chemical parameters simulated by ECHAM5-HAM to estimate the maximum supersaturation at the cloud base, and subsequently the cloud drop number concentration (CDNC due to activation. In-cloud sulfate production occurs through oxidation of dissolved SO2 by ozone and hydrogen peroxide. The model simulates realistic distributions for annually averaged CDNC although it is underestimated especially in remote marine regions. On average, CDNC is dominated by particles from the accumulation mode, with smaller contributions from the Aitken and coarse modes. The simulations indicate that in-cloud sulfate production is a potentially important source of accumulation mode sized cloud condensation nuclei, due to chemical growth of activated Aitken particles and to enhanced coalescence of processed particles. The strength of this source depends on the distribution of produced sulfate over the activated modes. This distribution is affected by uncertainties in many parameters that play a direct role in particle activation, such as the updraft velocity, the aerosol chemical composition and the organic solubility, and the simulated CDNC is found to be relatively sensitive to these uncertainties.

  17. Surface-active substances in atmospheric aerosol: an electrochemical approach

    Directory of Open Access Journals (Sweden)

    S. Frka

    2012-05-01

    Full Text Available We characterised surface-active substances (SASs in aqueous extract of atmospheric aerosols by using phase sensitive alternating current voltammetry. The electrochemical method has mainly been used for the quantification of surfactants in sea water but has not been applied to atmospheric aerosols yet. The advantage of the method is its simplicity and sensitivity that enables direct analysis of aerosol extracts without the need for sample concentration. Aerosol samples were collected at Middle Adriatic Martinska station influenced by different air masses as well as from urban (Zagreb, Croatia and rural (K-puszta, Hungary areas from late spring to early autumn in 2010. The highest SAS concentrations, expressed in equivalents of T-X-100, ranging from 0.34 to 0.91 µg m−3 were detected in urban samples. The SAS concentrations obtained for marine, regional and continental samples ranged from 0.14 to 0.31, 0.18 to 0.42 and 0.07 to 0.28 µg m−3, respectively. The SAS concentrations in K-puszta aerosols ranged from 0.13 to 0.46 µg m−3. Investigation of humic-like substances isolated from K-puszta samples (2008 confirmed their significant surfactant nature. Different SAS chemistry was noticed for urban and non-urban samples. Investigations at different pH revealed anionic character of SASs in aerosol samples.

  18. Secondary organic aerosols. Chemical aging, hygroscopicity, and cloud droplet activation

    Energy Technology Data Exchange (ETDEWEB)

    Buchholz, Angela

    2011-07-06

    Atmospheric aerosols have an important impact on the radiation balance, and thus, on the climate of the Earth. Aerosol particles scatter and absorb incoming solar and terrestrial radiation. Apart from this direct effect, aerosol particles act as cloud condensation nuclei (CCN), thereby greatly influencing the microphysics of clouds. Secondary organic aerosols (SOA) are an important fraction of the total aerosol mass. In many environments these organic compounds are mainly products of the oxidation of biogenic volatile organic compounds (VOC). In this study the hygroscopic growth and CCN activation of biogenic SOA were investigated which was formed by the oxidation of VOC with O{sub 3} and photochemically formed OH radicals under low NO{sub x} conditions. For this purpose, a complex mixture of VOC emitted by boreal tree species as gas-phase precursors was used in the Juelich Plant Atmosphere Chamber (JPAC). In long-term studies in the atmosphere simulation chamber SAPHIR {alpha}-pinene or a defined mixture of {alpha}-pinene, {beta}-pinene, limonene, ocimene, {delta}-3-carene served as precursors. Initial precursor concentrations between 40 and 1000 ppbC were investigated. The observed SOA particles were slightly hygroscopic with an average hygroscopicity parameter {kappa}(CCN) = 0.10 {+-} 0.02 and {kappa}(90%RH) = 0.05 {+-} 0.01. Closure between hygroscopic growth and CCN activation data could be achieved allowing either surface tension reduction, limited solubility, or non-ideality of the solution in the droplet. The SOA solutions in equilibrium with RH <95% are possible highly non-ideal. Therefore the organic-water interaction were investigated by applying the UNIFAC model. Calculations for surrogate compounds exhibited the same strong concentration (i.e. RH) dependence of {kappa} at sub-saturation. The growth curves could be fitted and CCN activation predicted by assuming a binary mixture of water and one hypothetical organic compound. The occurrence of

  19. Ambient Aerosol in Southeast Asia: High Resolution Aerosol Mass Spectrometer Measurements Over Oil Palm (Elaeis guineensis)

    Science.gov (United States)

    Phillips, G.; Dimarco, C.; Misztal, P.; Nemitz, E.; Farmer, D.; Kimmel, J.; Jimenez, J.

    2008-12-01

    The emission of organic compounds in the troposphere is important factor in the formation of secondary organic aerosol (SOA). A very large proportion of organic material emitted globally is estimated to arise from biogenic sources, with almost half coming from tropical and sub-tropical forests. Preliminary analyses of leave cuvette emission studies suggest that oil palm (Elaeis guineensis) is a significantly larger source of isoprene than tropical forest. Much larger sources of isoprene over oil palm allied with a larger anthropogenic component of local emissions contrast greatly with the remote tropical forest environment and therefore the character of SOA formed may differ significantly. These issues, allied with the high price of palm oil on international markets leading to increased use of land for oil palm production, could give rise to rapidly changing chemical and aerosol regimes in the tropics. It is therefore important to understand the current emissions and composition of organic aerosol over all important land-uses in the tropical environment. This in turn will lead to a greater understanding of the present, and to an improvement in predictive capacity for the future system. To help address these issues, a high resolution time of flight aerosol mass spectrometer (HR-ToF-AMS) was deployed in the Sabahmas (PPB OIL) oil palm plantation near Lahad Datu, in Eastern Sabah, as part of the field component of the Aerosol Coupling in the Earth System (ACES) project, part of the UK NERC APPRAISE program. This project was allied closely with measurements made of similar chemical species and aerosol components at a forest site in the Danum Valley as part of the UK Oxidant and Particle Photochemical Processes above a Southeast Asian tropical rainforest (OP3) project. Measurements of submicron non- refractory aerosol composition are presented along with some preliminary analysis of chemically resolved aerosol fluxes made with a new eddy covariance system, based on the

  20. Cloud condensation nuclei activation of limited solubility organic aerosol

    Science.gov (United States)

    Huff Hartz, Kara E.; Tischuk, Joshua E.; Chan, Man Nin; Chan, Chak K.; Donahue, Neil M.; Pandis, Spyros N.

    The cloud condensation nuclei (CCN) activation of 19 organic species with water solubilities ( Csat) ranging from 10 -4 to 10 2 g solute 100 g -1 H 2O was measured. The organic particles were generated by nebulization of an aqueous or an alcohol solution. Use of alcohols as solvents enables the measurement of low solubility, non-volatile organic CCN activity and reduces the likelihood of residual water in the aerosol. The activation diameter of organic species with very low solubility in water ( Csat<0.3 g 100 g -1 H 2O) is in agreement with Köhler theory using the bulk solubility (limited solubility case) of the organic in water. Many species, including 2-acetylbenzoic acid, aspartic acid, azelaic acid, glutamic acid, homophthalic acid, phthalic acid, cis-pinonic acid, and salicylic acid are highly CCN active in spite of their low solubility (0.3 g 100 g -1 H 2O< Csat<1 g 100 g -1 H 2O), and activate almost as if completely water soluble. The CCN activity of most species is reduced, if the particles are produced using non-aqueous solvents. The existence of the particles in a metastable state at low RH can explain the observed enhancement in CCN activity beyond the levels suggested by their solubility.

  1. Cloud droplet activation through oxidation of organic aerosol influenced by temperature and particle phase state

    Science.gov (United States)

    Slade, Jonathan H.; Shiraiwa, Manabu; Arangio, Andrea; Su, Hang; Pöschl, Ulrich; Wang, Jian; Knopf, Daniel A.

    2017-02-01

    Chemical aging of organic aerosol (OA) through multiphase oxidation reactions can alter their cloud condensation nuclei (CCN) activity and hygroscopicity. However, the oxidation kinetics and OA reactivity depend strongly on the particle phase state, potentially influencing the hydrophobic-to-hydrophilic conversion rate of carbonaceous aerosol. Here, amorphous Suwannee River fulvic acid (SRFA) aerosol particles, a surrogate humic-like substance (HULIS) that contributes substantially to global OA mass, are oxidized by OH radicals at different temperatures and phase states. When oxidized at low temperature in a glassy solid state, the hygroscopicity of SRFA particles increased by almost a factor of two, whereas oxidation of liquid-like SRFA particles at higher temperatures did not affect CCN activity. Low-temperature oxidation appears to promote the formation of highly-oxygenated particle-bound fragmentation products with lower molar mass and greater CCN activity, underscoring the importance of chemical aging in the free troposphere and its influence on the CCN activity of OA.

  2. Size-resolved CCN distributions and activation kinetics of aged continental and marine aerosol

    Directory of Open Access Journals (Sweden)

    A. Bougiatioti

    2011-04-01

    Full Text Available We present size-segregated measurements of cloud condensation nucleus (CCN activity of aged aerosol sampled at Finokalia, Crete, during the Finokalia Aerosol Measurement Experiment of summer 2007 (FAME07. From analysis of the data, hygroscopicity and activation kinetics distributions are derived. The CCN are found to be highly hygroscopic, (expressed by a size- and time-averaged hygroscopicity parameter κ ~ 0.22, with the majority of particles activating at ~0.5–0.6% supersaturation. Air masses originating from Central-Eastern Europe tend to be associated with higher CCN concentrations and slightly lower hygroscopicity (κ ~ 0.18 than for other airmass types. The particles were always well mixed, as reflected by the high activation ratios and narrow hygroscopicity distribution widths. Smaller particles (~30 nm were found to be more hygroscopic (~0.1 κ units higher than the larger ones (~100 nm. The particles with diameters less than 80 nm exhibited a diurnal hygroscopicity cycle (with κ peaking at ~14:00 h local time, consistent with photochemical aging and volatilization of less hygroscopic material from the aerosol. Use of bulk chemical composition and the aerosol number distribution results in excellent CCN closure when applying Köhler theory in its simplest form. Using asymptotic and threshold droplet growth analysis, the "aged" organics present in the aerosol were found not to suppress or delay the water uptake kinetics of particles in this environment.

  3. Cloud condensation nucleus activation properties of biogenic secondary organic aerosol

    Science.gov (United States)

    Vanreken, Timothy M.; Ng, Nga L.; Flagan, Richard C.; Seinfeld, John H.

    2005-04-01

    Organic aerosols in general and secondary organic aerosol (SOA) in particular are known to contribute significantly to the atmospheric population of cloud condensation nuclei (CCN). However, current knowledge is limited with respect to the nature of this contribution. This study presents a series of experiments wherein the potential for biogenically derived SOA to act as CCN is explored. Five compounds were studied: four monoterpenes (α-pinene, β-pinene, limonene, and Δ3-carene) and one terpenoid alcohol (terpinene-4-ol). In each case the aerosol formation was driven by the reaction of ozone with the biogenic precursor. The SOA produced in each experiment was allowed to age for several hours, during which CCN concentrations were periodically measured at four supersaturations: S = 0.27%, 0.32%, 0.54%, and 0.80%. The calculated relationships between particle dry diameter and critical supersaturation were found to fall in the range of previously reported data for single-component organic aerosols; of the systems studied, α-pinene SOA was the least CCN active, while limonene SOA exhibited the strongest CCN activity. Interestingly, the inferred critical supersaturation of the SOA products was considerably more sensitive to particle diameter than was found in previous studies. Furthermore, the relationships between particle size and critical supersaturation for the monoterpene SOA shifted considerably over the course of the experiments, with the aerosol becoming less hygroscopic over time. These results are consistent with the progressive oligomerization of the SOA.

  4. Aerosol production by high-velocity molten-metal droplets

    Energy Technology Data Exchange (ETDEWEB)

    Rader, D J; Benson, D A

    1988-06-01

    This report presents the results of an experimental study of the aerosol produced by high-velocity molten-metal droplets. These tests are intended to simulate the reduction of high-velocity fragments into aerosol in high-explosive detonations or reactor accidents involving nuclear materials. The primary droplets are produced by the heating and electromagnetic launch of metal wires; velocities approaching Mach 1 can be obtained at present. Size distributions obtained tungsten and zirconium droplets burning in air. Lognormal size distributions were observed in both cases with DMPS-equivalent mean diameters of about 0.4 ..mu..m and geometric standard deviations of about two. SEM and TEM analysis of aerosol samples collected by a point-to-plane electrostatic precipitator showed that the majority of these particles were web-like chain agglomerates. Tests performed in argon atmospheres produced several orders-of-magnitude less aerosol mass than in equivalent air tests, supporting the key role combustion plays in secondary aerosol generation. 26 refs., 14 figs., 2 tabs.

  5. Aerosol cloud precipitation interactions. Part 1. The nature and sources of cloud-active aerosols

    Science.gov (United States)

    Andreae, M. O.; Rosenfeld, D.

    2008-07-01

    Atmospheric aerosol particles serve as condensation nuclei for the formation of both, cloud droplets and atmospheric ice particles. As a result, they exert a substantial influence on the microphysical properties of water and ice clouds, which in turn affect the processes that lead to the formation of rain, snow, hail, and other forms of precipitation. In recent years, considerable progress has been made in understanding the chemical composition of aerosols, their microphysical properties, and the factors that enable them to act as cloud condensation nuclei (CCN) and ice nuclei (IN). The first part of this review article will focus on the nature and sources of CCN and IN. We discuss the fundamentals of the cloud droplet and ice nucleation processes, and the role that the chemical composition and particle size play in this process. We show that, in many instances, the influence of chemical composition can be represented by a simple parameterization, which leaves particle size as the main variable controlling CCN efficiency. Aerosol particles are produced either directly by anthropogenic and natural sources (dust, sea salt, soot, biological particles, etc.), or they are formed in the atmosphere by condensation of low-volatility compounds (e.g., sulfuric acid or oxidized organic compounds). We discuss the magnitude of these sources, and the CCN and IN characteristics of the particles they produce. In contrast to previous assessments, which focused on the aerosol mass, we are emphasizing the number of particles being produced, as this is the key variable in cloud microphysics. Large uncertainties still exist for many aerosol sources, e.g., the submicron part of the seaspray aerosol, the particles produced by the biosphere, and the secondary organic aerosol. We conclude with a discussion on what particle concentrations may have been in the pristine atmosphere, before the onset on anthropogenic pollution. Model calculations and observations in remote continental regions

  6. Evaluation of aerosol properties simulated by the high resolution global coupled chemistry-aerosol-microphysics model C-IFS-GLOMAP

    Science.gov (United States)

    Dhomse, Sandip; Mann, Graham; Carslaw, Ken; Flemming, Johannes; Morcrette, Jean-Jacques; Engelen, Richard; Remy, Samuel; Boucher, Olivier; Benduhn, Francois; Hewson, Will; Woodhouse, Matthew

    2016-04-01

    The EU Framework Programme GEMS and MACC consortium projects co-ordinated by the European Centre for Medium-range Weather Forecasts (ECMWF) have developed an operational global forecasting and reanalysis system (Composition-IFS) for atmospheric composition including greenhouse gases, reactive gases and aerosol. The current operational C-IFS system uses a mass-based aerosol model coupled to data assimilation of Aerosol Optical Depth measured by satellite (MODIS) to predict global aerosol properties. During MACC, the GLOMAP-mode aerosol microphysics scheme was added to the system, providing information on aerosol size and number for improved representation of aerosol-radiation and aerosol-cloud interactions, accounting also for simulated global variations in size distribution and internally-mixed particle composition. The IFS-GLOMAP system has recently been upgraded to couple with the sulphur cycle simulated in the online TM5 tropospheric chemistry module for global reactive gases. This C-IFS-GLOMAP system is also being upgraded to use a new "nitrate-extended" version of GLOMAP which realistically treats the size-resolved gas-particle partitioning of semi volatile gases ammonia and nitric acid. In this poster we described C-IFS-GLOMAP and present an evaluation of the global sulphate aerosol distribution simulated in this coupled aerosol-chemistry C-IFS-GLOMAP, comparing to surface observations in Europe, North America and the North Atlantic and contrasting to the fixed timescale sulphate production scheme developed in GEMS. We show that the coupling to the TM5 sulphur chemistry improves the seasonal cycle of sulphate aerosol, for example addressing a persistent wintertime sulphate high bias in northern Europe. The improved skill in simulated sulphate aerosol seasonal cycle is a pre-requisite to realistically characterise nitrate aerosol since biases in sulphate affect the amount of free ammonia available to form ammonium nitrate.

  7. Quantifying the Relationship between Organic Aerosol Composition and Hygroscopicity/CCN Activity

    Energy Technology Data Exchange (ETDEWEB)

    Ziemann, Paul J. [Univ. of California, Riverside, CA (United States); Kreidenweis, Sonia M. [Colorado State Univ., Fort Collins, CO (United States); Petters, Markus D. [North Carolina State Univ., Raleigh, NC (United States)

    2013-06-30

    The overall objective for this project was to provide the data and underlying process level understanding necessary to facilitate the dynamic treatment of organic aerosol CCN activity in future climate models. The specific objectives were as follows: (1) employ novel approaches to link organic aerosol composition and CCN activity, (2) evaluate the effects of temperature and relative humidity on organic aerosol CCN activity, and (3) develop parameterizations to link organic aerosol composition and CCN activity.

  8. Aerosol Characteristics at a High Altitude Location in Central Himalayas: Optical Properties and Radiative Forcing

    CERN Document Server

    Pant, P; Dumka, U C; Sagar, R; Satheesh, S K; Moorthy, K K; Sagar, Ram

    2006-01-01

    Collocated measurements of the mass concentrations of aerosol black carbon (BC) and composite aerosols near the surface were carried out along with spectral aerosol optical depths (AODs) from a high altitude station, Manora Peak in Central Himalayas, during a comprehensive aerosol field campaign in December 2004. Despite being a pristine location in the Shivalik Ranges of Central Himalayas, and having a monthly mean AOD (at 500 nm) of 0.059 $\\pm$ 0.033 (typical to this site), total suspended particulate (TSP) concentration was in the range 15 - 40 micro g m^(-3) (mean value 27.1 $\\pm$ 8.3 micro g m^(-3)). Interestingly, aerosol BC had a mean concentration of 1.36 $\\pm$ 0.99 micro g m^(-3), contributed to ~5.0 $\\pm$ 1.3 % to the composite aerosol mass. This large abundance of BC is found to have linkages to the human activities in the adjoining valley and to the boundary layer dynamics. Consequently, the inferred single scattering albedo lies in the range of 0.87 to 0.94 (mean value 0.90 $\\pm$ 0.03), indicatin...

  9. Lidar observations of high-altitude aerosol layers (cirrus clouds)

    Science.gov (United States)

    Deleva, Atanaska D.; Grigorov, Ivan V.

    2013-03-01

    Aerosols, clouds and aerosol-cloud interactions are recognized as the key factors influencing the climate. Clouds are the primary modulators of the Earth's radiative budget. This paper focuses on the detection of high-altitude aerosol layers in the troposphere over mid-latitude lidar station in Sofia, Bulgaria. They are situated in the height-region 6 km÷16 km, with thickness in the range 0.2 km÷5 km and have varying optical characteristics. On the basis of the general utilized classification of the Cirrus clouds, high values of the calculated atmospheric backscatter coefficient and Angströmexponent estimation results we conclude that the registered strongly scattered aerosol layers are Cirrus clouds. Lidar measurements are performed with an aerosol lidar, equipped with Nd:YAG laser at wavelengths 532 nm and 1064 nm. Mainly, lidar data are presented in terms of vertical atmospheric backscatter coefficient profiles. We also include 2Dcolormap in height-time coordinates build on the basis of so called range corrected signals. It shows in general changes of the aerosol stratification over the lidar station during the measurement period. We employed HYSPLIT backward trajectories and DREAM forecasts to analyze the lidar profile outlines and characterize the events during which Cirrus cloud samples were observed. So was remarked that most of the results were obtained during Saharan dust long-way transport over the city of Sofia. Reported experimental examples are extracted from regular lidar investigations of the atmosphere within the frame of European project EARLINET.

  10. Active and passive smoking - New insights on the molecular composition of different cigarette smoke aerosols by LDI-FTICRMS

    Science.gov (United States)

    Schramm, Sébastien; Carré, Vincent; Scheffler, Jean-Luc; Aubriet, Frédéric

    2014-08-01

    The aerosol generated when a cigarette is smoked is a significant indoor contaminant. Both smokers and non-smokers can be exposed to this class of pollutants. Nevertheless, they are not exposed to the same kind of smoke. The active smoker breathes in the mainstream smoke (MSS) during a puff, whereas the passive smoker inhales not only the smoke generated by the lit cigarette between two puffs (SSS) but also the smoke exhaled by active smokers (EXS). The aerosol fraction of EXS has until now been poorly documented; its composition is expected to be different from MSS. This study aims to investigate the complex composition of aerosol from EXS to better understand the difference in exposure between active and passive smokers. To address this, the in-situ laser desorption ionisation Fourier transform ion cyclotron mass spectrometry (LDI-FTICRMS) was used to characterise the aerosol composition of EXS from two different smokers. Results clearly indicated many similarities between EXS samples but also significant differences with MSS and SSS aerosol. The comparison of MSS and EXS aerosol allowed the chemicals retained by the active smoker's lungs to be identified, whereas the convolution of the EXS and SSS aerosol compositions were considered relevant to the exposition of a passive smoker. As a consequence, active smokers are thought to be mainly exposed to polar and poorly unsaturated oxygenated and nitrogenated organics, compared with poorly oxygenated but highly unsaturated compounds in passive smokers.

  11. Aerosol physicochemical effects on CCN activation simulated with the chemistry-climate model EMAC

    Science.gov (United States)

    Chang, D. Y.; Lelieveld, J.; Tost, H.; Steil, B.; Pozzer, A.; Yoon, J.

    2017-08-01

    This study uses the EMAC atmospheric chemistry-climate model to simulate cloud properties with a prognostic cloud droplet nucleation scheme. We present modeled global distributions of cloud condensation nuclei (CCN) number concentrations and CCN activation rates, together with the effective hygroscopicity parameter κ, to describe the aerosol chemical composition effect on CCN activation. Large particles can easily activate into cloud droplets, even at low κ values due to the dominant size effect in cloud droplet formation. Small particles are less efficiently activated as CCN, and are more sensitive to aerosol composition and supersaturation. Since the dominant fraction of small particles generally originates from anthropogenic precursor emissions over land, this study focuses on the influence of the continental atmosphere, using a prognostic cloud droplet nucleation scheme that considers aerosol-cloud interactions during cloud formation, together with a double-moment cloud microphysics scheme. The agreement of simulated clouds and climate with observations generally improves over the Northern Hemisphere continents, particularly high air pollution regions such as Eastern US, Europe, East Asia by accounting for aerosol-cloud interactions that include impacts of chemical composition on CCN activation.

  12. Modeling the Thermodynamics of Mixed Organic-Inorganic Aerosols to Predict Water Activities and Phase Equilibria

    Science.gov (United States)

    Zuend, A.; Marcolli, C.; Luo, B.; Peter, T.

    2008-12-01

    Tropospheric aerosol particles contain mixtures of inorganic salts, acids, water, and a large variety of organic compounds. Interactions between these substances in liquid mixtures lead to discrepancies from ideal thermodynamic behavior. While the thermodynamics of aqueous inorganic systems at atmospheric temperatures are well established, little is known about the physicochemistry of mixed organic-inorganic particles. Salting-out and salting-in effects result from organic-inorganic interactions and are used to improve industrial separation processes. In the atmosphere, they may influence the aerosol phases. Liquid-liquid phase separations into a mainly polar (aqueous) and a less polar organic phase may considerably influence the gas/particle partitioning of semi-volatile substances compared to a single phase estimation. Moreover, the phases present in the aerosol define the reaction medium for heterogeneous and multiphase chemistry occurring in aerosol particles. A correct description of these phases is needed when gas- or cloud-phase reaction schemes are adapted to aerosols. Non-ideal thermodynamic behavior in mixtures is usually described by an expression for the excess Gibbs energy. We present the group-contribution model AIOMFAC (Aerosol Inorganic-Organic Mixtures Functional groups Activity Coefficients), which explicitly accounts for molecular interactions between solution constituents, both organic and inorganic, to calculate activities, chemical potentials and the total Gibbs energy of mixed systems. This model allows to compute vapor-liquid (VLE), liquid-liquid (LLE) and solid-liquid (SLE) equilibria within one framework. Focusing on atmospheric applications we considered eight different cations, five anions and a wide range of alcohols/polyols as organic compounds. With AIOMFAC, the activities of the components within an aqueous electrolyte solution are very well represented up to high ionic strength. We show that the semiempirical middle

  13. Experiments on aerosol removal by high-pressure water spray

    Energy Technology Data Exchange (ETDEWEB)

    Corno, Ada del, E-mail: delcorno@rse-web.it [RSE, Power Generation Technologies and Materials Dept, via Rubattino 54, I-20134 Milano (Italy); Morandi, Sonia, E-mail: morandi@rse-web.it [RSE, Power Generation Technologies and Materials Dept, via Rubattino 54, I-20134 Milano (Italy); Parozzi, Flavio, E-mail: parozzi@rse-web.it [RSE, Power Generation Technologies and Materials Dept, via Rubattino 54, I-20134 Milano (Italy); Araneo, Lucio, E-mail: lucio.araneo@polimi.it [Politecnico di Milano, Department of Energy, via Lambruschini 4A, I-20156 Milano (Italy); CNR-IENI, via Cozzi 53, I-20125 Milano (Italy); Casella, Francesco, E-mail: francesco2.casella@mail.polimi.it [Politecnico di Milano, Department of Energy, via Lambruschini 4A, I-20156 Milano (Italy)

    2017-01-15

    Highlights: • Experimental research to measure the efficiency of high-pressure sprays in capturing aerosols if applied to a filtered containment venting system in case of severe accident. • Cloud of monodispersed SiO{sub 2} particles with sizes 0.5 or 1.0 μm and initial concentration in the range 2–90 mg/m{sup 3}. • Carried out in a chamber 0.5 × 1.0 m and 1.5 m high, with transparent walls equipped with a high pressure water spray with single nozzle. • Respect to low-pressure sprays, removal efficiency turned out significant: the half-life for 1 μm particles with a removal high-pressure spray system is orders of magnitude shorter than that with a low-pressure sprays system. - Abstract: An experimental research was managed in the framework of the PASSAM European Project to measure the efficiency of high-pressure sprays in capturing aerosols when applied to a filtered containment venting system in case of severe accident. The campaign was carried out in a purposely built facility composed by a scrubbing chamber 0.5 × 1.0 m and 1.5 m high, with transparent walls to permit the complete view of the aerosol removal process, where the aerosol was injected to form a cloud of specific particle concentration. The chamber was equipped with a high pressure water spray system with a single nozzle placed on its top. The test matrix consisted in the combination of water pressure injections, in the range 50–130 bar, on a cloud of monodispersed SiO{sub 2} particles with sizes 0.5 or 1.0 μm and initial concentration ranging between 2 and 99 mg/m{sup 3}. The spray was kept running for 2 min and the efficiency of the removal was evaluated, along the test time, using an optical particle sizer. With respect to low-pressure sprays, the removal efficiency turned out much more significant: the half-life for 1 μm particles with a removal high-pressure spray system is orders of magnitude shorter than that with a low-pressure spray system. The highest removal rate was

  14. The effect of phase partitioning of semivolatile compounds on the measured CCN activity of aerosol particles

    Directory of Open Access Journals (Sweden)

    S. Romakkaniemi

    2013-09-01

    Full Text Available The effect of inorganic semivolatile aerosol compounds on the CCN activity of aerosol particles was studied by using a computational model for a DMT-CCN counter, a cloud parcel model for condensation kinetics and experiments to quantify the modelled results. Concentrations of water vapour and semivolatiles as well as aerosol trajectories in the CCN column were calculated by a computational fluid dynamics model. These trajectories and vapour concentrations were then used as an input for the cloud parcel model to simulate mass transfer kinetics of water and semivolatiles between aerosol particles and the gas phase. Two different questions were studied: (1 how big fraction of semivolatiles is evaporated from particles before activation in the CCN counter? (2 How much the CCN activity can be increased due to condensation of semivolatiles prior to the maximum water supersaturation in the case of high semivolatile concentration in the gas phase? The results show that, to increase the CCN activity of aerosol particles, a very high gas phase concentration (as compared to typical ambient conditions is needed. We used nitric acid as a test compound. A concentration of several ppb or higher is needed for measurable effect. In the case of particle evaporation, we used ammonium nitrate as a test compound and found that it partially evaporates before maximum supersaturation is reached in the CCN counter, thus causing an underestimation of CCN activity. The effect of evaporation is clearly visible in all supersaturations, leading to an underestimation of the critical dry diameter by 10 to 15 nanometres in the case of ammonium nitrate particles in different supersaturations. This result was also confirmed by measurements in supersaturations between 0.1 and 0.7%.

  15. Opposite long-term trends in aerosols between low and high altitudes: a testimony to the aerosol-PBL feedback

    Science.gov (United States)

    Dong, Zipeng; Li, Zhanqing; Yu, Xing; Cribb, Maureen; Li, Xingmin; Dai, Jin

    2017-06-01

    Interactions between absorbing aerosols and the planetary boundary layer (PBL) play an important role in affecting air pollution near the surface. In this study, a unique feature of the aerosol-PBL interaction is identified that has important implications in monitoring and combating air pollution. Opposite trends in aerosol loading between the lower and upper PBL are shown on a wide range of timescales and data acquired by various platforms: from a short-term field experiment to decadal satellite observations and multidecadal ground observations in China. A novel method is proposed to obtain the vertical profiles of aerosol loading from passive sensors by virtue of varying elevations. The analyses of visibility, aerosol optical depth, and extinction with different temporal scales exhibit the similar trend, i.e., increasing in the lower atmosphere but decreasing in the upper atmosphere. Integration of the reversal aerosol trend below and above the PBL resulted in a much less change in the column-integrated quantities. The surface cooling effect, together with the change in the heating rate induced by the absorbing aerosol, unevenly modifies the atmospheric temperature profile, causing a more stable atmosphere inside the PBL but a destabilized atmosphere above the PBL. Such a change in the atmospheric stability favors the accumulation of pollutants near the surface and the vertical diffusion of aerosol particles in the upper atmosphere, both of which are consistent with the observed reversal aerosol trends. These findings have multiple implications in understanding and combating air pollution, especially in many developing countries with high emissions of light-absorbing aerosols.

  16. Single-particle characterization of the High Arctic summertime aerosol

    Directory of Open Access Journals (Sweden)

    B. Sierau

    2014-01-01

    Full Text Available Single-particle mass spectrometric measurements were carried out in the High Arctic north of 80° during summer 2008. The campaign took place onboard the icebreaker \\textit{Oden} and was part of the Arctic Summer Cloud Ocean Study (ASCOS. The instrument deployed was an Aerosol Time-of-Flight Mass Spectrometer (ATOFMS that provides information on the chemical composition of individual particles and their mixing state in real-time. Aerosols were sampled in the marine boundary layer at stations in the open ocean, in the marginal ice zone, and in the pack ice region. The largest fraction of particles detected for subsequent analysis in the size range of the ATOFMS between approximately 200 nm to 3000 nm in diameter showed mass spectrometric patterns indicating an internal mixing state and a biomass burning and/or biofuel source. The majority of these particles were connected to an air mass layer of elevated particle concentration mixed into the surface mixed layer from the upper part of the marine boundary layer. The second largest fraction was represented by sea salt particles. The chemical analysis of the over-ice sea salt aerosol revealed tracer compounds that reflect chemical aging of the particles during their long-range advection from the marginal ice zone, or open waters south thereof prior to detection at the ship. From our findings we conclude that long-range transport of particles is one source of aerosols in the High Arctic. To assess the importance of long-range particle sources for aerosol–cloud interactions over the inner Arctic in comparison to local and regional biogenic primary aerosol sources, the chemical composition of the detected particles was analyzed for indicators of marine biological origin. Only a~minor fraction showed chemical signatures of potentially ocean-derived primary particles of that kind. However, a chemical bias in the ATOFMS's detection capabilities observed during ASCOS might suggest a presence of a

  17. Comparison of Aerosol Classification from Airborne High Spectral Resolution Lidar and the CALIPSO Vertical Feature Mask

    Science.gov (United States)

    Burton, S. P.; Ferrare, R. A.; Omar, A. H.; Hostetler, C. A.; Hair, J. W.; Rogers, R.; Obland, M. D.; Butler, C. F.; Cook, A. L.; Harper, D. B.

    2012-12-01

    The NASA Langley Research Center (LaRC) airborne High Spectral Resolution Lidar (HSRL-1) on the NASA B200 aircraft has acquired large datasets of aerosol extinction (532nm), backscatter (532 and 1064nm), and depolarization (532 and 1064nm) profiles during 349 science flights in 19 field missions across North America since 2006. The extinction-to-backscatter ratio ("lidar ratio"), aerosol depolarization ratios, and backscatter color ratio measurements from HSRL-1 are scale-invariant parameters that depend on aerosol type but not concentration. These four aerosol intensive parameters are combined to qualitatively classify HSRL aerosol measurements into eight separate composition types. The classification methodology uses models formed from "training cases" with known aerosol type. The remaining measurements are then compared with these models using the Mahalanobis distance. Aerosol products from the CALIPSO satellite include aerosol type information as well, which is used as input to the CALIPSO aerosol retrieval. CALIPSO aerosol types are inferred using a mix of aerosol loading-dependent parameters, estimated aerosol depolarization, and location, altitude, and surface type information. The HSRL instrument flies beneath the CALIPSO satellite orbit track, presenting the opportunity for comparisons between the HSRL aerosol typing and the CALIPSO Vertical Feature Mask Aerosol Subtype product, giving insight into the performance of the CALIPSO aerosol type algorithm. We find that the aerosol classification from the two instruments frequently agree for marine aerosols and pure dust, and somewhat less frequently for pollution and smoke. In addition, the comparison suggests that the CALIPSO polluted dust type is overly inclusive, encompassing cases of dust combined with marine aerosol as well as cases without much evidence of dust. Qualitative classification of aerosol type combined with quantitative profile measurements of aerosol backscatter and extinction has many useful

  18. Separating Dust Mixtures and Other External Aerosol Mixtures Using Airborne High Spectral Resolution Lidar Data

    Science.gov (United States)

    Burton, S. P.; Ferrare, R. A.; Vaughan, M.; Hostetler, C. A.; Rogers, R. R.; Hair, J. W.; Cook, A. L.; Harper, D. B.

    2013-12-01

    Knowledge of aerosol type is important for source attribution and for determining the magnitude and assessing the consequences of aerosol radiative forcing. The NASA Langley Research Center airborne High Spectral Resolution Lidar (HSRL-1) has acquired considerable datasets of both aerosol extensive parameters (e.g. aerosol optical depth) and intensive parameters (e.g. aerosol depolarization ratio, lidar ratio) that can be used to infer aerosol type. An aerosol classification methodology has been used extensively to classify HSRL-1 aerosol measurements of different aerosol types including dust, smoke, urban pollution, and marine aerosol. However, atmospheric aerosol is frequently not a single pure type, but instead occurs as a mixture of types, and this mixing affects the optical and radiative properties of the aerosol. Here we present a comprehensive and unified set of rules for characterizing external mixtures using several key aerosol intensive parameters: extinction-to-backscatter ratio (i.e. lidar ratio), backscatter color ratio, and depolarization ratio. Our mixing rules apply not just to the scalar values of aerosol intensive parameters, but to multi-dimensional normal distributions with variance in each measurement dimension. We illustrate the applicability of the mixing rules using examples of HSRL-1 data where mixing occurred between different aerosol types, including advected Saharan dust mixed with the marine boundary layer in the Caribbean Sea and locally generated dust mixed with urban pollution in the Mexico City surroundings. For each of these cases we infer a time-height cross section of mixing ratio along the flight track and we partition aerosol extinction into portions attributed to the two pure types. Since multiple aerosol intensive parameters are measured and included in these calculations, the techniques can also be used for cases without significant depolarization (unlike similar work by earlier researchers), and so a third example of a

  19. Aerosol Composition in the Los Angeles Basin Studied by High Resolution Aerosol Mass Spectrometry

    Science.gov (United States)

    Hayes, P. L.; Ortega, A. M.; Cubison, M.; Hu, W.; Toohey, D. W.; Flynn, J. H.; Grossberg, N.; Lefer, B. L.; Alvarez, S. L.; Rappenglueck, B.; Allan, J. D.; Taylor, J.; Holloway, J. S.; Gilman, J. B.; Kuster, W. C.; De Gouw, J. A.; Massoli, P.; Zhang, X.; Weber, R.; Zhao, Y.; Cliff, S. S.; Wexler, A. S.; Isaacman, G. A.; Worton, D. R.; Kreisberg, N. M.; Hering, S. V.; Goldstein, A. H.; Jimenez, J. L.

    2011-12-01

    Atmospheric aerosols impact climate and health, but their sources and composition are poorly understood. To address this knowledge gap, a high-resolution aerosol mass spectrometer (AMS) and complementary instrumentation were deployed during the 2010 CalNex campaign to characterize aerosol composition in the Los Angeles (LA) area. Total mass concentrations as well as the species concentrations measured by the AMS compare well with most other instruments. Nitrate dominates in the mornings, but its concentration is reduced in the afternoon when organic aerosols (OA) increase and dominate. The diurnal variations in concentrations are strongly influenced by emission transport from the source-rich western basin. The average OA to enhanced CO ratio increases with photochemical age from 25 to 80 μg m-3 ppm-1, which indicates significant secondary OA (SOA) production and that a large majority of OA is secondary in aged air. The ratio values are similar to those from Mexico City as well as New England and the Mid-Atlantic States. Positive matrix factorization (PMF) is used to assess the concentrations of different OA components. The major OA classes are oxygenated OA (OOA, a surrogate for total SOA), and hydrocarbon-like OA (HOA, a surrogate for primary combustion OA). Several subclasses of OA are identified as well including diesel-influenced HOA (DI-HOA) and non-diesel HOA. DI-HOA exhibits low concentrations on Sundays consistent with the well-known weekday/weekend effect in LA. PMF analysis finds that OOA is 67% of the total OA concentration. A strong correlation between OOA and Ox (O3 + NO2) concentrations is observed with a slope of 0.15 that suggests the production of fresh SOA in Pasadena. Plotting the OA elemental ratios in a Van Krevelen diagram (H:C vs. O:C) yields a slope of -0.6, which is less steep than that observed in Riverside during the SOAR-2005 campaign. The difference in slopes may be attributed to the highly oxidized HOA present in Pasadena that is

  20. Characterizing Aerosol Distributions and Optical Properties Using the NASA Langley High Spectral Resolution Lidar

    Energy Technology Data Exchange (ETDEWEB)

    Hostetler, Chris; Ferrare, Richard

    2013-02-14

    The objective of this project was to provide vertically and horizontally resolved data on aerosol optical properties to assess and ultimately improve how models represent these aerosol properties and their impacts on atmospheric radiation. The approach was to deploy the NASA Langley Airborne High Spectral Resolution Lidar (HSRL) and other synergistic remote sensors on DOE Atmospheric Science Research (ASR) sponsored airborne field campaigns and synergistic field campaigns sponsored by other agencies to remotely measure aerosol backscattering, extinction, and optical thickness profiles. Synergistic sensors included a nadir-viewing digital camera for context imagery, and, later in the project, the NASA Goddard Institute for Space Studies (GISS) Research Scanning Polarimeter (RSP). The information from the remote sensing instruments was used to map the horizontal and vertical distribution of aerosol properties and type. The retrieved lidar parameters include profiles of aerosol extinction, backscatter, depolarization, and optical depth. Products produced in subsequent analyses included aerosol mixed layer height, aerosol type, and the partition of aerosol optical depth by type. The lidar products provided vertical context for in situ and remote sensing measurements from other airborne and ground-based platforms employed in the field campaigns and was used to assess the predictions of transport models. Also, the measurements provide a data base for future evaluation of techniques to combine active (lidar) and passive (polarimeter) measurements in advanced retrieval schemes to remotely characterize aerosol microphysical properties. The project was initiated as a 3-year project starting 1 January 2005. It was later awarded continuation funding for another 3 years (i.e., through 31 December 2010) followed by a 1-year no-cost extension (through 31 December 2011). This project supported logistical and flight costs of the NASA sensors on a dedicated aircraft, the subsequent

  1. Highly reactive free radicals in electronic cigarette aerosols.

    Science.gov (United States)

    Goel, Reema; Durand, Erwann; Trushin, Neil; Prokopczyk, Bogdan; Foulds, Jonathan; Elias, Ryan J; Richie, John P

    2015-09-21

    Electronic cigarette (EC) usage has increased exponentially, but limited data are available on its potential harmful effects. We tested for the presence of reactive, short-lived free radicals in EC aerosols by electron paramagnetic resonance spectroscopy (EPR) using the spin-trap phenyl-N-tert-butylnitrone (PBN). Radicals were detected in aerosols from all ECs and eliquids tested (2.5 × 10(13) to 10.3 × 10(13) radicals per puff at 3.3 V) and from eliquid solvents propylene glycol and glycerol and from "dry puffing". These results demonstrate, for the first time, the production of highly oxidizing free radicals from ECs which may present a potential toxicological risk to EC users.

  2. Size-resolved morphological properties of the high Arctic summer aerosol during ASCOS-2008

    OpenAIRE

    Hamacher-Barth, Evelyne; Leck, Caroline; Jansson, Kjell

    2016-01-01

    The representation of aerosol properties and processes in climate models is fraught with large uncertainties. Especially at high northern latitudes a strong underprediction of aerosol concentrations and nucleation events is observed and can only be constrained by in situ observations based on the analysis of individual aerosol particles. To further reduce the uncertainties surrounding aerosol properties and their potential role as cloud condensation nuclei this study provide...

  3. Aerosol classification using airborne High Spectral Resolution Lidar measurements – methodology and examples

    Directory of Open Access Journals (Sweden)

    S. P. Burton

    2012-01-01

    Full Text Available The NASA Langley Research Center (LaRC airborne High Spectral Resolution Lidar (HSRL on the NASA B200 aircraft has acquired extensive datasets of aerosol extinction (532 nm, aerosol optical depth (AOD (532 nm, backscatter (532 and 1064 nm, and depolarization (532 and 1064 nm profiles during 18 field missions that have been conducted over North America since 2006. The lidar measurements of aerosol intensive parameters (lidar ratio, depolarization, backscatter color ratio, and spectral depolarization ratio are shown to vary with location and aerosol type. A methodology based on observations of known aerosol types is used to qualitatively classify the extensive set of HSRL aerosol measurements into eight separate types. Several examples are presented showing how the aerosol intensive parameters vary with aerosol type and how these aerosols are classified according to this new methodology. The HSRL-based classification reveals vertical variability of aerosol types during the NASA ARCTAS field experiment conducted over Alaska and northwest Canada during 2008. In two examples derived from flights conducted during ARCTAS, the HSRL classification of biomass burning smoke is shown to be consistent with aerosol types derived from coincident airborne in situ measurements of particle size and composition. The HSRL retrievals of AOD and inferences of aerosol types are used to apportion AOD to aerosol type; results of this analysis are shown for several experiments.

  4. Ambient Observations of Organic Nitrogen Compounds in Submicrometer Aerosols in New York Using High Resolution Aerosol Mass Spectrometry

    Science.gov (United States)

    Zhou, S.; Ge, X.; Xu, J.; Sun, Y.; Zhang, Q.

    2015-12-01

    Organic nitrogen (ON) compounds, which include amines, nitriles, organic nitrates, amides, and N-containing aromatic heterocycles, are an important class of compounds ubiquitously detected in atmospheric particles and fog and cloud droplets. Previous studies indicate that these compounds can make up a significant fraction (20-80%) of the total nitrogen (N) content in atmospheric condensed phases and play important roles in new particle formation and growth and affecting the optical and hygroscopicity of aerosols. In this study, we report the observation of ON compounds in submicrometer particles (PM1) at two locations in New York based on measurements using Aerodyne high-resolution time-of-flight mass spectrometer (HR-ToF-AMS). One study was conducted as part of the US Department of Energy funded Aerosol Lifecyle - Intensive Operation Period (ALC-IOP) campaign at Brookhaven National Lab (BNL, 40.871˚N, 72.89˚W) in summer, 2011 and the other was conducted at the Queen's College (QC) in New York City (NYC) in summer, 2009. We observed a notable amount of N-containing organic fragment ions, CxHyNp+ and CxHyOzNp+, in the AMS spectra of organic aerosols at both locations and found that they were mainly associated with amino functional groups. Compared with results from lab experiments, the C3H8N+ at m/z = 58 was primarily attributed to trimethylamine. In addition, a significant amount of organonitrates was observed at BNL. Positive matrix factorization (PMF) analysis of the high resolution mass spectra (HRMS) of organic aerosols identified a unique nitrogen-enriched OA (NOA) factor with elevated nitrogen-to-carbon (N/C) at both BNL and QC. Analysis of the size distributions, volatility profiles, and correlations with external tracer indicates that acid-base reactions of amino compounds with sulfate and acidic gas were mainly responsible for the formation of amine salts. Photochemical production was also observed to play a role in the formation of NOA. Bivariate polar

  5. Chemical composition, sources, and processes of urban aerosols during summertime in Northwest China: insights from High Resolution Aerosol Mass Spectrometry

    Science.gov (United States)

    Xu, J.; Zhang, Q.; Chen, M.; Ge, X.; Ren, J.; Qin, D.

    2014-06-01

    An aerodyne High Resolution Time-of-Flight Aerosol Mass Spectrometer (HR-ToF-AMS) was deployed along with a Scanning Mobility Particle Sizer (SMPS) and a Multi Angle Absorption Photometers (MAAP) to measure the temporal variations of the mass loading, chemical composition, and size distribution of sub-micrometer particulate matter (PM1) in Lanzhou, northwest China, during 12 July-7 August 2012. The average PM1 mass concentration including non-refractory PM1 (NR-PM1) measured by HR-ToF-AMS and black carbon (BC) measured by MAAP during this study was 24.5 μg m-3 (ranging from 0.86 to 105μg m-3), with a mean composition consisting of 47% organics, 16% sulfate, 12% BC, 11% ammonium, 10% nitrate, and 4% chloride. The organics was consisted of 70% carbon, 21% oxygen, 8% hydrogen, and 1% nitrogen, with the average oxygen-to-carbon ratio (O / C) of 0.33 and organic mass-to-carbon ratio (OM / OC) of 1.58. Positive matrix factorization (PMF) of the high-resolution mass spectra of organic aerosols (OA) identified four distinct factors which represent, respectively, two primary OA (POA) emission sources (traffic and food cooking) and two secondary OA (SOA) types - a fresher, semi-volatile oxygenated OA (SV-OOA) and a more aged, low-volatility oxygenated OA (LV-OOA). Traffic-related hydrocarbon-like OA (HOA) and BC displayed distinct diurnal patterns both with peak at ~07:00-11:00 (BJT: UTC +8) corresponding to the morning rush hours, while cooking OA (COA) peaked during three meal periods. The diurnal profiles of sulfate and LV-OOA displayed a broad peak between ∼07:00-15:00, while those of nitrate, ammonium, and SV-OOA showed a narrower peak at ~08:00-13:00. The later morning and early afternoon peak in the diurnal profiles of secondary aerosol species was likely caused by mixing down of pollutants aloft, which were likely produced in the residual layer decoupled from the boundary layer during night time. The mass spectrum of SV-OOA also showed similarity with that of

  6. OH-initiated heterogeneous aging of highly oxidized organic aerosol

    Energy Technology Data Exchange (ETDEWEB)

    Kessler, Sean H.; Nah, Theodora; Daumit, Kelly E.; Smith, Jared D.; Leone, Stephen R.; Kolb, Charles E.; Worsnop, Douglas R.; Wilson, Kevin R.; Kroll, Jesse H.

    2011-12-05

    The oxidative evolution (“aging”) of organic species in the atmosphere is thought to have a major influence on the composition and properties of organic particulate matter, but remains poorly understood, particularly for the most oxidized fraction of the aerosol. Here we measure the kinetics and products of the heterogeneous oxidation of highly oxidized organic aerosol, with an aim of better constraining such atmospheric aging processes. Submicron particles composed of model oxidized organics—1,2,3,4-butanetetracarboxylic acid (C{sub 8}H{sub 10}O{sub 8}), citric acid (C{sub 6}H{sub 8}O{sub 7}), tartaric acid (C{sub 4}H{sub 6}O{sub 6}), and Suwannee River fulvic acid—were oxidized by gas-phase OH in a flow reactor, and the masses and elemental composition of the particles were monitored as a function of OH exposure. In contrast to our previous studies of less-oxidized model systems (squalane, erythritol, and levoglucosan), particle mass did not decrease significantly with heterogeneous oxidation. Carbon content of the aerosol always decreased somewhat, but this mass loss was approximately balanced by an increase in oxygen content. The estimated reactive uptake coefficients of the reactions range from 0.37 to 0.51 and indicate that such transformations occur at rates corresponding to 1-2 weeks in the atmosphere, suggesting their importance in the atmospheric lifecycle of organic particulate matter.

  7. A study on aerosol-cloud condensation nuclei (CCN) activation over eastern Himalaya in India

    Science.gov (United States)

    Roy, Arindam; Chatterjee, Abhijit; Sarkar, Chirantan; Das, Sanat Kumar; Ghosh, Sanjay Kumar; Raha, Sibaji

    2017-06-01

    Simultaneous measurements of condensation nuclei (CN) and cloud condensation nuclei (CCN) has been performed over a high altitude site Darjeeling (27°01‧N, 88°15‧E, 2200 m asl) at eastern part of Himalaya in India. The study was carried out during dry seasons (October 2015-May 2016) to investigate the temporal variability of CN and CCN concentrations and the major factors controlling CN-CCN activation. CCN concentrations measured at 0.2, 0.3, 0.4, 0.5, 0.6, 0.7, 0.8 and 0.9% super saturations have been reported in this study. The number concentrations of CN ranged between 694 and 23,643 cm- 3 with an average of 6563 ± 2160 cm- 3 whereas that of CCN (at 0.5% super saturation) ranged between 262 and 13,382 cm- 3 with an average of 1761 ± 856 cm- 3 during the entire study period. CN and CCN showed prominent monthly and seasonal variations controlled by local emissions, meteorological factors and long-range transport. Indo-Gangetic Plain (IGP) was found to be the most contributing region for CN and CCN over Darjeeling mainly during winter and premonsoon. A clear indication of the contribution of aerosols from plain land regions driven by up-slope valley wind was observed during premonsoon from diurnal variability of CN and CCN. Overall, 30-32% aerosols were observed to activate to CCN during winter and premonsoon whereas 24% activation was observed during postmonsoon. Chemical nature and hence solubility of aerosols controlled CCN activation more in night-time than day-time as observed from the correlations between activation ratios and hygroscopicity parameter, k. Strong seasonal dependence of CCN and activation ratio on super saturation and aerosol loading was observed. We observed higher CN and CCN loading and lower activation ratio over Darjeeling compared to western Himalayan high altitude station suggesting higher influence of local and long-range aerosols over eastern Himalaya and significant difference in chemical nature of aerosols between these two

  8. Impacts of new particle formation on aerosol cloud condensation nuclei (CCN activity in Shanghai: case study

    Directory of Open Access Journals (Sweden)

    C. Leng

    2014-07-01

    Full Text Available New particle formation (NPF events and their impacts on cloud condensation nuclei (CCN were investigated using continuous measurements collected in urban Shanghai from 1 to 30 April 2012. During the campaign, NPF occurred in 8 out of the 30 days and enhanced CCN number concentration (NCCN by a actor of 1.2–1.8, depending on supersaturation (SS. The NPF event on 3 April 2012 was chosen as an example to investigate the NPF influence on CCN activity. In this NPF event, secondary aerosols were produced continuously and increased PM2.5 mass concentration at a~rate of 4.33 μg cm−3 h−1, and the growth rate (GR and formation rate (FR were on average 5 nm h−1 and 0.36 cm−3 s−1, respectively. The newly formed particles grew quickly from nucleation mode (10–20 nm into CCN size range. NCCN increased rapidly at SS of 0.4–1.0% but weakly at SS of 0.2%. Correspondingly, aerosol CCN activities (fractions of activated aerosol particles in total aerosols, NCCN / NCN were significantly enhanced from 0.24–0.60 to 0.30–0.91 at SS of 0.2–1.0% due to the NPF. On the basis of the κ-Köhler theory, aerosol size distributions and chemical composition measured simultaneously were used to predict NCCN. There was a good agreement between the predicted and measured NCCN (R2 = 0.96, Npredicted / Nmeasured = 1.04. This study reveals that NPF exerts large impacts on aerosol particle abundance and size spectra, thus significantly promotes NCCN and aerosol CCN activity in this urban environment. The GR of NPF is the key factor controlling the newly formed particles to become CCN at all SS levels, whereas the FR is an effective factor only under high SS (e.g. 1.0% conditions.

  9. Formation of highly porous aerosol particles by atmospheric freeze-drying in ice clouds.

    Science.gov (United States)

    Adler, Gabriela; Koop, Thomas; Haspel, Carynelisa; Taraniuk, Ilya; Moise, Tamar; Koren, Ilan; Heiblum, Reuven H; Rudich, Yinon

    2013-12-17

    The cycling of atmospheric aerosols through clouds can change their chemical and physical properties and thus modify how aerosols affect cloud microphysics and, subsequently, precipitation and climate. Current knowledge about aerosol processing by clouds is rather limited to chemical reactions within water droplets in warm low-altitude clouds. However, in cold high-altitude cirrus clouds and anvils of high convective clouds in the tropics and midlatitudes, humidified aerosols freeze to form ice, which upon exposure to subsaturation conditions with respect to ice can sublimate, leaving behind residual modified aerosols. This freeze-drying process can occur in various types of clouds. Here we simulate an atmospheric freeze-drying cycle of aerosols in laboratory experiments using proxies for atmospheric aerosols. We find that aerosols that contain organic material that undergo such a process can form highly porous aerosol particles with a larger diameter and a lower density than the initial homogeneous aerosol. We attribute this morphology change to phase separation upon freezing followed by a glass transition of the organic material that can preserve a porous structure after ice sublimation. A porous structure may explain the previously observed enhancement in ice nucleation efficiency of glassy organic particles. We find that highly porous aerosol particles scatter solar light less efficiently than nonporous aerosol particles. Using a combination of satellite and radiosonde data, we show that highly porous aerosol formation can readily occur in highly convective clouds, which are widespread in the tropics and midlatitudes. These observations may have implications for subsequent cloud formation cycles and aerosol albedo near cloud edges.

  10. Observations of fluorescent aerosol-cloud interactions in the free troposphere at the Sphinx high Alpine research station, Jungfraujoch

    Science.gov (United States)

    Crawford, I.; Lloyd, G.; Bower, K. N.; Connolly, P. J.; Flynn, M. J.; Kaye, P. H.; Choularton, T. W.; Gallagher, M. W.

    2015-09-01

    The fluorescent nature of aerosol at a high Alpine site was studied using a wide-band integrated bioaerosol (WIBS-4) single particle multi-channel ultra violet-light induced fluorescence (UV-LIF) spectrometer. This was supported by comprehensive cloud microphysics and meteorological measurements with the aims of cataloguing concentrations of bio-fluorescent aerosols at this high altitude site and also investigating possible influences of UV-fluorescent particle types on cloud-aerosol processes. Analysis of background free tropospheric air masses, using a total aerosol inlet, showed there to be a minor but statistically insignificant increase in the fluorescent aerosol fraction during in-cloud cases compared to out of cloud cases. The size dependence of the fluorescent aerosol fraction showed the larger aerosol to be more likely to be fluorescent with 80 % of 10 μm particles being fluorescent. Whilst the fluorescent particles were in the minority (NFl/NAll = 0.27±0.19), a new hierarchical agglomerative cluster analysis approach, Crawford et al. (2015) revealed the majority of the fluorescent aerosol were likely to be representative of fluorescent mineral dust. A minor episodic contribution from a cluster likely to be representative of primary biological aerosol particles (PBAP) was also observed with a wintertime baseline concentration of 0.1±0.4 L-1. Given the low concentration of this cluster and the typically low ice active fraction of studied PBAP (e.g. pseudomonas syringae) we suggest that the contribution to the observed ice crystal concentration at this location is not significant during the wintertime.

  11. Impact of mixing state and hygroscopicity on CCN activity of biomass burning aerosol in Amazonia

    Science.gov (United States)

    Sánchez Gácita, Madeleine; Longo, Karla M.; Freire, Julliana L. M.; Freitas, Saulo R.; Martin, Scot T.

    2017-02-01

    Smoke aerosols prevail throughout Amazonia because of widespread biomass burning during the dry season, and external mixing, low variability in the particle size distribution and low particle hygroscopicity are typical. There can be profound effects on cloud properties. This study uses an adiabatic cloud model to simulate the activation of smoke particles as cloud condensation nuclei (CCN) for three hypothetical case studies, chosen as to resemble biomass burning aerosol observations in Amazonia. The relative importance of variability in hygroscopicity, mixing state, and activation kinetics for the activated fraction and maximum supersaturation is assessed. For a population with κp = 0.04, an overestimation of the cloud droplet number concentration Nd for the three selected case studies between 22.4 ± 1.4 and 54.3 ± 3.7 % was obtained when assuming a hygroscopicity parameter κp = 0.20. Assuming internal mixing of the aerosol population led to overestimations of up to 20 % of Nd when a group of particles with medium hygroscopicity was present in the externally mixed population cases. However, the overestimations were below 10 % for external mixtures between very low and low-hygroscopicity particles, as seems to be the case for Amazon smoke particles. Kinetic limitations were significant for medium- and high-hygroscopicity particles, and much lower for very low and low-hygroscopicity particles. When particles were assumed to be at equilibrium and to respond instantly to changes in the air parcel supersaturation, the overestimation of the droplet concentration was up to ˜ 100 % in internally mixed populations, and up to ˜ 250 % in externally mixed ones, being larger for the higher values of hygroscopicity. In addition, a perceptible delay between the times when maximum supersaturation and maximum aerosol activated fraction are reached was noticed and, for aerosol populations with effective hygroscopicity κpeff higher than a certain threshold value, the delay in

  12. Leaks in nuclear grade high efficiency aerosol filters

    Energy Technology Data Exchange (ETDEWEB)

    Scripsick, Ronald Clyde [Univ. of California, Davis, CA (United States)

    1994-07-01

    Nuclear grade high efficiency aerosol filters, also known as high efficiency particulate air (HEPA) filters, are commonly used in air cleaning systems for removal of hazardous aerosols. Performance of the filter units is important in assuring health and environmental protection. The filter units are constructed from pleated packs of fiberglass filter media sealed into rigid frames. Results of previous studies on such filter units indicate that their performance may not be completely predicted by ideal performance of the fibrous filter media. In this study, departure from ideal performance is linked to leaks existing in filter units and overall filter unit performance is derived from independent performance of the individual filter unit components. The performance of 14 nuclear grade HEPA filter units (size 1, 25 cfm) with plywood frames was evaluated with a test system that permitted independent determination of penetration as a function of particle size for the whole filter unit, the filter unit frame, and the filter media pack. Tests were performed using a polydisperse aerosol of di-2-ethylhexyl phthalate with a count median diameter of 0.2 {mu}m and geometric standard deviation of 1.6. Flow rate and differential pressure were controlled from 1% to 100% of design values. Particle counts were made upstream and downstream of the filter unit with an optical particle counter (OPC). The OPC provided count information in 28 size channels over the particle diameter range from 0.1 to 0.7 μm. Results provide evidence for a two component leak model of filler unit performance with: (1) external leaks through filter unit frames, and (2) internal leaks through defects in the media and through the seal between the media pack and frame. For the filter units evaluated, these leaks dominate overall filter unit performance over much of the flow rate and particle size ranges tested.

  13. Atmospheric aerosol brown carbon in the high Himalayas

    Science.gov (United States)

    Kirillova, Elena; Decesari, Stefano; Marinoni, Angela; Bonasoni, Paolo; Vuillermoz, Elisa; Facchini, M. Cristina; Fuzzi, Sandro

    2016-04-01

    Anthropogenic light-absorbing atmospheric aerosol can reach very high concentrations in the planetary boundary layer in South-East Asia ("brown clouds"), affecting atmospheric transparency and generating spatial gradients of temperature over land with a possible impact on atmospheric dynamics and monsoon circulation. Besides black carbon (BC), an important light-absorbing component of anthropogenic aerosols is the organic carbon component known as 'brown carbon' (BrC). In this research, we provided first measurements of atmospheric aerosol BrC in the high Himalayas during different seasons. Aerosol sampling was conducted at the GAW-WMO Global station "Nepal Climate Observatory-Pyramid" (NCO-P) located in the high Khumbu valley at 5079 m a.s.l. in the foothills of Mt. Everest. PM10 aerosol samples were collected from July 2013 to November 2014. The sampling strategy was set up in order to discriminate the daytime valley breeze bringing polluted air masses up to the observatory and free tropospheric air during nighttime. Water-soluble BrC (WS-BrC) and methanol-soluble BrC (MeS-BrC) were extracted and analyzed using a UV/VIS spectrophotometer equipped with a 50 cm liquid waveguide capillary cell. In the polluted air masses, the highest levels of the BrC light absorption coefficient at 365 nm (babs365) were observed during the pre-monsoon season (1.83±1.46 Mm-1 for WS-BrC and 2.86±2.49 Mm-1 for MeS-BrC) and the lowest during the monsoon season (0.21±0.22 Mm-1 for WS-BrC and 0.32±0.29 Mm-1 for MeS-BrC). The pre-monsoon season is the most frequently influenced by a strong atmospheric brown cloud (ABC) transport to NCO-P due to increased convection and mixing layer height over South Asia combined with the highest up-valley wind speed and the increase of the emissions from open fires due to the agricultural practice along the Himalayas foothills and the Indo-Gangetic Plain. In contrast, the monsoon season is characterized by a weakened valley wind regime and an

  14. The electrical charging of inactive aerosols in high ionised atmosphere, the electrical charging of artificial beta radioactive aerosols; Le processus de charge electrique: des aerosols non radioactifs en milieu fortement ionise, des aerosols radioactifs artificiels emetteurs beta

    Energy Technology Data Exchange (ETDEWEB)

    Gensdarmes, F

    2000-07-01

    The electrical properties of aerosols greatly influence their transport and deposition in a containment. In a bipolar ionic atmosphere, a neutral electric charge on aerosols is commonly assumed. However, many studies report a different charge distribution in some situations, like highly ionised atmosphere or in the case of radioactive aerosols. Such situations could arise from a hypothetical accident in a nuclear power plant. Within the framework of safety studies which are carried out at IPSN, our aims were the study of electrical properties of aerosols in highly ionised atmosphere, and the study of artificial radioactive aerosols, in order to suggest experimental validation of available theories. For this purpose, we designed an experimental device that allows us to measure non-radioactive aerosol charge distribution under high gamma irradiation, up to 10{sup 4} Gy/h. With our experimental device we also studied the properties of small ions in the medium. Our results show a variation of the charge distribution in highly ionised atmosphere. The charge increases with the dose of gamma ray. We have related this variation with the one of the small ions in the gases, according to theoretical prediction. However, the model overestimates slightly our experimental results. In the case of the radioactive aerosols, we have designed an original experimental device, which allows us to study the charge distribution of a {sup 137}Cs aerosol. Our results show that the electric charging of such aerosols is strongly dependent on evolution parameters in a containment. So, our results underline a great enhancement of self-charging of particles which are sampled in a confined medium. Our results are qualitatively in agreement with the theoretical model; nevertheless the latter underestimates appreciably the self-charging, owing to the fact that wall effects are not taken into account. (author)

  15. Aerosol typing - key information from aerosol studies

    Science.gov (United States)

    Mona, Lucia; Kahn, Ralph; Papagiannopoulos, Nikolaos; Holzer-Popp, Thomas; Pappalardo, Gelsomina

    2016-04-01

    Aerosol typing is a key source of aerosol information from ground-based and satellite-borne instruments. Depending on the specific measurement technique, aerosol typing can be used as input for retrievals or represents an output for other applications. Typically aerosol retrievals require some a priori or external aerosol type information. The accuracy of the derived aerosol products strongly depends on the reliability of these assumptions. Different sensors can make use of different aerosol type inputs. A critical review and harmonization of these procedures could significantly reduce related uncertainties. On the other hand, satellite measurements in recent years are providing valuable information about the global distribution of aerosol types, showing for example the main source regions and typical transport paths. Climatological studies of aerosol load at global and regional scales often rely on inferred aerosol type. There is still a high degree of inhomogeneity among satellite aerosol typing schemes, which makes the use different sensor datasets in a consistent way difficult. Knowledge of the 4d aerosol type distribution at these scales is essential for understanding the impact of different aerosol sources on climate, precipitation and air quality. All this information is needed for planning upcoming aerosol emissions policies. The exchange of expertise and the communication among satellite and ground-based measurement communities is fundamental for improving long-term dataset consistency, and for reducing aerosol type distribution uncertainties. Aerosol typing has been recognized as one of its high-priority activities of the AEROSAT (International Satellite Aerosol Science Network, http://aero-sat.org/) initiative. In the AEROSAT framework, a first critical review of aerosol typing procedures has been carried out. The review underlines the high heterogeneity in many aspects: approach, nomenclature, assumed number of components and parameters used for the

  16. A high-resolution study of surfactant partitioning and kinetic limitations for two-component internally mixed aerosols

    Science.gov (United States)

    Suda, S. R.; Petters, M. D.

    2013-12-01

    Atmospheric aerosols serve as cloud condensation nuclei (CCN), altering cloud properties and ultimately affecting climate through their effect on the radiative balance. Aerosol CCN activity depends in part on aerosol composition and surfactant compounds are of particular interest because surfactants are enriched at the water/air interface, resulting in a radial concentration gradient within the aqueous droplet. Accurate treatment of the surfactant concentration gradient complicates the otherwise straightforward predictions of CCN activity for aerosols of known composition. To accurately evaluate predictions made by theory, laboratory studies investigating the relationship between critical supersaturation and dry diameter of particles that include surfactants require significant reduction in measurement uncertainty for both water-uptake and CCN measurements. Furthermore, uncertainties remain regarding kinetic limitations to surfactant partitioning that could result in deviation from predictions based on equilibrium thermodynamics. This study attempts to address some of these issues through high-resolution analysis of CCN activity of two-component mixed surfactant/non-surfactant aerosols at different internal mixing ratios performed with and without a water-uptake time delay to ascertain whether or not the observed effects are kinetically limited. We present new data for the aerosols consisting of 1) the ionic surfactant sodium dodecyl sulfate (SDS) with ammonium sulfate, 2) SDS with sodium chloride and 3) the strong non-ionic fluorosurfactant Zonyl with an organic proxy glucose. As a point of reference we also evaluated the mixture of ammonium sulfate with glucose. Aerosol activation diameters were determined using CCN analysis in conjunction with scanning mobility size classification and high sheath-to-aerosol flow ratios. This resulted in CCN-derived kappa values that could be determined within +/-5% relative error. To test whether dynamic surfactant partitioning

  17. Airborne High Spectral Resolution Lidar Aerosol Measurements during MILAGRO and TEXAQS/GOMACCS

    Science.gov (United States)

    Ferrare, Richard; Hostetler, Chris; Hair, John; Cook Anthony; Harper, David; Burton, Sharon; Clayton, Marian; Clarke, Antony; Russell, Phil; Redemann, Jens

    2007-01-01

    Two1 field experiments conducted during 2006 provided opportunities to investigate the variability of aerosol properties near cities and the impacts of these aerosols on air quality and radiative transfer. The Megacity Initiative: Local and Global Research Observations (MILAGRO) /Megacity Aerosol Experiment in Mexico City (MAX-MEX)/Intercontinental Chemical Transport Experiment-B (INTEX-B) joint experiment conducted during March 2006 investigated the evolution and transport of pollution from Mexico City. The Texas Air Quality Study (TEXAQS)/Gulf of Mexico Atmospheric Composition and Climate Study (GoMACCS) (http://www.al.noaa.gov/2006/) conducted during August and September 2006 investigated climate and air quality in the Houston/Gulf of Mexico region. During both missions, the new NASA Langley airborne High Spectral Resolution Lidar (HSRL) was deployed on the NASA Langley B200 King Air aircraft and measured profiles of aerosol extinction, backscattering, and depolarization to: 1) characterize the spatial and vertical distributions of aerosols, 2) quantify aerosol extinction and optical thickness contributed by various aerosol types, 3) investigate aerosol variability near clouds, 4) evaluate model simulations of aerosol transport, and 5) assess aerosol optical properties derived from a combination of surface, airborne, and satellite measurements.

  18. Separating mixtures of aerosol types in airborne High Spectral Resolution Lidar data

    Science.gov (United States)

    Burton, S. P.; Vaughan, M. A.; Ferrare, R. A.; Hostetler, C. A.

    2014-02-01

    Knowledge of aerosol type is important for determining the magnitude and assessing the consequences of aerosol radiative forcing, and can provide useful information for source attribution studies. However, atmospheric aerosol is frequently not a single pure type, but instead occurs as a mixture of types, and this mixing affects the optical and radiative properties of the aerosol. This paper extends the work of earlier researchers by using the aerosol intensive parameters measured by the NASA Langley Research Center airborne High Spectral Resolution Lidar (HSRL-1) to develop a comprehensive and unified set of rules for characterizing the external mixing of several key aerosol intensive parameters: extinction-to-backscatter ratio (i.e., lidar ratio), backscatter color ratio, and depolarization ratio. We present the mixing rules in a particularly simple form that leads easily to mixing rules for the covariance matrices that describe aerosol distributions, rather than just single values of measured parameters. These rules can be applied to infer mixing ratios from the lidar-observed aerosol parameters, even for cases without significant depolarization. We demonstrate our technique with measurement curtains from three HSRL-1 flights which exhibit mixing between two aerosol types, urban pollution plus dust, marine plus dust, and smoke plus marine. For these cases, we infer a time-height cross-section of extinction mixing ratio along the flight track, and partition aerosol extinction into portions attributed to the two pure types.

  19. Separating mixtures of aerosol types in airborne High Spectral Resolution Lidar data

    Directory of Open Access Journals (Sweden)

    S. P. Burton

    2013-09-01

    Full Text Available Knowledge of aerosol type is important for source attribution and for determining the magnitude and assessing the consequences of aerosol radiative forcing. However, atmospheric aerosol is frequently not a single pure type, but instead occurs as a mixture of types, and this mixing affects the optical and radiative properties of the aerosol. This paper extends the work of earlier researchers by using the aerosol intensive parameters measured by the NASA Langley Research Center airborne High Spectral Resolution Lidar (HSRL-1 to develop a comprehensive and unified set of rules for characterizing the external mixing of several key aerosol intensive parameters: extinction-to-backscatter ratio (i.e. lidar ratio, backscatter color ratio, and depolarization ratio. We present the mixing rules in a particularly simple form that leads easily to mixing rules for the covariance matrices that describe aerosol distributions, rather than just scalar values of measured parameters. These rules can be applied to infer mixing ratios from the lidar-observed aerosol parameters, even for cases without significant depolarization. We demonstrate our technique with measurement curtains from three HSRL-1 flights which exhibit mixing between two aerosol types, urban pollution plus dust, marine plus dust, and smoke plus marine. For these cases, we infer a time-height cross-section of mixing ratio along the flight track, and partition aerosol extinction into portions attributed to the two pure types.

  20. Sources of optically active aerosol particles over the Amazon forest

    Science.gov (United States)

    Guyon, Pascal; Graham, Bim; Roberts, Gregory C.; Mayol-Bracero, Olga L.; Maenhaut, Willy; Artaxo, Paulo; Andreae, Meinrat O.

    Size-fractionated ambient aerosol samples were collected at a pasture site and a primary rainforest site in the Brazilian Amazon Basin during two field campaigns (April-May and September-October 1999), as part of the European contribution to the Large-Scale Biosphere-Atmosphere Experiment in Amazonia (LBA-EUSTACH). The samples were analyzed for up to 19 trace elements by particle-induced X-ray emission analysis (PIXE), for equivalent black carbon (BC e) by a light reflectance technique and for mass concentration by gravimetric analysis. Additionally, we made continuous measurements of absorption and light scattering by aerosol particles. The vertical chemical composition gradients at the forest site have been discussed in a companion article (Journal of Geophysical Research-Atmospheres 108 (D18), 4591 (doi:4510.1029/2003JD003465)). In this article, we present the results of a source identification and quantitative apportionment study of the wet and dry season aerosols, including an apportionment of the measured scattering and absorption properties of the total aerosol in terms of the identified aerosol sources. Source apportionments (obtained from absolute principal component analysis) revealed that the wet and dry season aerosols contained the same three main components, but in different (absolute and relative) amounts: the wet season aerosol consisted mainly of a natural biogenic component, whereas pyrogenic aerosols dominated the dry season aerosol mass. The third component identified was soil dust, which was often internally mixed with the biomass-burning aerosol. All three components contributed significantly to light extinction during both seasons. At the pasture site, up to 47% of the light absorption was attributed to biogenic particles during the wet season, and up to 35% at the tower site during the wet-to-dry transition period. The results from the present study suggest that, in addition to pyrogenic particles, biogenic and soil dust aerosols must be

  1. Interfacing the NRL 1-D High Vertical Resolution Aerosol Model with COAMPS

    Science.gov (United States)

    2016-06-13

    mechanistic model that predicts the evolution of the aerosol size and composition distribution. From such a model, aerosol extinction of EM radiation can be...calculated in a highly structured atmospheric marine boundary layer (AMBL) and used to evaluate and predict the performance of systems that operate...sea-salt AOD ranging from 0.01 - 0.10 (0.05 - 0.10 under moderate winds). IMPACT/APPLICATIONS Aerosols scatter and absorb EM radiation and are

  2. Cloud Condensation Nuclei Activity of Aerosols during GoAmazon 2014/15 Field Campaign Report

    Energy Technology Data Exchange (ETDEWEB)

    Wang, J. [Brookhaven National Lab. (BNL), Upton, NY (United States); Martin, S. T. [Harvard Univ., Cambridge, MA (United States); Kleinman, L. [Brookhaven National Lab. (BNL), Upton, NY (United States); Thalman, R. M. [Brookhaven National Lab. (BNL), Upton, NY (United States)

    2016-03-01

    Aerosol indirect effects, which represent the impact of aerosols on climate through influencing the properties of clouds, remain one of the main uncertainties in climate predictions (Stocker et al. 2013). Reducing this large uncertainty requires both improved understanding and representation of aerosol properties and processes in climate models, including the cloud activation properties of aerosols. The Atmospheric System Research (ASR) science program plan of January 2010 states that: “A key requirement for simulating aerosol-cloud interactions is the ability to calculate cloud condensation nuclei and ice nuclei (CCN and IN, respectively) concentrations as a function of supersaturation from the chemical and microphysical properties of the aerosol.” The Observations and Modeling of the Green Ocean Amazon (GoAmazon 2014/15) study seeks to understand how aerosol and cloud life cycles are influenced by pollutant outflow from a tropical megacity (Manaus)—in particular, the differences in cloud-aerosol-precipitation interactions between polluted and pristine conditions. One key question of GoAmazon2014/5 is: “What is the influence of the Manaus pollution plume on the cloud condensation nuclei (CCN) activities of the aerosol particles and the secondary organic material in the particles?” To address this question, we measured size-resolved CCN spectra, a critical measurement for GoAmazon2014/5.

  3. Aerosol chemistry over a high altitude station at northeastern Himalayas, India.

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    Abhijit Chatterjee

    Full Text Available BACKGROUND: There is an urgent need for an improved understanding of the sources, distributions and properties of atmospheric aerosol in order to control the atmospheric pollution over northeastern Himalayas where rising anthropogenic interferences from rapid urbanization and development is becoming an increasing concern. METHODOLOGY/PRINCIPAL FINDINGS: An extensive aerosol sampling program was conducted in Darjeeling (altitude approximately 2200 meter above sea level (masl, latitude 27 degrees 01'N and longitude 88 degrees 15'E, a high altitude station in northeastern Himalayas, during January-December 2005. Samples were collected using a respirable dust sampler and a fine dust sampler simultaneously. Ion chromatograph was used to analyze the water soluble ionic species of aerosol. The average concentrations of fine and coarse mode aerosol were found to be 29.5+/-20.8 microg m(-3 and 19.6+/-11.1 microg m(-3 respectively. Fine mode aerosol dominated during dry seasons and coarse mode aerosol dominated during monsoon. Nitrate existed as NH(4NO(3 in fine mode aerosol during winter and as NaNO(3 in coarse mode aerosol during monsoon. Gas phase photochemical oxidation of SO(2 during premonsoon and aqueous phase oxidation during winter and postmonsoon were the major pathways for the formation of SO(4(2- in the atmosphere. Long range transport of dust aerosol from arid regions of western India was observed during premonsoon. The acidity of fine mode aerosol was higher in dry seasons compared to monsoon whereas the coarse mode acidity was higher in monsoon compared to dry seasons. Biomass burning, vehicular emissions and dust particles were the major types of aerosol from local and continental regions whereas sea salt particles were the major types of aerosol from marine source regions. CONCLUSIONS/SIGNIFICANCE: The year-long data presented in this paper provide substantial improvements to the heretofore poor knowledge regarding aerosol chemistry over

  4. Chemical composition, sources, and processes of urban aerosols during summertime in Northwest China: insights from High Resolution Aerosol Mass Spectrometry

    Directory of Open Access Journals (Sweden)

    J. Xu

    2014-06-01

    Full Text Available An aerodyne High Resolution Time-of-Flight Aerosol Mass Spectrometer (HR-ToF-AMS was deployed along with a Scanning Mobility Particle Sizer (SMPS and a Multi Angle Absorption Photometers (MAAP to measure the temporal variations of the mass loading, chemical composition, and size distribution of sub-micrometer particulate matter (PM1 in Lanzhou, northwest China, during 12 July–7 August 2012. The average PM1 mass concentration including non-refractory PM1 (NR-PM1 measured by HR-ToF-AMS and black carbon (BC measured by MAAP during this study was 24.5 μg m−3 (ranging from 0.86 to 105μg m−3, with a mean composition consisting of 47% organics, 16% sulfate, 12% BC, 11% ammonium, 10% nitrate, and 4% chloride. The organics was consisted of 70% carbon, 21% oxygen, 8% hydrogen, and 1% nitrogen, with the average oxygen-to-carbon ratio (O / C of 0.33 and organic mass-to-carbon ratio (OM / OC of 1.58. Positive matrix factorization (PMF of the high-resolution mass spectra of organic aerosols (OA identified four distinct factors which represent, respectively, two primary OA (POA emission sources (traffic and food cooking and two secondary OA (SOA types – a fresher, semi-volatile oxygenated OA (SV-OOA and a more aged, low-volatility oxygenated OA (LV-OOA. Traffic-related hydrocarbon-like OA (HOA and BC displayed distinct diurnal patterns both with peak at ~07:00–11:00 (BJT: UTC +8 corresponding to the morning rush hours, while cooking OA (COA peaked during three meal periods. The diurnal profiles of sulfate and LV-OOA displayed a broad peak between ∼07:00–15:00, while those of nitrate, ammonium, and SV-OOA showed a narrower peak at ~08:00–13:00. The later morning and early afternoon peak in the diurnal profiles of secondary aerosol species was likely caused by mixing down of pollutants aloft, which were likely produced in the residual layer decoupled from the boundary layer during night time. The mass spectrum of SV-OOA also showed similarity

  5. DEVELOPMENT OF AN RH -DENUDED MIE ACTIVE SAMPLING SYSTEM AND TARGETED AEROSOL CALIBRATION

    Science.gov (United States)

    The MIE pDR 1200 nephelometer provides time resolved aerosol concentrations during personal and fixed-site sampling. Active (pumped) operation allows defining an upper PM2.5 particle size, however, this dramatically increases the aerosol mass passing through the phot...

  6. DEVELOPMENT OF AN RH -DENUDED MIE ACTIVE SAMPLING SYSTEM AND TARGETED AEROSOL CALIBRATION

    Science.gov (United States)

    The MIE pDR 1200 nephelometer provides time resolved aerosol concentrations during personal and fixed-site sampling. Active (pumped) operation allows defining an upper PM2.5 particle size, however, this dramatically increases the aerosol mass passing through the phot...

  7. Aerosol hygroscopicity and CCN activation kinetics in a boreal forest environment during the 2007 EUCAARI campaign

    Directory of Open Access Journals (Sweden)

    K. M. Cerully

    2011-12-01

    Full Text Available Measurements of size-resolved cloud condensation nuclei (CCN concentrations, subsaturated hygroscopic growth, size distribution, and chemical composition were collected from March through May, 2007, in the remote Boreal forests of Hyytiälä, Finland, as part of the European Integrated project on Aerosol Cloud Climate and Air Quality Interactions (EUCAARI campaign. Hygroscopicity parameter, κ, distributions were derived independently from Continuous Flow-Streamwise Thermal Gradient CCN Chamber (CFSTGC and Hygroscopicity Tandem Differential Mobility Analyzer (HTDMA measurements. CFSTGC-derived κ values for 40, 60, and 80 nm particles range mostly between 0.10 and 0.40 with an average characteristic of highly oxidized organics of 0.20 ± 0.10, indicating that organics play a dominant role for this environment. HTDMA-derived κ were generally 30% lower. Diurnal trends of κ show a minimum at sunrise and a maximum in the late afternoon; this trend covaries with inorganic mass fraction and the m/z 44 organic mass fraction given by a quadrupole aerosol mass spectrometer, further illustrating the importance of organics in aerosol hygroscopicity. The chemical dispersion inferred from the observed κ distributions indicates that while 60 and 80 nm dispersion increases around midday, 40 nm dispersion remains constant. Additionally, 80 nm particles show a markedly higher level of chemical dispersion than both 40 and 60 nm particles. An analysis of droplet activation kinetics for the sizes considered indicates that most of the CCN activate as rapidly as (NH42SO4 calibration aerosol.

  8. Cloud condensation nuclei activity of aliphatic amine secondary aerosol

    Science.gov (United States)

    Aliphatic amines can form secondary aerosol via oxidation with atmospheric radicals (e.g. hydroxyl radical and nitrate radical). The resulting particle composition can contain both secondary organic aerosol (SOA) and inorganic salts. The fraction of organic to inorganic materials in the particulate ...

  9. On the Water Uptake and CCN Activation of Tropospheric Organic Aerosols

    Science.gov (United States)

    Rastak, Narges; Pajunoja, Aki; Acosta Navarro, Juan-Camilo; Leong, Yu Jun; Cerully, Kate M.; Nenes, Athanasios; Kirkevåg, Alf; Topping, David; Virtanen, Annele; Riipinen, Ilona

    2016-04-01

    Aerosol particles introduce high uncertainties to radiative climate forcing. If exposed to a given relative humidity (RH), aerosol particles containing soluble material can absorb water and grow in size (hygroscopic growth). If RH is increased further beyond supersaturation (RH >100%) the particles can act as cloud condensation nuclei (CCN). Aerosol particles interactions with water vapour determine to a large extent their influence on climate. Organic aerosols (OA) contribute a large fraction (20-90%) of atmospheric submicron particulate mass, on the other hand they often consist of thousands of compounds with different properties. One of these properties is solubility, which affects the hygroscopic growth and cloud condensation nucleus (CCN) activation of the organic particles. We investigate the hygroscopic behaviour of complex organic aerosols accounting for the distribution of solubilities present in these mixtures. We use the SPARC method to estimate the solubility distributions of isoprene (IP) and monoterpene (MT) SOA based on their chemical composition, as predicted by the Master Chemical Mechanism (MCM). Combining these solubility distributions with the adsorption theory along with the non-ideal behaviour of organic mixtures, we predict the expected hygroscopic growth factors (HGFs), CCN activation behaviour and the related hygroscopicity parameters kappa for these mixtures. The predictions are compared to laboratory measurements as well as field data from MT- and IP-dominated measurement sites. The predicted solubility distributions do a good job in explaining the water uptake of these two mixture types at high relative humidities (RH around 90%), as well as their CCN activation - including the potential differences between the kappa values derived from HGF vs. CCN data. At lower relative humidities, however, the observed water uptake is higher than predicted on solubility alone, particularly for the MT-derived SOA. The data from the low RHs are further

  10. Activation of "synthetic ambient" aerosols - Relation to chemical composition of particles <100 nm

    Science.gov (United States)

    Burkart, J.; Hitzenberger, R.; Reischl, G.; Bauer, H.; Leder, K.; Puxbaum, H.

    2012-07-01

    Cloud condensation nuclei (CCN) are an important fraction of atmospheric aerosols because of their role in cloud formation. Experimental studies focus either on direct field measurements of complex ambient aerosols or laboratory investigations on well defined aerosols produced from single substances or substance mixtures. In this study, we focussed on the ultrafine aerosol because in terms of number concentration, the majority of the CCN are expected to have sizes in this range. A field study was performed from July 2007 to October 2008 to investigate the activation behaviour of the atmospheric aerosol in Vienna (Burkart et al., 2011). Filter samples of the aerosol aerosol in a nebulizer. Chemical analyses of the ultrafine water soluble material were also performed. The CCN properties of the "synthetic ambient" aerosol were obtained using the University of Vienna CCN counter (Giebl et al., 2002; Dusek et al., 2006b) at a nominal supersaturation (SS) of 0.5%. Activation diameters dact ranged from 54.5 nm to 66 nm, were larger than dact of typical single inorganic salts and showed no seasonal pattern in contrast to the fraction of water soluble organic carbon (WSOC), which ranged from 44% in spring to 15% in winter. The average hygroscopicity parameter κ (Petters and Kreidenweis, 2007) obtained from the activation curves ranged from 0.20 to 0.30 (average 0.24), which was significantly lower than κchem calculated from the chemical composition (0.43 ± 0.07).

  11. Tropospheric Aerosols

    Science.gov (United States)

    Buseck, P. R.; Schwartz, S. E.

    2003-12-01

    It is widely believed that "On a clear day you can see forever," as proclaimed in the 1965 Broadway musical of the same name. While an admittedly beautiful thought, we all know that this concept is only figurative. Aside from Earth's curvature and Rayleigh scattering by air molecules, aerosols - colloidal suspensions of solid or liquid particles in a gas - limit our vision. Even on the clearest day, there are billions of aerosol particles per cubic meter of air.Atmospheric aerosols are commonly referred to as smoke, dust, haze, and smog, terms that are loosely reflective of their origin and composition. Aerosol particles have arisen naturally for eons from sea spray, volcanic emissions, wind entrainment of mineral dust, wildfires, and gas-to-particle conversion of hydrocarbons from plants and dimethylsulfide from the oceans. However, over the industrial period, the natural background aerosol has been greatly augmented by anthropogenic contributions, i.e., those produced by human activities. One manifestation of this impact is reduced visibility (Figure 1). Thus, perhaps more than in other realms of geochemistry, when considering the composition of the troposphere one must consider the effects of these activities. The atmosphere has become a reservoir for vast quantities of anthropogenic emissions that exert important perturbations on it and on the planetary ecosystem in general. Consequently, much recent research focuses on the effects of human activities on the atmosphere and, through them, on the environment and Earth's climate. For these reasons consideration of the geochemistry of the atmosphere, and of atmospheric aerosols in particular, must include the effects of human activities. (201K)Figure 1. Impairment of visibility by aerosols. Photographs at Yosemite National Park, California, USA. (a) Low aerosol concentration (particulate matter of aerodynamic diameter less than 2.5 μm, PM2.5=0.3 μg m-3; particulate matter of aerodynamic diameter less than 10

  12. Heterogeneous chlorine activation on stratospheric aerosols and clouds in the Arctic polar vortex

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    T. Wegner

    2012-11-01

    Full Text Available Chlorine activation in the Arctic is investigated by examining different parameterizations for uptake coefficients on stratospheric aerosols, high-resolution in-situ measurements and vortex-wide satellite observations. The parameterizations for heterogeneous chemistry on liquid aerosols are most sensitive to temperature with the reaction rates doubling for every 1 K increase in temperature. However, differences between the currently available parameterizations are negligible. For Nitric Acid Trihydrate particles (NAT the major factors of uncertainty are the number density of nucleated particles and different parameterizations for heterogeneous chemistry. These two factors induce an uncertainty that covers several orders of magnitude on the reaction rate. Nonetheless, since predicted reaction rates on liquid aerosols always exceed those on NAT, the overall uncertainty for chlorine activation is small. In-situ observations of ClOx from Arctic winters in 2005 and 2010 are used to evaluate the heterogeneous chemistry parameterizations. The conditions for these measurements proved to be very different between those two winters with HCl being the limiting reacting partner for the 2005 measurements and ClONO2 for the 2010 measurements. Modeled levels of chlorine activation are in very good agreement with the in-situ observations and the surface area provided by Polar Stratospheric Clouds (PSCs has only a limited impact on modeled chlorine activation. This indicates that the parameterizations give a good representation of the processes in the atmosphere. Back-trajectories started on the location of the observations in 2005 indicate temperatures on the threshold for PSC formation, hence the surface area is mainly provided by the background aerosol. Still, the model shows additional chlorine activation during this time-frame, providing cautionary evidence for chlorine activation even in the absence of PSCs. Vortex-averaged satellite

  13. Characterisation of high dose dry powder aerosols by cascade impaction and laser diffraction analysis

    NARCIS (Netherlands)

    Grasmeijer, F.; Hagedoorn, P.; Frijlink, H.W.; De Boer, A.H.

    2011-01-01

    Background: Developments in high dose dry powder inhalationcontinue to challenge the viability of pharmacopoeialmethods for drug aerosol characterisation. Especiallythe occurrence of bounce effects can cause the amount offines (<1 lm) to be highly overestimated in particle sizedistributions (PSDs) o

  14. CCN Activation Properties of Multiple-Component, Smog Chamber Generated, and Ambient Aerosols

    Science.gov (United States)

    Raymond, T. M.; Pandis, S. N.

    2002-12-01

    Ambient aerosols are a complex mixture of inorganic and hundreds of organic compounds varying in structure and physical properties. Despite the considerable fraction of organic matter in atmospheric aerosol, relatively little is known about the ability of complex, mixed particles to act as cloud condensation nuclei (CCN). Previous work has focused on pure-component and dual-component aerosols and theoretical modeling of their activation. This work expands the investigation by studying the CCN-forming ability of multiple-component organic-inorganic mixed aerosol compounds produced in a smog chamber, and ambient aerosols. The CCN properties of aerosols produced in an indoor five cubic meter Teflon smog chamber and ambient aerosol are investigated experimentally combining a Tandem Differential Mobility Analyzer (TDMA) with a static diffusion CCN counter (M1 Model, DH Associates). Data was obtained for ozone oxidation products of alpha-pinene, beta-pinene, limonene, gasoline, and diesel fuel. Multiple-component aerosols were produced from atomizing a mixed solution of chemical components and studying the particles with the TDMA-CCNC system. Mixtures included ammonium sulfate, sodium chloride, pinonic acid, pinic acid, norpinic acid, glutamic acid, and leucine. Studies were performed at supersaturations of 0.3% and 1.0% with dry particle diameters ranging from 0.02 to 0.2 micrometers. The results were analyzed to gain insights into CCN properties of atmospheric aerosols composed of known mixtures of inorganic and organic species, mixed oxidation products of primary organic species, and actual ambient aerosols. The results are compared to the behavior of pure organic aerosols and theory.

  15. Compressed gas domestic aerosol valve design using high viscous product

    Directory of Open Access Journals (Sweden)

    A Nourian

    2016-10-01

    Full Text Available Most of the current universal consumer aerosol products using high viscous product such as cooking oil, antiperspirants, hair removal cream are primarily used LPG (Liquefied Petroleum Gas propellant which is unfriendly environmental. The advantages of the new innovative technology described in this paper are: i. No butane or other liquefied hydrocarbon gas is used as a propellant and it replaced with Compressed air, nitrogen or other safe gas propellant. ii. Customer acceptable spray quality and consistency during can lifetime iii. Conventional cans and filling technology There is only a feasible energy source which is inert gas (i.e. compressed air to replace VOCs (Volatile Organic Compounds and greenhouse gases, which must be avoided, to improve atomisation by generating gas bubbles and turbulence inside the atomiser insert and the actuator. This research concentrates on using "bubbly flow" in the valve stem, with injection of compressed gas into the passing flow, thus also generating turbulence. The new valve designed in this investigation using inert gases has advantageous over conventional valve with butane propellant using high viscous product (> 400 Cp because, when the valving arrangement is fully open, there are negligible energy losses as fluid passes through the valve from the interior of the container to the actuator insert. The use of valving arrangement thus permits all pressure drops to be controlled, resulting in improved control of atomising efficiency and flow rate, whereas in conventional valves a significant pressure drops occurs through the valve which has a complex effect on the corresponding spray.

  16. Linking Aerosol Source Activities to Present and Future Climate Effects

    Science.gov (United States)

    Koch, D.; Bond, T. C.; Streets, D.; Menon, S.; Unger, N.

    2007-05-01

    Aerosol source sectors (transport, power, industry, residential, biomass burning) generate distinct mixtures of aerosol species. These mixtures in turn have different effects on climate. As sectoral emissions change in coming decades, whether by regulation or not, it is helpful to link pollution from source types to climate consequences. We do so, using our global (GISS GCM) aerosol model for present and future IPCC SRES scenarios. According to our model, residential and transport sectors have net positive 1995 aerosol forcings (0.04 and 0.03 W m-2) due to their large black carbon contents. However, the sulfate-dominated power and industry sectors have net negative 1995 forcings (-0.10 and -0.09 W m-2). Due to the near-balance of absorbing and scattering components, biomass burning forcing is small. For the 2050 SRES A1B scenario, the net (negative) aerosol forcing is double 1995 due primarily to increased sulfur emissions in the industry and power sectors. For 2050 B1 the net (negative) forcing decreases relative to 1995, as sulfur emissions are reduced. Both future scenarios project decreasing residential emissions. Yet transport emissions are expected to remain significant and thus become the dominant source of warming aerosols in the future. Aerosol pollution is projected to shift southward relative to the present, as the current industrialized regions generally reduce emissions and tropical and southern hemispheric regions continue to develop. Similar to these SRES scenarios, IIASA scenarios project a decline in residential emissions; however IIASA is more optimistic about transport sector emissions reductions. We will conduct present-day climate experiments, including aerosol direct and indirect effects, to study impacts of power and transport sectors on climate features such as air temperature and hydrologic cycle.

  17. Aerosol profile information from high resolution oxygen A-Band measurements from space

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    A. Geddes

    2014-06-01

    Full Text Available Aerosols are an important factor of the Earth climatic system and they play a key role for air quality and public health. Observations of the oxygen A-Band at 760 nm can provide information on the vertical distribution of aerosols from passive satellite sensors, that can be of great interest for operational monitoring applications with high coverage if the aerosol information is obtained with sufficient precision, accuracy and vertical resolution. To address this issue, retrieval simulations of the aerosol vertical profile retrieval from O2 A Band observations by GOSAT, the upcoming OCO-2 and Sentinel 5-P mission and the proposed CarbonSat mission have been carried out. Precise retrievals of AOD within the boundary layer were found to favour low resolution, high SNR instruments such as Sentinel-5 P, whereas higher resolution instruments such as OCO-2 showed greater performance at higher altitudes and in information content above the boundary layer. Accurate retrievals of the AOD in the 0–2 km range appears difficult from all studied instruments and the retrieval errors typically exceed a value of 0.05. Constraining the surface albedo is a promising and effective way of improving the retrieval of aerosol, but the required level of a priori knowledge is very high. Due to the limited information content of the aerosol profile retrieval, the use of a parameterised aerosol distribution has been assessed and we show that the AOD and height of an aerosol layer can be retrieved well if the aerosol layer is uplifted to the free troposphere but errors are often large for aerosol layers in the boundary layer. Additional errors will be introduced by incorrect assumptions on surface pressure and aerosol type which can both bias retrieved AOD and height by up to 40%. We conclude the aerosol profile retrievals from O2 A Band using existing or upcoming satellite sensors will only provide limited information on aerosols in the boundary layer but such

  18. Vaporization front in the interaction of a high-energy laser with aerosols - A solitary wave

    Science.gov (United States)

    Lee, C. T.; Miller, T. G.

    1982-06-01

    If a high-energy laser beam were to propagate through highly absorbent aerosols, the aerosols might be subject to extinction by evaporation. This could occur, for instance, if a high-energy CO2 laser beam were to propagate through a medium containing a mist of water droplets. The incident energy would evaporate the droplets, thus increasing the transmission with time. In this paper, solitary waves are obtained as the asymptotic solution to the coupled nonlinear equations describing such an interaction.

  19. Fast Airborne Aerosol Size and Chemistry Measurements with the High Resolution Aerosol Mass Spectrometer during the MILAGRO Campaign

    Science.gov (United States)

    DeCarlo, P. F.; Dunlea, E. J.; Kimmel, J. R.; Aiken, A. C.; Sueper, D.; Crounse, J.; Wennberg, P. O.; Emmons, L.; Shinozuka, Y.; Clarke, A.; Zhou, J.; Tomlinson, J.; Collins,D. R.; Knapp, D.; Weinheimer, A. J.; Montzka,D. D.; Campos,T.; Jimenez, J. L.

    2007-01-01

    The concentration, size, and composition of non-refractory submicron aerosol (NR-PM(sub l)) was measured over Mexico City and central Mexico with a High-Resolution Time-of-Flight Aerosol Mass Spectrometer (HR-ToF-AMS) onboard the NSF/NCAR C-130 aircraft as part of the MILAGRO field campaign. This was the first aircraft deployment of the HR-ToF-AMS. During the campaign the instrument performed very well, and provided 12 s data. The aerosol mass from the AMS correlates strongly with other aerosol measurements on board the aircraft. Organic aerosol (OA) species dominate the NR-PM(sub l) mass. OA correlates strongly with CO and HCN indicating that pollution (mostly secondary OA, SOA) and biomass burning (BB) are the main OA sources. The OA to CO ratio indicates a typical value for aged air of around 80 microg/cubic m (STP) ppm(exp -1). This is within the range observed in outflow from the Northeastern US, which could be due to a compensating effect between higher BB but lower biogenic VOC emissions during this study. The O/C atomic ratio for OA is calculated from the HR mass spectra and shows a clear increase with photochemical age, as SOA forms rapidly and quickly overwhelms primary urban OA, consistent with Volkamer et al. (2006) and Kleinman et al. (2008). The stability of the OA/CO while O/C increases with photochemical age implies a net loss of carbon from the OA. BB OA is marked by signals at m/z 60 and 73, and also by a signal enhancement at large m/z indicative of larger molecules or more resistance to fragmentation. The main inorganic components show different spatial patterns and size distributions. Sulfate is regional in nature with clear volcanic and petrochemical/power plant sources, while the urban area is not a major regional source for this species. Nitrate is enhanced significantly in the urban area and immediate outflow, and is strongly correlated with CO indicating a strong urban source. The importance of nitrate decreases with distance from the city

  20. Fast airborne aerosol size and chemistry measurements with the high resolution aerosol mass spectrometer during the MILAGRO Campaign

    Science.gov (United States)

    Decarlo, P. F.; Dunlea, E. J.; Kimmel, J. R.; Aiken, A. C.; Sueper, D.; Crounse, J.; Wennberg, P. O.; Emmons, L.; Shinozuka, Y.; Clarke, A.; Zhou, J.; Tomlinson, J.; Collins, D. R.; Knapp, D.; Weinheimer, A. J.; Montzka, D. D.; Campos, T.; Jimenez, J. L.

    2007-12-01

    The concentration, size, and composition of non-refractory submicron aerosol (NR-PM1) was measured over Mexico City and central Mexico with a High-Resolution Time-of-Flight Aerosol Mass Spectrometer (HR-ToF-AMS) onboard the NSF/NCAR C-130 aircraft as part of the MILAGRO field campaign. This was the first aircraft deployment of the HR-ToF-AMS, in which the instrument performed very well, and provided 12 s data. The aerosol mass from the AMS correlates strongly with other aerosol measurements on board the aircraft. Organic aerosol (OA) species dominate the NR-PM1 mass. OA correlates strongly with CO and HCN indicating that pollution (mostly secondary OA, SOA) and biomass burning (BB) are the main OA sources. The OA to CO ratio indicates a typical value for aged air of around 80 μg m-3 (STP) ppm-1. This is within the range observed in outflow from the Northeastern US, which could be due to a compensating effect between higher BB but lower biogenic VOC emissions during this study. The O/C atomic ratio for OA is calculated from the HR mass spectra and shows a clear increase with photochemical age, as SOA forms rapidly and quickly overwhelms primary urban OA, consistent with Volkamer et al. (2006) and Kleinman et al. (2007b). BB OA is marked by signals at m/z 60 and 73, and also by a signal enhancement at large m/z indicative of larger molecules or more resistance to fragmentation. The main inorganic components show different spatial patterns and size distributions. Sulfate is regional in nature with clear volcanic and petrochemical/power plant sources, while the urban area is not a major source for this species. Nitrate is enhanced significantly in the urban area and immediate outflow, and is strongly correlated with CO indicating a strong urban source. The importance of nitrate decreases with distance from the city likely due to evaporation. BB does not appear to be a strong source of nitrate despite its high emissions of nitrogen oxides, presumably due to low ammonia

  1. Fast airborne aerosol size and chemistry measurements with the high resolution aerosol mass spectrometer during the MILAGRO Campaign

    Directory of Open Access Journals (Sweden)

    P. F. DeCarlo

    2007-12-01

    Full Text Available The concentration, size, and composition of non-refractory submicron aerosol (NR-PM1 was measured over Mexico City and central Mexico with a High-Resolution Time-of-Flight Aerosol Mass Spectrometer (HR-ToF-AMS onboard the NSF/NCAR C-130 aircraft as part of the MILAGRO field campaign. This was the first aircraft deployment of the HR-ToF-AMS, in which the instrument performed very well, and provided 12 s data. The aerosol mass from the AMS correlates strongly with other aerosol measurements on board the aircraft. Organic aerosol (OA species dominate the NR-PM1 mass. OA correlates strongly with CO and HCN indicating that pollution (mostly secondary OA, SOA and biomass burning (BB are the main OA sources. The OA to CO ratio indicates a typical value for aged air of around 80 μg m−3 (STP ppm−1. This is within the range observed in outflow from the Northeastern US, which could be due to a compensating effect between higher BB but lower biogenic VOC emissions during this study. The O/C atomic ratio for OA is calculated from the HR mass spectra and shows a clear increase with photochemical age, as SOA forms rapidly and quickly overwhelms primary urban OA, consistent with Volkamer et al. (2006 and Kleinman et al. (2007b. BB OA is marked by signals at m/z 60 and 73, and also by a signal enhancement at large m/z indicative of larger molecules or more resistance to fragmentation. The main inorganic components show different spatial patterns and size distributions. Sulfate is regional in nature with clear volcanic and petrochemical/power plant sources, while the urban area is not a major source for this species. Nitrate is enhanced significantly in the urban area and immediate outflow, and is strongly correlated with CO indicating a strong urban source. The importance of nitrate decreases with distance from the city likely due to evaporation. BB does not appear to be a strong source of nitrate

  2. Establishing the Impact of Model Surfactants on Cloud Condensation Nuclei Activation of Sea Spray Aerosols

    Science.gov (United States)

    Forestieri, S.; Cappa, C. D.; Ruehl, C. R.

    2016-12-01

    Aerosol impacts on cloud properties, also known as indirect effects, remain a major source of uncertainty in modeling global radiative forcing. To reduce this uncertainty necessitates better understanding of how aerosol chemical composition impacts the cloud-forming ability of aerosols. It is well established that both size and hygroscopicity impact the cloud condensation nuclei (CCN) activity of aerosols. Previous studies demonstrate that the presence of surface-active organic material in aerosols can also reduce the surface tension of activating droplets, thereby enhancing CCN activity. We quantified surface tension of microscopic droplets using a continuous-flow stream-wise thermal gradient chamber at humidities close to activation for multi-component lab-generated sea spray aerosol (SSA) proxies. The SSA proxies used were atomized NaCl or synthetic sea salt coated with one to many various fatty acids found in nascent SSA particles. Observed surface tension values near the point of activation as a function of chemical composition for various SSA proxies will be presented.

  3. Sources and atmospheric processing of winter aerosols in Seoul, Korea: insights from real-time measurements using a high-resolution aerosol mass spectrometer

    Science.gov (United States)

    Kim, Hwajin; Zhang, Qi; Bae, Gwi-Nam; Kim, Jin Young; Bok Lee, Seung

    2017-02-01

    Highly time-resolved chemical characterization of nonrefractory submicrometer particulate matter (NR-PM1) was conducted in Seoul, the capital and largest metropolis of Korea, using an Aerodyne high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS). The measurements were performed during winter, when elevated particulate matter (PM) pollution events are often observed. This is the first time that detailed real-time aerosol measurement results have been reported from Seoul, Korea, and they reveal valuable insights into the sources and atmospheric processes that contribute to PM pollution in this region. The average concentration of submicron aerosol (PM1 = NR-PM1+ black carbon (BC)) was 27.5 µg m-3, and the total mass was dominated by organics (44 %), followed by nitrate (24 %) and sulfate (10 %). The average atomic ratios of oxygen to carbon (O / C), hydrogen to carbon (H / C), and nitrogen to carbon (N / C) of organic aerosols (OA) were 0.37, 1.79, and 0.018, respectively, which result in an average organic mass-to-carbon (OM / OC) ratio of 1.67. The concentrations (2.6-90.7 µg m-3) and composition of PM1 varied dynamically during the measurement period due to the influences of different meteorological conditions, emission sources, and air mass origins. Five distinct sources of OA were identified via positive matrix factorization (PMF) analysis of the HR-ToF-AMS data: vehicle emissions represented by a hydrocarbon-like OA factor (HOA, O / C = 0.06), cooking activities represented by a cooking OA factor (COA, O / C = 0.14), wood combustion represented by a biomass burning OA factor (BBOA, O / C = 0.34), and secondary organic aerosol (SOA) represented by a semivolatile oxygenated OA factor (SV-OOA, O / C = 0.56) and a low-volatility oxygenated OA factor (LV-OOA, O / C = 0.68). On average, primary OA (POA = HOA + COA + BBOA) accounted for 59 % the OA mass, whereas SV-OOA and LV-OOA contributed 15 and 26 %, respectively. Our results indicate that air

  4. Hygroscopic growth and activation of HULIS particles: experimental data and a new iterative parameterization scheme for complex aerosol particles

    Directory of Open Access Journals (Sweden)

    A. Massling

    2008-03-01

    Full Text Available The hygroscopic growth and activation of two HULIS (HUmic LIke Substance and one Aerosol-Water-Extract sample, prepared from urban-type aerosol, were investigated. All samples were extracted from filters, redissolved in water and atomized for the investigations presented here. The hygroscopic growth measurements were done using LACIS (Leipzig Aerosol Cloud Interaction Simulator together with a HH-TDMA (High Humidity Tandem Differential Mobility Analyzer. Hygroscopic growth was determined for relative humidities (RHs up to 99.75%. The critical diameters for activation were measured for supersaturations between 0.2 and 1%. All three samples showed a similar hygroscopic growth behavior, and the two HULIS samples also were similar in their activation behavior, while the Aerosol-Water-Extract turned out to be more CCN active than the HULIS samples. The experimental data was used to derive parameterizations for the hygroscopic growth and activation of HULIS particles. The concept of ρion (Wex et al., 2007a and the Szyszkowski-equation (Szyszkowski, 1908; Facchini, 1999 were used for parameterizing the Raoult and the Kelvin (surface tension terms of the Köhler equation, respectively. This concept proved to be very successful for the HULIS samples in the saturation range from RHs larger than 98% up to activation. It was also shown to work well with data on HULIS taken from literature. Here, different atmospheric life-times and/or different sources for the different samples showed up in different coefficients for the parameterization. However, the parameterization did not work out well for the Aerosol-Water-Extract.

  5. Factor analysis of combined organic and inorganic aerosol mass spectra from high resolution aerosol mass spectrometer measurements

    Directory of Open Access Journals (Sweden)

    Y. L. Sun

    2012-05-01

    Full Text Available The high resolution mass spectra of organic and inorganic aerosols from aerosol mass spectrometer (AMS measurements were first combined into positive matrix factorization (PMF analysis to investigate the sources and evolution processes of atmospheric aerosols. The new approach is able to study the mixing of organic aerosols (OA and inorganic species, the acidity of OA factors, and the fragment ion patterns related to photochemical processing. In this study, PMF analysis of the unified AMS spectral matrices resolved 8 factors for the submicron aerosols measured at Queens College in New York City in summer 2009. The hydrocarbon-like OA (HOA and cooking OA (COA contain very minor inorganic species, indicating the different sources and mixing characteristics between primary OA and secondary species. The two factors that are primarily ammonium sulfate (SO4-OA and ammonium nitrate (NO3-OA, respectively, are overall neutralized, of which the OA in SO4-OA shows the highest oxidation state (O/C = 0.69 among OA factors. The semi-volatile oxygenated OA comprises two components, i.e., a less oxidized (LO-OOA and a more oxidized (MO-OOA. The MO-OOA represents a local photochemical product with the diurnal profile exhibiting a pronounced noon peak, consistent with those of formaldehyde (HCHO and Ox (= O3+NO2. The much higher NO+/NO2+ fragment ion ratio in MO-OOA than that from ammonium nitrate alone provides evidence for the formation of organic nitrates. The amine-related nitrogen-enriched OA (NOA contains ~25% of acidic inorganic salts, elucidating the formation of secondary OA from amines in acidic environments. The size distributions derived from 3-dimensional size-resolved mass spectra show distinct diurnal evolving behaviors for different OA factors, but overall a progressing evolution from smaller to larger particle mode as a function of oxidation states

  6. Quantification of marine aerosol subgrid variability and its correlation with clouds based on high-resolution regional modeling: Quantifying Aerosol Subgrid Variability

    Energy Technology Data Exchange (ETDEWEB)

    Lin, Guangxing; Qian, Yun; Yan, Huiping; Zhao, Chun; Ghan, Steven J.; Easter, Richard C.; Zhang, Kai

    2017-06-16

    One limitation of most global climate models (GCMs) is that with the horizontal resolutions they typically employ, they cannot resolve the subgrid variability (SGV) of clouds and aerosols, adding extra uncertainties to the aerosol radiative forcing estimation. To inform the development of an aerosol subgrid variability parameterization, here we analyze the aerosol SGV over the southern Pacific Ocean simulated by the high-resolution Weather Research and Forecasting model coupled to Chemistry. We find that within a typical GCM grid, the aerosol mass subgrid standard deviation is 15% of the grid-box mean mass near the surface on a 1 month mean basis. The fraction can increase to 50% in the free troposphere. The relationships between the sea-salt mass concentration, meteorological variables, and sea-salt emission rate are investigated in both the clear and cloudy portion. Under clear-sky conditions, marine aerosol subgrid standard deviation is highly correlated with the standard deviations of vertical velocity, cloud water mixing ratio, and sea-salt emission rates near the surface. It is also strongly connected to the grid box mean aerosol in the free troposphere (between 2 km and 4 km). In the cloudy area, interstitial sea-salt aerosol mass concentrations are smaller, but higher correlation is found between the subgrid standard deviations of aerosol mass and vertical velocity. Additionally, we find that decreasing the model grid resolution can reduce the marine aerosol SGV but strengthen the correlations between the aerosol SGV and the total water mixing ratio (sum of water vapor, cloud liquid, and cloud ice mixing ratios).

  7. Aerosol nucleation induced by a high energy particle beam

    DEFF Research Database (Denmark)

    Enghoff, Martin Andreas Bødker; Pedersen, Jens Olaf Pepke; Uggerhøj, Ulrik I.

    atmospheric conditions using a 580 MeV electron beam to ionize the volume of the reaction chamber. We find a clear and significant contribution from ion induced nucleation and consider this to be an unambiguous observation of the ion-effect on aerosol nucleation using a particle beam under conditions not far......The effect of ions in aerosol nucleation is a subject where much remains to be discovered. That ions can enhance nucleation has been shown by theory, observations, and experiments. However, the exact mechanism still remains to be determined. One question is if the nature of the ionization affects...... the nucleation. This is an essential question since many experiments have been performed using radioactive sources that ionize differently than the cosmic rays which are responsible for the majority of atmospheric ionization. Here we report on an experimental study of sulphuric acid aerosol nucleation under near...

  8. Development of a high-spectral-resolution lidar for continuous observation of aerosols in South America

    Science.gov (United States)

    Jin, Yoshitaka; Sugimoto, Nobuo; Nishizawa, Tomoaki; Ristori, Pablo; Papandrea, Sebastian; Otero, Lidia; Quel, Eduardo; Mizuno, Akira

    2016-05-01

    Continuous monitoring of aerosol profiles using lidar is helpful for a quasi-real-time indication of aerosol concentration. For instance, volcanic ash concentration and its height distribution are essential information for plane flights. Depolarization ratio and multi-wavelength measurements are useful for characterizing aerosol types such as volcanic ash, smoke, dust, sea-salt, and air pollution aerosols. High spectral resolution lidar (HSRL) and Raman scattering lidar can contribute to such aerosol characterization significantly since extinction coefficients can be measured independently from backscattering coefficients. In particular, HSRL can measure aerosol extinction during daytime and nighttime with a high sensitivity. We developed an HSRL with the iodine filter method for continuous observation of aerosols at 532nm in the northern region of Argentina in the framework of the South American Environmental Atmospheric Risk Management Network (SAVER.Net)/SATREPS project. The laser wavelength of the HSRL was controlled by a feedback system to tune the laser wavelength to the center of an iodine absorption line. The stability of the laser wavelength with the system satisfied the requirement showing very small systematic errors in the retrieval of extinction and backscatter.

  9. A thermodynamic model of mixed organic-inorganic aerosols to predict activity coefficients

    Science.gov (United States)

    Zuend, A.; Marcolli, C.; Luo, B. P.; Peter, T.

    2008-08-01

    Tropospheric aerosols contain mixtures of inorganic salts, acids, water, and a large variety of organic compounds. Interactions between these substances in liquid mixtures lead to discrepancies from ideal thermodynamic behaviour. By means of activity coefficients, non-ideal behaviour can be taken into account. We present here a thermodynamic model named AIOMFAC (Aerosol Inorganic-Organic Mixtures Functional groups Activity Coefficients) that is able to calculate activity coefficients covering inorganic, organic, and organic-inorganic interactions in aqueous solutions over a wide concentration range. This model is based on the activity coefficient model LIFAC by Yan et al. (1999) that we modified and reparametrised to better describe atmospherically relevant conditions and mixture compositions. Focusing on atmospheric applications we considered H+, Li+, Na+, K+, NH+4, Mg2+, Ca2+, Cl-, Br-, NO-3, HSO-4, and SO2-4 as cations and anions and a wide range of alcohols/polyols composed of the functional groups CHn and OH as organic compounds. With AIOMFAC, the activities of the components within an aqueous electrolyte solution are well represented up to high ionic strength. Most notably, a semi-empirical middle-range parametrisation of direct organic-inorganic interactions in alcohol+water+salt solutions strongly improves the agreement between experimental and modelled activity coefficients. At room temperature, this novel thermodynamic model offers the possibility to compute equilibrium relative humidities, gas/particle partitioning and liquid-liquid phase separations with high accuracy. In further studies, other organic functional groups will be introduced. The model framework is not restricted to specific ions or organic compounds and is therefore also applicable for other research topics.

  10. A thermodynamic model of mixed organic-inorganic aerosols to predict activity coefficients

    Directory of Open Access Journals (Sweden)

    A. Zuend

    2008-08-01

    Full Text Available Tropospheric aerosols contain mixtures of inorganic salts, acids, water, and a large variety of organic compounds. Interactions between these substances in liquid mixtures lead to discrepancies from ideal thermodynamic behaviour. By means of activity coefficients, non-ideal behaviour can be taken into account. We present here a thermodynamic model named AIOMFAC (Aerosol Inorganic-Organic Mixtures Functional groups Activity Coefficients that is able to calculate activity coefficients covering inorganic, organic, and organic-inorganic interactions in aqueous solutions over a wide concentration range. This model is based on the activity coefficient model LIFAC by Yan et al. (1999 that we modified and reparametrised to better describe atmospherically relevant conditions and mixture compositions. Focusing on atmospheric applications we considered H+, Li+, Na+, K+, NH+4, Mg2+, Ca2+, Cl, Br, NO3, HSO4, and SO2−4 as cations and anions and a wide range of alcohols/polyols composed of the functional groups CHn and OH as organic compounds. With AIOMFAC, the activities of the components within an aqueous electrolyte solution are well represented up to high ionic strength. Most notably, a semi-empirical middle-range parametrisation of direct organic-inorganic interactions in alcohol+water+salt solutions strongly improves the agreement between experimental and modelled activity coefficients. At room temperature, this novel thermodynamic model offers the possibility to compute equilibrium relative humidities, gas/particle partitioning and liquid-liquid phase separations with high accuracy. In further studies, other organic functional groups will be introduced. The model framework is not restricted to specific ions or organic compounds and is therefore also

  11. A thermodynamic model of mixed organic-inorganic aerosols to predict activity coefficients

    Directory of Open Access Journals (Sweden)

    A. Zuend

    2008-03-01

    Full Text Available Tropospheric aerosols contain mixtures of inorganic salts, acids, water, and a large variety of organic compounds. Interactions between these substances in liquid mixtures lead to discrepancies from ideal thermodynamic behaviour. By means of activity coefficients, non-ideal behaviour can be taken into account. We present here a thermodynamic model named AIOMFAC (Aerosol Inorganic–Organic Mixtures Functional groups Activity Coefficients that is able to calculate activity coefficients covering inorganic, organic, and organic–inorganic interactions in aqueous solutions over a wide concentration range. This model is based on the activity coefficient model LIFAC by Yan et al. (1999 that we modified and reparametrised to better describe atmospherically relevant conditions and mixture compositions. Focusing on atmospheric applications we considered H+, Li+, Na+, K+, NH4+, Mg2+, Ca2+, Cl, Br, NO3, HSO4, and SO42− as cations and anions and a wide range of alcohols/polyols composed of the functional groups CHn and OH as organic compounds. With AIOMFAC, the activities of the components within an aqueous electrolyte solution are well represented up to high ionic strength. Most notably, a semi-empirical middle-range parametrisation of direct organic–inorganic interactions in alcohol + water + salt solutions strongly improves the agreement between experimental and modelled activity coefficients. At room temperature, this novel thermodynamic model offers the possibility to compute equilibrium relative humidities, gas/particle partitioning and liquid–liquid phase separations with high accuracy. In further studies, other organic functional groups will be introduced. The model framework is not restricted to specific ions or organic compounds and is therefore

  12. Development and testing of an aerosol-stratus cloud parameterization scheme for middle and high latitudes

    Energy Technology Data Exchange (ETDEWEB)

    Olsson, P.Q.; Meyers, M.P.; Kreidenweis, S.; Cotton, W.R. [Colorado State Univ., Fort Collins, CO (United States)

    1996-04-01

    The aim of this new project is to develop an aerosol/cloud microphysics parameterization of mixed-phase stratus and boundary layer clouds. Our approach is to create, test, and implement a bulk-microphysics/aerosol model using data from Atmospheric Radiation Measurement (ARM) Cloud and Radiation Testbed (CART) sites and large-eddy simulation (LES) explicit bin-resolving aerosol/microphysics models. The primary objectives of this work are twofold. First, we need the prediction of number concentrations of activated aerosol which are transferred to the droplet spectrum, so that the aerosol population directly affects the cloud formation and microphysics. Second, we plan to couple the aerosol model to the gas and aqueous-chemistry module that will drive the aerosol formation and growth. We begin by exploring the feasibility of performing cloud-resolving simulations of Arctic stratus clouds over the North Slope CART site. These simulations using Colorado State University`s regional atmospheric modeling system (RAMS) will be useful in designing the structure of the cloud-resolving model and in interpreting data acquired at the North Slope site.

  13. Airborne high spectral resolution lidar observation of pollution aerosol during EUCAARI-LONGREX

    Directory of Open Access Journals (Sweden)

    S. Groß

    2012-10-01

    Full Text Available Airborne high spectral resolution lidar observations over Europe during the EUCAARI field experiment in May 2008 are analysed with respect to spatial distribution and optical properties of continental pollution aerosol. Continental aerosol is characterized by its depolarisation and lidar ratio. Mean values of 6%±1% for the particle linear depolarisation ratio, and 56 sr±6 sr for the lidar ratio were found for pollution aerosol. Both, lidar ratio and depolarisation ratio at 532 nm show virtually no variations for all analysed days during the measurement campaign.

  14. The role of the particle size distribution in assessing aerosol composition effects on simulated droplet activation

    Directory of Open Access Journals (Sweden)

    D. S. Ward

    2010-02-01

    Full Text Available Variations in the chemical composition of atmospheric aerosols alter their hygroscopicity and can lead to changes in the cloud-active fraction of the aerosols, or cloud condensation nuclei (CCN number concentration. To investigate the importance of this effect under different atmospheric conditions, cloud droplet formation was simulated with a Lagrangian parcel model. Initial values of updraft speed and temperature were systematically varied along with aerosol number concentration, size and hygroscopicity (represented by the hygroscopicity parameter, κ. A previous study classifies the sensitivity of CCN activity to compositional changes based on the supersaturation reached in the parcel model. We found that these classifications could not be generalized to a range of aerosol size distribution median radii. Instead, variations in sensitivity with size depend on the location of the dry critical radius for droplet activation relative to the size distribution median radius. The parcel model output was used to construct droplet activation lookup tables based on κ that were implemented in the Regional Atmospheric Modeling System (RAMS microphysical scheme. As a first application of this system, aerosol hygroscopicity and size were varied in a series of RAMS mesoscale simulations designed to investigate the sensitivity of a mixed-phase orographic cloud case to the parameter variations. Observations from a recent field campaign in northwestern Colorado provided the basis for the aerosol field initializations. Model results show moderate sensitivity in the distribution of total case precipitation to extreme changes in κ, and minimal sensitivity to observed changes in estimated κ. The impact of varying aerosol hygroscopicity diminished with increasing median radius, as expected from the parcel model results. The conclusions drawn from these simulations could simplify similar research in other cloud regimes by defining the need, or lack of need, for

  15. Role of aerosols in modulating cloud properties during active-break cycle of Indian summer monsoon

    Science.gov (United States)

    Bhattacharya, A.; Chakraborty, A.; Venugopal, V.

    2016-11-01

    In this study, the weather research and forecast model coupled with chemistry (WRF-Chem), is used to understand the impact of aerosol-cloud interaction during the active-break cycles of the Indian summer monsoon. Two sets of simulations are performed, one with a fixed aerosol concentration (ConstantAero) and the other with an observation-based prescription of the rate of change of aerosol concentration as a function of precipitation (VaryingAero). This prescription is derived based on satellite-retrieved daily rainrate and concurrent observations of aerosol optical depth from aerosol robotic network. The proposed modification is necessitated by the lack of realistic emission estimates over the Indian region as well as the presence of inherent biases in monsoon simulation in WRF-Chem. In the VaryingAero simulation, unlike in the ConstantAero run, we find that the break-to-active monsoon phase has more cloud liquid water (CLW) and less rain efficiency than in the active-to-break phase. This is primarily due to the indirect effect of increased aerosol loading in the break phase. This result is in accordance with the observed behaviour of CLW estimtes from microwave imager (TRMM 2A12) and radar reflectivity (TRMM precipitation radar). We also find that the proposed interactive aerosol loading results in higher spatial variability in CLW and enhances the likelihood of increased cloud cover via formation of larger clouds. The modification also alters the diurnal cycle of clouds in break and break-to-active phases as compared to other phases due to aerosol loading, with a stronger diurnal cycle of upper level clouds in these phases in the VaryingAero model as compared to ConstantAero model.

  16. Role of aerosols in modulating cloud properties during active-break cycle of Indian summer monsoon

    Science.gov (United States)

    Bhattacharya, A.; Chakraborty, A.; Venugopal, V.

    2017-09-01

    In this study, the weather research and forecast model coupled with chemistry (WRF-Chem), is used to understand the impact of aerosol-cloud interaction during the active-break cycles of the Indian summer monsoon. Two sets of simulations are performed, one with a fixed aerosol concentration ( ConstantAero) and the other with an observation-based prescription of the rate of change of aerosol concentration as a function of precipitation ( VaryingAero). This prescription is derived based on satellite-retrieved daily rainrate and concurrent observations of aerosol optical depth from aerosol robotic network. The proposed modification is necessitated by the lack of realistic emission estimates over the Indian region as well as the presence of inherent biases in monsoon simulation in WRF-Chem. In the VaryingAero simulation, unlike in the ConstantAero run, we find that the break-to-active monsoon phase has more cloud liquid water (CLW) and less rain efficiency than in the active-to-break phase. This is primarily due to the indirect effect of increased aerosol loading in the break phase. This result is in accordance with the observed behaviour of CLW estimtes from microwave imager (TRMM 2A12) and radar reflectivity (TRMM precipitation radar). We also find that the proposed interactive aerosol loading results in higher spatial variability in CLW and enhances the likelihood of increased cloud cover via formation of larger clouds. The modification also alters the diurnal cycle of clouds in break and break-to-active phases as compared to other phases due to aerosol loading, with a stronger diurnal cycle of upper level clouds in these phases in the VaryingAero model as compared to ConstantAero model.

  17. Lidar detection of high concentrations of ozone and aerosol transported from northeastern Asia over Saga, Japan

    Science.gov (United States)

    Uchino, Osamu; Sakai, Tetsu; Izumi, Toshiharu; Nagai, Tomohiro; Morino, Isamu; Yamazaki, Akihiro; Deushi, Makoto; Yumimoto, Keiya; Maki, Takashi; Tanaka, Taichu Y.; Akaho, Taiga; Okumura, Hiroshi; Arai, Kohei; Nakatsuru, Takahiro; Matsunaga, Tsuneo; Yokota, Tatsuya

    2017-02-01

    To validate products of the Greenhouse gases Observing SATellite (GOSAT), we observed vertical profiles of aerosols, thin cirrus clouds, and tropospheric ozone with a mobile-lidar system that consisted of a two-wavelength (532 and 1064 nm) polarization lidar and a tropospheric ozone differential absorption lidar (DIAL). We used these lidars to make continuous measurements over Saga (33.24° N, 130.29° E) during 20-31 March 2015. High ozone and high aerosol concentrations were observed almost simultaneously in the altitude range 0.5-1.5 km from 03:00 to 20:00 Japan Standard Time (JST) on 22 March 2015. The maximum ozone volume mixing ratio was ˜ 110 ppbv. The maxima of the aerosol extinction coefficient and optical depth at 532 nm were 1.2 km-1 and 2.1, respectively. Backward trajectory analysis and the simulations by the Model of Aerosol Species IN the Global AtmospheRe (MASINGAR) mk-2 and the Meteorological Research Institute Chemistry-Climate Model, version 2 (MRI-CCM2), indicated that mineral dust particles from the Gobi Desert and an air mass with high ozone and aerosol (mainly sulfate) concentrations that originated from the North China Plain could have been transported over the measurement site within about 2 days. These high ozone and aerosol concentrations impacted surface air quality substantially in the afternoon of 22 March 2015. After some modifications of its physical and chemical parameters, MRI-CCM2 approximately reproduced the high ozone volume mixing ratio. MASINGAR mk-2 successfully predicted high aerosol concentrations, but the predicted peak aerosol optical thickness was about one-third of the observed value.

  18. Reduction of photosynthetically active radiation under extreme stratospheric aerosol loads

    Energy Technology Data Exchange (ETDEWEB)

    Gerstl, S.A.W.; Zardecki, A.

    1981-08-01

    The recently published hypothesis that the Cretaceous-Tertiary extinctions might be caused by an obstruction of sunlight is tested by model calculations. First we compute the total mass of stratospheric aerosols under normal atmospheric conditions for four different (measured) aerosol size distributions and vertical profiles. For comparison, the stratospheric dust masses after four volcanic eruptions are also evaluated. Detailed solar radiative transfer calculations are then performed for artificially increased aerosol amounts until the postulated darkness scenario is obtained. Thus we find that a total stratospheric aerosol mass between 1 and 4 times 10/sup 1/ g is sufficient to reduce photosynthesis to 10/sup -3/ of normal. We also infer from this result tha the impact of a 0.4- to 3-km-diameter asteroid or a close encounter with a Halley-size comet may deposit that amount of particulates into the stratosphere. The darkness scenario of Alvarez et al. is thus shown to be a possible extinction mechanism, even with smaller size asteroids of comets than previously estimated.

  19. Characterization of aerosol photooxidation flow reactors: heterogeneous oxidation, secondary organic aerosol formation and cloud condensation nuclei activity measurements

    Directory of Open Access Journals (Sweden)

    A. T. Lambe

    2011-03-01

    Full Text Available Motivated by the need to develop instrumental techniques for characterizing organic aerosol aging, we report on the performance of the Toronto Photo-Oxidation Tube (TPOT and Potential Aerosol Mass (PAM flow tube reactors under a variety of experimental conditions. The PAM system was designed with lower surface-area-to-volume (SA/V ratio to minimize wall effects; the TPOT reactor was designed to study heterogeneous aerosol chemistry where wall loss can be independently measured. The following studies were performed: (1 transmission efficiency measurements for CO2, SO2, and bis(2-ethylhexyl sebacate (BES particles, (2 H2SO4 yield measurements from the oxidation of SO2, (3 residence time distribution (RTD measurements for CO2, SO2, and BES particles, (4 aerosol mass spectra, O/C and H/C ratios, and cloud condensation nuclei (CCN activity measurements of BES particles exposed to OH radicals, and (5 aerosol mass spectra, O/C and H/C ratios, CCN activity, and yield measurements of secondary organic aerosol (SOA generated from gas-phase OH oxidation of m-xylene and α-pinene. OH exposures ranged from (2.0 ± 1.0 × 1010 to (1.8 ± 0.3 × 1012 molec cm−3 s. Where applicable, data from the flow tube reactors are compared with published results from the Caltech smog chamber. The TPOT yielded narrower RTDs. However, its transmission efficiency for SO2 was lower than that for the PAM. Transmission efficiency for BES and H2SO4 particles was size-dependent and was similar for the two flow tube designs. Oxidized BES particles had similar O/C and H/C ratios and CCN activity at OH exposures greater than 1011 molec cm−3 s, but different CCN activity at lower OH exposures. The O/C ratio, H/C ratio, and yield of m-xylene and α-pinene SOA was strongly affected by reactor design and

  20. Comparative Antimicrobial Activities of Aerosolized Sodium Hypochlorite, Chlorine Dioxide, and Electrochemically Activated Solutions Evaluated Using a Novel Standardized Assay

    Science.gov (United States)

    Thorn, R. M. S.; Robinson, G. M.

    2013-01-01

    The main aim of this study was to develop a standardized experimental assay to enable differential antimicrobial comparisons of test biocidal aerosols. This study represents the first chlorine-matched comparative assessment of the antimicrobial activities of aerosolized sodium hypochlorite, chlorine dioxide, and electrochemically activated solution (ECAS) to determine their relative abilities to decontaminate various surface-associated health care-relevant microbial challenges. Standard microbiological challenges were developed by surface-associating typed Pseudomonas aeruginosa, Staphylococcus aureus, Bacillus subtilis spores, or a clinical methicillin-resistant S. aureus (MRSA) strain on stainless steel, polypropylene, or fabric. All test coupons were subjected to 20-min biocidal aerosols of chlorine-matched (100 ppm) sodium hypochlorite, chlorine dioxide, or ECAS within a standard aerosolization chamber using a commercial humidifier under defined conditions. Biocidal treatment type and material surface had a significant effect on the number of microorganisms recovered from various material surfaces following treatment exposure. Under the conditions of the assay, the order of antimicrobial efficacy of biocidal aerosol treatment was as follows: ECAS > chlorine dioxide > sodium hypochlorite. For all biocides, greater antimicrobial reductions were seen when treating stainless steel and fabric than when treating plastic-associated microorganisms. The experimental fogging system and assay protocol designed within this study were shown capable of differentiating the comparative efficacies of multiple chlorine-matched biocidal aerosols against a spectrum of target organisms on a range of test surface materials and would be appropriate for testing other biocidal aerosol treatments or material surfaces. PMID:23459480

  1. Comparative antimicrobial activities of aerosolized sodium hypochlorite, chlorine dioxide, and electrochemically activated solutions evaluated using a novel standardized assay.

    Science.gov (United States)

    Thorn, R M S; Robinson, G M; Reynolds, D M

    2013-05-01

    The main aim of this study was to develop a standardized experimental assay to enable differential antimicrobial comparisons of test biocidal aerosols. This study represents the first chlorine-matched comparative assessment of the antimicrobial activities of aerosolized sodium hypochlorite, chlorine dioxide, and electrochemically activated solution (ECAS) to determine their relative abilities to decontaminate various surface-associated health care-relevant microbial challenges. Standard microbiological challenges were developed by surface-associating typed Pseudomonas aeruginosa, Staphylococcus aureus, Bacillus subtilis spores, or a clinical methicillin-resistant S. aureus (MRSA) strain on stainless steel, polypropylene, or fabric. All test coupons were subjected to 20-min biocidal aerosols of chlorine-matched (100 ppm) sodium hypochlorite, chlorine dioxide, or ECAS within a standard aerosolization chamber using a commercial humidifier under defined conditions. Biocidal treatment type and material surface had a significant effect on the number of microorganisms recovered from various material surfaces following treatment exposure. Under the conditions of the assay, the order of antimicrobial efficacy of biocidal aerosol treatment was as follows: ECAS > chlorine dioxide > sodium hypochlorite. For all biocides, greater antimicrobial reductions were seen when treating stainless steel and fabric than when treating plastic-associated microorganisms. The experimental fogging system and assay protocol designed within this study were shown capable of differentiating the comparative efficacies of multiple chlorine-matched biocidal aerosols against a spectrum of target organisms on a range of test surface materials and would be appropriate for testing other biocidal aerosol treatments or material surfaces.

  2. Microfluidic electrochemical sensor for on-line monitoring of aerosol oxidative activity.

    Science.gov (United States)

    Sameenoi, Yupaporn; Koehler, Kirsten; Shapiro, Jeff; Boonsong, Kanokporn; Sun, Yele; Collett, Jeffrey; Volckens, John; Henry, Charles S

    2012-06-27

    Particulate matter (PM) air pollution has a significant impact on human morbidity and mortality; however, the mechanisms of PM-induced toxicity are poorly defined. A leading hypothesis states that airborne PM induces harm by generating reactive oxygen species in and around human tissues, leading to oxidative stress. We report here a system employing a microfluidic electrochemical sensor coupled directly to a particle-into-liquid sampler (PILS) system to measure aerosol oxidative activity in an on-line format. The oxidative activity measurement is based on the dithiothreitol (DTT) assay, where, after being oxidized by PM, the remaining reduced DTT is analyzed by the microfluidic sensor. The sensor consists of an array of working, reference, and auxiliary electrodes fabricated in a poly(dimethylsiloxane)-based microfluidic device. Cobalt(II) phthalocyanine-modified carbon paste was used as the working electrode material, allowing selective detection of reduced DTT. The electrochemical sensor was validated off-line against the traditional DTT assay using filter samples taken from urban environments and biomass burning events. After off-line characterization, the sensor was coupled to a PILS to enable on-line sampling/analysis of aerosol oxidative activity. Urban dust and industrial incinerator ash samples were aerosolized in an aerosol chamber and analyzed for their oxidative activity. The on-line sensor reported DTT consumption rates (oxidative activity) in good correlation with aerosol concentration (R(2) from 0.86 to 0.97) with a time resolution of approximately 3 min.

  3. Ultraviolet Raman lidar for high-accuracy profiling of aerosol extinction coefficient

    Institute of Scientific and Technical Information of China (English)

    Fei Gao; Xiaoquan Song; Yufeng Wang; Yi Zhou; Dengxin Hua

    2009-01-01

    An ultraviolet (UV) Raman lidar system at 354.7 nm has been developed for accurately measuring the aerosol extinction profiles. A spectroscopic filter combining a high-spectral-resolution grating with two narrowband mirrors is used to separate the vibrational Raman scattering signal of N2 at a central wave-length of 386.7 nm and the elastic scattering signal at 354.7 nm. The aerosol extinction is derived from the Raman scattering of N2 and the elastic scattering by the use of Raman method and Klett method, respectively. The derived results of aerosol extinction are used to compare the difference of two retrieval methods, and the preliminary experiment shows that the Raman lidar system operated in analog detection mode has the capability of measuring aerosol profiles up to a height of 3 km with a laser energy of 250 mJ and an integration time of 8 min.

  4. Evaluating the Role of Aerosol Mixing State in Cloud Droplet Nucleation using a New Activation Parameterization

    Science.gov (United States)

    Rothenberg, D. A.; Wang, C.

    2013-12-01

    An important source contributing to uncertainty in simulations with global climate models arises from the influence of aerosols on cloud properties. These so-called aerosol indirect effects arise from a single coupling in the model, representing how aerosols activate and serve as cloud condensation nuclei and ultimately cloud droplets. While it is possible to build explicit numerical models which describe this process in detail, these class of tools are untenable for use in global climate models due to their complexity. Instead, physically- or empirically-based parameterizations of activation are used in their place to efficiently approximate cloud droplet nucleation as a function of a few meteorological and aerosol physical/chemical properties. As global climate models are outfitted with more complex, size- and mixing state-resolving aerosol models, activation parameterizations are increasingly called upon to handle aerosol populations against which their performance has not been explicitly benchmarked. Here, a simple scheme is proposed to evaluate the performance of activation parameterizations against a spectrum of mixing states, and two schemes commonly used in global models are studied using this framework. It is shown that each scheme exhibits systematic biases when a complex mixing state is present. To help resolve these issues, a new scheme is derived using Polynomial Chaos Expansion to build meta-models representing a full complexity parcel model. The meta-models are shown to accurately handle activation in both single-mode and mixture cases. In addition, a global sensitivity analysis is applied to benchmark the performance of the meta-models and the activation parameterizations against a detailed parcel model, and it is shown that the meta-models tend to more accurately attribute variability in activation dynamics to each input parameter and their interactions with others when compared to the physically-based parameterizations. A variety of experiments

  5. Incorporating an advanced aerosol activation parameterization into WRF-CAM5: Model evaluation and parameterization intercomparison: An Advanced Aerosol Activation Scheme

    Energy Technology Data Exchange (ETDEWEB)

    Zhang, Yang [Department of Marine, Earth, and Atmospheric Sciences, North Carolina State University, Raleigh North Carolina USA; Collaborative Innovation Center for Regional Environmental Quality, Beijing China; Zhang, Xin [Department of Marine, Earth, and Atmospheric Sciences, North Carolina State University, Raleigh North Carolina USA; Wang, Kai [Department of Marine, Earth, and Atmospheric Sciences, North Carolina State University, Raleigh North Carolina USA; He, Jian [Department of Marine, Earth, and Atmospheric Sciences, North Carolina State University, Raleigh North Carolina USA; Leung, L. Ruby [Pacific Northwest National Laboratory, Richland Washington USA; Fan, Jiwen [Pacific Northwest National Laboratory, Richland Washington USA; Nenes, Athanasios [School of Earth and Atmospheric Sciences, Georgia Institute of Technology, Atlanta Georgia USA; School of Chemical and Biomolecular Engineering, Georgia Institute of Technology, Atlanta Georgia USA

    2015-07-22

    Aerosol activation into cloud droplets is an important process that governs aerosol indirect effects. The advanced treatment of aerosol activation by Fountoukis and Nenes (2005) and its recent updates, collectively called the FN series, have been incorporated into a newly developed regional coupled climate-air quality model based on the Weather Research and Forecasting model with the physics package of the Community Atmosphere Model version 5 (WRF-CAM5) to simulate aerosol-cloud interactions in both resolved and convective clouds. The model is applied to East Asia for two full years of 2005 and 2010. A comprehensive model evaluation is performed for model predictions of meteorological, radiative, and cloud variables, chemical concentrations, and column mass abundances against satellite data and surface observations from air quality monitoring sites across East Asia. The model performs overall well for major meteorological variables including near-surface temperature, specific humidity, wind speed, precipitation, cloud fraction, precipitable water, downward shortwave and longwave radiation, and column mass abundances of CO, SO2, NO2, HCHO, and O3 in terms of both magnitudes and spatial distributions. Larger biases exist in the predictions of surface concentrations of CO and NOx at all sites and SO2, O3, PM2.5, and PM10 concentrations at some sites, aerosol optical depth, cloud condensation nuclei over ocean, cloud droplet number concentration (CDNC), cloud liquid and ice water path, and cloud optical thickness. Compared with the default Abdul-Razzack Ghan (2000) parameterization, simulations with the FN series produce ~107–113% higher CDNC, with half of the difference attributable to the higher aerosol activation fraction by the FN series and the remaining half due to feedbacks in subsequent cloud microphysical processes. With the higher CDNC, the FN series are more skillful in simulating cloud water path, cloud optical thickness, downward shortwave radiation

  6. Aerosol nucleation induced by a high energy particle beam

    DEFF Research Database (Denmark)

    Enghoff, Martin Andreas Bødker; Pedersen, Jens Olaf Pepke; Uggerhøj, Ulrik I.

    2011-01-01

    We have studied sulfuric acid aerosol nucleation in an atmospheric pressure reaction chamber using a 580 MeV electron beam to ionize the volume of the reaction chamber. We find a clear contribution from ion-induced nucleation and consider this to be the first unambiguous observation of the ion......-effect on aerosol nucleation using a particle beam under conditions that resemble the Earth's atmosphere. By comparison with ionization using a gamma source we further show that the nature of the ionizing particles is not important for the ion-induced component of the nucleation. This implies that inexpensive...... ionization sources - as opposed to expensive accelerator beams - can be used for investigations of ion-induced nucleation....

  7. Real-time measurement of aerosol particle concentration at high temperatures; Hiukkaspitoisuuden reaaliaikainen mittaaminen korkeassa laempoetilassa

    Energy Technology Data Exchange (ETDEWEB)

    Keskinen, J.; Hautanen, J.; Laitinen, A. [Tampere Univ. of Technology (Finland). Physics

    1997-10-01

    The aim of this project is to develop a new method for continuous aerosol particle concentration measurement at elevated temperatures (up to 800-1000 deg C). The measured property of the aerosol particles is the so called Fuchs surface area. This quantity is relevant for diffusion limited mass transfer to particles. The principle of the method is as follows. First, aerosol particles are charged electrically by diffusion charging process. The charging takes place at high temperature. After the charging, aerosol is diluted and cooled. Finally, aerosol particles are collected and the total charge carried by the aerosol particles is measured. Particle collection and charge measurement take place at low temperature. Benefits of this measurement method are: particles are charged in-situ, charge of the particles is not affected by the temperature and pressure changes after sampling, particle collection and charge measurement are carried out outside the process conditions, and the measured quantity is well defined. The results of this study can be used when the formation of the fly ash particles is studied. Another field of applications is the study and the development of gasification processes. Possibly, the method can also be used for the monitoring the operation of the high temperature particle collection devices. (orig.)

  8. NASA LaRC airborne high spectral resolution lidar aerosol measurements during MILAGRO: observations and validation

    Directory of Open Access Journals (Sweden)

    L. I. Kleinman

    2009-07-01

    Full Text Available The NASA Langley Research Center (LaRC airborne High Spectral Resolution Lidar (HSRL measures vertical profiles of aerosol extinction, backscatter, and depolarization at both 532 nm and 1064 nm. In March of 2006 the HSRL participated in the Megacity Initiative: Local and Global Research Observations (MILAGRO campaign along with several other suites of instruments deployed on both aircraft and ground based platforms. This paper presents high spatial and vertical resolution HSRL measurements of aerosol extinction and optical depth from MILAGRO and comparisons of those measurements with similar measurements from other sensors and model predictions. HSRL measurements coincident with airborne in situ aerosol scattering and absorption measurements from two different instrument suites on the C-130 and G-1 aircraft, airborne aerosol optical depth (AOD and extinction measurements from an airborne tracking sunphotometer on the J-31 aircraft, and AOD from a network of ground based Aerosol Robotic Network (AERONET sun photometers are presented as a validation of the HSRL aerosol extinction and optical depth products. Regarding the extinction validation, we find bias differences between HSRL and these instruments to be less than 3% (0.01 km−1 at 532 nm, the wavelength at which the HSRL technique is employed. The rms differences at 532 nm were less than 50% (0.015 km−1. To our knowledge this is the most comprehensive validation of the HSRL measurement of aerosol extinction and optical depth to date. The observed bias differences in ambient aerosol extinction between HSRL and other measurements is within 15–20% at visible wavelengths, found by previous studies to be the differences observed with current state-of-the-art instrumentation (Schmid et al., 2006.

  9. NASA LaRC airborne high spectral resolution lidar aerosol measurements during MILAGRO: observations and validation

    Directory of Open Access Journals (Sweden)

    R. R. Rogers

    2009-04-01

    Full Text Available The NASA Langley Research Center (LaRC airborne High Spectral Resolution Lidar (HSRL measures vertical profiles of aerosol extinction, backscatter, and depolarization at both 532 nm and 1064 nm. In March of 2006 the HSRL participated in the Megacity Initiative: Local and Global Research Observations (MILAGRO campaign along with several other suites of instruments deployed on both aircraft and ground based platforms. This paper presents high spatial and vertical resolution HSRL measurements of aerosol extinction and optical depth from MILAGRO and comparisons of those measurements with similar measurements from other sensors and model predictions. HSRL measurements coincident with airborne in situ aerosol scattering and absorption measurements from two different instrument suites on the C-130 and G-1 aircraft, airborne aerosol optical depth (AOD and extinction measurements from an airborne tracking sunphotometer on the J-31 aircraft, and AOD from a network of ground based Aerosol Robotic Network (AERONET sun photometers are presented as a validation of the HSRL aerosol extinction and optical depth products. Regarding the extinction validation, we find bias differences between HSRL and these instruments to be less than 3% (0.01 km−1 at 532 nm, the wavelength at which the HSRL technique is employed. The rms differences at 532 nm were less than 50% (0.015 km−1. To our knowledge this is the most comprehensive validation of the HSRL measurement of aerosol extinction and optical depth to date. The observed bias differences in ambient aerosol extinction between HSRL and other measurements is within 15–20% at visible wavelengths, found by previous studies to be the differences observed with current state-of-the-art instrumentation (Schmid et al., 2006.

  10. Hygroscopic properties of urban aerosols and their cloud condensation nuclei activities measured in Seoul during the MAPS-Seoul campaign

    Science.gov (United States)

    Kim, Najin; Park, Minsu; Yum, Seong Soo; Park, Jong Sung; Song, In Ho; Shin, Hye Jung; Ahn, Joon Young; Kwak, Kyung-Hwan; Kim, Hwajin; Bae, Gwi-Nam; Lee, Gangwoong

    2017-03-01

    Aerosol physical properties, chemical compositions, hygroscopicity and cloud condensation nuclei (CCN) activities were measured in Seoul, the highly populated capital city of Korea, during the Megacity Air Pollution Studies (MAPS-Seoul) campaign, in May-June 2015. The average aerosol concentration for particle diameters >10 nm was 11787 ± 7421 cm-3 with dominant peaks at morning rush hours and in the afternoon due to frequent new particle formation (NPF) events. The average CCN concentration was 4075 ± 1812 cm-3 at 0.6% supersaturation, with little diurnal variation. The average hygroscopicity parameter (κ) value determined using a humidified tandem differential mobility analyzer (HTDMA) ranged 0.17-0.27 for a range of particle diameters (30-150 nm). The κ values derived using the aerosol mass spectrometer (AMS) data with three different methods were 0.32-0.34, significantly higher than those from HTDMA due to the uncertainties in the hygroscopicity values of different chemical compositions, especially organics and black carbon. Factors affecting the aerosol hygroscopicity seemed to be traffic and chemical processes during the NPF events. The CCN concentration predicted based on HTDMA κ data showed very good agreement with the measured one. Because of the overestimation of κ, CCN closure with the predicted CCN concentration based on AMS κ data over-predicted CCN concentration although the linear correlation between measured and predicted CCN concentration was still very good.

  11. Ozone oxidation of oleic acid surface films decreases aerosol cloud condensation nuclei activity

    Science.gov (United States)

    Schwier, A. N.; Sareen, N.; Lathem, T. L.; Nenes, A.; McNeill, V. F.

    2011-08-01

    Heterogeneous oxidation of aerosols composed of pure oleic acid (C18H34O2, an unsaturated fatty acid commonly found in continental and marine aerosol) by gas-phase O3 is known to increase aerosol hygroscopicity and activity as cloud condensation nuclei (CCN). Whether this trend is preserved when the oleic acid is internally mixed with other electrolytes is unknown and addressed in this study. We quantify the CCN activity of sodium salt aerosols (NaCl and Na2SO4) internally mixed with sodium oleate (SO) and oleic acid (OA). We find that particles containing roughly one monolayer of SO/OA show similar CCN activity to pure salt particles, whereas a tenfold increase in organic concentration slightly depresses CCN activity. O3 oxidation of these multicomponent aerosols has little effect on the critical diameter for CCN activation for unacidified particles at all conditions studied, and the activation kinetics of the CCN are similar in each case to those of pure salts. SO-containing particles which are acidified to atmospherically relevant pH before analysis in order to form oleic acid, however, show depressed CCN activity upon oxidation. This effect is more pronounced at higher organic concentrations. The behavior after oxidation is consistent with the disappearance of the organic surface film, supported by Köhler Theory Analysis (KTA). The κ-Köhler calculations show a small decrease in hygroscopicity after oxidation. The important implication of this finding is that oxidative aging may not always enhance the hygroscopicity of internally mixed inorganic-organic aerosols.

  12. Evaluation and application of passive and active optical remote sensing methods for the measurement of atmospheric aerosol properties

    Energy Technology Data Exchange (ETDEWEB)

    Mielonen, T.

    2010-07-01

    Atmospheric aerosol particles affect the atmosphere's radiation balance by scattering and absorbing sunlight. Moreover, the particles act as condensation nuclei for clouds and affect their reflectivity. In addition, aerosols have negative health effects and they reduce visibility. Aerosols are emitted into the atmosphere from both natural and anthropogenic sources. Different types of aerosols have different effects on the radiation balance, thus global monitoring and typing of aerosols is of vital importance. In this thesis, several remote sensing methods used in the measurement of atmospheric aerosols are evaluated. Remote sensing of aerosols can be done with active and passive instruments. Passive instruments measure radiation emitted by the sun and the Earth while active instruments have their own radiation source, for example a black body radiator or laser. The instruments utilized in these studies were sun photometers (PFR, Cimel), lidars (POLLYXT, CALIOP), transmissiometer (OLAF) and a spectroradiometer (MODIS). Retrieval results from spaceborne instruments (MODIS, CALIOP) were evaluated with ground based measurements (PFR, Cimel). In addition, effects of indicative aerosol model assumptions on the calculated radiative transfer were studied. Finally, aerosol particle mass at the ground level was approximated from satellite measurements and vertical profiles of aerosols measured with a lidar were analyzed. For the evaluation part, these studies show that the calculation of aerosol induced attenuation of radiation based on aerosol size distribution measurements is not a trivial task. In addition to dry aerosol size distribution, the effect of ambient relative humidity on the size distribution and the optical properties of the aerosols need to be known in order to achieve correct results from the calculations. Furthermore, the results suggest that aerosol size parameters retrieved from passive spaceborne measurements depend heavily on surgace reflectance

  13. High Resolution Modelling of Aerosols-Meteorology Interactions over Northern Europe and Arctic regions

    Science.gov (United States)

    Mahura, Alexander; Nuterman, Roman; Baklanov, Alexander

    2017-04-01

    Aerosols have influence on weather, air quality and climate. Multi-scale modelling, and especially long-range atmospheric transport, dispersion, and deposition of aerosols from remote sources is especially challenging in northern latitudes. It is due to complexity of meteorological, chemical and biological processes, their interactions and especially within and above the surface layer, linking to climate change, and influence on ecosystems. The online integrated meteorology-chemistry-aerosols model Enviro-HIRLAM (Environment - High Resolution Limited Area Model) was employed for evaluating spatio-temporal variability of atmospheric aerosols and their interactions and effects on meteorology with a focus on the Northern Europe and Arctic regions. The model setup covers domain having 510 x 568 grids of latitude vs. longitude, horizontal resolution of 0.15 deg, 40 vertical hybrid levels, time step of 360 sec, 6 h meteorological surface data assimilation. The model was run for January and July-August 2010 at DMI's CRAY-XC30 supercomputer. Emissions used are anthropogenic (ECLIPSE v5), shipping (combined AU_RCP and FMI), wildfires (IS4FIRES), and interactive sea salt, dust and DMS. The boundary conditions were obtained from ECMWF: for meteorology (from IFS at 0.15 and 0.25 deg. for summer and winter, respectively) and atmospheric composition (from MACC Reanalysis at 1.125 deg. resolution). The Enviro-HIRLAM model was employed in 4 modes: the reference run (e.g. without aerosols influence on meteorology) and 3 modified runs (direct aerosol effect (DAE), indirect aerosol effect (IDAE), and both effects DAE and IDAE included). The differences between the reference run and the runs with mentioned aerosol effects were estimated on a day-by-day, monthly and diurnal cycle bases over the domain, Arctic areas, European and Nordic countries. The results of statistical analyses are summarized and presented.

  14. Development and Applications of a New, High-Resolution, Operational MISR Aerosol Product

    Science.gov (United States)

    Garay, M. J.; Diner, D. J.; Kalashnikova, O.

    2014-12-01

    Since early 2000, the Multi-angle Imaging SpectroRadiometer (MISR) instrument on NASA's Terra satellite has been providing aerosol optical depth (AOD) and particle property retrievals at 17.6 km spatial resolution. Capitalizing on the capabilities provided by multi-angle viewing, the operational MISR algorithm performs well, with about 75% of MISR AOD retrievals falling within 0.05 or 20% × AOD of the paired validation data from the ground-based Aerosol Robotic Network (AERONET), and is able to distinguish aerosol particles by size and sphericity, over both land and water. These attributes enable a variety of applications, including aerosol transport model validation and global air quality assessment. Motivated by the adverse impacts of aerosols on human health at the local level, and taking advantage of computational speed advances that have occurred since the launch of Terra, we have implemented an operational MISR aerosol product with 4.4 km spatial resolution that maintains, and sometimes improves upon, the quality of the 17.6 km resolution product. We will describe the performance of this product relative to the heritage 17.6 km product, the global AERONET validation network, and high spatial density AERONET-DRAGON sites. Other changes that simplify product content, and make working with the data much easier for users, will also be discussed. Examples of how the new product demonstrates finer spatial variability of aerosol fields than previously retrieved, and ways this new dataset can be used for studies of local aerosol effects, will be shown.

  15. Aerosol mixing state, hygroscopic growth and cloud activation efficiency during MIRAGE 2006

    Directory of Open Access Journals (Sweden)

    S. Lance

    2013-05-01

    Full Text Available Observations of aerosol hygroscopic growth and CCN activation spectra for submicron particles are reported for the T1 ground site outside of Mexico City during the MIRAGE 2006 campaign. κ-Köhler theory is used to evaluate the characteristic hygroscopicity parameter, κ*, for the CCN active aerosol population using both size-resolved HTMDA and size-resolved CCNc measurements. Organic mass fractions (forg are evaluated from size-resolved aerosol mass spectrometer (AMS measurements, from which predictions of the hygroscopicity parameter are compared against κ*. Strong diurnal changes in aerosol water uptake parameters and aerosol composition are observed. We find that new particle formation (NPF events are correlated with an increased κ* and CCN-active fraction during the daytime, with greater impact on smaller particles. During NPF events, the number concentration of 40 nm particles acting as CCN at 0.51% ± 0.06% supersaturation can surpass by more than a factor of two the corresponding concentrations of 100 nm particles. We also find that at 06:00–08:00 LT throughout the campaign, fresh traffic emissions result in substantial changes to the chemical distribution of the aerosol, with on average 65% externally mixed fraction for 40 nm particles and 30% externally mixed fraction for 100 nm particles, whereas at midday nearly all particles of both sizes can be described as "internally mixed". Average activation spectra and growth factor distributions are analyzed for different time periods characterizing the daytime (with and without NPF events, the early morning "rush hour" and the entire campaign. We show that κ* derived from CCNc measurements decreases as a function of size during all time periods, while the CCN-active fraction increases as a function of size. Size-resolved AMS measurements do not predict the observed trend for κ* versus particle size, which can be attributed to unresolved mixing state and the presence of refractory

  16. Chemical composition, sources, and processes of urban aerosols during summertime in northwest China: insights from high-resolution aerosol mass spectrometry

    Science.gov (United States)

    Xu, J.; Zhang, Q.; Chen, M.; Ge, X.; Ren, J.; Qin, D.

    2014-12-01

    An Aerodyne high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS) was deployed along with a scanning mobility particle sizer (SMPS) and a multi-angle absorption photometer (MAAP) to measure the temporal variations of the mass loading, chemical composition, and size distribution of submicron particulate matter (PM1) in Lanzhou, northwest China, during 11 July-7 August 2012. The average (PM1 mass concentration including non-refractory (PM1 (NR-(PM1) measured by HR-ToF-AMS and black carbon (BC) measured by MAAP during this study was 24.5 μg m-3 (ranging from 0.86 to 105 μg m-3), with a mean composition consisting of 47% organics, 16% sulfate, 12% BC, 11% ammonium, 10% nitrate, and 4% chloride. Organic aerosol (OA) on average consisted of 70% carbon, 21% oxygen, 8% hydrogen, and 1% nitrogen, with the average oxygen-to-carbon ratio (O / C) of 0.33 and organic mass-to-carbon ratio (OM / OC) of 1.58. Positive matrix factorization (PMF) of the high-resolution organic mass spectra identified four distinct factors which represent, respectively, two primary OA (POA) emission sources (traffic and food cooking) and two secondary OA (SOA) types - a fresher, semi-volatile oxygenated OA (SV-OOA) and a more aged, low-volatility oxygenated OA (LV-OOA). Traffic-related hydrocarbon-like OA (HOA) and BC displayed distinct diurnal patterns, both with peak at ~ 07:00-11:00 (BJT: UTC +8), corresponding to the morning rush hours, while cooking-emission related OA (COA) peaked during three meal periods. The diurnal profiles of sulfate and LV-OOA displayed a broad peak between ~ 07:00 and 15:00, while those of nitrate, ammonium, and SV-OOA showed a narrower peak between ~ 08:00-13:00. The later morning and early afternoon maximum in the diurnal profiles of secondary aerosol species was likely caused by downward mixing of pollutants aloft, which were likely produced in the residual layer decoupled from the boundary layer during nighttime. The mass spectrum of SV-OOA was

  17. Size-resolved and bulk activation properties of aerosols in the North China plain: the importance of aerosol size distribution in the prediction of CCN number concentration

    Directory of Open Access Journals (Sweden)

    Z. Z. Deng

    2011-01-01

    Full Text Available Size-resolved and bulk activation properties of aerosols were measured at a regional/suburban site in the North China Plain (NCP, which is occasionally heavily polluted by anthropogenic aerosol particles and gases. A CCN (Cloud Condensation Nuclei closure study is conducted with bulk CCN number concentration (NCCN and calculated NCCN based on the aerosol number size distribution and size-resolved activation properties.

    The observed NCCN are higher than those observed in other locations than China, with average NCCN of roughly 2000, 3000, 6000, 10 000 and 13 000 cm−3 at supersaturations of 0.056, 0.083, 0.17, 0.35 and 0.70%, respectively. An inferred critical dry diameter (Dm is calculated based on the measured NCCN and aerosol number size distribution assuming homogeneous chemical composition. This inferred cut off diameter varies in a wide range, indicating that it is impossible to predict NCCN with a fixed critical diameter.

    Size-resolved activation measurements show that most of the 300 nm particles are activated at the investigated supersaturations, while almost no particles of 30 nm are activated even at the highest supersaturation of 0.72%. The activation ratio increases with increasing supersaturation and particle size. The slopes of the activation curves for ambient aerosols are not as steep as those observed in calibrations with ammonium sulfate suggesting that the observed aerosols is an external mixture of more hygroscopic and hydrophobic particles. This conclusion is confirmed by hygroscopicity measurements performed during two intensive field studies in 2009.

    The calculated NCCN based on the size-resolved activation ratio and aerosol number size distribution correlate well with the measured NCCN, and show an average overestimation

  18. Aerosol Chemistry Resolved by Mass Spectrometry: Linking Field Measurements of Cloud Condensation Nuclei Activity to Organic Aerosol Composition.

    Science.gov (United States)

    Vogel, Alexander L; Schneider, Johannes; Müller-Tautges, Christina; Phillips, Gavin J; Pöhlker, Mira L; Rose, Diana; Zuth, Christoph; Makkonen, Ulla; Hakola, Hannele; Crowley, John N; Andreae, Meinrat O; Pöschl, Ulrich; Hoffmann, Thorsten

    2016-10-06

    Aerosol hygroscopic properties were linked to its chemical composition by using complementary online mass spectrometric techniques in a comprehensive chemical characterization study at a rural mountaintop station in central Germany in August 2012. In particular, atmospheric pressure chemical ionization mass spectrometry ((-)APCI-MS) provided measurements of organic acids, organosulfates, and nitrooxy-organosulfates in the particle phase at 1 min time resolution. Offline analysis of filter samples enabled us to determine the molecular composition of signals appearing in the online (-)APCI-MS spectra. Aerosol mass spectrometry (AMS) provided quantitative measurements of total submicrometer organics, nitrate, sulfate, and ammonium. Inorganic sulfate measurements were achieved by semionline ion chromatography and were compared to the AMS total sulfate mass. We found that up to 40% of the total sulfate mass fraction can be covalently bonded to organic molecules. This finding is supported by both on- and offline soft ionization techniques, which confirmed the presence of several organosulfates and nitrooxy-organosulfates in the particle phase. The chemical composition analysis was compared to hygroscopicity measurements derived from a cloud condensation nuclei counter. We observed that the hygroscopicity parameter (κ) that is derived from organic mass fractions determined by AMS measurements may overestimate the observed κ up to 0.2 if a high fraction of sulfate is bonded to organic molecules and little photochemical aging is exhibited.

  19. Consistency of aerosols above clouds characterization from A-Train active and passive measurements

    Science.gov (United States)

    Deaconu, Lucia T.; Waquet, Fabien; Josset, Damien; Ferlay, Nicolas; Peers, Fanny; Thieuleux, François; Ducos, Fabrice; Pascal, Nicolas; Tanré, Didier; Pelon, Jacques; Goloub, Philippe

    2017-09-01

    This study presents a comparison between the retrieval of optical properties of aerosol above clouds (AAC) from different techniques developed for the A-Train sensors CALIOP/CALIPSO and POLDER/PARASOL. The main objective is to analyse the consistency between the results derived from the active and the passive measurements. We compare the aerosol optical thickness (AOT) above optically thick clouds (cloud optical thickness (COT) larger than 3) and their Ångström exponent (AE). These parameters are retrieved with the CALIOP operational method, the POLDER operational polarization method and the CALIOP-based depolarization ratio method (DRM) - for which we also propose a calibrated version (denominated DRMSODA, where SODA is the Synergized Optical Depth of Aerosols). We analyse 6 months of data over three distinctive regions characterized by different types of aerosols and clouds. Additionally, for these regions, we select three case studies: a biomass-burning event over the South Atlantic Ocean, a Saharan dust case over the North Atlantic Ocean and a Siberian biomass-burning event over the North Pacific Ocean. Four and a half years of data are studied over the entire globe for distinct situations where aerosol and cloud layers are in contact or vertically separated. Overall, the regional analysis shows a good correlation between the POLDER and the DRMSODA AOTs when the microphysics of aerosols is dominated by fine-mode particles of biomass-burning aerosols from southern Africa (correlation coefficient (R2) of 0.83) or coarse-mode aerosols of Saharan dust (R2 of 0.82). A good correlation between these methods (R2 of 0.68) is also observed in the global treatment, when the aerosol and cloud layers are separated well. The analysis of detached layers also shows a mean difference in AOT of 0.07 at 532 nm between POLDER and DRMSODA at a global scale. The correlation between the retrievals decreases when a complex mixture of aerosols is expected (R2 of 0.37) - as in the

  20. Identification of columnar aerosol types under high aerosol optical depth conditions for a single AERONET site in Korea

    Science.gov (United States)

    Choi, Yongjoo; Ghim, Young Sung; Holben, B. N.

    2016-02-01

    Dominant aerosol types were classified using level 2 inversion products for the Anmyon Aerosol Robotic Network (AERONET) site in Korea for the period 1999-2007. The aerosol types were mineral dust (MD), MD mixed with carbon, and black carbon mixed coarse particles (BCCP) for coarse mode aerosols, black carbon (BC), organic carbon (OC), and secondary inorganic ions (SII) for fine mode aerosols, and mixed particles between. The classification was carried out using a clustering method based on parameters, including single scattering albedo (SSA), absorption Angstrom exponent (AAE), and fine mode volume fraction (FMVF). Among the seven aerosol types, MD was distinct, with the highest AAE and a very low FMVF and SII with the highest SSA and FMVF. BCCP was introduced to designate coarse particles mixed with BC, of which the AAE was lower than 1, despite a low FMVF. In addition to a large difference in AAE between BC and OC, the SSA of OC was larger than that of BC, indicating the effects of the white smoke produced from the smoldering phase of biomass burning. Monthly variations of the aerosol types were well interpreted by meteorology and emissions and coincided with those in the previous studies. Applying our results to well-characterized global AERONET sites, we confirmed that the aerosol types at Anmyon were valid at other sites. However, the results also showed that the mean properties for aerosol types were influenced by the specific aerosols prevalent at the study sites.

  1. Comparison of activity coefficient models for atmospheric aerosols containing mixtures of electrolytes, organics, and water

    Science.gov (United States)

    Tong, Chinghang; Clegg, Simon L.; Seinfeld, John H.

    Atmospheric aerosols generally comprise a mixture of electrolytes, organic compounds, and water. Determining the gas-particle distribution of volatile compounds, including water, requires equilibrium or mass transfer calculations, at the heart of which are models for the activity coefficients of the particle-phase components. We evaluate here the performance of four recent activity coefficient models developed for electrolyte/organic/water mixtures typical of atmospheric aerosols. Two of the models, the CSB model [Clegg, S.L., Seinfeld, J.H., Brimblecombe, P., 2001. Thermodynamic modelling of aqueous aerosols containing electrolytes and dissolved organic compounds. Journal of Aerosol Science 32, 713-738] and the aerosol diameter dependent equilibrium model (ADDEM) [Topping, D.O., McFiggans, G.B., Coe, H., 2005. A curved multi-component aerosol hygroscopicity model framework: part 2—including organic compounds. Atmospheric Chemistry and Physics 5, 1223-1242] treat ion-water and organic-water interactions but do not include ion-organic interactions; these can be referred to as "decoupled" models. The other two models, reparameterized Ming and Russell model 2005 [Raatikainen, T., Laaksonen, A., 2005. Application of several activity coefficient models to water-organic-electrolyte aerosols of atmospheric interest. Atmospheric Chemistry and Physics 5, 2475-2495] and X-UNIFAC.3 [Erdakos, G.B., Change, E.I., Pandow, J.F., Seinfeld, J.H., 2006. Prediction of activity coefficients in liquid aerosol particles containing organic compounds, dissolved inorganic salts, and water—Part 3: Organic compounds, water, and ionic constituents by consideration of short-, mid-, and long-range effects using X-UNIFAC.3. Atmospheric Environment 40, 6437-6452], include ion-organic interactions; these are referred to as "coupled" models. We address the question—Does the inclusion of a treatment of ion-organic interactions substantially improve the performance of the coupled models over

  2. CCN activity and hygroscopic growth of organic aerosols following reactive uptake of ammonia.

    Science.gov (United States)

    Dinar, E; Anttila, T; Rudich, Y

    2008-02-01

    Recent field observations suggest that ammonium salts of organic acids may be very important in accounting for aerosols' properties in many environments. In this study we present laboratory experiments and calculations on the influence of ammonia reaction with organic aerosol components and its effect upon their (1) subsaturation hygroscopic growth (HG) and (2) supersaturation cloud condensation nuclei (CCN) activity. By using adipic acid (slightly soluble), citric acid (soluble), and di(ethylene glycol) monovinyl ether (DEGMVE, nonacidic compound) aerosols we show the feasibility and importance of atmospherically relevant acid-base neutralization by ammonia for different organic species. It is suggested that the formation of ammonium salts due to reaction of ammonia with slightly soluble organic acids (such as adipic acid) can affect the CCN activity and hygroscopic growth of aerosols with a significant organic component. It is further confined that the reaction involves carboxylic groups, it requires presence of water in the aerosol, and that the effects are stronger for less soluble organic acids.

  3. The Influence of Aerosol Concentration on Changes in the Volumetric Activities of Indoor Radon Short-Term Decay Products

    Directory of Open Access Journals (Sweden)

    Diana Politova

    2011-02-01

    Full Text Available The article describes the influence of aerosol concentration on changes in the volumetric activities of indoor radon short-term decay products. The concentration of aerosol in the air, equilibrium factors and unattached fraction were measured under normal living conditions when the concentration of aerosol increases, i.e. burning a candle or frankincense in accommodations, smoke-filled accommodations, a steamy kitchen etc. It has been established that when the concentration of aerosol in the air rises, the number of free atoms of radon short-term decay products attached to aerosol particles also increases, and therefore higher volumetric activity of alpha particles is fixed. A tight positive connection of the correlation between equilibrium factor (F and aerosol particle concentration in the air of accommodations as well as a negative correlation between unattached fraction and an equilibrium factor have been determined.Article in Lithuanian

  4. Eddy covariance measurements with high-resolution time-of-flight aerosol mass spectrometry: a new approach to chemically-resolved aerosol fluxes

    Directory of Open Access Journals (Sweden)

    D. K. Farmer

    2010-12-01

    Full Text Available Although laboratory studies show that biogenic volatile organic compounds (VOCs yield substantial secondary organic aerosol (SOA, production of biogenic SOA as indicated by upward fluxes has not been conclusively observed over forests. Further, while aerosols are known to deposit to surfaces, few techniques exist to provide chemically-resolved particle deposition fluxes. To better constrain aerosol sources and sinks, we have developed a new technique to directly measure fluxes of chemically-resolved submicron aerosols using the high-resolution time-of-flight aerosol mass spectrometer (HR-AMS in a new, fast eddy covariance mode. This approach takes advantage of the instrument's ability to quantitatively identify both organic and inorganic components, including ammonium, sulphate and nitrate, at a temporal resolution of several Hz. The new approach has been successfully deployed over a temperate ponderosa pine plantation in California during the BEARPEX-2007 campaign, providing both total and chemically resolved non-refractory (NR PM1 fluxes. Average deposition velocity for total NR-PM1 aerosol at noon was 2.05 ± 0.04 mm/s. Using a high resolution measurement of the NH2+ and NH3+ fragments, we demonstrate the first eddy covariance flux measurements of particulate ammonium, which show a noon-time deposition velocity of 1.9 ± 0.7 mm/s and are dominated by deposition of ammonium sulphate.

  5. Absorbing aerosols at high relative humidity: linking hygroscopic growth to optical properties

    Directory of Open Access Journals (Sweden)

    J. Michel Flores

    2012-06-01

    Full Text Available One of the major uncertainties in the understanding of Earth's climate system is the interaction between solar radiation and aerosols in the atmosphere. Aerosols exposed to high humidity will change their chemical, physical, and optical properties due to their increased water content. To model hydrated aerosols, atmospheric chemistry and climate models often use the volume weighted mixing rule to predict the complex refractive index (RI of aerosols when they interact with high relative humidity, and, in general, assume homogeneous mixing. This study explores the validity of these assumptions. A humidified cavity ring down aerosol spectrometer (CRD-AS and a tandem hygroscopic DMA (differential mobility analyzer are used to measure the extinction coefficient and hygroscopic growth factors of humidified aerosols, respectively. The measurements are performed at 80% and 90%RH at wavelengths of 532 nm and 355 nm using size-selected aerosols with different degrees of absorption; from purely scattering to highly absorbing particles. The ratio of the humidified to the dry extinction coefficients (fRHext(%RH, Dry is measured and compared to theoretical calculations based on Mie theory. Using the measured hygroscopic growth factors and assuming homogeneous mixing, the expected RIs using the volume weighted mixing rule are compared to the RIs derived from the extinction measurements.

    We found a weak linear dependence or no dependence of fRH(%RH, Dry with size for hydrated absorbing aerosols in contrast to the non-monotonically decreasing behavior with size for purely scattering aerosols. No discernible difference could be made between the two wavelengths used. Less than 7% differences were found between the real parts of the complex refractive indices derived and those calculated using the volume weighted mixing rule, and the imaginary parts had up to a 20% difference. However, for substances with growth factor less than 1

  6. Consistency of aerosols above clouds characterization from A-Train active and passive measurements

    Directory of Open Access Journals (Sweden)

    L. T. Deaconu

    2017-09-01

    Full Text Available This study presents a comparison between the retrieval of optical properties of aerosol above clouds (AAC from different techniques developed for the A-Train sensors CALIOP/CALIPSO and POLDER/PARASOL. The main objective is to analyse the consistency between the results derived from the active and the passive measurements. We compare the aerosol optical thickness (AOT above optically thick clouds (cloud optical thickness (COT larger than 3 and their Ångström exponent (AE. These parameters are retrieved with the CALIOP operational method, the POLDER operational polarization method and the CALIOP-based depolarization ratio method (DRM – for which we also propose a calibrated version (denominated DRMSODA, where SODA is the Synergized Optical Depth of Aerosols. We analyse 6 months of data over three distinctive regions characterized by different types of aerosols and clouds. Additionally, for these regions, we select three case studies: a biomass-burning event over the South Atlantic Ocean, a Saharan dust case over the North Atlantic Ocean and a Siberian biomass-burning event over the North Pacific Ocean. Four and a half years of data are studied over the entire globe for distinct situations where aerosol and cloud layers are in contact or vertically separated. Overall, the regional analysis shows a good correlation between the POLDER and the DRMSODA AOTs when the microphysics of aerosols is dominated by fine-mode particles of biomass-burning aerosols from southern Africa (correlation coefficient (R2 of 0.83 or coarse-mode aerosols of Saharan dust (R2 of 0.82. A good correlation between these methods (R2 of 0.68 is also observed in the global treatment, when the aerosol and cloud layers are separated well. The analysis of detached layers also shows a mean difference in AOT of 0.07 at 532 nm between POLDER and DRMSODA at a global scale. The correlation between the retrievals decreases when a complex mixture of aerosols is expected (R2 of 0.37

  7. A new method to discriminate secondary organic aerosols from different sources using high-resolution aerosol mass spectra

    Science.gov (United States)

    Heringa, M. F.; Decarlo, P. F.; Chirico, R.; Tritscher, T.; Clairotte, M.; Mohr, C.; Crippa, M.; Slowik, J. G.; Pfaffenberger, L.; Dommen, J.; Weingartner, E.; Prévôt, A. S. H.; Baltensperger, U.

    2012-02-01

    Organic aerosol (OA) represents a significant and often major fraction of the non-refractory PM1 (particulate matter with an aerodynamic diameter da car and a two-stroke Euro 2 scooter were characterized with an Aerodyne high-resolution time-of-flight aerosol mass spectrometer (HR-TOF-AMS) and compared to SOA from α-pinene. The emissions were sampled from the chimney/tailpipe by a heated inlet system and filtered before injection into a smog chamber. The gas phase emissions were irradiated by xenon arc lamps to initiate photo-chemistry which led to nucleation and subsequent particle growth by SOA production. Duplicate experiments were performed for each SOA type, with the averaged organic mass spectra showing Pearson's r values >0.94 for the correlations between the four different SOA types after five hours of aging. High-resolution mass spectra (HR-MS) showed that the dominant peaks in the MS, m/z 43 and 44, are dominated by the oxygenated ions C2H3O+ and CO2+, respectively, similarly to the relatively fresh semi-volatile oxygenated OA (SV-OOA) observed in the ambient aerosol. The atomic O:C ratios were found to be in the range of 0.25-0.55 with no major increase during the first five hours of aging. On average, the diesel SOA showed the lowest O:C ratio followed by SOA from wood burning, α-pinene and the scooter emissions. Grouping the fragment ions revealed that the SOA source with the highest O:C ratio had the largest fraction of small ions. The HR data of the four sources could be clustered and separated using principal component analysis (PCA). The model showed a significant separation of the four SOA types and clustering of the duplicate experiments on the first two principal components (PCs), which explained 79% of the total variance. Projection of ambient SV-OOA spectra resolved by positive matrix factorization (PMF) showed that this approach could be useful to identify large contributions of the tested SOA sources to SV-OOA. The first results from this

  8. CCN activity and volatility of β-caryophyllene secondary organic aerosol

    DEFF Research Database (Denmark)

    Frosch, M.; Bilde, Merete; Nenes, A.

    2013-01-01

    In a series of smog chamber experiments, the cloud condensation nuclei (CCN) activity of secondary organic aerosol (SOA) generated from ozonolysis of beta-caryophyllene was characterized by determining the CCN derived hygroscopicity parameter, kappa(CCN), from experimental data. Two types of CCN...

  9. Laboratory Studies of Processing of Carbonaceous Aerosols by Atmospheric Oxidants/Hygroscopicity and CCN Activity of Secondary & Processed Primary Organic Aerosols

    Energy Technology Data Exchange (ETDEWEB)

    Ziemann, P.J.; Arey, J.; Atkinson, R.; Kreidenweis, S.M.; Petters, M.D.

    2012-06-13

    The atmosphere is composed of a complex mixture of gases and suspended microscopic aerosol particles. The ability of these particles to take up water (hygroscopicity) and to act as nuclei for cloud droplet formation significantly impacts aerosol light scattering and absorption, and cloud formation, thereby influencing air quality, visibility, and climate in important ways. A substantial, yet poorly characterized component of the atmospheric aerosol is organic matter. Its major sources are direct emissions from combustion processes, which are referred to as primary organic aerosol (POA), or in situ processes in which volatile organic compounds (VOCs) are oxidized in the atmosphere to low volatility reaction products that subsequent condense to form particles that are referred to as secondary organic aerosol (SOA). POA and VOCs are emitted to the atmosphere from both anthropogenic and natural (biogenic) sources. The overall goal of this experimental research project was to conduct laboratory studies under simulated atmospheric conditions to investigate the effects of the chemical composition of organic aerosol particles on their hygroscopicity and cloud condensation nucleation (CCN) activity, in order to develop quantitative relationships that could be used to more accurately incorporate aerosol-cloud interactions into regional and global atmospheric models. More specifically, the project aimed to determine the products, mechanisms, and rates of chemical reactions involved in the processing of organic aerosol particles by atmospheric oxidants and to investigate the relationships between the chemical composition of organic particles (as represented by molecule sizes and the specific functional groups that are present) and the hygroscopicity and CCN activity of oxidized POA and SOA formed from the oxidation of the major classes of anthropogenic and biogenic VOCs that are emitted to the atmosphere, as well as model hydrocarbons. The general approach for this project was

  10. Can we better use existing and emerging computing hardware to embed activity coefficient predictions in complex atmospheric aerosol models?

    Science.gov (United States)

    Topping, David; Alibay, Irfan; Ruske, Simon; Hindriksen, Vincent; Noisternig, Michael

    2016-04-01

    To predict the evolving concentration, chemical composition and ability of aerosol particles to act as cloud droplets, we rely on numerical modeling. Mechanistic models attempt to account for the movement of compounds between the gaseous and condensed phases at a molecular level. This 'bottom up' approach is designed to increase our fundamental understanding. However, such models rely on predicting the properties of molecules and subsequent mixtures. For partitioning between the gaseous and condensed phases this includes: saturation vapour pressures; Henrys law coefficients; activity coefficients; diffusion coefficients and reaction rates. Current gas phase chemical mechanisms predict the existence of potentially millions of individual species. Within a dynamic ensemble model, this can often be used as justification for neglecting computationally expensive process descriptions. Indeed, on whether we can quantify the true sensitivity to uncertainties in molecular properties, even at the single aerosol particle level it has been impossible to embed fully coupled representations of process level knowledge with all possible compounds, typically relying on heavily parameterised descriptions. Relying on emerging numerical frameworks, and designed for the changing landscape of high-performance computing (HPC), in this study we show that comprehensive microphysical models from single particle to larger scales can be developed to encompass a complete state-of-the-art knowledge of aerosol chemical and process diversity. We focus specifically on the ability to capture activity coefficients in liquid solutions using the UNIFAC method, profiling traditional coding strategies and those that exploit emerging hardware.

  11. Contributions of local sources, long-range and mountain wind transport for aerosols over an eastern Himalayan high-altitude station in India

    Science.gov (United States)

    Chatterjee, Abhijit; Sarkar, Chirantan; Singh, Ajay; Ghosh, Sanjay; Raha, Sibaji; Das, Sanat

    A long-term study (2010-2013) on aerosols mass concentrations (PM2.5), number concentrations of size segregated aerosols and mass concentration of total suspended black carbon aerosols has been made over Darjeeling (27.01 N, 88.15 E), a high altitude (2200 m asl) station at eastern Himalaya in India. Seasonal and diurnal variation of all types of aerosols, their chemical composition and source apportionment revealed that aerosols over this part of Himalaya are mainly of two types; locally generated and long-range transported aerosols. The diurnal variation of aerosols including black carbon showed distinct feature of up-slope mountain wind transport mainly during premonsoon (Mar-May) which brings aerosol particles from low land regions. This present study focuses on the estimation of the individual contributions from local emissions (LE), long-range transport (LRT) and mountain wind transport (MWT) towards the total aerosol loading over Darjeeling. Several strike events (called by local political party) were observed at Darjeeling over the entire period of study (2008-2013) when all the local activities (schools, colleges, offices, vehicular, industrial etc) were stopped fully. Most of the strike events occurred during premonsoon. We have observed three types of events during premonsoon over the entire study period; 1) strike events with the contribution of LRT+MWT with zero local emissions (LE=0), 2) normal days with the contribution of LE+LRT+MWT, 3) normal days with the contribution of LE+MWT with zero long-range contribution (LRT=0). On normal days, the diurnal variation of aerosols during premonsoon showed sharp morning and evening peaks associated to local anthropogenic activities with the effect of up-slope mountain wind during afternoon. During strike events, the morning and evening peaks were absent but a broad peak was observed during afternoon associated to up-slope mountain wind. The increase in aerosol concentrations during afternoon on strike days

  12. Evidence for a High Proportion of Atmospheric Organic Aerosol from Isoprene

    Science.gov (United States)

    Robinson, Niall H.; Hamilton, Jacqueline F.; Langford, Ben; Oram, David E.; Barley, Mark H.; Jenkin, Michael E.; Rickard, Andrew R.; Coe, Hugh; McFiggans, Gordon

    2010-05-01

    The tropics emit a huge amount of volatile organic compounds (VOCs) into the Earth's atmosphere. The processes by which these gases are oxidised to form secondary organic aerosol (SOA) are currently not well understood or quantified. Intensive field measurements were carried out as part of the Oxidant and Particle Photochemical Processes (OP3) and the Aerosol Coupling in the Earth System (ACES) projects around pristine rainforest in Malaysian Borneo. This is the first campaign of its type in a South East Asian rainforest. We present detailed organic aerosol composition measurements made using an Aerodyne High Resolution Time of Flight Aerosol Mass Spectrometer (HR-ToF-AMS) at Bukit Atur, a Global Atmosphere Watch site located in the Danum Valley Conservation Area. This is a state-of-the-art field deployable instrument that can provide real time composition, mass loading and aerodynamic particle sizing information. In addition, the mass spectral resolution is sufficient to perform an analysis of the elemental composition of the organic species present. Off line analysis of filter samples was performed using comprehensive two-dimensional gas chromatography coupled to time of flight mass spectrometry (GCxGC/ToFMS). This technique provides a more detailed chemical characterisation of the SOA, allowing direct links back to gas phase precursors. The ground site data are compared with Aerodyne Compact Time of Flight Aerosol Mass Spectrometer (C-ToF-AMS) measurements made on the UK Facility for Airborne Atmospheric Measurements (FAAM) BAe-146 research aircraft. Airborne measurements were made above pristine rainforest surrounding the Danum Valley site, as well as nearby oil palm agricultural sites and palm oil rendering plants. Proton Transfer Reaction Mass Spectrometry (PTRMS) measurements of VOCs were made at the ground site and from the FAAM aircraft. Novel organic aerosol was measured by both AMSs, and identified as being isoprenoid in origin by GCxGC/ToFMS analysis

  13. Connecting the solubility and CCN activation of complex organic aerosols: a theoretical study using solubility distributions

    Science.gov (United States)

    Riipinen, I.; Rastak, N.; Pandis, S. N.

    2015-06-01

    We present a theoretical study investigating the cloud activation of multicomponent organic particles. We modeled these complex mixtures using solubility distributions (analogous to volatility distributions in the VBS, i.e., volatility basis set, approach), describing the mixture as a set of surrogate compounds with varying water solubilities in a given range. We conducted Köhler theory calculations for 144 different mixtures with varying solubility range, number of components, assumption about the organic mixture thermodynamics and the shape of the solubility distribution, yielding approximately 6000 unique cloud condensation nucleus (CCN)-activation points. The results from these comprehensive calculations were compared to three simplifying assumptions about organic aerosol solubility: (1) complete dissolution at the point of activation; (2) combining the aerosol solubility with the molar mass and density into a single effective hygroscopicity parameter κ; and (3) assuming a fixed water-soluble fraction ϵeff. The complete dissolution was able to reproduce the activation points with a reasonable accuracy only when the majority (70-80%) of the material was dissolved at the point of activation. The single-parameter representations of complex mixture solubility were confirmed to be powerful semi-empirical tools for representing the CCN activation of organic aerosol, predicting the activation diameter within 10% in most of the studied supersaturations. Depending mostly on the condensed-phase interactions between the organic molecules, material with solubilities larger than about 0.1-100 g L-1 could be treated as soluble in the CCN activation process over atmospherically relevant particle dry diameters and supersaturations. Our results indicate that understanding the details of the solubility distribution in the range of 0.1-100 g L-1 is thus critical for capturing the CCN activation, while resolution outside this solubility range will probably not add

  14. Assessment of aerosol-cloud interactions during southern African biomass burning activity, employing cloud parameterizations

    Science.gov (United States)

    Wiston, Modise; McFiggans, Gordon; Schultz, David

    2015-04-01

    In this study, we perform a simulation of the spatial distributions of particle and gas concentrations from a significantly large source of pollution event during a dry season in southern Africa and their interactions with cloud processes. Specific focus is on the extent to which cloud-aerosol interactions are affected by various inputs (i.e. emissions) and parameterizations and feedback mechanisms in a coupled mesoscale chemistry-meteorology model -herein Weather Research and Forecasting model with chemistry (WRF-Chem). The southern African dry season (May-Sep) is characterised by biomass burning (BB) type of pollution. During this period, BB particles are frequently observed over the subcontinent, at the same time a persistent deck of stratocumulus covers the south West African coast, favouring long-range transport over the Atlantic Ocean of aerosols above clouds. While anthropogenic pollutants tend to spread more over the entire domain, biomass pollutants are concentrated around the burning areas, especially the savannah and tropical rainforest of the Congo Basin. BB is linked to agricultural practice at latitudes south of 10° N. During an intense burning event, there is a clear signal of strong interactions of aerosols and cloud microphysics. These species interfere with the radiative budget, and directly affect the amount of solar radiation reflected and scattered back to space and partly absorbed by the atmosphere. Aerosols also affect cloud microphysics by acting as cloud condensation nuclei (CCN), modifying precipitation pattern and the cloud albedo. Key area is to understand the role of pollution on convective cloud processes and its impacts on cloud dynamics. The hypothesis is that an environment of potentially high pollution enables the probability of interactions between co-located aerosols and cloud layers. To investigate this hypothesis, we outline an approach to integrate three elements: i) focusing on regime(s) where there are strong indications of

  15. A new method to discriminate secondary organic aerosols from different sources using high-resolution aerosol mass spectra

    Directory of Open Access Journals (Sweden)

    M. F. Heringa

    2012-02-01

    Full Text Available Organic aerosol (OA represents a significant and often major fraction of the non-refractory PM1 (particulate matter with an aerodynamic diameter da < 1 μm mass. Secondary organic aerosol (SOA is an important contributor to the OA and can be formed from biogenic and anthropogenic precursors. Here we present results from the characterization of SOA produced from the emissions of three different anthropogenic sources. SOA from a log wood burner, a Euro 2 diesel car and a two-stroke Euro 2 scooter were characterized with an Aerodyne high-resolution time-of-flight aerosol mass spectrometer (HR-TOF-AMS and compared to SOA from α-pinene.

    The emissions were sampled from the chimney/tailpipe by a heated inlet system and filtered before injection into a smog chamber. The gas phase emissions were irradiated by xenon arc lamps to initiate photo-chemistry which led to nucleation and subsequent particle growth by SOA production.

    Duplicate experiments were performed for each SOA type, with the averaged organic mass spectra showing Pearson's r values >0.94 for the correlations between the four different SOA types after five hours of aging. High-resolution mass spectra (HR-MS showed that the dominant peaks in the MS, m/z 43 and 44, are dominated by the oxygenated ions C2H3O+ and CO2+, respectively, similarly to the relatively fresh semi-volatile oxygenated OA (SV-OOA observed in the ambient aerosol. The atomic O:C ratios were found to be in the range of 0.25–0.55 with no major increase during the first five hours of aging. On average, the diesel SOA showed the lowest O:C ratio followed by SOA from wood burning, α-pinene and the scooter emissions. Grouping the fragment ions revealed that the SOA source with the highest O:C ratio had the largest fraction of small ions.

    The HR data of the four sources could be clustered and separated using

  16. A new method to discriminate secondary organic aerosols from different sources using high-resolution aerosol mass spectra

    Directory of Open Access Journals (Sweden)

    M. F. Heringa

    2011-10-01

    Full Text Available Organic aerosol (OA represents a significant and often major fraction of the non-refractory PM1 (particulate matter with an aerodynamic diameter da < 1 μm mass. Secondary organic aerosol (SOA is an important contributor to the OA and can be formed from biogenic and anthropogenic precursors. Here we present results from the characterization of SOA produced from the emissions of three different anthropogenic sources. SOA from a log wood burner, a Euro 2 diesel car and a two-stroke Euro 2 scooter were characterized with an Aerodyne high-resolution time-of-flight aerosol mass spectrometer (HR-TOF-AMS and compared to SOA from α-pinene.

    The emissions were sampled from the chimney/tailpipe by a heated inlet system and filtered before injection into a smog chamber. The gas phase emissions were irradiated by xenon arc lamps to initiate photo-chemistry which led to nucleation and subsequent particle growth by SOA production.

    Duplicate experiments were performed for each SOA type, with the averaged organic mass spectra in the m/z range 12–250 showing Pearson's r values >0.94 for the correlations between the different SOA types after 5 h of aging. High-resolution mass spectra (HR-MS showed that the dominant peaks in the MS, m/z 43 and 44, are dominated by the oxygenated ions C2H3O+ and CO2+, respectively, similarly to the relatively fresh semi-volatile oxidized OA (SV-OOA observed in the ambient aerosol. The atomic O : C ratios were found to be in the range of 0.25–0.55 with no major increase during the first 5 h of aging. On average, the diesel SOA showed the lowest O : C ratio followed by SOA from wood burning, α-pinene and the scooter emissions. Grouping the fragment ions based on their carbon number revealed that the SOA source with the highest O : C ratio had the largest fraction of small ions. Fragment ions

  17. Comparison of high order algorithms in Aerosol and Aghora for compressible flows

    Directory of Open Access Journals (Sweden)

    Mbengoue D. A.

    2013-12-01

    Full Text Available This article summarizes the work done within the Colargol project during CEMRACS 2012. The aim of this project is to compare the implementations of high order finite element methods for compressible flows that have been developed at ONERA and at INRIA for about one year, within the Aghora and Aerosol libraries.

  18. Hygroscopicity of aerosol particles and CCN activity of nearly hydrophobic particles in the urban atmosphere over Japan during summer

    Science.gov (United States)

    Ogawa, Shuhei; Setoguchi, Yoshitaka; Kawana, Kaori; Nakayama, Tomoki; Ikeda, Yuka; Sawada, Yuuki; Matsumi, Yutaka; Mochida, Michihiro

    2016-06-01

    We investigated the hygroscopicity of 150 nm particles and the number-size distributions and the cloud condensation nuclei (CCN) activity of nearly hydrophobic particles in aerosols over Nagoya, Japan, during summer. We analyzed the correlations between the number concentrations of particles in specific hygroscopic growth factor (g) ranges and the mass concentrations of chemical components. This analysis suggests the association of nearly hydrophobic particles with hydrocarbon-like organic aerosol, elemental carbon and semivolatile oxygenated organic aerosol (SV-OOA), that of less hygroscopic particles with SV-OOA and nitrate and that of more hygroscopic particles with low-volatile oxygenated organic aerosol (LV-OOA) and sulfate. The hygroscopicity parameter (κ) of organics was derived based on the g distributions and chemical composition of 150 nm particles. The κ of the organics correlated positively with the fraction of the total organic mass spectral signal at m/z 44 and the volume fraction of the LV-OOA to the organics, indicating that organics with highly oxygenated structures including carboxylic acid groups contribute to the water uptake. The number-size distributions of the nearly hydrophobic particles with g around 1.0 and 1.1 correlated with the mass concentrations of chemical components. The results show that the chemical composition of the particles with g around 1.0 was different between the Aitken mode and the accumulation mode size ranges. An analysis for a parameter Fmax of the curves fitted to the CCN efficiency spectra of the particles with g around 1.0 suggests that the coating by organics associated with SV-OOA elevated the CCN activity of these particles.

  19. Preparation of active layers in polymer solar cells by aerosol jet printing.

    Science.gov (United States)

    Yang, Chunhe; Zhou, Erjun; Miyanishi, Shoji; Hashimoto, Kazuhito; Tajima, Keisuke

    2011-10-01

    Active layers of polymer solar cells were prepared by aerosol jet printing of organic inks. Various solvents and additives with high boiling points were screened for the preparation of high-quality polymer films. The effects on device performance of treating the films by thermal and solvent vapor annealing were also investigated. The components of the solvent were important for controlling the drying rate of the liquid films, reducing the number of particle-like protrusions on the film surface, and realizing high molecular ordering in the polymer phases. The optimized solar cell device with poly(3-hexylthiophene) and a C(60) derivative showed a high fill factor of 67% and power conversion efficiency of 2.53% without thermal annealing. The combination of poly[N-9-heptadecanyl-2,7-carbazole-alt-3,6-bis(thiophen-5-yl)-2,5-diethylhexyl-2,5-dihydropyrrolo-[3,4-]pyrrole-1,4-dione] and a C(70) derivative led to power conversion efficiency of 3.92 and 3.14% for device areas of 0.03 and 1 cm(2), respectively.

  20. Characterization of high-resolution aerosol mass spectra of primary organic aerosol emissions from Chinese cooking and biomass burning

    Directory of Open Access Journals (Sweden)

    L.-Y. He

    2010-09-01

    Full Text Available Aerosol Mass Spectrometer (AMS has proved to be a powerful tool to measure submicron particulate composition with high time resolution. Factor analysis of mass spectra (MS collected worldwide by AMS demonstrates that submicron organic aerosol (OA is usually composed of several major components, such as oxygenated (OOA, hydrocarbon-like (HOA, biomass burning (BBOA, and other primary OA. In order to help interpretation of component MS from factor analysis of ambient OA datasets, AMS measurement of different primary sources is required for comparison. Such work, however, has been very scarce in the literature, especially for high resolution MS (HR-MS measurement, which performs improved characterization by separating the ions of different elemental compositions at each m/z in comparison with unit mass resolution MS (UMR-MS measurement. In this study, primary emissions from four types of Chinese cooking (CC and six types of biomass burning (BB were simulated systemically and measured using an Aerodyne High-Resolution Time-of-Flight AMS (HR-ToF-AMS. The MS of the CC emissions show high similarity with m/z 41 and m/z 55 being the highest signals; the MS of the BB emissions also show high similarity with m/z 29 and m/z 43 being the highest signals. The MS difference between the CC and BB emissions is much bigger than that between different CC (or BB types, especially for the HR-MS. The O/C ratio of OA ranges from 0.08 to 0.13 for the CC emissions while from 0.18 to 0.26 for the BB emissions. The ions of m/z 43, m/z 44, m/z 57, and m/z 60, usually used as tracer ions in AMS measurement, were examined for their HR-MS characteristics in the CC and BB emissions. Moreover, the MS of the CC and BB emissions are also used to compare with component MS from factor analysis of ambient OA datasets observed in China, as well as with other AMS measurements of primary sources in the literature. The MS

  1. South African night sky brightness during high aerosol epochs

    CERN Document Server

    Winkler, Hartmut; Marang, Fred

    2014-01-01

    Sky conditions in the remote, dry north-western interior of South Africa are now the subject of considerable interest in view of the imminent construction of numerous solar power plants in this area. Furthermore, the part of this region in which the core of the SKA is to be located (which includes SALT) has been declared an Astronomical Advantage Zone, for which sky brightness monitoring will now be mandatory. In this project we seek to characterise the sky brightness profile under a variety of atmospheric conditions. Key factors are of course the lunar phase and altitude, but in addition the sky brightness is also significantly affected by the atmospheric aerosol loading, as that influences light beam scattering. In this paper we chose to investigate the sky characteristics soon after the Mount Pinatubo volcanic eruption in 1991, which resulted in huge ash masses reaching the stratosphere (where they affected solar irradiance for several years). We re-reduced photometric sky measurements from the South Afric...

  2. Activity Concentration Monitoring for Alpha Radioactive Aerosol in CRARL after Reprocessing Experiments

    Institute of Scientific and Technical Information of China (English)

    WANG; Xiang-li; LIU; Ning; WANG; Xiao-rong; BAI; Yang; JIAO; Xiao-yan; XU; Xin; MA; Hao-ran

    2015-01-01

    The activity concentration for alpha radioactive aerosol in CRARL after reprocessing experiments was analyzed.Through the decay method of activity concentration monitoring,the processed result shows the background is 3.05×10-3 s-1,σ(0)=2.25×10-3,LC=2.33×10-3 Bq/m3,LD=4.66×10-3 Bq/m3.The result indicated

  3. Research Note Difference between low-volume and high-volume Andersen samplers in measuring atmospheric aerosols

    Institute of Scientific and Technical Information of China (English)

    Fengfu Fu; Nobuo Shinohaya; Mitsuo Ito; Xueqin Xu; Mincong Shen; Liangjun Xu

    2008-01-01

    The mass concentration and size distribution of aerosols in Tokaimura were investigated using a high-volume and a low-volume Andersen sampler. A difference was found using the two samplers: the concentration of total aerosols determined with the high-volume sampler is smaller than that of the low-volume sampler by 70-90% throughout the year. Compared to the high-volume sampler, low-volume sampler gave lower concentration for aerosols7μm, higher concentration for aerosols of 3.3-7.0μm and<1.1μm, though similar results for aerosols of 1.1-3.3μm. The low-volume sampler was found to have better separation efficiency and higher accuracy.

  4. Aerosol composition and sources during high and low pollution periods in Ningbo, China

    Science.gov (United States)

    Xu, Jing-Sha; Xu, Hong-Hui; Xiao, Hang; Tong, Lei; Snape, Colin E.; Wang, Cheng-Jun; He, Jun

    2016-09-01

    Due to the rapid industrialization of the Yangtze River Delta (YRD) region in China, heavy air pollution episodes have occurred frequently over the past five years which are of great concern due to their environmental and health impacts. To investigate the chemical characteristics of the highly polluted aerosols in this region, a sampling campaign had been conducted in Ningbo from 3 December 2012 to 27 June 2013, during which a month long high pollution episode had been captured. Daily average PM2.5 concentrations during high and low pollution periods were 111 μg m-3 and 53 μg m-3, respectively. The most polluted day was 8 January 2013 with a PM2.5 concentration up to 175 μg m- 3. To understand the origin of the highly polluted aerosols, meteorological conditions, air mass backward trajectories, distribution of fire spots in surrounding areas and various categories of aerosol pollutants were analyzed, including trace metals, inorganic species, PAHs and anhydrosugars. Total metal concentrations were 3.8 and 1.6 μg m-3 for the high and low pollution episodes, respectively, accounting for 3.4% and 3.1% of the total PM2.5 mass. Total concentrations of ionic species accounted for more than 50.0% of the PM2.5 by mass, with dominant ions (nitrate, sulfate, ammonium) accounting for over 42.0% of the PM2.5 mass concentrations in both periods. During the high pollution episode, enhanced Cd-Pb and biomarker (levoglucosan, mannosan) levels indicated the contributions from coal combustion, traffic and biomass burning to fine aerosol PM2.5. The average diagnostic ratio of Fla/(Fla + Pyr) was 0.54 in high pollution episode, which was intermediate between that for wood (> 0.50) and coal combustion (0.58). BaP/Bpe was 0.49 and 0.30 for the highly and lightly polluted aerosols respectively, associated with the significant non-traffic emissions (pollution period and long-range transport of air masses from heavy industries and biomass burning from northern China to Ningbo could be

  5. Survival and ice nucleation activity of bacteria as aerosols in a cloud simulation chamber

    Directory of Open Access Journals (Sweden)

    P. Amato

    2015-02-01

    Full Text Available The residence time of bacterial cells in the atmosphere is predictable by numerical models. However, estimations of their aerial dispersion as living entities are limited by lacks of information concerning survival rates and behavior in relation to atmospheric water. Here we investigate the viability and ice nucleation (IN activity of typical atmospheric ice nucleation active bacteria (Pseudomonas syringae and P. fluorescens when airborne in a cloud simulation chamber (AIDA, Karlsruhe, Germany. Cell suspensions were sprayed into the chamber and aerosol samples were collected by impingement at designated times over a total duration of up to 18 h, and at some occasions after dissipation of a cloud formed by depressurization. Aerosol concentration was monitored simultaneously by online instruments. The cultivability of airborne cells decreased exponentially over time with a half-life time of 250 ± 30 min (about 3.5 to 4.5 h. In contrast, IN activity remained unchanged for several hours after aerosolization, demonstrating that IN activity was maintained after cell death. Interestingly, the relative abundance of IN active cells still airborne in the chamber was strongly decreased after cloud formation and dissipation. This illustrates the preferential precipitation of IN active cells by wet processes. Our results indicate that from 106 = cells aerosolized from a surface, one would survive the average duration of its atmospheric journey estimated at 3.4 days. Statistically, this corresponds to the emission of 1 cell that achieves dissemination every ~33 min per m2 of cultivated crops fields, a strong source of airborne bacteria. Based on the observed survival rates, depending on wind speed, the trajectory endpoint could be situated several hundreds to thousands of kilometers from the emission source. These results should improve the representation of the aerial dissemination of bacteria in numeric models.

  6. Size-resolved and bulk activation properties of aerosols in the North China Plain

    Directory of Open Access Journals (Sweden)

    Z. Z. Deng

    2011-04-01

    Full Text Available Size-resolved and bulk activation properties of aerosols were measured at a regional/suburban site in the North China Plain (NCP, which is occasionally heavily polluted by anthropogenic aerosol particles and gases. A Cloud Condensation Nuclei (CCN closure study is conducted with bulk CCN number concentration (NCCN and calculated CCN number concentration based on the aerosol number size distribution and size-resolved activation properties.

    The observed CCN number concentration (NCCN-obs are higher than those observed in other locations than China, with average NCCN-obs of roughly 2000, 3000, 6000, 10 000 and 13 000 cm−3 at supersaturations of 0.056, 0.083, 0.17, 0.35 and 0.70%, respectively. An inferred critical dry diameter (Dm is calculated based on the NCCN-obs and aerosol number size distribution assuming homogeneous chemical composition. The inferred cut-off diameters are in the ranges of 190–280, 160–260, 95–180, 65–120 and 50–100 nm at supersaturations of 0.056, 0.083, 0.17, 0.35 and 0.7%, with their mean values 230.1, 198.4, 128.4, 86.4 and 69.2 nm, respectively.

    Size-resolved activation measurements show that most of the 300 nm particles are activated at the investigated supersaturations, while almost no particles of 30 nm are activated even at the highest supersaturation of 0.72%. The activation ratio increases with increasing supersaturation and particle size. The slopes of the activation curves for ambient aerosols are not as steep as those observed in calibrations with ammonium sulfate suggesting that the observed aerosols is an external mixture of more hygroscopic and hydrophobic particles.

    The calculated CCN number concentrations (NCCN-calc based on the size-resolved activation ratio and aerosol number size distribution correlate well with the NCCN-obs, and

  7. Characterization of the sources and processes of organic and inorganic aerosols in New York City with a high-resolution time-of-flight aerosol mass spectrometer

    Directory of Open Access Journals (Sweden)

    Y.-L. Sun

    2010-10-01

    cooking emissions and a distinct diurnal pattern peaking around local lunch and dinner times. In addition, NOA is characterized with prominent CxH2x+2N+ peaks likely from amine compounds. Our results indicate that cooking-related activities are a major source of POA in NYC, releasing comparable amounts of POA as traffic emissions. POA=HOA+COA on average accounts for ~30% of the total OA mass during this study while SOA dominates the OA composition with SV-OOA and LV-OOA on average accounting for 34% and 30%, respectively, of the total OA mass. The chemical evolution of SOA in NYC involves a~continuous oxidation from SV-OOA to LV-OOA, which is further supported by a gradual increase of O/C ratio and a simultaneous decrease of H/C ratio in total OOA. Detailed analysis of NOA (5.8% of OA presents evidence that nitrogen-containing organic species such as amines might have played an important role in the atmospheric processing of OA in NYC, likely involving acid-base chemistry. Analysis of air mass trajectories and satellite imagery of aerosol optical depth (AOD indicates that the high potential source regions of secondary sulfate and aged OA are mainly located in regions to the west and southwest of the city.

  8. Aerosol mixingstate, hygroscopic growth and cloud activation efficiency during MIRAGE 2006

    Energy Technology Data Exchange (ETDEWEB)

    Lance, Sara; Raatikainen, T.; Onasch, Timothy B.; Worsnop, Douglas R.; Yu, Xiao-Ying; Alexander, M. L.; Stolzenberg, Mark; McMurry, Peter; Smith, James N.; Nenes, Athanasios

    2013-05-15

    Observations of aerosol hygroscopic growth and CCN activation spectra for submicron particles are reported for the T1 ground site outside of Mexico City during the MIRAGE 2006 campaign. K¨ohler theory is used to evaluate the characteristic water uptake coefficient, k*, for the CCN active aerosol population using both size-resolved HTMDA and size-resolved CCNc measurements. Organic mass fractions, (forg), are evaluated from size-resolved aerosol mass spectrometer (AMS) measurements, from which kAMS is inferred and compared against k*. Strong diurnal profiles of aerosol water uptake parameters and aerosol composition are observed. We find that new particle formation (NPF) events are correlated with an increased k* and CCN-active fraction during the daytime, with greater impact on smaller particles. During NPF events, the number concentration of 40 nm particles acting as CCN can surpass by more than a factor of two the concentrations of 100 nm particles acting as CCN, at supersaturations of 0.51% +/- 0.06%. We also find that at 0600-0800 in the morning throughout the campaign, fresh traffic emissions result in substantial changes to the chemical distribution of the aerosol, with on average 65% externally-mixed fraction for 40 nm particles and 30% externally-mixed fraction for 100 nm particles, whereas at midday nearly all particles of both sizes can be described as “internally-mixed”. Average activation spectra and growth factor distributions are analyzed for different time periods characterizing the daytime (with and without NPF events), the early morning “rush hour”, and the entire campaign. We show that k* derived from CCNc measurements decreases as a function of size during all time periods, while the CCN-active fraction increases as a function of size. Size-resolved AMS measurements do not predict the observed trend for k* versus particle size, which can be attributed to unresolved mixing-state and the presence of refractory material not measured by the

  9. Incorporation of Advanced Activation Treatments into CESM/CAM5: Model Evaluation and Impacts on Aerosol Indirect Forcing

    Science.gov (United States)

    Gantt, B.; He, J.; Zhang, X.; Zhang, Y.; Nenes, A.

    2013-12-01

    One of the greatest sources of uncertainty in climate science is the influence of aerosols on clouds through indirect effects, especially processes affecting the activation of aerosols into cloud droplets. Aerosol activation parameterizations incorporate much of the complexity of these processes, but the small differences between parameterizations can have a large impact on the spatiotemporal distribution of activated aerosols and the resulting cloud properties. Currently, most models simulate aerosol activation using the Abdul-Razzak and Ghan [2000] (AR-G00) scheme which derives an empiric calculation of the maximum parcel supersaturation based on the regression of numerical parcel calculations. The Community Atmosphere Model version 5.1.1 within the Community Earth Systems Model version 1.0.5 (CESM/CAM5) is an online-coupled Earth Systems model that simulates the interactions among aerosols, clouds, and radiation. CESM/CAM5 uses the AR-G00 scheme to simulate aerosol activation. In this work, we update CESM/CAM5 by incorporating a series of explicit aerosol activation schemes (Fountoukis and Nenes [2005]; Barahona and Nenes [2007]; Kumar et al. [2009]; and Barahona et al. [2010]) which account for the impacts of insoluble aerosol adsorption, giant cloud condensation nuclei activation kinetics, and entrainment on cloud droplet number concentrations (CDNC). CESM/CAM5 results with the empiric and explicit aerosol activation schemes are evaluated against several global datasets including observed low-level CDNC and satellite-derived cloud optical thickness (COT), liquid water path (LWP), and shortwave cloud forcing (SWCF). Globally, the incorporation of all explicit schemes leads to an average increase in column CDNC of 155%, increase (more negative) in SWCF of 13%, and decrease in surface shortwave radiation of -4%. In terms of climate impacts, these schemes result in an annual mean decrease in surface temperature and precipitation of -0.9 K (~0.2%) and -0.04 mm day

  10. High formation of secondary organic aerosol from the photo-oxidation of toluene

    Directory of Open Access Journals (Sweden)

    L. Hildebrandt

    2009-01-01

    Full Text Available Toluene and other aromatics have long been viewed as the dominant anthropogenic secondary organic aerosol (SOA precursors, but the SOA mass yields from toluene reported in previous studies vary widely. Experiments conducted in the Carnegie Mellon University environmental chamber to study SOA formation from the photo-oxidation of toluene show significantly larger SOA production than parameterizations employed in current air-quality models. Aerosol mass yields depend on experimental conditions: yields are higher under higher UV intensity, under low-NOx conditions and at lower temperatures. The extent of oxidation of the aerosol also varies with experimental conditions, consistent with ongoing, progressive photochemical aging of the toluene SOA. Measurements using a thermodenuder system suggest that the aerosol formed under high- and low-NOx conditions is semi-volatile. These results suggest that SOA formation from toluene depends strongly on ambient conditions. An approximate parameterization is proposed for use in air-quality models until a more thorough treatment accounting for the dynamic nature of this system becomes available.

  11. High formation of secondary organic aerosol from the photo-oxidation of toluene

    Directory of Open Access Journals (Sweden)

    L. Hildebrandt

    2009-05-01

    Full Text Available Toluene and other aromatics have long been viewed as the dominant anthropogenic secondary organic aerosol (SOA precursors, but the SOA mass yields from toluene reported in previous studies vary widely. Experiments conducted in the Carnegie Mellon University environmental chamber to study SOA formation from the photo-oxidation of toluene show significantly larger SOA production than parameterizations employed in current air-quality models. Aerosol mass yields depend on experimental conditions: yields are higher under higher UV intensity, under low-NOx conditions and at lower temperatures. The extent of oxidation of the aerosol also varies with experimental conditions, consistent with ongoing, progressive photochemical aging of the toluene SOA. Measurements using a thermodenuder system suggest that the aerosol formed under high- and low-NOx conditions is semi-volatile. These results suggest that SOA formation from toluene depends strongly on ambient conditions. An approximate parameterization is proposed for use in air-quality models until a more thorough treatment accounting for the dynamic nature of this system becomes available.

  12. Manipulating API and AOD data to distinguish transportation of aerosol at high altitude in Penang, Malaysia

    Science.gov (United States)

    Tan, F.; Lim, H. S.; Abdullah, K.; Yoon, T. L.; Matjafri, M. Z.; Holben, B.

    2014-02-01

    Air pollution index (API) is an index commonly used in Malaysia to determine the air quality level. It is a ground truth data measurement which is unable to unambiguously quantify air quality level at higher atmosphere. On the other hand, aerosol optical depth (AOD) from AERONET data obtained using sun photometer provides reading of the air quality for a column of atmosphere from ground surface. We first determine the quantitative correlation between the API and AOD data collected in Penang, Malaysia, between January - September, 2012, using two independent methods, one based on regression analysis and the other interpolation. Our purpose is to establish a systematic numerical procedure to determine whether aerosol transported in high altitude from other location has occurred. Two independent methods for establishing the quantitative relationship between the API and AOD data were used as a way to facilitate the verification of our approach. In our method, data from southwest monsoon period (August to September) were used as "calibration dataset" to establish the quantitative correlation between the AOD and API data. The established calibrated coefficients is then used to predict the AOD of other months, which are then compared against the data actually measured. Discrepancy between the predicted and measured AOD data can then be interpreted as an indication of whether the atmosphere at high altitude is polluted by aerosol transported from other location. If the predicted AOD is much larger than that measured, back trajectory analysis was applied to identify the aerosol transported source. This procedure is very helpful to investigate the aerosol transportation and distribution patterns during monsoon and non monsoon periods.

  13. Size-resolved morphological properties of the high Arctic summer aerosol during ASCOS-2008

    Science.gov (United States)

    Hamacher-Barth, Evelyne; Leck, Caroline; Jansson, Kjell

    2016-05-01

    The representation of aerosol properties and processes in climate models is fraught with large uncertainties. Especially at high northern latitudes a strong underprediction of aerosol concentrations and nucleation events is observed and can only be constrained by in situ observations based on the analysis of individual aerosol particles. To further reduce the uncertainties surrounding aerosol properties and their potential role as cloud condensation nuclei this study provides observational data resolved over size on morphological and chemical properties of aerosol particles collected in the summer high Arctic, north of 80° N. Aerosol particles were imaged with scanning and transmission electron microscopy and further evaluated with digital image analysis. In total, 3909 aerosol particles were imaged and categorized according to morphological similarities into three gross morphological groups: single particles, gel particles, and halo particles. Single particles were observed between 15 and 800 nm in diameter and represent the dominating type of particles (82 %). The majority of particles appeared to be marine gels with a broad Aitken mode peaking at 70 nm and accompanied by a minor fraction of ammonium (bi)sulfate with a maximum at 170 nm in number concentration. Gel particles (11 % of all particles) were observed between 45 and 800 nm with a maximum at 154 nm in diameter. Imaging with transmission electron microscopy allowed further morphological discrimination of gel particles in "aggregate" particles, "aggregate with film" particles, and "mucus-like" particles. Halo particles were observed above 75 nm and appeared to be ammonium (bi)sulfate (59 % of halo particles), gel matter (19 %), or decomposed gel matter (22 %), which were internally mixed with sulfuric acid, methane sulfonic acid, or ammonium (bi)sulfate with a maximum at 161 nm in diameter. Elemental dispersive X-ray spectroscopy analysis of individual particles revealed a prevalence of the monovalent

  14. Composition, size and cloud condensation nuclei activity of biomass burning aerosol from northern Australian savannah fires

    Science.gov (United States)

    Mallet, Marc D.; Cravigan, Luke T.; Milic, Andelija; Alroe, Joel; Ristovski, Zoran D.; Ward, Jason; Keywood, Melita; Williams, Leah R.; Selleck, Paul; Miljevic, Branka

    2017-03-01

    The vast majority of Australia's fires occur in the tropical north of the continent during the dry season. These fires are a significant source of aerosol and cloud condensation nuclei (CCN) in the region, providing a unique opportunity to investigate the biomass burning aerosol (BBA) in the absence of other sources. CCN concentrations at 0.5 % supersaturation and aerosol size and chemical properties were measured at the Australian Tropical Atmospheric Research Station (ATARS) during June 2014. CCN concentrations reached over 104 cm-3 when frequent and close fires were burning - up to 45 times higher than periods with no fires. Both the size distribution and composition of BBA appeared to significantly influence CCN concentrations. A distinct diurnal trend in the proportion of BBA activating to cloud droplets was observed, with an activation ratio of 40 ± 20 % during the night and 60 ± 20 % during the day. BBA was, on average, less hygroscopic during the night (κ = 0. 04 ± 0.03) than during the day (κ = 0.07 ± 0.05), with a maximum typically observed just before midday. Size-resolved composition of BBA showed that organics comprised a constant 90 % of the aerosol volume for aerodynamic diameters between 100 and 200 nm. While this suggests that the photochemical oxidation of organics led to an increase in the hygroscopic growth and an increase in daytime activation ratios, it does not explain the decrease in hygroscopicity after midday. Modelled CCN concentrations assuming typical continental hygroscopicities produced very large overestimations of up to 200 %. Smaller, but still significant, overpredictions up to ˜ 100 % were observed using aerosol mass spectrometer (AMS)- and hygroscopicity tandem differential mobility analyser (H-TDMA)-derived hygroscopicities as well as campaign night and day averages. The largest estimations in every case occurred during the night, when the small variations in very weakly hygroscopic species corresponded to large

  15. Enhancing non-refractory aerosol apportionment from an urban industrial site through receptor modelling of complete high time-resolution aerosol mass spectra

    Directory of Open Access Journals (Sweden)

    M. L. McGuire

    2014-02-01

    the ability to better understand the chemical nature of atypical factors from high resolution mass spectra. Second, utilizing PMF to extract factors containing inorganic species allowed for the determination of extent of neutralization, which could have implications for aerosol parameterization. Third, subtler differences in organic aerosol components were resolved through the incorporation of inorganic mass into the PMF matrix. The additional temporal features provided by the inorganic aerosol components allowed for the resolution of more types of oxygenated organic aerosol than could be reliably resolved from PMF of organics alone. Comparison of findings from the PMFFull MS and PMFOrg MS methods showed that for the Windsor airshed, the PMFFull MS method enabled additional conclusions to be drawn in terms of aerosol sources and chemical processes. While performing PMFOrg MS can provide important distinctions between types of organic aerosol, it is shown that including inorganic species in the PMF analysis can permit further apportionment of organics for unit mass resolution AMS mass spectra.

  16. On the impacts of phytoplankton-derived organic matter on the properties of the primary marine aerosol – Part 2: Composition, hygroscopicity and cloud condensation activity

    Directory of Open Access Journals (Sweden)

    E. Fuentes

    2011-03-01

    Full Text Available The effect of nanogel colloidal and dissolved organic matter <0.2 μm, secreted by marine biota, on the hygroscopic growth and droplet activation behaviour of the primary marine aerosol was studied. Seawater proxies were prepared by the combination of artificial seawater devoid of marine organics and natural seawater enriched in organic exudate released by laboratory-grown phytoplankton cultures, as described in a companion paper. The primary aerosol was produced by bubble bursting, using a plunging multijet system as an aerosol generator.

    The aerosol generated from seawater proxies enriched with marine exudate presented organic volume fractions on the order of 8–37%, as derived by applying a simple mixing rule. The hygroscopic growth and cloud condensation nuclei (CCN activity of the marine organics-enriched particles where 9–17% and 5–24% lower, respectively, than those of the aerosol produced from artificial seawater devoid of exudate. Experiments in a companion paper indicated that the cloud nuclei formation could be enhanced in diatom bloom areas because of the increase in the primary particle production induced by marine organics. The experiments in the present study, however, indicate that the impacts of such an enhancement would be counteracted by the reduction in the CCN activity of the primary particles enriched in marine organics.

    The extent of the effect of the biogenic matter on the particle behaviour was dependent on the seawater organic concentration and type of algal exudate. Aerosol produced from seawater proxies containing diatomaceous exudate presented higher hydrophobicity and lower CCN activity than those enriched with nanoplankton exudate. The organic fraction of the particles was found to correlate with the seawater organic concentration, without observing saturation of the particle organic mass fraction even for unrealistically high organic matter concentration in seawater. These findings are

  17. Eddy covariance measurements with high-resolution time-of-flight aerosol mass spectrometry: a new approach to chemically resolved aerosol fluxes

    Directory of Open Access Journals (Sweden)

    D. K. Farmer

    2011-06-01

    Full Text Available Although laboratory studies show that biogenic volatile organic compounds (VOCs yield substantial secondary organic aerosol (SOA, production of biogenic SOA as indicated by upward fluxes has not been conclusively observed over forests. Further, while aerosols are known to deposit to surfaces, few techniques exist to provide chemically-resolved particle deposition fluxes. To better constrain aerosol sources and sinks, we have developed a new technique to directly measure fluxes of chemically-resolved submicron aerosols using the high-resolution time-of-flight aerosol mass spectrometer (HR-AMS in a new, fast eddy covariance mode. This approach takes advantage of the instrument's ability to quantitatively identify both organic and inorganic components, including ammonium, sulphate and nitrate, at a temporal resolution of several Hz. The new approach has been successfully deployed over a temperate ponderosa pine plantation in California during the BEARPEX-2007 campaign, providing both total and chemically resolved non-refractory (NR PM1 fluxes. Average deposition velocities for total NR-PM1 aerosol at noon were 2.05 ± 0.04 mm s−1. Using a high resolution measurement of the NH2+ and NH3+ fragments, we demonstrate the first eddy covariance flux measurements of particulate ammonium, which show a noon-time deposition velocity of 1.9 ± 0.7 mm s−1 and are dominated by deposition of ammonium sulphate.

  18. Plume-exit modeling to determine cloud condensation nuclei activity of aerosols from residential biofuel combustion

    Science.gov (United States)

    Mena, Francisco; Bond, Tami C.; Riemer, Nicole

    2017-08-01

    Residential biofuel combustion is an important source of aerosols and gases in the atmosphere. The change in cloud characteristics due to biofuel burning aerosols is uncertain, in part, due to the uncertainty in the added number of cloud condensation nuclei (CCN) from biofuel burning. We provide estimates of the CCN activity of biofuel burning aerosols by explicitly modeling plume dynamics (coagulation, condensation, chemical reactions, and dilution) in a young biofuel burning plume from emission until plume exit, defined here as the condition when the plume reaches ambient temperature and specific humidity through entrainment. We found that aerosol-scale dynamics affect CCN activity only during the first few seconds of evolution, after which the CCN efficiency reaches a constant value. Homogenizing factors in a plume are co-emission of semi-volatile organic compounds (SVOCs) or emission at small particle sizes; SVOC co-emission can be the main factor determining plume-exit CCN for hydrophobic or small particles. Coagulation limits emission of CCN to about 1016 per kilogram of fuel. Depending on emission factor, particle size, and composition, some of these particles may not activate at low supersaturation (ssat). Hygroscopic Aitken-mode particles can contribute to CCN through self-coagulation but have a small effect on the CCN activity of accumulation-mode particles, regardless of composition differences. Simple models (monodisperse coagulation and average hygroscopicity) can be used to estimate plume-exit CCN within about 20 % if particles are unimodal and have homogeneous composition, or when particles are emitted in the Aitken mode even if they are not homogeneous. On the other hand, if externally mixed particles are emitted in the accumulation mode without SVOCs, an average hygroscopicity overestimates emitted CCN by up to a factor of 2. This work has identified conditions under which particle populations become more homogeneous during plume processes. This

  19. Activity level of gross α and gross β in airborne aerosol samples around the Qinshan NPP

    Institute of Scientific and Technical Information of China (English)

    CHEN Bin; YE Jida; CHEN Qianyuan; WU Xiaofei; SONG Weili; WANG Hongfeng

    2007-01-01

    The monitoring results of gross α and gross β activity from 2001 to 2005 for environmental airborne aerosol samples around the Qinshan NPP base are presented in this paper. A total of 170 aerosol samples were collected from monitoring sites of Caichenmen village, Qinlian village, Xiajiawan village and Yangliucun village around the Qinshan NPP base. The measured specific activity of gross α and gross β are in the range of 0.02 ~ 0.38 mBq/m3 and 0.10 ~ 1.81 mBq/m3, respectively, with an average of 0.11 mBq/m3 and 0.45mBq/m3, respectively. They are lower than the average of 0.15 mBq/m3 and 0.52mBq/m3, of reference site at Hangzhou City. It is indicated that the specific activity of gross α and gross β for environmental aerosol samples around the Qinshan NPP base had not been increased in normal operating conditions of the NPP.

  20. Levoglucosan indicates high levels of biomass burning aerosols over oceans from the Arctic to Antarctic

    Science.gov (United States)

    Hu, Q.; Xie, Z.; Wang, X.; Kang, H.; Zhang, P.

    2015-12-01

    Biomass burning discharges numerous kinds of gases and aerosols, such as carbon dioxide (CO2), carbon monoxide (CO), methane (CH4), black carbon (BC), alcohols, organic acids and persistent organic pollutants (POPs), and is known to affect air quality, global carbon cycle, and climate. However, the extent to which biomass burning gases/aerosols are present on a global scale, especially in the marine atmosphere, is poorly understood. Here we measure levoglucosan, a superior molecular tracer of biomass burning aerosols because of its single source, in marine air from the Arctic Ocean through the North and South Pacific Ocean to coastal Antarctica during burning season. Levoglucosan was found to be present in all regions at ng/m3 levels. As a whole, levoglucosan concentrations in the Southern Hemisphere were comparable to those in the Northern Hemisphere. Marine air in the mid-latitudes (30°-60° N and S) has the highest levoglucosan loading due to the emission from adjacent lands. Air over the Arctic Ocean which affected by biomass burning in the east Siberia has intermediate loading. Equatorial latitudes is the main source of biomass burning emissions, however, levoglucosan is in relatively low level. Large amount of precipitation and high hydroxyl radical concentration in this region cause more deposition and degradation of levoglucosan during transport. Previous studies were debatable on the influence of biomass burning on the Antarctic because of uncertain source of BC. Here via levoglucosan, it is proved that although far away from emission sources, the Antarctic is still affected by biomass burning aerosols which may be derived from South America. Biomass burning has a significant impact on mercury (Hg) and water-soluble organic carbon (WSOC) in marine aerosols from pole to pole, with more contribution to WSOC in the Northern Hemisphere than in the Southern Hemisphere.

  1. Study of particle size distribution and formation mechanism of radioactive aerosols generated in high-energy neutron fields

    CERN Document Server

    Endo, A; Noguchi, H; Tanaka, S; Iida, T; Furuichi, S; Kanda, Y; Oki, Y

    2003-01-01

    The size distributions of sup 3 sup 8 Cl, sup 3 sup 9 Cl, sup 8 sup 2 Br and sup 8 sup 4 Br aerosols generated by irradiations of argon and krypton gases containing di-octyl phthalate (DOP) aerosols with 45 MeV and 65 MeV quasi-monoenergetic neutrons were measured in order to study the formation mechanism of radioactive particles in high energy radiation fields. The effects of the size distribution of the radioactive aerosols on the size of the added DOP aerosols, the energy of the neutrons and the kinds of nuclides were studied. The observed size distributions of the radioactive particles were explained by attachment of the radioactive atoms generated by the neutron-induced reactions to the DOP aerosols. (author)

  2. Aerosol Characteristics at a high-altitude station Nainital during the ISRO-GBP Land Campaign-II

    CERN Document Server

    Saha, A; Dumka, U C; Hegde, P; Srivastava, M K; Sagar, R; Saha, Auromeet; Srivastava, Manoj K.; Sagar, Ram

    2006-01-01

    During the second land campaign (LC-II) organised by ISRO-GBP, extensive ground-based measurements of aerosol characteristics were carried out over Manora Peak (29.4oN; 79.5oE; 1951 metres above mean sea level), Nainital (a high altitude station located in the Shivalik ranges of Central Himalayas) during the dry, winter season (December) of 2004. These measurements included the spectral aerosol optical depths (AOD), columnar water vapour content (W), Total Columnar Ozone (TCO), total number concentration (NT) of near surface aerosols, mass concentration of black carbon (MB), aerosol mass loading (MT), and Global Solar Radiation. Based on these measured parameters, we present the results on the near-surface and columnar properties of atmospheric aerosols at Nainital.

  3. Highly-controlled, reproducible measurements of aerosol emissions from African biomass combustion

    Science.gov (United States)

    Haslett, Sophie; Thomas, J. Chris; Morgan, William; Hadden, Rory; Liu, Dantong; Allan, James; Williams, Paul; Sekou, Keïta; Liousse, Catherine; Coe, Hugh

    2017-04-01

    Particulate emissions from biomass burning can alter the atmosphere's radiative balance and cause significant harm to human health. However, the relationship between these emissions and fundamental combustion processes is, to date, poorly characterised. In atmospheric models, aerosol emissions are represented by emission factors based on mass loss, which are averaged over an entire combustion event for each particulate species. This approach, however, masks huge variability in emissions during different phases of the combustion period. Laboratory tests have shown that even small changes to the burning environment can lead to huge variation in observed aerosol emission factors (Akagi et al., 2011). In order to address this gap in understanding, in this study, small wood samples sourced from Côte D'Ivoire were burned in a highly-controlled laboratory environment. The shape and mass of samples, available airflow and surrounding heat were carefully regulated. Organic aerosol and refractory black carbon emissions were measured in real-time using an Aerosol Mass Spectrometer and a Single Particle Soot Photometer, respectively. Both of these instruments are used regularly to measure aerosol concentrations in the field. This methodology produced remarkably repeatable results, allowing three different phases of combustion to be identified by their emissions. Black carbon was emitted predominantly during flaming combustion; organic aerosols were emitted during pyrolysis before ignition and from smouldering-dominated behaviour near the end of combustion. During the flaming period, there was a strong correlation between the emission of black carbon and the rate of mass loss, which suggests there is value in employing a mass-based emission factor for this species. However, very little correlation was seen between organic aerosol and mass loss throughout the tests. As such, results here suggest that emission factors averaged over an entire combustion event are unlikely to be

  4. First lidar measurements of water vapor and aerosols from a high-altitude aircraft

    Science.gov (United States)

    Browell, Edward V.; Ismail, Syed

    1995-01-01

    Water vapor plays an important role in many atmospheric processes related to radiation, climate change, atmospheric dynamics, meteorology, the global hydrologic cycle, and atmospheric chemistry, and yet our knowledge of the global distribution of water vapor is very limited. The differential absorption lidar (DIAL) technique has the potential of providing needed high resolution water vapor measurements from aircraft and from space, and the Lidar Atmospheric Sensing Experiment (LASE) is a key step in the development of this capability. The LASE instrument is the first fully engineered, autonomous DIAL system, and it is designed to operate from a high-altitude aircraft (ER-2) and to make water vapor and aerosol profile measurements across the troposphere. The LASE system was flown from the NASA Wallops Flight Facility in a series of engineering flights during September 1994. This paper discusses the characteristics of the LASE system and presents the first LASE measurements of water vapor and aerosol profiles.

  5. Single-particle characterization of the high-Arctic summertime aerosol

    Directory of Open Access Journals (Sweden)

    B. Sierau

    2014-07-01

    Full Text Available Single-particle mass-spectrometric measurements were carried out in the high Arctic north of 80° during summer 2008. The campaign took place onboard the icebreaker Oden and was part of the Arctic Summer Cloud Ocean Study (ASCOS. The instrument deployed was an aerosol time-of-flight mass spectrometer (ATOFMS that provides information on the chemical composition of individual particles and their mixing state in real time. Aerosols were sampled in the marine boundary layer at stations in the open ocean, in the marginal ice zone, and in the pack ice region. The largest fraction of particles detected for subsequent analysis in the size range of the ATOFMS between approximately 200 and 3000 nm in diameter showed mass-spectrometric patterns, indicating an internal mixing state and a biomass burning and/or biofuel source. The majority of these particles were connected to an air mass layer of elevated particle concentration mixed into the surface mixed layer from the upper part of the marine boundary layer. The second largest fraction was represented by sea salt particles. The chemical analysis of the over-ice sea salt aerosol revealed tracer compounds that reflect chemical aging of the particles during their long-range advection from the marginal ice zone, or open waters south thereof prior to detection at the ship. From our findings we conclude that long-range transport of particles is one source of aerosols in the high Arctic. To assess the importance of long-range particle sources for aerosol–cloud interactions over the inner Arctic in comparison to local and regional biogenic primary aerosol sources, the chemical composition of the detected particles was analyzed for indicators of marine biological origin. Only a minor fraction showed chemical signatures of potentially ocean-derived primary particles of that kind. However, a chemical bias in the ATOFMS's detection capabilities observed during ASCOS might suggest the presence of a particle type of

  6. Aerosol activity distribution on aerodynamic diameter inside the object ''Shelter'': physical and dosimetric aspects

    Energy Technology Data Exchange (ETDEWEB)

    Bondarenko, O.A.; Aryasov, P.B.; Medvedev, S.Yu.; Nesmiyan, I.M. [Radiation Protection Inst., Kiev (Ukraine); Zhidkov, A.V. [ISTC ' ' Shelter' ' , Chernobyl, Kiev (Ukraine)

    2001-07-01

    Experimental results of the aerosol size distribution inside the Object ''Shelter'' are evaluated in the work. The results show a consistent and significant contribution of sub-micron fraction to the total aerosol activity. Different methods of interpretation of impactor data series are evaluated in terms of adequate assessment of the separate sub-micron aerosol fraction. The contribution of the sub-micron component to the total aerosol activity was found to be about 35%. Results of this research were also compared to those of other authors conducted with by using identical impactor equipment, e.g. results of aerosol sampling at a Czech NPP Dukovany. It is demonstrated in the work that observation of such a significant contribution of the sub-micron fraction for the Shelter aerosol can be hardly explained by systematic failure of the sampling equipment. Also physical mechanisms and corresponding observations of sub-micron aerosol generation inside the Shelter as well as subsequent dosimetric aspects are discussed. (orig.)

  7. Relating cloud condensation nuclei activity and oxidation level of alpha-pinene secondary organic aerosols

    DEFF Research Database (Denmark)

    Foverskov, Mia Frosch Mogensbæk; Bilde, M.; DeCarlo, P. F.

    2011-01-01

    and the CCN-derived single hygroscopicity parameter kappa for different experimental conditions: varying precursor concentrations (10-40 ppb), different OH sources (photolysis of HONO either with or without the addition of NO or ozonolysis of tetramethylethylene), and exposure to light. Oxygenation......During a series of smog chamber experiments, the effects of chemical and photochemical aging on the ability of organic aerosols generated from ozonolysis of alpha-pinene to act as cloud condensation nuclei (CCN) were investigated. In particular, the study focused on the relation between oxygenation...... was described by the contribution of the aerosol mass spectrometer (AMS) mass fragment m/z 44 to the total organic signal (f(44)) and the oxygen to carbon molar ratio (O/C), likewise determined with AMS. CCN activity, described by the hygroscopicity parameter kappa, was determined with a CCN counter...

  8. Hygroscopicity and CCN activity of atmospheric aerosol particles and their relation to organics: Characteristics of urban aerosols in Nagoya, Japan

    Science.gov (United States)

    Kawana, Kaori; Nakayama, Tomoki; Mochida, Michihiro

    2016-04-01

    The size-resolved distributions of hygroscopic growth factor g and the ratios of cloud condensation nuclei (CCN) to condensation nuclei of atmospheric aerosols were investigated in Nagoya, Japan. The average of the distributions of g at 85% relative humidity was bimodal. The size-resolved mean κ derived from g showed an increasing trend with diameter: 0.17-0.33 at 24-359 nm. The κ values calculated from CCN activation curves were 37% higher than those derived from g. Only 9% of the 37% difference is explained by the difference in the κ of inorganics under subsaturated and supersaturated conditions, suggesting a contribution of organics to the remaining 28% difference. The size-averaged κ of organics (κorg) was calculated as 0.14 and 0.19 by two different methods. The number fractions of CCN predicted from the hygroscopicity data over the range of 24-359 nm are loosely consistent with those observed if the size- and time-averaged g is applied to all particles (differences: -30% to +10%). This consistency improves if size- and time-resolved g and g distribution are used (differences: -19% to -3%). Whereas the number fractions of CCN predicted from the composition data are greatly underestimated if organics are assumed to be insoluble (differences: -64% to -45%), they are more consistent if κorg of 0.14 or 0.19 is applied (differences: -10% to +14%). The results demonstrate the importance of the dependence of the g of particles on time and particle size and the hygroscopicity of organics for CCN number concentrations in the urban atmosphere.

  9. Aerosol formation from high-velocity uranium drops: Comparison of number and mass distributions. Final report

    Energy Technology Data Exchange (ETDEWEB)

    Rader, D.J.; Benson, D.A.

    1995-05-01

    This report presents the results of an experimental study of the aerosol produced by the combustion of high-velocity molten-uranium droplets produced by the simultaneous heating and electromagnetic launch of uranium wires. These tests are intended to simulate the reduction of high-velocity fragments into aerosol in high-explosive detonations or reactor accidents involving nuclear materials. As reported earlier, the resulting aerosol consists mainly of web-like chain agglomerates. A condensation nucleus counter was used to investigate the decay of the total particle concentration due to coagulation and losses. Number size distributions based on mobility equivalent diameter obtained soon after launch with a Differential Mobility Particle Sizer showed lognormal distributions with an initial count median diameter (CMD) of 0.3 {mu}m and a geometric standard deviation, {sigma}{sub g} of about 2; the CMD was found to increase and {sigma}{sub g} decrease with time due to coagulation. Mass size distributions based on aerodynamic diameter were obtained for the first time with a Microorifice Uniform Deposit Impactor, which showed lognormal distributions with mass median aerodynamic diameters of about 0.5 {mu}m and an aerodynamic geometric standard deviation of about 2. Approximate methods for converting between number and mass distributions and between mobility and aerodynamic equivalent diameters are presented.

  10. Chemical Aging and Cloud Condensation Nuclei Activity of Biomass Burning Aerosol Proxies in the Presence of OH Radicals

    Science.gov (United States)

    Slade, Jonathan H., Jr.

    Biomass burning aerosol (BBA) can adversely impact regional and global air quality and represents a significant source of organic aerosol (OA) to the atmosphere that can affect climate. Aerosol particles can alter the transfer of radiation in earth's atmosphere directly by scattering and absorbing radiation or indirectly via cloud formation. Gas-to-particle, also termed heterogeneous, oxidation reactions can significantly alter the particle's physical and chemical properties. In turn, this can lead to the degradation of biomolecular markers for air quality-related aerosol source apportionment studies, the particles' lifetime, and modify the particles' abilities to serve as cloud condensation nuclei (CCN). However, the rates, mechanisms, and conditions by which these multiphase oxidation reactions occur and influence the CCN activity of OA is not well understood. The work presented here aims to determine the reactivity and products from the interaction of BBA surrogate-particles and trace gas-phase oxidants and to link the effects of OA chemical aging on the particles' ability to nucleate clouds. The reactive uptake of OH by BBA surrogate-substrates and particles, including levoglucosan, nitroguaiacol, abietic acid, and methyl-nitrocatechol, was determined as a function of both OH concentration and relative humidity (RH) using chemical ionization mass spectrometry coupled to various flow reactors. OH reactive uptake decreased with increasing OH concentration, indicative of OH adsorption followed by reaction. OH oxidation led to significant volatilization, i.e. mass loss of the organic material, as determined by application of high resolution proton transfer reaction time-of-flight mass spectrometry. Volatilized reaction products were identified, providing mechanistic insight of the chemical pathways in the heterogeneous OH oxidation of BBA. The reactive uptake of OH by levoglucosan particles increased with RH due to enhanced OH and organic bulk diffusivity. In

  11. High performance liquid chromatography study of complex oxygenated alkane mixtures from organic aerosols

    Science.gov (United States)

    Kalafut-Pettibone, Alicia J.; Klems, Joseph P.; McGivern, W. Sean

    2013-05-01

    The composition of secondary organic aerosol particles is of primary importance both in identifying particle sources and in determining physical parameters, such as cloud condensation nucleus propensity. Further, measurements of composition are valuable in determining the chemistry of formation and aging. In this work, we describe the application of a recently-developed derivatization technique to a complex synthetic organic aerosol derived from the photolysis of 1-iodooctane. The technique utilizes high-performance liquid chromatography (HPLC) coupled to both ultravioletvisible (UV/VIS) spectroscopy and tandem mass spectrometry (MS-MS) to determine the overall distribution of hydroxyl (OH), non-acid carbonyl (C=O), and carboxylic acid (COOH) moieties as well as the specific identities of chromatographically separated products. This composition data will then be used to constrain models of the particle formation mechanisms.

  12. Aerosolized Antibiotics.

    Science.gov (United States)

    Restrepo, Marcos I; Keyt, Holly; Reyes, Luis F

    2015-06-01

    Administration of medications via aerosolization is potentially an ideal strategy to treat airway diseases. This delivery method ensures high concentrations of the medication in the targeted tissues, the airways, with generally lower systemic absorption and systemic adverse effects. Aerosolized antibiotics have been tested as treatment for bacterial infections in patients with cystic fibrosis (CF), non-CF bronchiectasis (NCFB), and ventilator-associated pneumonia (VAP). The most successful application of this to date is treatment of infections in patients with CF. It has been hypothesized that similar success would be seen in NCFB and in difficult-to-treat hospital-acquired infections such as VAP. This review summarizes the available evidence supporting the use of aerosolized antibiotics and addresses the specific considerations that clinicians should recognize when prescribing an aerosolized antibiotic for patients with CF, NCFB, and VAP.

  13. Dominant aerosol processes during high-pollution episodes over Greater Tokyo

    CERN Document Server

    Sartelet, Karine; Sportisse, Bruno

    2007-01-01

    This paper studies two high-pollution episodes over Greater Tokyo: 9 and 10 December 1999, and 31 July and 1 August 2001. Results obtained with the chemistry-transport model (CTM) Polair3D are compared to measurements of inorganic PM2.5. To understand to which extent the aerosol processes modeled in Polair3D impact simulated inorganic PM2.5, Polair3D is run with different options in the aerosol module, e.g. with/without heterogeneous reactions. To quantify the impact of processes outside the aerosol module, simulations are also done with another CTM (CMAQ). In the winter episode, sulfate is mostly impacted by condensation, coagulation, long-range transport, and deposition to a lesser extent. In the summer episode, the effect of long-range transport largely dominates. The impact of condensation/evaporation is dominant for ammonium, nitrate and chloride in both episodes. However, the impact of the thermodynamic equilibrium assumption is limited. The impact of heterogeneous reactions is large for nitrate and amm...

  14. Generalized high-spectral-resolution lidar technique with a multimode laser for aerosol remote sensing.

    Science.gov (United States)

    Cheng, Zhongtao; Liu, Dong; Zhang, Yupeng; Liu, Chong; Bai, Jian; Wang, Dan; Wang, Nanchao; Zhou, Yudi; Luo, Jing; Yang, Yongying; Shen, Yibing; Su, Lin; Yang, Liming

    2017-01-23

    High-spectral-resolution lidar (HSRL) is a powerful tool for atmospheric aerosol remote sensing. The current HSRL technique often requires a single longitudinal mode laser as the transmitter to accomplish the spectral discrimination of the aerosol and molecular scattering conveniently. However, single-mode laser is cumbersome and has very strict requirements for ambient stability, making the HSRL instrument not so robust in many cases. In this paper, a new HSRL concept, called generalized HSRL technique with a multimode laser (MML-gHSRL), is proposed, which can work using a multimode laser. The MML-gHSRL takes advantage of the period characteristic of the spectral function of the interferometric spectral discrimination filter (ISDF) thoroughly. By matching the free spectral range of the ISDF with the mode interval of the multimode laser, fine spectral discrimination for the lidar return from each longitudinal mode can be realized. Two common ISDFs, i.e., the Fabry-Perot interferometer (FPI) and field-widened Michelson interferometer (FWMI), are introduced to develop the MML-gHSRL, and their performance is quantitatively analyzed and compared. The MML-gHSRL is a natural but significant generalization for the current HSRL technique based on the IDSF. It is potential that this technique would be a good entrance to future HSRL developments, especially in airborne and satellite-borne aerosol remote sensing applications.

  15. Aerosol black carbon characteristics over a high-altitude Western Ghats location in Southern India

    Science.gov (United States)

    Udayasoorian, C.; Jayabalakrishnan, R. M.; Suguna, A. R.; Gogoi, Mukunda M.; Babu, S. Suresh

    2014-10-01

    Aerosol black carbon (BC) mass concentrations were continuously monitored over a period of 2 years (April 2010 to May 2012) from a high-altitude location Ooty in the Nilgiris Mountain range in southern India to characterize the distinct nature of absorbing aerosols and their seasonality. Despite being remote and sparsely inhabited, BC concentrations showed significant seasonality with higher values (~ 0.96 ± 0.35 μg m-3) in summer (March to May), attributed to increased vertical transport of effluents in the upwind valley regions, which might have been confined to the surrounding valley regions within the very shallow winter boundary layer. The local atmospheric boundary layer (ABL) influence in summer was further modulated by the long-range transported aerosols from the eastern locations of Ooty. During monsoon (June-August), the concentrations were far reduced (~ 0.23 ± 0.06 μg m-3) due to intense precipitation. Diurnal variations were found conspicuous mainly during summer season associated with local ABL. The spectral absorption coefficients (αabs) depicted, in general, flatter distribution (mostly < 1.0 for more than 85% of daily mean values), suggesting the relative dominance of fossil fuel combustion, though showed marginal seasonal change with higher values of αabs in summer.

  16. Chemical composition of free tropospheric aerosol for PM1 and coarse mode at the high alpine site Jungfraujoch

    Directory of Open Access Journals (Sweden)

    J. Cozic

    2008-01-01

    Full Text Available The chemical composition of submicron (fine mode and supermicron (coarse mode aerosol particles has been investigated at the Jungfraujoch high alpine research station (3580 m a.s.l., Switzerland as part of the GAW aerosol monitoring program since 1999. A clear seasonality was observed for all major components throughout the period with low concentrations in winter (predominantly free tropospheric aerosol and higher concentrations in summer (enhanced vertical transport of boundary layer pollutants. In addition, mass closure was attempted during intensive campaigns in March 2004, February–March 2005 and August 2005. Ionic, carbonaceous and non-refractory components of the aerosol were quantified as well as the PM1 and coarse mode total aerosol mass concentrations. A relatively low conversion factor of 1.8 for organic carbon (OC to particulate organic matter (OM was found in winter (February–March 2005. Organics, sulfate, ammonium, and nitrate were the major components of the fine aerosol fraction that were identified, while calcium and nitrate were the only two measured components contributing to the coarse mode. The aerosol mass concentrations for fine and coarse mode aerosol measured during the intensive campaigns were not typical of the long-term seasonality due largely to dynamical differences. Average fine and coarse mode concentrations during the intensive field campaigns were 1.7 μg m−3 and 2.4 μg m−3 in winter and 2.5 μg m−3 and 2.0 μg m−3 in summer, respectively. The mass balance of aerosols showed higher contributions of calcium and nitrate in the coarse mode during Saharan dust events (SDE than without SDE.

  17. Chemical composition of free tropospheric aerosol for PM1 and coarse mode at the high alpine site Jungfraujoch

    Directory of Open Access Journals (Sweden)

    J. Cozic

    2007-08-01

    Full Text Available The chemical composition of submicron (fine mode and supermicron (coarse mode aerosol particles has been investigated since 1999 within the GAW aerosol monitoring program at the high alpine research station Jungfraujoch (3580 m a.s.l., Switzerland. Clear seasonality was observed for all major components in the last 9 years with low concentrations in winter (predominantly free tropospheric aerosol and higher concentrations in summer (enhanced vertical transport of boundary layer pollutants. In addition, mass closure was attempted during intensive experiments in March 2004, February–March 2005 and August 2005. Ionic, carbonaceous and refractory components of the aerosol were quantified as well as the PM1 and coarse mode total aerosol mass concentrations. A relatively low conversion factor of 1.8 for organic carbon (OC to particulate organic matter (OM in winter (February–March 2005 was found. Organics, sulfate, ammonium, and nitrate were the major identified components of the fine aerosol fraction, while calcium and nitrate were the two major measured components in the coarse mode. The aerosol mass concentrations for fine and coarse mode aerosol during the intensive campaigns were not typical of the long term seasonality due largely to dynamical differences. Average fine and coarse mode concentrations during the intensive field campaigns were 1.7 μg m−3 and 2.4 μg m−3 in winter and 2.5 μg m−3 and 2.0 μg m−3 in summer, respectively. The mass balance of aerosols showed higher contributions of calcium and nitrate in the coarse mode during Saharan dust events (SDE than without SDE.

  18. Modeling regional air quality and climate: improving organic aerosol and aerosol activation processes in WRF/Chem version 3.7.1

    Science.gov (United States)

    Yahya, Khairunnisa; Glotfelty, Timothy; Wang, Kai; Zhang, Yang; Nenes, Athanasios

    2017-06-01

    Air quality and climate influence each other through the uncertain processes of aerosol formation and cloud droplet activation. In this study, both processes are improved in the Weather, Research and Forecasting model with Chemistry (WRF/Chem) version 3.7.1. The existing Volatility Basis Set (VBS) treatments for organic aerosol (OA) formation in WRF/Chem are improved by considering the following: the secondary OA (SOA) formation from semi-volatile primary organic aerosol (POA), a semi-empirical formulation for the enthalpy of vaporization of SOA, and functionalization and fragmentation reactions for multiple generations of products from the oxidation of VOCs. Over the continental US, 2-month-long simulations (May to June 2010) are conducted and results are evaluated against surface and aircraft observations during the Nexus of Air Quality and Climate Change (CalNex) campaign. Among all the configurations considered, the best performance is found for the simulation with the 2005 Carbon Bond mechanism (CB05) and the VBS SOA module with semivolatile POA treatment, 25 % fragmentation, and the emissions of semi-volatile and intermediate volatile organic compounds being 3 times the original POA emissions. Among the three gas-phase mechanisms (CB05, CB6, and SAPRC07) used, CB05 gives the best performance for surface ozone and PM2. 5 concentrations. Differences in SOA predictions are larger for the simulations with different VBS treatments (e.g., nonvolatile POA versus semivolatile POA) compared to the simulations with different gas-phase mechanisms. Compared to the simulation with CB05 and the default SOA module, the simulations with the VBS treatment improve cloud droplet number concentration (CDNC) predictions (normalized mean biases from -40.8 % to a range of -34.6 to -27.7 %), with large differences between CB05-CB6 and SAPRC07 due to large differences in their OH and HO2 predictions. An advanced aerosol activation parameterization based on the Fountoukis and Nenes

  19. Synthesis of Trace Gas and Aerosol Observations and Evaluation of Modelled Short-lived Climate Pollutants Across the Pan-Eurasian High Latitudes

    Science.gov (United States)

    Arnold, S.; Nieminen, T.

    2015-12-01

    Model calculations suggest that changes in short-lived climate pollutants (SLCPs) such as ozone and aerosol may have contributed significantly to rapid Arctic warming over the past century. Arctic tropospheric budgets of SLCPs are impacted by long-range transport of trace gases and aerosols from Europe, Asia and N. America, but also by local sources such as gas flaring, shipping and boreal fires. Recently, the POLARCAT Model Intercomparison Project (POLMIP) showed that significant model biases persist through the depth of the European and North American high latitude troposphere in modelled trace-gas abundances. Evaluation of models over the Siberian high latitudes is challenging due to a severe paucity of available observations, despite the potential importance of this region as a route for European pollution export to the Arctic. Despite the existence of a number of limited datasets, which could be used for model evaluation in this region, until now no effort has been made to synthesise and exploit these observations to evaluate modelled abundances of SLCPs such as tropospheric ozone & aerosol. In this presentation, we will show evaluation of simulated aerosol, tropospheric ozone, and precursor species in several global chemical transport models, using a synthesis of available surface, aircraft and satellite observations over the high latitude pan-Eurasian region. We use models and observations to investigate source regions contributing to remote Siberian SLCP abundances over the annual cycle, and show substantial biases in simulated aerosol and trace gas concentrations that are consistent across a suite of different models. These comparisons constitute the first multi-model evaluation of tropospheric composition in the pan-Eurasin region using observations from across the broad region. Finally, we use the model simulations to determine optimum locations for the development of future monitoring activities in high latitude Eurasia with an aim of better

  20. Cloud droplet activity changes of soot aerosol upon smog chamber ageing

    Directory of Open Access Journals (Sweden)

    C. Wittbom

    2014-04-01

    Full Text Available Particles containing soot, or black carbon, are generally considered to contribute to global warming. However, large uncertainties remain in the net climate forcing resulting from anthropogenic emissions of black carbon (BC, to a large extent due to the fact that BC is co-emitted with gases and primary particles, both organic and inorganic, and subject to atmospheric ageing processes. In this study, diesel exhaust particles and particles from a flame soot generator spiked with light aromatic secondary organic aerosol (SOA precursors were processed by UV-radiation in a 6 m3 Teflon chamber in the presence of NOx. The time-dependent changes of the soot nanoparticle properties were characterised using a Cloud Condensation Nuclei Counter, an Aerosol Particle Mass Analyzer and a Soot Particle Aerosol Mass Spectrometer. The results show that freshly emitted soot particles do not activate into cloud droplets at supersaturations ≤ 2%, i.e. the black carbon core coated with primary organic aerosol (POA from the exhaust is limited in hygroscopicity. Before the onset of UV radiation it is unlikely that any substantial SOA formation is taking place. An immediate change in cloud-activation properties occurs at the onset of UV exposure. This change in hygroscopicity is likely attributed to SOA formed from intermediate volatile organic compounds (IVOC in the diesel engine exhaust. The change of cloud condensation nuclei (CCN properties at the onset of UV radiation implies that the lifetime of soot particles in the atmosphere is affected by the access to sunlight, which differs between latitudes. The ageing of soot particles progressively enhances their ability to act as cloud condensation nuclei, due to changes in: (I organic fraction of the particle, (II chemical properties of this fraction (POA or SOA, (III particle size, and (IV particle morphology. Applying κ-Köhler theory, using a κSOA value of 0.13 (derived from independent input parameters

  1. Characterization of urban aerosol in Cork city (Ireland using aerosol mass spectrometry

    Directory of Open Access Journals (Sweden)

    M. Dall'Osto

    2013-05-01

    Full Text Available Ambient wintertime background urban aerosol in Cork city, Ireland, was characterized using aerosol mass spectrometry. During the three-week measurement study in 2009, 93% of the ca. 1 350 000 single particles characterized by an Aerosol Time-of-Flight Mass Spectrometer (TSI ATOFMS were classified into five organic-rich particle types, internally mixed to different proportions with elemental carbon (EC, sulphate and nitrate, while the remaining 7% was predominantly inorganic in nature. Non-refractory PM1 aerosol was characterized using a High Resolution Time-of-Flight Aerosol Mass Spectrometer (Aerodyne HR-ToF-AMS and was also found to comprise organic aerosol as the most abundant species (62%, followed by nitrate (15%, sulphate (9% and ammonium (9%, and chloride (5%. Positive matrix factorization (PMF was applied to the HR-ToF-AMS organic matrix, and a five-factor solution was found to describe the variance in the data well. Specifically, "hydrocarbon-like" organic aerosol (HOA comprised 20% of the mass, "low-volatility" oxygenated organic aerosol (LV-OOA comprised 18%, "biomass burning" organic aerosol (BBOA comprised 23%, non-wood solid-fuel combustion "peat and coal" organic aerosol (PCOA comprised 21%, and finally a species type characterized by primary extit{m/z}~peaks at 41 and 55, similar to previously reported "cooking" organic aerosol (COA, but possessing different diurnal variations to what would be expected for cooking activities, contributed 18%. Correlations between the different particle types obtained by the two aerosol mass spectrometers are also discussed. Despite wood, coal and peat being minor fuel types used for domestic space heating in urban areas, their relatively low combustion efficiencies result in a significant contribution to PM1 aerosol mass (44% and 28% of the total organic aerosol mass and non-refractory total PM1, respectively.

  2. Characteristics of Aerosol Spectral Optical Depths over Manora Peak, Nainital $-$ A High Altitude Station in the Central Himalayas

    CERN Document Server

    Sagar, R; Dumka, U C; Moorthy, K K; Pant, P

    2003-01-01

    We present for the first time spectral behaviour of aerosol optical depths (AODs) over Manora Peak, Nainital located at an altitude of ~2 km in the central Himalayas. The observations were carried out using a Multi-Wavelength Solar Radiometer during January to December 2002. The primary features of the study are (i) larger AOD during afternoon periods compared to forenoon, attributable to change in the ray path from comparatively cleaner environment in the forenoon to polluted environment in the afternoon (ii) extremely low AODs during local winter and a remarkable increase to high values in summer (iii) a distinct change in the spectral dependencies of AODs from a relatively steeper spectra during winter to a shallower one in summer representing both transparent (meteorological aerosols) and polluted summer (urban haze aerosols) skies.The mean aerosol extinction law at Nainital during 2002 is best represented by $0.10 \\lambda^{-0.61}$.

  3. Organic Aerosol Formation in the Humid, Photochemically-Active Southeastern US: SOAS Experiments and Simulations

    Science.gov (United States)

    Sareen, N.; Lim, Y. B.; Carlton, A. G.; Turpin, B. J.

    2013-12-01

    Aqueous multiphase chemistry in the atmosphere can lead to rapid transformation of organic compounds, forming highly oxidized low volatility organic aerosol and, in some cases, light absorbing (brown) carbon. Because liquid water is globally abundant, this chemistry could substantially impact climate, air quality, health, and the environment. Gas-phase precursors released from biogenic and anthropogenic sources are oxidized and fragmented forming water-soluble gases that can undergo reactions in the aqueous phase (in clouds, fogs, and wet aerosols) leading to the formation of secondary organic aerosol (SOAAQ). Recent studies have highlighted the role of certain precursors like glyoxal, methylglyoxal, glycolaldehyde, acetic acid, acetone, and epoxides in the formation of SOAAQ. The goal of this work is to identify other precursors that are atmospherically important. In this study, ambient mixtures of water-soluble gases were scrubbed from the atmosphere at Brent, Alabama during the Southern Oxidant and Aerosol Study (SOAS). Four mist chambers in parallel collected ambient gases in a DI water medium at 20-25 LPM with a 4 hr collection time. Total organic carbon (TOC) values in daily composited samples were 64-180 μM. Aqueous OH radical oxidation experiments were conducted with these mixtures in a newly designed cuvette chamber to understand the formation of SOA through gas followed by aqueous chemistry. OH radicals (3.5E-2 μM [OH] s-1) were formed in-situ in the chamber, continuously by H2O2 photolysis. Precursors and products of these aqueous OH experiments were characterized using ion chromatography (IC), electrospray ionization mass spectrometry (ESI-MS), and IC-ESI-MS. ESI-MS results from a June 12th, 2013 sample showed precursors to be primarily odd, positive mode ions, indicative of the presence of non-nitrogen containing alcohols, aldehydes, organic peroxides, or epoxides. Products were seen in the negative mode and included organic acid ions like pyruvate

  4. High T(sub c) superconductors fabricated by plasma aerosol mist deposition technique

    Science.gov (United States)

    Wang, X. W.; Vuong, K. D.; Leone, A.; Shen, C. Q.; Williams, J.; Coy, M.

    1995-01-01

    We report new results on high T(sub c) superconductors fabricated by a plasma aerosol mist deposition technique, in atmospheric environment. Materials fabricated are YBaCuO, BiPbSrCaCuO, BaCaCuO precursor films for TlBaCaCuO, and other buffers such as YSZ. Depending on processing conditions, sizes of crystallites and/or particles are between dozens of nano-meters and several micrometers. Superconductive properties and other material characteristics can also be tailored.

  5. Temperature dependence of bromine activation due to reaction with ozone in a proxy for organic aerosols

    Science.gov (United States)

    Edebeli, Jacinta; Ammann, Markus; Gilgen, Anina; Eichler, Anja; Schneebeli, Martin; Bartels-Rausch, Thorsten

    2016-04-01

    The discovery of boundary layer ozone depletion events in the Polar Regions [1] and in the mid-latitudes [2], two areas of very different temperature regimes, begs the question of temperature dependence of reactions responsible for these observations [3]. These ODEs have been attributed to ozone reacting with halides leading to reactive halogens (halogen activation) of which bromide is extensively studied, R1 - R3 [4, 5] (R1 is a multiphase reaction). O3 + Br-→ O2 + OBr- (R1) OBr- + H+ ↔ HOBr (R2) HOBr + H+ + Br-→ Br2 + H2O (R3) Despite extensive studies of ozone-bromide interactions, the temperature dependence of bromine activation is not clear [3]. This limits parameterization of the involved reactions and factors in atmospheric models [3, 6]. Viscosity changes in the matrix (such as organic aerosols) due to temperature have been shown to influence heterogeneous reaction rates and products beyond pure temperature effect [7]. With the application of coated wall flow-tubes, the aim of this study is therefore to investigate the temperature dependence of bromine activation by ozone interaction while attempting to characterize the contributions of the bulk and surface reactions to observed ozone uptake. Citric acid is used in this study as a hygroscopically characterized matrix whose viscosity changes with temperature and humidity. Here, we present reactive ozone uptake measured between 258 and 289 K. The data show high reproducibility. Comparison of measured uptake with modelled bulk uptake at different matrix compositions (and viscosities) indicate that bulk reactive uptake dominates, but there are other factors which still need further consideration in the model. References 1. Barrie, L.A., et al., Nature, 1988. 334: p. 138 - 141. 2. Hebestreit, K., et al., Science, 1999. 283: p. 55-57. 3. Simpson, W.R., et al., Atmospheric Chemistry and Physics, 2007. 7: p. 4375 - 4418. 4. Haag, R.W. and J. Hoigné, Environ Sci Technol, 1983. 17: p. 261-267. 5. Oum, K.W., et

  6. On the aerosol-cloud relationship at a high-alpine site

    Energy Technology Data Exchange (ETDEWEB)

    Baltensperger, U.; Schwikowski, M.; Jost, D.T.; Nyeki, S.; Gaeggeler, H.W. [Paul Scherrer Inst. (PSI), Villigen (Switzerland)

    1997-09-01

    Field experiments at the Jungfraujoch showed that during the presence of a cloud, most of the aerosol mass is transferred into the cloud phase. This results in smaller cloud droplets for increasing aerosol concentration, which increases the albedo of clouds (known as the indirect effect of climate forcing by aerosol particles). (author) 1 fig., 4 refs.

  7. Molecular composition of organic aerosols in central Amazonia: an ultra-high-resolution mass spectrometry study

    Science.gov (United States)

    Kourtchev, Ivan; Godoi, Ricardo H. M.; Connors, Sarah; Levine, James G.; Archibald, Alex T.; Godoi, Ana F. L.; Paralovo, Sarah L.; Barbosa, Cybelli G. G.; Souza, Rodrigo A. F.; Manzi, Antonio O.; Seco, Roger; Sjostedt, Steve; Park, Jeong-Hoo; Guenther, Alex; Kim, Saewung; Smith, James; Martin, Scot T.; Kalberer, Markus

    2016-09-01

    The Amazon Basin plays key role in atmospheric chemistry, biodiversity and climate change. In this study we applied nanoelectrospray (nanoESI) ultra-high-resolution mass spectrometry (UHRMS) for the analysis of the organic fraction of PM2.5 aerosol samples collected during dry and wet seasons at a site in central Amazonia receiving background air masses, biomass burning and urban pollution. Comprehensive mass spectral data evaluation methods (e.g. Kendrick mass defect, Van Krevelen diagrams, carbon oxidation state and aromaticity equivalent) were used to identify compound classes and mass distributions of the detected species. Nitrogen- and/or sulfur-containing organic species contributed up to 60 % of the total identified number of formulae. A large number of molecular formulae in organic aerosol (OA) were attributed to later-generation nitrogen- and sulfur-containing oxidation products, suggesting that OA composition is affected by biomass burning and other, potentially anthropogenic, sources. Isoprene-derived organosulfate (IEPOX-OS) was found to be the most dominant ion in most of the analysed samples and strongly followed the concentration trends of the gas-phase anthropogenic tracers confirming its mixed anthropogenic-biogenic origin. The presence of oxidised aromatic and nitro-aromatic compounds in the samples suggested a strong influence from biomass burning especially during the dry period. Aerosol samples from the dry period and under enhanced biomass burning conditions contained a large number of molecules with high carbon oxidation state and an increased number of aromatic compounds compared to that from the wet period. The results of this work demonstrate that the studied site is influenced not only by biogenic emissions from the forest but also by biomass burning and potentially other anthropogenic emissions from the neighbouring urban environments.

  8. Improving estimates of aerosol radiative forcing through a particle-based aerosol microphysical scheme

    Science.gov (United States)

    Fierce, L.; McGraw, R. L.

    2016-12-01

    Forcing by atmospheric aerosols remains a large source of uncertainty in assessing human influences on the climate. Although global models have moved toward including more detailed representations of aerosol populations, aerosol microphysical schemes have been evaluated against benchmark models in only limited cases. Here we introduce a new framework for simulating atmospheric aerosols based on the Quadrature Method of Moments. This new aerosol model has been designed to reproduce key features of benchmark populations simulated by the particle-resolved model PartMC-MOSAIC, while tracking as little information about aerosol distributions as is necessary. The quadrature-based model simulates the aerosol evolution using a small number of weighted particles and is, therefore, decided as a reduced particle-based model. By applying principles of maximum entropy, the quadrature-based model efficiently reproduces distributions with respect to key aerosol properties, such as critical supersaturation for cloud condensation nuclei activation and optical cross sections, with high accuracy. In addition to providing an optimized aerosol model, the present study also describes how multi-scale modeling can be used as a tool for development of advanced aerosol microphysical schemes.

  9. Fluorescence spectra and biological activity of aerosolized bacillus spores and MS2 bacteriophage exposed to ozone at different relative humidities in a rotating drum

    Science.gov (United States)

    Ratnesar-Shumate, Shanna; Pan, Yong-Le; Hill, Steven C.; Kinahan, Sean; Corson, Elizabeth; Eshbaugh, Jonathan; Santarpia, Joshua L.

    2015-03-01

    Biological aerosols (bioaerosols) released into the environment may undergo physical and chemical transformations when exposed to atmospheric constituents such as solar irradiation, reactive oxygenated species, ozone, free radicals, water vapor and pollutants. Aging experiments were performed in a rotating drum chamber subjecting bioaerosols, Bacillus thuringiensis Al Hakam (BtAH) spores and MS2 bacteriophages to ozone at 0 and 150 ppb, and relative humidities (RH) at 10%, 50%, and 80+%. Fluorescence spectra and intensities of the aerosols as a function of time in the reaction chamber were measured with a single particle fluorescence spectrometer (SPFS) and an Ultra-Violet Aerodynamic Particle Sizer® Spectrometer (UV-APS). Losses in biological activity were measured by culture and quantitative polymerase chain reaction (q-PCR) assay. For both types of aerosols the largest change in fluorescence emission was between 280 and 400 nm when excited at 263 nm followed by fluorescence emission between 380 and 700 nm when excited at 351 nm. The fluorescence for both BtAH and MS2 were observed to decrease significantly at high ozone concentration and high RH when excited at 263 nm excitation. The decreases in 263 nm excited fluorescence are indicative of hydrolysis and oxidation of tryptophan in the aerosols. Fluorescence measured with the UV-APS (355-nm excitation) increased with time for both BtAH and MS2 aerosols. A two log loss of MS2 bacteriophage infectivity was observed in the presence of ozone at ~50% and 80% RH when measured by culture and normalized for physical losses by q-PCR. Viability of BtAH spores after exposure could not be measured due to the loss of genomic material during experiments, suggesting degradation of extracelluar DNA attributable to oxidation. The results of these studies indicate that the physical and biological properties of bioaerosols change significantly after exposure to ozone and water vapor.

  10. The effect of hygroscopicity on sea-spray aerosol fluxes: a comparison of high-rate and bulk correction methods

    Directory of Open Access Journals (Sweden)

    D. A. J. Sproson

    2012-09-01

    Full Text Available The eddy covariance technique is the most direct of the methods that have been used to measure the flux of sea-spray aerosol between the ocean and atmosphere, but has been applied in only a handful of studies. However, unless the aerosol is dried before the eddy covariance measurements are made, the hygroscopic nature of sea-spray may combine with a relative humidity flux to result in a bias in the calculated aerosol flux. "Bulk" methods have been presented to account for this bias, however they rely on assumptions of the shape of the aerosol spectra which may not be valid for near-surface measurements of sea-spray.

    Here we describe a method of correcting aerosol spectra for relative humidity induced size variations at the high frequency (10 Hz measurement timescale, where counting statistics are poor and the spectral shape cannot be well represented by a simple power law. Such a correction allows the effects of hygroscopicity and relative humidity flux on the aerosol flux to be explicitly evaluated and compared to the bulk corrections, both in their original form and once reformulated to better represent the measured mean aerosol spectra. In general, the bulk corrections – particularly when reformulated for the measured mean aerosol spectra – perform relatively well, producing flux corrections of the right sign and approximate magnitude. However, there are times when the bulk methods either significantly over- or underestimate the required flux correction. We thus conclude that, where possible, relative humidity corrections should be made at the measurement frequency.

  11. Optimized sparse-particle aerosol representations for modeling cloud-aerosol interactions

    Science.gov (United States)

    Fierce, Laura; McGraw, Robert

    2016-04-01

    Sparse representations of atmospheric aerosols are needed for efficient regional- and global-scale chemical transport models. Here we introduce a new framework for representing aerosol distributions, based on the method of moments. Given a set of moment constraints, we show how linear programming can be used to identify collections of sparse particles that approximately maximize distributional entropy. The collections of sparse particles derived from this approach reproduce CCN activity of the exact model aerosol distributions with high accuracy. Additionally, the linear programming techniques described in this study can be used to bound key aerosol properties, such as the number concentration of CCN. Unlike the commonly used sparse representations, such as modal and sectional schemes, the maximum-entropy moment-based approach is not constrained to pre-determined size bins or assumed distribution shapes. This study is a first step toward a new aerosol simulation scheme that will track multivariate aerosol distributions with sufficient computational efficiency for large-scale simulations.

  12. Structure, electrical characteristics, and high-temperature stability of aerosol jet printed silver nanoparticle films

    Science.gov (United States)

    Rahman, Md Taibur; McCloy, John; Ramana, C. V.; Panat, Rahul

    2016-08-01

    Printed electronics has emerged as a versatile eco-friendly fabrication technique to create sintered nanoparticle (NP) films on arbitrary surfaces with an excellent control over the film microstructure. While applicability of such films for high-temperature applications is not explored previously, herein we report the high-temperature electrical stability of silver (Ag) metal NP films fabricated using an Aerosol Jet based printing technique and demonstrate that this behavior is dictated by changes in the film microstructure. In-situ high temperature (24-500 °C) impedance spectroscopy measurements show that the real part of the impedance increases with increasing temperature up to 150 °C, at which point a decreasing trend prevails until 300 °C, followed again by an increase in impedance. The electrical behavior is correlated with the in-situ grain growth of the Ag NP films, as observed afterwards by scanning electron microscopy and X-ray diffraction (XRD), and could be tailored by controlling the initial microstructure through sintering conditions. Using combined diffraction and spectroscopic analytical methods, it is demonstrated the Aerosol Jet printed Ag NP films exhibit enhanced thermal stability and oxidation resistance. In addition to establishing the conditions for stability of Ag NP films, the results provide a fundamental understanding of the effect of grain growth and reduction in grain boundary area on the electrical stability of sintered NP films.

  13. Refractive Index and Absorption Attribution of Highly Absorbing Brown Carbon Aerosols from an Urban Indian City-Kanpur

    Science.gov (United States)

    Shamjad, P. M.; Tripathi, S. N.; Thamban, Navaneeth M.; Vreeland, Heidi

    2016-11-01

    Atmospheric aerosols influence Earth’s radiative balance, having both warming and cooling effects. Though many aerosols reflect radiation, carbonaceous aerosols such as black carbon and certain organic carbon species known as brown carbon have the potential to warm the atmosphere by absorbing light. Black carbon absorbs light over the entire solar spectrum whereas brown carbon absorbs near-UV wavelengths and, to a lesser extent, visible light. In developing countries, such as India, where combustion sources are prolific, the influence of brown carbon on absorption may be significant. In order to better characterize brown carbon, we present experimental and modeled absorption properties of submicron aerosols measured in an urban Indian city (Kanpur). Brown carbon here is found to be fivefold more absorbing at 365 nm wavelength compared to previous studies. Results suggest ~30% of total absorption in Kanpur is attributed to brown carbon, with primary organic aerosols contributing more than secondary organics. We report the spectral brown carbon refractive indices along with an experimentally constrained estimate of the influence of aerosol mixing state on absorption. We conclude that brown carbon in Kanpur is highly absorbing in nature and that the mixing state plays an important role in light absorption from volatile species.

  14. CCN activity and droplet growth kinetics of fresh and aged monoterpene secondary organic aerosol

    Directory of Open Access Journals (Sweden)

    G. J. Engelhart

    2008-01-01

    Full Text Available The ability of secondary organic aerosol (SOA produced from the ozonolysis of α-pinene and monoterpene mixtures (α-pinene, β-pinene, limonene and 3-carene to become cloud droplets was investigated. Monoterpene SOA is quite active and would likely be a good source of cloud condensation nuclei (CCN in the atmosphere. A static CCN counter and a Scanning Mobility CCN Analyser (a Scanning Mobility Particle Sizer coupled with a Continuous Flow counter were used for the CCN measurements. A decrease in CCN activation diameter for α-pinene SOA of approximately 3 nm h−1 was observed as the aerosol continued to react with oxidants. Hydroxyl radicals further oxidize the SOA particles thereby enhancing the particle CCN activity with time. The initial concentrations of ozone and monoterpene precursor (for concentrations lower than 40 ppb do not appear to affect the activity of the resulting SOA. Köhler Theory Analysis (KTA is used to infer the molar mass of the SOA sampled online and offline from atomized filter samples. KTA suggests that the aged aerosol (both from α-pinene and the mixed monoterpene oxidation is primarily water-soluble (around 70–80%, with an estimated average molar mass of 180±55 g mol−1 (consistent with existing SOA speciation studies. CCN activity measurements of the SOA mixed with (NH42SO4 suggest that the organic can depress surface tension by as much as 10 nM m−1 (with respect to pure water. The droplet growth kinetics of SOA samples are similar to (NH42SO4, except at low supersaturation, where SOA tends to grow more slowly. The CCN activity of α-pinene and mixed monoterpene SOA can be modelled by a very simple implementation of Köhler theory, assuming complete dissolution of the particles, no dissociation into ions, molecular weight of 180 g mol−1, density of 1.5 g cm−3, and surface tension to

  15. CCN activity and droplet growth kinetics of fresh and aged monoterpene secondary organic aerosol

    Directory of Open Access Journals (Sweden)

    G. J. Engelhart

    2008-07-01

    Full Text Available The ability of secondary organic aerosol (SOA produced from the ozonolysis of α-pinene and monoterpene mixtures (α-pinene, β-pinene, limonene and 3-carene to become cloud droplets was investigated. A static CCN counter and a Scanning Mobility CCN Analyser (a Scanning Mobility Particle Sizer coupled with a Continuous Flow counter were used for the CCN measurements. Consistent with previous studies monoterpene SOA is quite active and would likely be a good source of cloud condensation nuclei (CCN in the atmosphere. A decrease in CCN activation diameter for α-pinene SOA of approximately 3 nm hr−1 was observed as the aerosol continued to react with oxidants. Hydroxyl radicals further oxidize the SOA particles thereby enhancing the particle CCN activity with time. The initial concentrations of ozone and monoterpene precursor (for concentrations lower than 40 ppb do not appear to affect the activity of the resulting SOA. Köhler Theory Analysis (KTA is used to infer the molar mass of the SOA sampled online and offline from atomized filter samples. The estimated average molar mass of online SOA was determined to be 180±55 g mol−1 (consistent with existing SOA speciation studies assuming complete solubility. KTA suggests that the aged aerosol (both from α-pinene and the mixed monoterpene oxidation is primarily water-soluble (around 65%. CCN activity measurements of the SOA mixed with (NH42SO4 suggest that the organic can depress surface tension by as much as 10 N m−1 (with respect to pure water. The droplet growth kinetics of SOA samples are similar to (NH42SO4, except at low supersaturation, where SOA tends to grow more slowly. The CCN activation diameter of α-pinene and mixed monoterpene SOA can be modelled to within 10–15% of experiments by a simple implementation of Köhler theory, assuming complete dissolution of the particles, no

  16. Soot Aerosol Particles as Cloud Condensation Nuclei: from Ice Nucleation Activity to Ice Crystal Morphology

    Science.gov (United States)

    Pirim, Claire; Ikhenazene, Raouf; Ortega, Isamel Kenneth; Carpentier, Yvain; Focsa, Cristian; Chazallon, Bertrand; Ouf, François-Xavier

    2016-04-01

    Emissions of solid-state particles (soot) from engine exhausts due to incomplete fuel combustion is considered to influence ice and liquid water cloud droplet activation [1]. The activity of these aerosols would originate from their ability to be important centers of ice-particle nucleation, as they would promote ice formation above water homogeneous freezing point. Soot particles are reported to be generally worse ice nuclei than mineral dust because they activate nucleation at higher ice-supersaturations for deposition nucleation and at lower temperatures for immersion freezing than ratios usually expected for homogeneous nucleation [2]. In fact, there are still numerous opened questions as to whether and how soot's physico-chemical properties (structure, morphology and chemical composition) can influence their nucleation ability. Therefore, systematic investigations of soot aerosol nucleation activity via one specific nucleation mode, here deposition nucleation, combined with thorough structural and compositional analyzes are needed in order to establish any association between the particles' activity and their physico-chemical properties. In addition, since the morphology of the ice crystals can influence their radiative properties [3], we investigated their morphology as they grow over both soot and pristine substrates at different temperatures and humidity ratios. In the present work, Combustion Aerosol STandart soot samples were produced from propane using various experimental conditions. Their nucleation activity was studied in deposition mode (from water vapor), and monitored using a temperature-controlled reactor in which the sample's relative humidity is precisely measured with a cryo-hygrometer. Formation of water/ice onto the particles is followed both optically and spectroscopically, using a microscope coupled to a Raman spectrometer. Vibrational signatures of hydroxyls (O-H) emerge when the particle becomes hydrated and are used to characterize ice

  17. Aerosol particles at a high-altitude site on the Southeast Tibetan Plateau, China: Implications for pollution transport from South Asia

    Science.gov (United States)

    Zhao, Zhuzi; Cao, Junji; Shen, Zhenxing; Xu, Baiqing; Zhu, Chongshu; Chen, L.-W. Antony; Su, Xiaoli; Liu, Suixin; Han, Yongming; Wang, Gehui; Ho, Kinfai

    2013-10-01

    aerosol samples were collected from 16 July 2008 to 26 July 2009 at Lulang, a high-altitude (>3300m above sea level) site on the southeast Tibetan Plateau (TP); objectives were to determine chemical characteristics of the aerosol and identify its major sources. We report aerosol (total suspended particulate, TSP) mass levels and the concentrations of selected elements, carbonaceous species, and water-soluble inorganic ions. Significant buildup of aerosol mass and chemical species (organic carbon, element carbon, nitrate, and sulfate) occurred during the premonsoon, while lower concentrations were observed during the monsoon. Seasonal variations in aerosol and chemical species were driven by precipitation scavenging and atmospheric circulation. Two kinds of high-aerosol episodes were observed: one was enriched with dust indicators (Fe and Ca2+), and the other was enhanced with organic and elemental carbon (OC and EC), SO42-, NO3-, and Fe. The TSP loadings during the latter were 3 to 6 times those on normal days. The greatest aerosol optical depths (National Centers for Environmental Protection/National Center for Atmospheric Research reanalysis) occurred upwind, in eastern India and Bangladesh, and trajectory analysis indicates that air pollutants were transported from the southwest. Northwesterly winds brought high levels of natural emissions (Fe, Ca2+) and low levels of pollutants (SO42-, NO3-, K+, and EC); this was consistent with high aerosol optical depths over the western deserts and Gobi. Our work provides evidence that both geological and pollution aerosols from surrounding regions impact the aerosol population of the TP.

  18. Exposure to aerosols during high-pressure cleaning and relationship with health effects.

    Science.gov (United States)

    Madsen, Anne Mette; Matthiesen, Christoffer B

    2013-01-01

    In different occupations cleaning has been identified as the work task causing the highest exposure to aerosol components. High pressure cleaning (hpc) is a cleaning method used in many environments and seems to be considered as a cleaning method causing high exposure. In the presented study, the literature concerning exposure to aerosols during hpc is reviewed. Only a few studies have been published about exposure to aerosols during hpc. Exposure during hpc has been measured on farms, at waste water treatment plants, at a chemical factory and for graffiti removers. High exposures to bacterial endotoxin or chemical components were found in these environments during hpc. Few cases have been published documenting acute health effects caused by exposure to microorganisms and endotoxin during hpc. High pressure cleaners are also used in private settings but no papers have been found about exposure or related health effects during work in private settings. The use of clean water during hpc is important since effluent water or roof-collected rain water can cause a higher exposure to bioaerosols and related health effects. However, tap water in some areas also seems to have a high content of endotoxin, and this too should be considered when deliberating the protection of the airways of workers. Different attempts have been made to reduce workers' exposure and the health effects of exposure during hpc, among them the use of respiratory protection, ventilation and automation of work processes have been used with some degree of success. However, some of these studies only show tendencies. A high number of repeats seem to be necessary in order to obtain conclusive results. The material to be cleaned, as well as the degree of dirtiness, highly influences the exposure level; therefore, in comparative studies it is important also to consider these parameters. No study has been found which compares exposure during the use of different high pressure cleaners. The comparison of

  19. High Resolution Aerosol Optical Depth Retrieval Using Gaofen-1 WFV Camera Data

    Directory of Open Access Journals (Sweden)

    Kun Sun

    2017-01-01

    Full Text Available Aerosol Optical Depth (AOD is crucial for urban air quality assessment. However, the frequently used moderate-resolution imaging spectroradiometer (MODIS AOD product at 10 km resolution is too coarse to be applied in a regional-scale study. Gaofen-1 (GF-1 wide-field-of-view (WFV camera data, with high spatial and temporal resolution, has great potential in estimation of AOD. Due to the lack of shortwave infrared (SWIR band and complex surface reflectivity brought from high spatial resolution, it is difficult to retrieve AOD from GF-1 WFV data with traditional methods. In this paper, we propose an improved AOD retrieval algorithm for GF-1 WFV data. The retrieved AOD has a spatial resolution of 160 m and covers all land surface types. Significant improvements in the algorithm include: (1 adopting an improved clear sky composite method by using the MODIS AOD product to identify the clearest days and correct the background atmospheric effect; and (2 obtaining local aerosol models from long-term CIMEL sun-photometer measurements. Validation against MODIS AOD and ground measurements showed that the GF-1 WFV AOD has a good relationship with MODIS AOD (R2 = 0.66; RMSE = 0.27 and ground measurements (R2 = 0.80; RMSE = 0.25. Nevertheless, the proposed algorithm was found to overestimate AOD in some cases, which will need to be improved upon in future research.

  20. Characterization of submicron aerosols during a serious pollution month in Beijing (2013 using an aerodyne high-resolution aerosol mass spectrometer

    Directory of Open Access Journals (Sweden)

    J. K. Zhang

    2013-07-01

    Full Text Available In January 2013, Beijing experienced several serious haze events. To achieve a better understanding of the characteristics, sources and processes of aerosols during this month, an Aerodyne High-Resolution Time-of-Flight Aerosol Mass Spectrometer (HR-ToF-AMS was deployed at an urban site between 1 January and 1 February 2013 to obtain the size-resolved chemical composition of non-refractory submicron particles (NR-PM1. During this period, the mean measured NR-PM1 mass concentration was 87.4 μg m-3 and was composed of organics (49.8%, sulfate (21.4%, nitrate (14.6%, ammonium (10.4%, and chloride (3.8%. Moreover, inorganic matter, such as sulfate and nitrate comprised an increasing fraction of the NR-PM1 load as NR-PM1 loading increased, denoting their key roles in particulate pollution during this month. The average size distributions of the species were all dominated by an accumulation mode peaking at approximately 600 nm in vacuum aerodynamic diameter and organics characterized by an additional smaller size (∼200 nm. Elemental analyses showed that the average O/C, H/C, and N/C (molar ratio of organic matter were 0.34, 1.44 and 0.015, respectively, corresponding to an OM/OC ratio (mass ratio of organic matter to organic carbon of 1.60. Positive matrix factorization (PMF analyses of the high-resolution organic mass spectral dataset differentiated the organic aerosol into four components, i.e., oxygenated organic aerosols (OOA, cooking-related (COA, nitrogen-containing (NOA and hydrocarbon-like (HOA, which on average accounted for 40.0, 23.4, 18.1 and 18.5% of the total organic mass, respectively. Back trajectory clustering analyses indicated that the WNW air masses were associated with the highest NR-PM1 pollution during the campaign. Aerosol particles in southern air masses were especially rich in inorganic and oxidized organic species, whereas northern air masses contained a large fraction of primary species.

  1. Long-term study of cloud condensation nuclei (CCN) activation of the atmospheric aerosol in Vienna

    Science.gov (United States)

    Burkart, J.; Steiner, G.; Reischl, G.; Hitzenberger, R.

    2011-10-01

    During a total of 11 months, cloud condensation nuclei (CCN at super-saturation S 0.5%) and condensation nuclei (CN) concentrations were measured in the urban background aerosol of Vienna, Austria. For several months, number size distributions between 13.22 nm and 929 nm were also measured with a scanning mobility particle spectrometer (SMPS). Activation ratios (i.e. CCN/CN ratios) were calculated and apparent activation diameters obtained by integrating the SMPS size distributions. Variations in all CCN parameters (concentration, activation ratio, apparent activation diameter) are quite large on timescales of days to weeks. Passages of fronts influenced CCN parameters. Concentrations decreased with the passage of a front. No significant differences were found for fronts from different sectors (for Vienna mainly north to west and south to east). CCN concentrations at 0.5% S ranged from 160 cm-3 to 3600 cm-3 with a campaign average of 820 cm-3. Activation ratios were quite low (0.02-0.47, average: 0.13) and comparable to activation ratios found in other polluted regions (e.g. Cubison et al., 2008). Apparent activation diameters were found to be much larger (campaign average: 169 nm, range: (69-370) nm) than activation diameters for single-salt particles (around 50 nm depending on the salt). Contrary to CN concentrations, which are influenced by source patterns, CCN concentrations did not exhibit distinct diurnal patterns. Activation ratios showed diurnal variations counter-current to the variations of CN concentrations.

  2. Observations of fluorescent and biological aerosol at a high-altitude site in Central France

    Directory of Open Access Journals (Sweden)

    A. M. Gabey

    2013-01-01

    >
    Analysis of organic mass spectra recorded using an Aerosol Mass Spectrometer (AMS; Aerodyne Inc. suggests that aerosol reaching the site at night was more aged than that during the day, indicative of sampling the residual layer at night. Supplementary meteorological data and previous work also show that pdD lies in the residual layer/free troposphere at night, and this is thought to cause the observed diurnal cycles in organic-type and fluorescent aerosol particles.

    Based on the observed disparity between bacteria and fluorescent particle concentrations, fluorescent non-PBA is likely to be important in the WIBS-3 data and the surprisingly high fluorescent concentration in the residual layer/free troposphere raises questions about a ubiquitous background in continental air during the summer.

  3. Observations of fluorescent and biological aerosol at a high-altitude site in central France

    Science.gov (United States)

    Gabey, A. M.; Vaitilingom, M.; Freney, E.; Boulon, J.; Sellegri, K.; Gallagher, M. W.; Crawford, I. P.; Robinson, N. H.; Stanley, W. R.; Kaye, P. H.

    2013-08-01

    an aerosol mass spectrometer (AMS; Aerodyne Inc.) suggests that aerosol reaching the site at night was more aged than that during the day, indicative of sampling the residual layer at night. Supplementary meteorological data and previous work also show that PdD lies in the residual layer/free troposphere at night, and this is thought to cause the observed diurnal cycles in organic-type and fluorescent aerosol particles. Based on the observed disparity between bacteria and fluorescent particle concentrations, fluorescent non-PBA is likely to be important in the WIBS-3 data and the surprisingly high fluorescent concentration in the residual layer/free troposphere raises questions about a ubiquitous background in continental air during the summer.

  4. Use of aerosolized tissue plasminogen activator in the treatment of plastic bronchitis.

    Science.gov (United States)

    Lubcke, Nicole L; Nussbaum, Vicki M; Schroth, Mary

    2013-03-01

    To present a case of nebulized tissue plasminogen activator (t-PA) treatment for symptomatic plastic bronchitis in a pediatric patient years after a Fontan procedure. A 13-year-old boy with a history of corrected congenital heart disease was admitted to the pediatric intensive care unit after 2 weeks of worsening respiratory distress. A chest radiograph and subsequent bronchoscopy revealed extensive mucus plugging due to plastic bronchitis. Casts reaccumulated quickly after manual removal of the mucus and a regimen of aerosolized t-PA was initiated to break down the casts and prevent further cast formation over the 17-day hospital course. The treatment was successful and the patient was discharged home without evidence of bronchial casts. Plastic bronchitis is a potentially devastating condition in which pulmonary infiltrates line the bronchial tree, forming casts and prohibiting effective oxygen exchange. There are few effective treatment options for this condition. The use of aerosolized t-PA for the treatment of plastic bronchitis has been reported to be safe and effective in 4 cases but no consistent regimen, dose, or duration of treatment has been established. t-PA can be nebulized and inhaled for successful inhibition of bronchial cast formation. More information to determine the most effective dose and duration of therapy is needed to effectively improve the lives of people with plastic bronchitis.

  5. Hygroscopicity distribution concept for measurement data analysis and modeling of aerosol particle mixing state with regard to hygroscopic growth and CCN activation

    Science.gov (United States)

    Su, H.; Rose, D.; Cheng, Y. F.; Gunthe, S. S.; Massling, A.; Stock, M.; Wiedensohler, A.; Andreae, M. O.; Pöschl, U.

    2010-08-01

    This paper presents a general concept and mathematical framework of particle hygroscopicity distribution for the analysis and modeling of aerosol hygroscopic growth and cloud condensation nucleus (CCN) activity. The cumulative distribution function of particle hygroscopicity, H(κ, Dd) is defined as the number fraction of particles with a given dry diameter, Dd, and with an effective hygroscopicity parameter smaller than the parameter κ. From hygroscopicity tandem differential mobility analyzer (HTDMA) and size-resolved CCN measurement data, H(κ, Dd can be derived by solving the κ-Köhler model equation. Alternatively, H(κ, Dd can be predicted from measurement or model data resolving the chemical composition of single particles. A range of model scenarios are used to explain and illustrate the concept, and exemplary practical applications are shown with HTDMA and CCN measurement data from polluted megacity and pristine rainforest air. Lognormal distribution functions are found to be suitable for approximately describing the hygroscopicity distributions of the investigated atmospheric aerosol samples. For detailed characterization of aerosol hygroscopicity distributions, including externally mixed particles of low hygroscopicity such as freshly emitted soot, we suggest that size-resolved CCN measurements with a wide range and high resolution of water vapor supersaturation and dry particle diameter should be combined with comprehensive HTDMA measurements and size-resolved or single-particle measurements of aerosol chemical composition, including refractory components. In field and laboratory experiments, hygroscopicity distribution data from HTDMA and CCN measurements can complement mixing state information from optical, chemical and volatility-based techniques. Moreover, we propose and intend to use hygroscopicity distribution functions in model studies investigating the influence of aerosol mixing state on the formation of cloud droplets.

  6. High-spectral-resolution radiometric measurements of aerosol extinction over an urban region in India

    Science.gov (United States)

    Devara, P. C. S.; Ramkumar, M.; Maheskumar, R. S.; Pandithurai, G.

    2001-06-01

    Concurrent observations of aerosol optical depth (AOD) were carried out using a high-spectral-resolution radiometer (HSRR) and solar radiometer (SR) at the Indian Institute of Tropical Meteorology (IITM), Pune, India, on all clear-sky days available during November 1995-February 1996. The HSRR observations were collected at 5 nm intervals throughout the 400-700 nm spectrum while the SR measurements were made at discrete wavelengths of 400, 600, 940, 1060 and 1630 nm. In order to study the effect of integrated spectral observations on the derived AODs as compared to such depths from a single spectrum, multi-spectral observations at 2 nm intervals were collected. The AODs and their wavelength dependence from the HSRR and SR are compared and fairly good agreement found. The HSRR derived AODs at 400 nm and 700 nm from the present data sets are compared with those obtained during the winters of 1993-94 and 1994-95. The results reveal greater AODs, indicating abundance of aerosol particle concentration, during 1995-96 as compared to 1993-94 and 1994-95.

  7. Automated high-volume aerosol sampling station for environmental radiation monitoring

    Energy Technology Data Exchange (ETDEWEB)

    Toivonen, H.; Honkamaa, T.; Ilander, T.; Leppaenen, A.; Nikkinen, M.; Poellaenen, R.; Ylaetalo, S

    1998-07-01

    An automated high-volume aerosol sampling station, known as CINDERELLA.STUK, for environmental radiation monitoring has been developed by the Radiation and Nuclear Safety Authority (STUK), Finland. The sample is collected on a glass fibre filter (attached into a cassette), the airflow through the filter is 800 m{sup 3}/h at maximum. During the sampling, the filter is continuously monitored with Na(I) scintillation detectors. After the sampling, the large filter is automatically cut into 15 pieces that form a small sample and after ageing, the pile of filter pieces is moved onto an HPGe detector. These actions are performed automatically by a robot. The system is operated at a duty cycle of 1 d sampling, 1 d decay and 1 d counting. Minimum detectable concentrations of radionuclides in air are typically 1Ae10 x 10{sup -6} Bq/m{sup 3}. The station is equipped with various sensors to reveal unauthorized admittance. These sensors can be monitored remotely in real time via Internet or telephone lines. The processes and operation of the station are monitored and partly controlled by computer. The present approach fulfils the requirements of CTBTO for aerosol monitoring. The concept suits well for nuclear material safeguards, too 10 refs.

  8. Molecular Chemistry of Organic Aerosols Through the Application of High Resolution Mass Spectrometry

    Energy Technology Data Exchange (ETDEWEB)

    Nizkorodov, Serguei; Laskin, Julia; Laskin, Alexander

    2011-01-05

    Understanding of molecular composition and fundamental chemical transformations of organic aerosols (OA) during their formation and aging is both a major challenge and the area of greatest uncertainty in atmospheric research. Particularly little is known about fundamental relationship between the chemical composition and physicochemical properties of OA, their atmospheric history, evolution, and impact on the environment. Ambient soft-ionization methods combined with high-resolution mass spectrometry (HR-MS) analysis provide detailed information on the molecular content of OA that is pivotal for improved understanding of their complex composition, multi-phase aging chemistry, direct (light absorption and scattering) and indirect (aerosol-cloud interactions) effects on atmospheric radiation and climate, and health effects. The HR-MS methods can detect thousands of individual OA constituents at once, provide their elemental formulae from accurate mass measurements, and provide structural information based on tandem mass spectrometry. Integration with additional analytical tools, such as chromatography and UV/Vis absorption spectroscopy, makes it possible to further separate OA compounds by their polarity and ability to absorb solar radiation. The goal of this perspective is to describe modern HR-MS methods, review recent applications to field and laboratory studies of OA, and explain how the information obtained from HR-MS methods can be translated into improved understanding of OA chemistry.

  9. Characterization of submicron aerosols at a rural site in Pearl River Delta of China using an Aerodyne High-Resolution Aerosol Mass Spectrometer

    Directory of Open Access Journals (Sweden)

    X.-F. Huang

    2010-11-01

    Full Text Available The Pearl River Delta (PRD region in South China is one of the most economically developed regions in China, but it is also noted for its severe air pollution due to industrial/metropolitan emissions. In order to continuously improve the understanding and quantification of air pollution in this region, an intensive campaign was executed in PRD during October–November 2008. Here, we report and analyze Aerodyne High-Resolution Aerosol Mass Spectrometer measurements at Kaiping, a rural site downwind of the highly-polluted central PRD area, to characterize the general features of submicron particulate pollution in the regional air. The mean measured PM1 mass concentration was 33.1 ± 18.1 μg m−3 during the campaign and composed of organic matter (33.8%, sulfate (33.7%, ammonium (14.0%, nitrate (10.7%, black carbon (6.7%, and chloride (1.1%, which is characterized by high fractions of inorganic ions due to huge emissions of SO2 and NOx in PRD. The average size distributions of the species (except BC were all dominated by an accumulation mode peaking at ~450 nm in vacuum aerodynamic diameter. Calculations based on high-resolution organic mass spectra indicate that C, H, O, and N on average contributed 56.6, 7.0, 35.1, and 1.3% to the total organic mass, respectively, corresponding to an organic matter mass to organic carbon mass ratio (OM/OC of 1.77 ± 0.08. Based on the high-resolution organic mass spectral dataset observed, Positive Matrix Factorization (PMF analysis differentiated the organic aerosol into three components, i.e., biomass burning (BBOA and two oxygenated (LV-OOA and SV-OOA organic aerosols, which on average accounted for 24.5, 39.6 and 35.8% of the total organic mass, respectively. The BBOA showed strong features of biomass burning emissions and has been mainly attributed to field rice straw burning after harvest. The LV-OOA and SV-OOA were found to correspond to more aged (and thus

  10. Cloud condensation nuclei in pristine tropical rainforest air of Amazonia: size-resolved measurements and modeling of atmospheric aerosol composition and CCN activity

    Science.gov (United States)

    Gunthe, S. S.; King, S. M.; Rose, D.; Chen, Q.; Roldin, P.; Farmer, D. K.; Jimenez, J. L.; Artaxo, P.; Andreae, M. O.; Martin, S. T.; Pöschl, U.

    2009-10-01

    Atmospheric aerosol particles serving as cloud condensation nuclei (CCN) are key elements of the hydrological cycle and climate. We have measured and characterized CCN at water vapor supersaturations in the range of S=0.10-0.82% in pristine tropical rainforest air during the AMAZE-08 campaign in central Amazonia. The effective hygroscopicity parameters describing the influence of chemical composition on the CCN activity of aerosol particles varied in the range of κ≍0.1-0.4 (0.16±0.06 arithmetic mean and standard deviation). The overall median value of κ≍0.15 was by a factor of two lower than the values typically observed for continental aerosols in other regions of the world. Aitken mode particles were less hygroscopic than accumulation mode particles (κ≍0.1 at D≍50 nm; κ≍0.2 at D≍200 nm), which is in agreement with earlier hygroscopicity tandem differential mobility analyzer (H-TDMA) studies. The CCN measurement results are consistent with aerosol mass spectrometry (AMS) data, showing that the organic mass fraction (forg) was on average as high as ~90% in the Aitken mode (D≤100 nm) and decreased with increasing particle diameter in the accumulation mode (~80% at D≍200 nm). The κ values exhibited a negative linear correlation with forg (R2=0.81), and extrapolation yielded the following effective hygroscopicity parameters for organic and inorganic particle components: κorg≍0.1 which can be regarded as the effective hygroscopicity of biogenic secondary organic aerosol (SOA) and κinorg≍0.6 which is characteristic for ammonium sulfate and related salts. Both the size dependence and the temporal variability of effective particle hygroscopicity could be parameterized as a function of AMS-based organic and inorganic mass fractions (κp=κorg×forg +κinorg×finorg). The CCN number concentrations predicted with κp were in fair agreement with the measurement results (~20% average deviation). The median CCN number concentrations at S=0

  11. Occurrence of weak, sub-micron, tropospheric aerosol events at high Arctic latitudes

    Science.gov (United States)

    O'Neill, N. T.; Pancrati, O.; Baibakov, K.; Eloranta, E.; Batchelor, R. L.; Freemantle, J.; McArthur, L. J. B.; Strong, K.; Lindenmaier, R.

    2008-07-01

    Numerous fine mode (sub-micron) aerosol optical events were observed during the summer of 2007 at the High Arctic atmospheric observatory (PEARL) located at Eureka, Nunavut, Canada. Half of these events could be traced to forest fires in southern and eastern Russia and the Northwest Territories of Canada. The most notable findings were that (a) a combination of ground-based measurements (passive sunphotometry, high spectral resolution lidar) could be employed to determine that weak (near sub-visual) fine mode events had occurred, and (b) this data combined with remote sensing imagery products (MODIS, OMI-AI, FLAMBE fire sources), Fourier transform spectroscopy and back trajectories could be employed to identify the smoke events.

  12. CCN activity and volatility of β-caryophyllene secondary organic aerosol

    Directory of Open Access Journals (Sweden)

    M. Frosch

    2013-02-01

    Full Text Available In a series of smog chamber experiments, the cloud condensation nuclei (CCN activity of secondary organic aerosol (SOA generated from ozonolysis of β-caryophyllene was characterized by determining the CCN derived hygroscopicity parameter, κCCN, from experimental data. Two types of CCN counters, operating at different temperatures, were used. The effect of semi-volatile organic compounds on the CCN activity of SOA was studied using a thermodenuder.

    Overall, SOA was only slightly CCN active (with κCCN in the range 0.001–0.16, and in dark experiments with no OH scavenger present, κCCN decreased when particles were sent through the thermodenuder (with a temperature up to 50 °C.

    SOA was generated under different experimental conditions: In some experiments, an OH scavenger (2-butanol was added. SOA from these experiments was less CCN active than SOA produced in experiments without an OH scavenger (i.e. where OH was produced during ozonolysis. In other experiments, lights were turned on, either without or with the addition of HONO (OH source. This led to the formation of more CCN active SOA.

    SOA was aged up to 30 h through exposure to ozone and (in experiments with no OH scavenger present to OH. In all experiments, the derived κCCN consistently increased with time after initial injection of β-caryophyllene, showing that chemical ageing increases the CCN activity of β-caryophyllene SOA. κCCN was also observed to depend on supersaturation, which was explained either as an evaporation artifact from semi-volatile SOA (only observed in experiments lacking light exposure or, alternatively, by effects related to chemical composition depending on dry particle size.

    Using the method of Threshold Droplet Growth Analysis it was also concluded that the activation kinetics of the SOA do not differ significantly from calibration ammonium sulphate aerosol for

  13. A case study of the highly time-resolved evolution of aerosol chemical and optical properties in urban Shanghai, China

    Directory of Open Access Journals (Sweden)

    Y. Huang

    2013-04-01

    Full Text Available Characteristics of the chemical and optical properties of aerosols in urban Shanghai and their relationship were studied over a three-day period in October 2011. A suite of real-time instruments, including an Aerosol Time-Of-Flight Mass Spectrometer (ATOFMS, a Monitor for AeRosols and GAses (MARGA, a Cavity Ring Down Spectrometer (CRDS, a nephelometer and a Scanning Mobility Particle Sizer (SMPS, was employed to follow the quick changes of the aerosol properties within the 72 h sampling period. The origin of the air mass arriving in Shanghai during this period shifted from the East China Sea to the northwest area of China, offering a unique opportunity to observe the evolution of aerosols influenced by regional transport from the most polluted areas in China. According to the meteorological conditions and temporal characterizations of the chemical and optical properties, the sampling period was divided into three periods. During Period 1 (00:00–23:00 LT, 13 October, the aerosols in urban Shanghai were mainly fresh and the single scattering albedo varied negatively with the emission of elemental carbon, indicating that local sources dominated. Period 2 (23:00 LT on 13 October to 10:00 LT on 15 October was impacted by regionally transported pollutants and had the highest particulate matter (PM mass loading and the lowest particle acidity, characterized by large fractions of aged particles and high secondary ion (nitrate, sulfate and ammonium mass concentrations. Comparison between ATOFMS particle acidity and quantitative particle acidity by MARGA indicated the significance of semi-quantitative calculation in ATOFMS. Two sub-periods were identified in Period 2 based on the scattering efficiency of PM1 mass. Period 3 (from 10:00 LT on 15 October to 00:00 LT on 16 October had a low PM1/PM10 ratio and a new particle formation event. The comparison of these sub-periods highlights the influence of particle mixing state on aerosol optical properties

  14. Laboratory and field studies of stratospheric aerosols: Phase changes under high supersaturation

    Science.gov (United States)

    Hallet, John

    1991-02-01

    It is well known that water in the form of isolated small droplets supercool as much as 40 C below their equilibrium melting point. Solutions similarly supercool (with respect to water) and supersaturate (with respect of the solute). Experiments are described in which bulk solutions typical of atmospheric aerosols (nitric acid, sulfuric acid, and hydrates; ammonium sulfate; ammonium bisulfate; sodium chloride) are supercooled and/or supersaturated and nucleated to initiate crystal growth. Supersaturation of 300 percent is readily attainable, with linear growth of crystals increasing roughly as (supercooling/supersaturation)sup 2. The implication of the experiments is that the situation of metastability in polar stratosphere clouds is very likely, with nucleation only occuring under a high degree of supercooling or supersaturation.

  15. Laboratory and field studies of stratospheric aerosols: Phase changes under high supersaturation

    Science.gov (United States)

    Hallet, John

    1991-01-01

    It is well known that water in the form of isolated small droplets supercool as much as 40 C below their equilibrium melting point. Solutions similarly supercool (with respect to water) and supersaturate (with respect of the solute). Experiments are described in which bulk solutions typical of atmospheric aerosols (nitric acid, sulfuric acid, and hydrates; ammonium sulfate; ammonium bisulfate; sodium chloride) are supercooled and/or supersaturated and nucleated to initiate crystal growth. Supersaturation of 300 percent is readily attainable, with linear growth of crystals increasing roughly as (supercooling/supersaturation)sup 2. The implication of the experiments is that the situation of metastability in polar stratosphere clouds is very likely, with nucleation only occuring under a high degree of supercooling or supersaturation.

  16. Pilot Study of Inhaled Aerosols Targeted via Magnetic Alignment of High Aspect Ratio Particles in Rabbits

    Directory of Open Access Journals (Sweden)

    Gillian E. S. Redman

    2011-01-01

    Full Text Available Recently, inhaled pharmaceutical aerosols have seen increased investigation in the treatment of lung cancer, where the inability to deliver adequate therapeutic drug concentrations to tumour sites may be overcome with improved targeted delivery to the site of the tumour. In this study, the feasibility of magnetically targeted delivery of high aspect ratio particles loaded with iron oxide nanoparticles was studied in 19 New Zealand White rabbits. Half of the exposed rabbits had a magnetic field placed externally over their right lung. Iron sensitive magnetic resonance images of the lungs were acquired to determine the iron concentrations in the right and left lung of each animal. The right/left ratio increased in the middle and basal regions of the lung where, due to the morphology of the rabbit lung, this method of targeting is most effective. With further optimization, this technique could be an effective method for increasing the dose of drug delivered to a specific site within the lung.

  17. Impact of Aerosols on Shortwave and Photosynthetically Active Radiation Balance over Sub-tropical Region in South Asia: Observational and Modeling Approach

    Science.gov (United States)

    Subba, T.; Pathak, B.

    2016-12-01

    The North-East Indian Region (NER) (22-30ºN, 89-98ºE) in south Asia sandwiched between two global biodiversity hotspots namely, Himalaya and Indo-Burma, assumes significance owing to its unique topography with mountains in the north, east and south and densely populated Indo Gangetic plains (IGP) towards the west resulting in complex aerosol system. Multi-year (2010-2014) concurrent measurements of aerosol properties and the shortwave radiation budget are examined over four geographically distinct stations of NER operational under Indian Space Research organization's ARFINET (Aerosol Radiative Forcing over India NETwork). An attempt has been made to lessen the ambiguity of forcing estimation by validating the radiative transfer modelled ARF with the CNR4 net radiometer measured values (r2 0.98). The Normalized Difference Vegetation Index and its dependence on the extinction of the photosynthetically active radiation (PAR) due to aerosol are assessed. The spring time enhancement of aerosols in the column has shown significant surface cooling (ARF = -48 ± 5 Wm-2) over the region, while the very high Black Carbon (BC) mass concentrations near the surface (SSA > 0.8) leads to significant atmospheric warming (ARF = +41 ± 7 Wm-2) in the shortwave range. Radiative forcing estimates reveal that the atmospheric forcing by BC could be as high as +30Wm-2 over the western part, which are significantly higher than the eastern part with a consequent heating rate of 1.5 K day-1 revealing an east-west asymmetry over NER. The impact of BC aerosols on the photosynthetic rate varies among different locations ranging from -5±2 Wm-2 to -25±3 Wm-2. Almost 70% of the total atmospheric shortwave radiative absorption is attributed to just 10% contribution of Black Carbon (BC) to total mass concentration and causes a reduction of more than 30% of PAR reaching the surface over Brahmaputra valley due to direct radiative effect. Comparison of previous and the present study shows highest

  18. Characterization of urban aerosol in Cork City (Ireland using aerosol mass spectrometry

    Directory of Open Access Journals (Sweden)

    M. Dall'Osto

    2012-11-01

    Full Text Available Ambient wintertime background urban aerosol in Cork City, Ireland, was characterized using aerosol mass spectrometry. During the three-week measurement study in 2009, 93% of the 1 200 000 single particles characterized by an Aerosol Time-Of-Flight Mass Spectrometer (TSI ATOFMS were classified into five organic-rich particle types, internally-mixed to different proportions with Elemental Carbon (EC, sulphate and nitrate while the remaining 7% was predominantly inorganic in nature. Non-refractory PM1 aerosol was also characterized using a High Resolution Time-Of-Flight Aerodyne Aerosol Mass Spectrometer (HR-ToF-AMS and was also found to comprise organic matter as the most abundant species (62%, followed by nitrate (15%, sulphate (9% and ammonium (9%, and then chloride (5%.

    Positive matrix factorization (PMF was applied to the HR-ToF-AMS organic matrix and a five-factor solution was found to describe the variance in the data well. Specifically, "Hydrocarbon-like" Organic Aerosol (HOA comprised 19% of the mass, "Oxygenated low volatility" Organic Aerosols (LV-OOA comprised 19%, "Biomass wood Burning" Organic Aerosol (BBOA comprised 23%, non-wood solid-fuel combustion "Peat and Coal" Organic Aerosol (PCOA comprised 21%, and finally, a species type characterized by primary m/z peaks at 41 and 55, similar to previously-reported "Cooking" Organic Aerosol (COA but possessing different diurnal variations to what would be expected for cooking activities, contributed 18%. Despite wood, cool and peat being minor fuel types used for domestic space heating in urban areas, their relatively low combustion efficiencies result in a significant contribution to PM1 aerosol mass (44% and 28% of the total organic aerosols mass and non refractory PM1, respectively.

  19. Long-term study of cloud condensation nuclei (CCN) activation of the atmospheric aerosol in Vienna

    Science.gov (United States)

    Burkart, J.; Steiner, G.; Reischl, G.; Hitzenberger, R.

    2011-01-01

    During a total of 11 months, cloud condensation nuclei (CCN at super-saturation S 0.5%) and condensation nuclei (CN) concentrations were measured in the urban background aerosol of Vienna, Austria. For several months, number size distributions between 13.22 nm and 929 nm were also measured with a scanning mobility particle spectrometer (SMPS). Activation ratios (i.e. CCN/CN ratios) were calculated and apparent activation diameters obtained by integrating the SMPS size distributions. Variations in all CCN parameters (concentration, activation ratio, apparent activation diameter) are quite large on timescales of days to weeks. Passages of fronts influenced CCN parameters. Concentrations decreased with the passage of a front. No significant differences were found for fronts from different sectors (for Vienna mainly north to west and south to east). CCN concentrations at 0.5% S ranged from 160 cm−3 to 3600 cm−3 with a campaign average of 820 cm−3. Activation ratios were quite low (0.02–0.47, average: 0.13) and comparable to activation ratios found in other polluted regions (e.g. Cubison et al., 2008). Apparent activation diameters were found to be much larger (campaign average: 169 nm, range: (69–370) nm) than activation diameters for single-salt particles (around 50 nm depending on the salt). Contrary to CN concentrations, which are influenced by source patterns, CCN concentrations did not exhibit distinct diurnal patterns. Activation ratios showed diurnal variations counter-current to the variations of CN concentrations. PMID:21977003

  20. Absorbing aerosols at high relative humidity: closure between hygroscopic growth and optical properties

    Directory of Open Access Journals (Sweden)

    J. M. Flores

    2012-01-01

    Full Text Available The extinction coefficient and growth factor of humidified aerosols, at 80% and 90% RH, and at 532 nm and 355 nm wavelengths were measured for size-selected particles for ammonium sulfate, IHSS Pahokee peat (a lightly absorbing humic-like substance proxy, nigrosine (a black dye to model highly absorbing substances, and a mixture of AS and nigrosine. The ratio of the humidified extinction coefficients to the dry (fRHext(%RH, Dry was explored. The measured fRHext(%RH, Dry was compared to theoretical calculations based on Mie theory, using the measured growth factors and assuming homogeneous mixing. The expected complex refractive indices (RIs using the volume weighted mixing rule were compared to the RIs derived from the extinction measurements. Moreover, the differences between assuming a core-shell structure or a homogeneous mixing of the substances is examined. The laboratory results were used as a basis to model the change in the total extinction, the single scattering albedo (ω, and the asymmetry parameter (g in the twilight zone of clouds at 355 nm and 532 nm.

    We found slightly linear to no dependency of fRH(%RH, Dry with size for absorbing substances in contrast to the decreasing exponential behavior with size for purely scattering substances. However, no discernable difference could be made between the two wavelengths used. Less than 5% differences were found between the real parts of the complex refractive indices derived and those calculated using the volume weighted mixing rule, and the imaginary parts had up to a 20% difference. Moreover, for substances with growth factor less than 1.15 there was, in average, less than 5% difference between the extinction efficiencies calculated using a core-shell model and assuming homogeneous mixing for size parameters less than 2.5. For x>2.5 the differences were greater causing and overestimation of the extinction efficiency (

  1. High Resolution Aerosol Data from MODIS Satellite for Urban Air Quality Studies

    Science.gov (United States)

    Chudnovsky, A.; Lyapustin, A.; Wang, Y.; Tang, C.; Schwartz, J.; Koutrakis, P.

    2013-01-01

    The Moderate Resolution Imaging Spectroradiometer (MODIS) provides daily global coverage, but the 10 km resolution of its aerosol optical depth (AOD) product is not suitable for studying spatial variability of aerosols in urban areas. Recently, a new Multi-Angle Implementation of Atmospheric Correction (MAIAC) algorithm was developed for MODIS which provides AOD at 1 km resolution. Using MAIAC data, the relationship between MAIAC AOD and PM(sub 2.5) as measured by the 27 EPA ground monitoring stations was investigated. These results were also compared to conventional MODIS 10 km AOD retrievals (MOD04) for the same days and locations. The coefficients of determination for MOD04 and for MAIAC are R(exp 2) =0.45 and 0.50 respectively, suggested that AOD is a reasonably good proxy for PM(sub 2.5) ground concentrations. Finally, we studied the relationship between PM(sub 2.5) and AOD at the intra-urban scale (10 km) in Boston. The fine resolution results indicated spatial variability in particle concentration at a sub-10 kilometer scale. A local analysis for the Boston area showed that the AOD-PM(sub 2.5) relationship does not depend on relative humidity and air temperatures below approximately 7 C. The correlation improves for temperatures above 7 - 16 C. We found no dependence on the boundary layer height except when the former was in the range 250-500 m. Finally, we apply a mixed effects model approach to MAIAC aerosol optical depth (AOD) retrievals from MODIS to predict PM(sub 2.5) concentrations within the greater Boston area. With this approach we can control for the inherent day-to-day variability in the AOD-PM(sub 2.5) relationship, which depends on time-varying parameters such as particle optical properties, vertical and diurnal concentration profiles and ground surface reflectance. Our results show that the model-predicted PM(sub 2.5) mass concentrations are highly correlated with the actual observations (out-of-sample R(exp 2) of 0.86). Therefore, adjustment

  2. Hygroscopicity Behavior, Activation Properties and Chemical Composition of Atmospheric Aerosol at a Background Site in the Megacity Region of Peking

    Science.gov (United States)

    Henning, Silvia; Nowak, Andreas; Mildenberger, Katrin; Göbel, Tina; Nekat, Bettina; van Pinxteren, Dominik; Herrmann, Hartmut; Zhao, Chunsheng; Wiedensohler, Alfred; Stratmann, Frank

    2010-05-01

    Large areas of China suffer from heavy air pollution (both gaseous and particulate) caused by strong economic growth in the last two decades. However, knowledge concerning the physical and chemical properties of the resulting aerosol particles populations, and their effects on the optical properties of the atmosphere, is still sparse. In the framework of the investigations presented here, comprehensive measurements concerning aerosol particle hygroscopicity, CCN ability, composition, and optical properties were performed. The investigations are part of the DFG-funded project HaChi (Haze in China) and are conducted in collaboration with the Peking University. A conclusive parameterization of aerosol hygroscopicity and activation data is aimed for, which will then be implemented in a meso-scale model to investigate aerosol-cloud-radiation and precipitation interactions. During two intensive measurements campaigns (March 2009 and July/ August 2009), in-situ aerosol measurements have been performed in an air-conditioned mobile laboratory next to the Wuqing Meteorological Station (39°23'8.53"N, 117°1'25.88"E), which is located between Bejing and Tijanjin and is thereby an ideal background site in a megacity region. The particle number size distribution (TDMPS), the particle optical properties (MAAP and nephelometer) and their hygroscopic properties at high RH (HH-TDMA, LACIS-mobile) were characterized as well as their cloud nucleating properties above supersaturation (DMT-CCNC). 24 h PM1 particle samples were continuously collected over the two campaigns in winter and summer using a DIGITEL high volume sampler (DHA-80). Additionally two 6h size-resolved samples (daytime and night-time) were collected each day applying an 11-stage Berner impactor. The size-selection of HH-TDMA, LACIS and the CCNC was synchronized with the Berner stages. Opening analysis of the winter campaign data showed that the HH-TDMA usually detected a hydrophobic and a hygroscopic mode, i.e., the

  3. Highly time-resolved trace element concentrations in aerosols during the Megapoli Paris campaigns

    Science.gov (United States)

    Furger, Markus; Visser, Suzanne; Slowik, Jay G.; Crippa, Monica; Poulain, Laurent; Appel, Karen; Flechsig, Uwe; Prevot, Andre S. H.; Baltensperger, Urs

    2014-05-01

    Trace elements contribute typically only a few percent to the total mass of air pollutants, however, they can affect the environment in significant ways, especially those that are toxic. Furthermore, they are advantageous with respect to a refinement of source apportionment when measured with high time resolution and appropriate size segregation. This approach is especially advantageous in an urban environment with numerous time-variant emission sources distributed across a relatively narrow space, as is typically the setting of a megacity. Two 1-month long field campaigns took place in the framework of the Megapoli project in Paris, France, in the summer of 2009 and in the winter of 2010. Rotating drum impactors (RDI) were operated at two sites in each campaign, one urban, the other one suburban. The RDI segregated the aerosols into three size ranges (PM10-2.5, PM2.5-1 and PM1-0.1) and sampled with 2-hour time resolution. The samples were analyzed with synchrotron radiation induced X-ray fluorescence spectrometry (SR-XRF) at the synchrotron facilities of Paul Scherrer Institute (SLS) and Deutsches Elektronen-Synchrotron (HASYLAB), where a broad range of elements (Na, Mg, Al, Si, P, S, Cl, K, Ca, Ti, V, Cr, Mn, Fe, Ni, Cu, Zn, Se, Sr, Zr, Cd, Sn, Sb, Ba, Pb) was analyzed for each size range. Time series of the analyzed elements for the different sites and campaigns were prepared to characterize the aerosol trace element composition and temporal behavior for the different weather situations and urban environments. They allow for the distinction of regional vs. local sources and transport, and provide a basis for source apportionment calculations. Local and regional contributions of traffic, including re-suspension, break wear and exhaust, wood burning, marine and other sources will be discussed. Indications of long-range transport from Polish coal emissions in the city center of Paris were also found.

  4. Modeling regional air quality and climate: improving organic aerosol and aerosol activation processes in WRF/Chem version 3.7.1

    Directory of Open Access Journals (Sweden)

    K. Yahya

    2017-06-01

    Full Text Available Air quality and climate influence each other through the uncertain processes of aerosol formation and cloud droplet activation. In this study, both processes are improved in the Weather, Research and Forecasting model with Chemistry (WRF/Chem version 3.7.1. The existing Volatility Basis Set (VBS treatments for organic aerosol (OA formation in WRF/Chem are improved by considering the following: the secondary OA (SOA formation from semi-volatile primary organic aerosol (POA, a semi-empirical formulation for the enthalpy of vaporization of SOA, and functionalization and fragmentation reactions for multiple generations of products from the oxidation of VOCs. Over the continental US, 2-month-long simulations (May to June 2010 are conducted and results are evaluated against surface and aircraft observations during the Nexus of Air Quality and Climate Change (CalNex campaign. Among all the configurations considered, the best performance is found for the simulation with the 2005 Carbon Bond mechanism (CB05 and the VBS SOA module with semivolatile POA treatment, 25 % fragmentation, and the emissions of semi-volatile and intermediate volatile organic compounds being 3 times the original POA emissions. Among the three gas-phase mechanisms (CB05, CB6, and SAPRC07 used, CB05 gives the best performance for surface ozone and PM2. 5 concentrations. Differences in SOA predictions are larger for the simulations with different VBS treatments (e.g., nonvolatile POA versus semivolatile POA compared to the simulations with different gas-phase mechanisms. Compared to the simulation with CB05 and the default SOA module, the simulations with the VBS treatment improve cloud droplet number concentration (CDNC predictions (normalized mean biases from −40.8 % to a range of −34.6 to −27.7 %, with large differences between CB05–CB6 and SAPRC07 due to large differences in their OH and HO2 predictions. An advanced aerosol activation

  5. Size-resolved aerosol chemistry on Whistler Mountain, Canada with a High-Resolution Aerosol Mass Spectrometer during INTEX-B

    Directory of Open Access Journals (Sweden)

    Y. Sun

    2008-12-01

    Full Text Available An Aerodyne High Resolution Time-of-Flight Aerosol Mass Spectrometer (HR-ToF-AMS was deployed at the peak of Whistler Mountain (elevation 2182 m-MSL, British Columbia, from 19 April to 16 May 2006, as part of the Intercontinental Chemical Transport Experiment Phase B (INTEX-B campaign. The mass concentrations and size distributions of non-refractory submicron particle (NR-PM1 species (i.e., sulfate, nitrate, ammonium, chloride, and organics were measured in situ every 5 min. The HR-ToF-AMS results agreed well with collocated measurements. The average concentration of non-refractory submicron particulate matter (NR-PM1; 1.9 μg m−3 is similar to those observed at other remote, high elevation sites in North America. Episodes of enhanced aerosol loadings were observed, due to influences of regional and trans-Pacific transport of air pollution. Organics and sulfate were the dominant species, on average accounting for 55% and 30%, respectively, of the NR-PM1 mass. The average size distributions of sulfate and ammonium both showed a~large accumulation mode peaking around 500–600 nm in Dva while those of organic aerosol (OA and nitrate peaked at ~300 nm. The size differences suggest that sulfate and OA were mostly present in external mixtures from different source origins. We also quantitatively determined the elemental composition of OA using the high resolution mass spectra. Overall, OA at Whistler Peak was highly oxygenated, with an average organic-mass-to-organic-carbon ratio (OM/OC of 2.28±0.23 and an atomic ratio of oxygen-to-carbon (O/C of 0.83±0.17. The nominal formula for OA was C1H1.66N0.03O0.83 for the entire study. Two significant trans-Pacific dust events originated from Asia were observed at Whistler Peak during this study. While both events were characterized with significant enhancements of coarse mode particles and mineral

  6. Submicron aerosol analysis and organic source apportionment in an urban atmosphere in Pearl River Delta of China using high-resolution aerosol mass spectrometry

    Science.gov (United States)

    He, Ling-Yan; Huang, Xiao-Feng; Xue, Lian; Hu, Min; Lin, Yun; Zheng, Jun; Zhang, Renyi; Zhang, Yuan-Hang

    2011-06-01

    The Pearl River Delta (PRD) region in South China is one of the most economically developed regions in China while also noted for its severe air pollution, especially in the urban environments. In order to understand in depth the aerosol chemistry and the emission sources in PRD, an Aerodyne high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS) was deployed at an urban site in the Hong Kong-Shenzhen metropolitan area between 25 October and 2 December 2009. Ten minute-resolved measurement data were analyzed, and an average mass concentration of 44.5 ± 34.0 μg m-3 was calculated for the entire campaign. On average, organic matter was the most abundant PM1 component accounting for 39.7% of the total mass, followed by sulfate (24.5%), black carbon (measured by aethalometer, 14.0%), ammonium (10.2%), nitrate (10.0%), and chloride (1.6%). Moreover, organic matter comprised an increasing fraction of the PM1 loading as the PM1 loading increased, denoting its key role in particulate pollution in this region. Calculations of organic elemental composition based on the high-resolution organic mass spectra obtained indicated that C, H, O, and N on average contributed 33.8%, 55.1%, 10.2%, and 0.9%, respectively, to the total atomic numbers of organic aerosol (OA), which corresponded to an OM/OC ratio (the ratio of organic matter mass/organic carbon mass) of 1.57 ± 0.08. Positive matrix factorization analysis was then conducted on the high-resolution organic mass spectral data set. Four OA components were identified, including a hydrocarbon-like (HOA), a biomass burning (BBOA), and two oxygenated (LV-OOA and SV-OOA) components, which on average accounted for 29.5%, 24.1%, 18.8%, and 27.6%, respectively, of the total organic mass. The HOA was found to have contributions from both fossil fuel combustion and cooking emissions, while the BBOA was well correlated with acetonitrile, a known biomass burning marker. The LV-OOA and SV-OOA corresponded to more aged and

  7. Cloud droplet activation mechanisms of amino acid aerosol particles: insight from molecular dynamics simulations

    Directory of Open Access Journals (Sweden)

    Xin Li

    2013-07-01

    Full Text Available Atmospheric amino acids constitute a large fraction of water-soluble organic nitrogen compounds in aerosol particles, and have been confirmed as effective cloud condensation nuclei (CCN materials in laboratory experiments. We present a molecular dynamics (MD study of six amino acids with different structures and chemical properties that are relevant to the remote marine atmospheric aerosol–cloud system, with the aim of investigating the detailed mechanism of their induced changes in surface activity and surface tension, which are important properties for cloud drop activation. Distributions and orientations of the amino acid molecules are studied; these l-amino acids are serine (SER, glycine (GLY, alanine (ALA, valine (VAL, methionine (MET and phenylalanine (PHE and are categorised as hydrophilic and amphiphilic according to their affinities to water. The results suggest that the presence of surface-concentrated amphiphilic amino acid molecules give rise to enhanced Lennard–Jones repulsion, which in turn results in decreased surface tension of a planar interface and an increased surface tension of the spherical interface of droplets with diameters below 10 nm. The observed surface tension perturbation for the different amino acids under study not only serves as benchmark for future studies of more complex systems, but also shows that amphiphilic amino acids are surface active. The MD simulations used in this study reproduce experimental results of surface tension measurements for planar interfaces and the method is therefore applicable for spherical interfaces of nano-size for which experimental measurements are not possible to conduct.

  8. An integrated approach using high time-resolved tools to study the origin of aerosols

    Energy Technology Data Exchange (ETDEWEB)

    Di Gilio, A. [Chemistry Department, University of Bari, via Orabona, 4, 70126 Bari (Italy); ARPA PUGLIA, Corso Trieste, 27, 70126 Bari (Italy); Gennaro, G. de, E-mail: gianluigi.degennaro@uniba.it [Chemistry Department, University of Bari, via Orabona, 4, 70126 Bari (Italy); ARPA PUGLIA, Corso Trieste, 27, 70126 Bari (Italy); Dambruoso, P. [Chemistry Department, University of Bari, via Orabona, 4, 70126 Bari (Italy); ARPA PUGLIA, Corso Trieste, 27, 70126 Bari (Italy); Ventrella, G. [Chemistry Department, University of Bari, via Orabona, 4, 70126 Bari (Italy)

    2015-10-15

    Long-range transport of natural and/or anthropogenic particles can contribute significantly to PM10 and PM2.5 concentrations and some European cities often fail to comply with PM daily limit values due to the additional impact of particles from remote sources. For this reason, reliable methodologies to identify long-range transport (LRT) events would be useful to better understand air pollution phenomena and support proper decision-making. This study explores the potential of an integrated and high time-resolved monitoring approach for the identification and characterization of local, regional and long-range transport events of high PM. In particular, the goal of this work was also the identification of time-limited event. For this purpose, a high time-resolved monitoring campaign was carried out at an urban background site in Bari (southern Italy) for about 20 days (1st–20th October 2011). The integration of collected data as the hourly measurements of inorganic ions in PM{sub 2.5} and their gas precursors and of the natural radioactivity, in addition to the analyses of aerosol maps and hourly back trajectories (BT), provided useful information for the identification and chemical characterization of local sources and trans-boundary intrusions. Non-sea salt (nss) sulfate levels were found to increase when air masses came from northeastern Europe and higher dispersive conditions of the atmosphere were detected. Instead, higher nitrate and lower nss-sulfate concentrations were registered in correspondence with air mass stagnation and attributed to local traffic source. In some cases, combinations of local and trans-boundary sources were observed. Finally, statistical investigations such as the principal component analysis (PCA) applied on hourly ion concentrations and the cluster analyses, the Potential Source Contribution Function (PSCF) and the Concentration Weighted Trajectory (CWT) models computed on hourly back-trajectories enabled to complete a cognitive

  9. Relating CCN activity, volatility, and droplet growth kinetics of β-caryophyllene secondary organic aerosol

    Directory of Open Access Journals (Sweden)

    A. Asa-Awuku

    2009-02-01

    Full Text Available This study investigates the droplet formation characteristics of secondary organic aerosol (SOA formed during the ozonolysis of sesquiterpene β-caryophyllene (with and without hydroxyl radicals present. Emphasis is placed on understanding the role of semi-volatile material on Cloud Condensation Nucleus (CCN activity and droplet growth kinetics. Aging of β-caryophyllene SOA significantly affects all CCN-relevant properties measured throughout the experiments. Using a thermodenuder and two CCN instruments, we find that CCN activity is a strong function of temperature (activation diameter at ~0.6% supersaturation: 100±10 nm at 20°C and 130±10 nm at 35°C, suggesting that the hygroscopic fraction of the SOA is volatile. The water-soluble organic carbon (WSOC is extracted from the SOA and characterized with Köhler Theory Analysis (KTA; the results suggest that the WSOC is composed of low molecular weight (<200 g mol−1 slightly surface-active material that constitute 5–15% of the SOA mass. These properties are similar to the water-soluble fraction of monoterpene SOA, suggesting that predictive understanding of SOA CCN activity requires knowledge of the WSOC fraction but not its exact speciation. Droplet growth kinetics of the CCN are found to be strongly anticorrelated with WSOC fraction, suggesting that the insoluble material in the SOA forms a kinetic barrier that delays droplet growth. Overall, volatilization effects can increase activation diameters by 30%, and depress droplet growth rate by a factor of two; these results may have important implications for the droplet formation characteristics of SOA, and the atmospheric relevance of CCN measurements carried out at temperatures different from ambient.

  10. Investigation of mineral aerosols radiative effects over High Mountain Asia in 1990-2009 using a regional climate model

    Science.gov (United States)

    Ji, Zhenming; Kang, Shichang; Zhang, Qianggong; Cong, Zhiyuan; Chen, Pengfei; Sillanpää, Mika

    2016-09-01

    Mineral aerosols scatter and absorb incident solar radiation in the atmosphere, and play an important role in the regional climate of High Mountain Asia (the domain includes the Himalayas, Tibetan Plateau, Pamir, Hindu-kush, Karakorum and Tienshan Mountains). Dust deposition on snow/ice can also change the surface albedo, resulting in perturbations in the surface radiation balance. However, most studies that have made quantitative assessments of the climatic effect of mineral aerosols over the High Mountain Asia region did not consider the impact of dust on snow/ice at the surface. In this study, a regional climate model coupled with an aerosol-snow/ice feedback module was used to investigate the emission, distribution, and deposition of dust and the climatic effects of aerosols over High Mountain Asia. Two sets of simulations driven by a reanalysis boundary condition were performed, i.e., with and without dust-climate feedback. Results indicated that the model captured the spatial and temporal features of the climatology and aerosol optical depth (AOD). High dust emission fluxes were simulated in the interior of the Tibetan Plateau (TP) and the Yarlung Tsangpo Valley in March-April-May (MAM), with a decreasing trend during 1990-2009. Dry deposition was controlled by the topography, and its spatial and seasonal features agreed well with the dust emission fluxes. The maximum wet deposition occurred in the western (southern and central) TP in MAM (JJA). A positive surface radiative forcing was induced by dust, including aerosol-snow/ice feedback, resulting in 2-m temperature increases of 0.1-0.5 °C over the western TP and Kunlun Mountains in MAM. Mineral dust also caused a decrease of 5-25 mm in the snow water equivalent (SWE) over the western TP, Himalayas, and Pamir Mountains in DJF and MAM. The long-term regional mean radiative forcing via dust deposition on snow showed an rising trend during 1990-2009, which suggested the contribution of aerosols surface

  11. In-canopy gradients, composition, and sources of optically active aerosols over the Amazon forest

    Science.gov (United States)

    Guyon, P.; Graham, B.; Roberts, G. C.; Mayol-Bracero, O. L.; Andreae, M. O.; Artaxo, P.; Maenhaut, W.

    2003-04-01

    As part of the European contribution to the Large-Scale Biosphere-Atmosphere Experiment in Amazonia (LBA-EUSTACH), size-fractionated aerosol samples were collected at a primary rainforest site in the Brazilian Amazon during the wet and dry seasons. Daytime-nighttime segregated sampling was carried out at three different heights (above, within and below canopy level) on a 54 m meteorological tower. The samples were analyzed for up to 19 trace elements, equivalent black carbon (BCe) and mass concentrations. Additionally, measurements of scattering and absorption coefficients were performed. Absolute principal component analysis revealed that the wet and dry season aerosols contained the same three main aerosol components, namely a natural biogenic, a pyrogenic, and a soil dust component, but that these were present in different (absolute and relative) amounts. The elements related to biomass burning and soil dust generally exhibited highest concentrations above the canopy and during daytime, whilst forest-derived aerosol was more concentrated underneath the canopy and during nighttime. These variations can be largely attributed to daytime convective mixing and the formation of a shallow nocturnal boundary layer, along with the possibility of enhanced nighttime release of biogenic aerosol particles. All three components contributed significantly to light extinction, suggesting that, in addition to pyrogenic particles, biogenic and soil dust aerosols must be taken into account when modeling the physical and optical properties of aerosols in forested regions such the Amazon Basin.

  12. The vapor pressures and activities of dicarboxylic acids reconsidered: the impact of the physical state of the aerosol

    Directory of Open Access Journals (Sweden)

    V. Soonsin

    2010-08-01

    Full Text Available We present vapor pressure data of the C2 to C5 dicarboxylic acids deduced from measured evaporation rates of single levitated particles as both, aqueous droplets and solid crystals. The data of aqueous solution particles over a wide concentration range allow us to directly calculate activities of the dicarboxylic acids and comparison of these activities with parameterizations reported in the literature. The data of the pure liquid state acids, i.e. the dicarboxylic acids in their supercooled melt state, exhibit no even-odd alternation in vapor pressure, while the acids in the solid form do. This observation is consistent with the known solubilities of the acids and our measured vapor pressures of the supercooled melt. Thus, the gas/particle partitioning of the different dicarboxylic acids in the atmosphere depends strongly on the physical state of the aerosol phase, the difference being largest for the even acids.

    Our results show also that, in general, measurements of vapor pressures of solid dicarboxylic acids may be compromised by the presence of amorphous fractions, polymorphic forms, crystalline structures with a high defect number, and/or solvent inclusions in the solid material, yielding a higher vapor pressure than the one of the thermodynamically stable crystalline form at the same temperature.

  13. The vapor pressures and activities of dicarboxylic acids reconsidered: the impact of the physical state of the aerosol

    Directory of Open Access Journals (Sweden)

    V. Soonsin

    2010-12-01

    Full Text Available We present vapor pressure data of the C2 to C5 dicarboxylic acids deduced from measured evaporation rates of single levitated particles as both, aqueous droplets and solid crystals. The data of aqueous solution particles over a wide concentration range allow us to directly calculate activities of the dicarboxylic acids and comparison of these activities with parameterizations reported in the literature. The data of the pure liquid state acids, i.e. the dicarboxylic acids in their supercooled melt state, exhibit no even-odd alternation in vapor pressure, while the acids in the solid form do. This observation is consistent with the known solubilities of the acids and our measured vapor pressures of the supercooled melt. Thus, the gas/particle partitioning of the different dicarboxylic acids in the atmosphere depends strongly on the physical state of the aerosol phase, the difference being largest for the even acids. Our results show also that, in general, measurements of vapor pressures of solid dicarboxylic acids may be compromised by the presence of polymorphic forms, crystalline structures with a high defect number, and/or solvent inclusions in the solid material, yielding a higher vapor pressure than the one of the thermodynamically stable crystalline form at the same temperature.

  14. Absence of detectable influenza RNA transmitted via aerosol during various human respiratory activities--experiments from Singapore and Hong Kong.

    Directory of Open Access Journals (Sweden)

    Julian W Tang

    Full Text Available Two independent studies by two separate research teams (from Hong Kong and Singapore failed to detect any influenza RNA landing on, or inhaled by, a life-like, human manikin target, after exposure to naturally influenza-infected volunteers. For the Hong Kong experiments, 9 influenza-infected volunteers were recruited to breathe, talk/count and cough, from 0.1 m and 0.5 m distance, onto a mouth-breathing manikin. Aerosolised droplets exhaled from the volunteers and entering the manikin's mouth were collected with PTFE filters and an aerosol sampler, in separate experiments. Virus detection was performed using an in-house influenza RNA reverse-transcription polymerase chain reaction (RT-PCR assay. No influenza RNA was detected from any of the PTFE filters or air samples. For the Singapore experiments, 6 influenza-infected volunteers were asked to breathe (nasal/mouth breathing, talk (counting in English/second language, cough (from 1 m/0.1 m away and laugh, onto a thermal, breathing manikin. The manikin's face was swabbed at specific points (around both eyes, the nostrils and the mouth before and after exposure to each of these respiratory activities, and was cleaned between each activity with medical grade alcohol swabs. Shadowgraph imaging was used to record the generation of these respiratory aerosols from the infected volunteers and their impact onto the target manikin. No influenza RNA was detected from any of these swabs with either team's in-house diagnostic influenza assays. All the influenza-infected volunteers had diagnostic swabs taken at recruitment that confirmed influenza (A/H1, A/H3 or B infection with high viral loads, ranging from 10(5-10(8 copies/mL (Hong Kong volunteers/assay and 10(4-10(7 copies/mL influenza viral RNA (Singapore volunteers/assay. These findings suggest that influenza RNA may not be readily transmitted from naturally-infected human source to susceptible recipients via these natural respiratory activities, within

  15. Sea Spray Aerosols

    DEFF Research Database (Denmark)

    Butcher, Andrew Charles

    emissions produced directly from bubble bursting as the result of air entrainment from breaking waves and particles generated from secondary emissions of volatile organic compounds. In the first paper, we study the chemical properties of particles produced from several sea water proxies with the use...... of a cloud condensation nuclei ounter. Proxy solutions with high inorganic salt concentrations and some organics produce sea spray aerosol particles with little change in cloud condensation activity relative to pure salts. Comparison is made between a frit based method for bubble production and a plunging...... a relationship between plunging jet particle ux, oceanic particle ux, and energy dissipation rate in both systems. Previous sea spray aerosol studies dissipate an order of magnitude more energy for the same particle ux production as the open ocean. A scaling factor related to the energy expended in air...

  16. Sea Spray Aerosols

    DEFF Research Database (Denmark)

    Butcher, Andrew Charles

    emissions produced directly from bubble bursting as the result of air entrainment from breaking waves and particles generated from secondary emissions of volatile organic compounds. In the first paper, we study the chemical properties of particles produced from several sea water proxies with the use...... of a cloud condensation nuclei ounter. Proxy solutions with high inorganic salt concentrations and some organics produce sea spray aerosol particles with little change in cloud condensation activity relative to pure salts. Comparison is made between a frit based method for bubble production and a plunging...... a relationship between plunging jet particle ux, oceanic particle ux, and energy dissipation rate in both systems. Previous sea spray aerosol studies dissipate an order of magnitude more energy for the same particle ux production as the open ocean. A scaling factor related to the energy expended in air...

  17. High-resolution modeling of the influences of absorbing aerosols on rainfall over northern India and the Himalaya foothills during boreal summer

    Science.gov (United States)

    Kim, K.; Lau, W. K.; Tao, W.; Shi, J. J.; Tan, Q.; Chin, M.; Matsui, T.; Kemp, E. M.; Peters-Lidard, C. D.

    2012-12-01

    High elevation and steep topography of Tibetan Plateau and the Himalayas foothills regions are important components of the South Asian summer monsoon system. Strong orographic forcing combined with abundant moisture from the Arabian Sea and the Bay of Bengal and aerosols stacked up against the southern slope of the Tibetan Plateau produce complex physical and dynamical effects on monsoon rainfall and circulation. In this work, we use the NASA Unified Weather Research and Forecasting (Nu-WRF) model to study the effect of aerosol radiative forcing on the short-term predictability (1-7 days) of the South Asian monsoon rainfall system. Two sets of 7-day forecasting experiments were conducted with and without aerosol radiative forcing. Each set consists of 34 7-day forcasts with initial conditions from daily reanalysis and GEOS-5 aerosol distribution (only for aerosol run) from June 11- July 14, 2008. Nu-WRF, without aerosol forcing captures the horizontal distribution of 7-day mean precipitation reasonably well, but it tends to over-estimates rainfall over the central India. The biases are especially larger in the upwind side of the western Ghats and northeast India and Bangladesh. Preliminary results show that inclusion of aerosol radiative forcing and interaction with dynamics reduces rainfall over the Indo-Gangetic plain where aerosol loadinng is high, but enhances rainfall downstream of the prevailing monsoon flow in the southern slope of Tibetan Plateau, especially over the northeast India and foothills regions, consistent with the EHP hypothesis. Effect of aerosol radiative forcing is small during the first two days of forecasts. Rainfall anomalies generated by atmospheric feedback induced by aerosol radiative forcing becomes statistically significant and large enough to be separable from growing model biases after three days of simulation. The results indicate the inclusion of aerosol radiative forcing may improve short-term (4-7 day) forecasting skill in

  18. Protection of air in premises and environment against beryllium aerosols

    Energy Technology Data Exchange (ETDEWEB)

    Bitkolov, N.Z.; Vishnevsky, E.P.; Krupkin, A.V. [Research Inst. of Industrial and Marine Medicine, St. Petersburg (Russian Federation)

    1998-01-01

    First and foremost, the danger of beryllium aerosols concerns a possibility of their inhalation. The situation is aggravated with high biological activity of the beryllium in a human lung. The small allowable beryllium aerosols` concentration in air poses a rather complex and expensive problem of the pollution prevention and clearing up of air. The delivery and transportation of beryllium aerosols from sites of their formation are defined by the circuit of ventilation, that forms aerodynamics of air flows in premises, and aerodynamic links between premises. The causes of aerosols release in air of premises from hoods, isolated and hermetically sealed vessels can be vibrations, as well as pulses of temperature and pressure. Furthermore, it is possible the redispersion of aerosols from dirty surfaces. The effective protection of air against beryllium aerosols at industrial plants is provided by a complex of hygienic measures: from individual means of breath protection up to collective means of the prevention of air pollution. (J.P.N.)

  19. High lightning activity in maritime clouds near Mexico

    Directory of Open Access Journals (Sweden)

    B. Kucienska

    2012-01-01

    Full Text Available Lightning activity detected by the World Wide Lightning Location Network (WWLLN over oceanic regions adjacent to Mexico is often as high as that observed over the continent. In order to explore the possible cause of the observed high flash density over those regions, the relationships between lightning, rainfall, vertical hydrometeor profiles, latent heating, wind variability and aerosol optical thickness are analyzed. The characteristics of lightning and precipitation over four oceanic zones adjacent to Mexican coastlines are contrasted against those over the continent. In addition, we compare two smaller regions over the Tropical Pacific Ocean: one located within the Inter-Tropical Converge Zone and characterized by high rainfall and weak lightning activity and the other influenced by a continental jet and presenting high rainfall and strong lightning activity over the Gulf of Tehuantepec. Maritime precipitating clouds that develop within the region influenced by offshore winds exhibit similar properties to continental clouds: large content of precipitation ice and an increased height range of coexistence of precipitation ice and cloud water. During the rainy season, monthly distribution of lightning within the region influenced by the continental jet is contrary to that of rainfall. Moreover, the monthly variability of lightning is very similar to the variability of the meridional wind component and it is also related to the variability of aerosol optical depth. The analysis strongly suggests that the high lightning activity observed over the Gulf of Tehuantepec is caused by continental cloud condensation nuclei advected over the ocean.

  20. High lightning activity in maritime clouds near Mexico

    Science.gov (United States)

    Kucienska, B.; Raga, G. B.; Romero-Centeno, R.

    2012-09-01

    Lightning activity detected by the World Wide Lightning Location Network (WWLLN) over oceanic regions adjacent to Mexico is often as high as that observed over the continent. In order to explore the possible causes of the observed high flash density over those regions, the relationships between lightning, rainfall, vertical hydrometeor profiles, latent heating, wind variability and aerosol optical depth are analyzed. The characteristics of lightning and precipitation over four oceanic zones adjacent to Mexican coastlines are contrasted against those over the continent. The number of flashes per rainfall over some coastal maritime regions is found to be higher than over the continent. The largest number of flashes per rainfall is observed during the biomass burning season. In addition, we compare two smaller areas of the Tropical Pacific Ocean: one located within the Inter-Tropical Convergence Zone and characterized by high rainfall and weak lightning activity and the other one influenced by a continental wind jet and characterized by high rainfall and strong lightning activity. During the rainy season, the monthly distribution of lightning within the region influenced by the continental wind jet is contrary to that of rainfall. Moreover, the monthly variability of lightning is very similar to the variability of the meridional wind component and it is also related to the variability of aerosol optical depth. The analysis suggests that the high lightning activity observed over coastal Pacific region is linked to the continental cloud condensation nuclei advected over the ocean. Analysis of daily observations indicates that the greatest lightning density is observed for moderate values of the aerosol optical depth, between 0.2 and 0.35.

  1. The application of single particle aerosol mass spectrometry for the detection and identification of high explosives and chemical warfare agents

    Energy Technology Data Exchange (ETDEWEB)

    Martin, Audrey Noreen [Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States)

    2006-01-01

    Single Particle Aerosol Mass Spectrometry (SPAMS) was evaluated as a real-time detection technique for single particles of high explosives. Dual-polarity time-of-flight mass spectra were obtained for samples of 2,4,6-trinitrotoluene (TNT), 1,3,5-trinitro-1,3,5-triazinane (RDX), and pentaerythritol tetranitrate (PETN); peaks indicative of each compound were identified. Composite explosives, Comp B, Semtex 1A, and Semtex 1H were also analyzed, and peaks due to the explosive components of each sample were present in each spectrum. Mass spectral variability with laser fluence is discussed. The ability of the SPAMS system to identify explosive components in a single complex explosive particle (~1 pg) without the need for consumables is demonstrated. SPAMS was also applied to the detection of Chemical Warfare Agent (CWA) simulants in the liquid and vapor phases. Liquid simulants for sarin, cyclosarin, tabun, and VX were analyzed; peaks indicative of each simulant were identified. Vapor phase CWA simulants were adsorbed onto alumina, silica, Zeolite, activated carbon, and metal powders which were directly analyzed using SPAMS. The use of metal powders as adsorbent materials was especially useful in the analysis of triethyl phosphate (TEP), a VX stimulant, which was undetectable using SPAMS in the liquid phase. The capability of SPAMS to detect high explosives and CWA simulants using one set of operational conditions is established.

  2. Quantifying the Impact of Icelandic Dust Storms on High-Latitude Aerosol

    Science.gov (United States)

    Browse, Jo; Dorsi, Kelly; Dagsson Waldhauserova, Pavla; Murray, Ben

    2017-04-01

    Using a combination of observations, meteorological climatologies and modelling we have developed an Icelandic dust storm emission inventory. Here we present results from a global modelling study quantifying the contribution of Icelandic dust to high-latitude: ice nucleating particles (INP), cloud condensation nuclei (CCN) and PM2.5. Our results suggest that Icelandic dust cannot explain the formation and persistence of summertime mixed-phase Arctic marine clouds, as summertime marine clouds are too warm for Icelandic dust to serve as INP. However, in colder regions (such as Greenland) Icelandic dust may sporadically contribute to INP. The contribution of Icelandic dust to high-latitude CCN was shown to be complex. Indeed, our results indicate a decrease in high-latitude CCN in the aftermath of Icelandic dust storms. This decrease is due to the short-term increase of the Arctic atmospheric condensation sink and the resulting suppression of nucleation processes (a significant source of Arctic summertime CCN). Finally, Icelandic dust storms are shown to significantly contribute to high-latitude summertime PM2.5 (and PM10) both during (˜100 {μ}gm-3) and in the aftermath (˜10 {μ}gm-3) of dust events. Our results suggest that Icelandic dust storms (neglected in most global climate models) may in the short term increase aerosol optical depth (strongly correlated to PM2.5) at high latitudes. Additionally, Icelandic dust storms are likely to contribute to poor air quality as well as reduced visibility in the Arctic boundary layer. Thus, we argue for the adoption of high-latitude dust emissions in climate and NWP models.

  3. High-Resolution Mass Spectroscopic Analysis of Secondary Organic Aerosol Generated by Ozonolysis of Isoprene

    Energy Technology Data Exchange (ETDEWEB)

    Nguyen, Tran B; Bateman, Adam P; Bones, David L; Nizkorodov, Serguei; Laskin, Julia; Laskin, Alexander

    2010-02-01

    The chemical composition of secondary organic aerosol (SOA) generated from the ozonolysis of isoprene (C5H8) in the presence of an OH scavenger was examined using high-resolution electrospray ionization mass spectrometry (ESI-MS). The chemical composition of SOA is complex, with more than 1000 assigned peaks observed in the positive and negative ion mode spectra. Only a small fraction of peaks corresponds to known products of isoprene oxidation, such as pyruvic acid, glycolic acid, methylglyoxal, etc. The absolute majority of the detected peaks correspond to highly oxidized oligomeric constituents of SOA, with an average O:C molar ratio of ~0.6. The corresponding organic mass (OM) to organic oxygen (OO) ratio is OM/OO ~2.4. Approximately 8% of oxygen atoms in SOA are in the form of peroxides as quantified with an iodide test. Double bond equivalency (DBE) factors, representing the sum of all double bonds and rings, increase by 1 for every 2-3 additional carbon atoms in the molecule. The prevalent oligomer building blocks are therefore carbonyls or carboxylic acids with a C2-C3 skeleton. Kendrick analysis suggests that simple aldehydes, specifically formaldehyde, acetaldehyde, and methylglyoxal can serve as monomeric building blocks in the observed oligomers. The large number of reactive functional groups, especially organic peroxides and carbonyls, suggests that isoprene/O3 SOA should be prone to chemical and photochemical aging.

  4. Application of several activity coefficient models to water-organic-electrolyte aerosols of atmospheric interest

    Directory of Open Access Journals (Sweden)

    T. Raatikainen

    2005-01-01

    Full Text Available In this work, existing and modified activity coefficient models are examined in order to assess their capabilities to describe the properties of aqueous solution droplets relevant in the atmosphere. Five different water-organic-electrolyte activity coefficient models were first selected from the literature. Only one of these models included organics and electrolytes which are common in atmospheric aerosol particles. In the other models, organic species were solvents such as alcohols, and important atmospheric ions like NH4+ could be missing. The predictions of these models were compared to experimental activity and solubility data in aqueous single electrolyte solutions with 31 different electrolytes. Based on the deviations from experimental data and on the capabilities of the models, four predictive models were selected for fitting of new parameters for binary and ternary solutions of common atmospheric electrolytes and organics. New electrolytes (H+, NH4+, Na+, Cl-, NO3- and SO42- and organics (dicarboxylic and some hydroxy acids were added and some modifications were made to the models if it was found useful. All new and most of the existing parameters were fitted to experimental single electrolyte data as well as data for aqueous organics and aqueous organic-electrolyte solutions. Unfortunately, there are very few data available for organic activities in binary solutions and for organic and electrolyte activities in aqueous organic-electrolyte solutions. This reduces model capabilities in predicting solubilities. After the parameters were fitted, deviations from measurement data were calculated for all fitted models, and for different data types. These deviations and the calculated property values were compared with those from other non-electrolyte and organic-electrolyte models found in the literature. Finally, hygroscopic growth factors were calculated for four 100 nm organic-electrolyte particles and these predictions were compared to

  5. A case study of high sea salt aerosol (SSA) concentrations as a hazard to aviation

    OpenAIRE

    2015-01-01

    Abstract: On the night of 2nd January 2014 an aircraft on approach to Cork airport was required to abort a landing attempt due to sea salt aerosol (SSA) accretion on the windscreen. The salt reduced forward facing visibility to dangerously low levels. This was the first time such an incident was recorded by Irelands Air Accident Investigation Unit. This paper describes the meteorological conditions at the time of the aborted landing approach. Sea salt aerosol formation mechanisms are ela...

  6. Evaluating the degree of oxygenation of organic aerosol during foggy and hazy days in Hong Kong using high-resolution time-of-flight aerosol mass spectrometry (HR-ToF-AMS

    Directory of Open Access Journals (Sweden)

    Y. J. Li

    2013-02-01

    Full Text Available The chemical characteristics of organic aerosol (OA are still poorly constrained. Here we present observation results of the degree of oxygenation of OA based on high-resolution time-of-flight aerosol mass spectrometry (HR-ToF-AMS measurements made at a coastal site in Hong Kong from late April to the end of May in 2011. Two foggy periods and one hazy period were chosen for detailed analysis to compare the changes in the degree of oxygenation of OA due to different processes. The Extended Aerosol Inorganic Model (E-AIM predicted a fine particle liquid water content (LWCfp up to 85 μg m−3 during the foggy days. Particle concentration as measured by HR-ToF-AMS was up to 60 μg m−3 during the hazy days and up to 30 μg m−3 during the foggy days. The degree of oxygenation of OA, as indicated by several parameters including the fraction of m/z 44 in organic mass spectra (f44, the elemental ratio of oxygen to carbon (O : C, and the carbon oxidation state (OSc, was evaluated against the odd oxygen (Ox concentration, LWCfp, ionic strength (IS, and in-situ pH (pHis. Results suggest that the high concentration of OA (on average 11 μg m−3 and the high degree of oxygenation (f44 = 0.15, O : C = 0.51, and OSc = −0.31 during the hazy period were mainly due to gas-phase oxidation. During the foggy periods with low photochemical activities, the degree of oxygenation of OA was almost as high as that on the hazy days and significantly higher than that during non-foggy/non-hazy days. However, the OA evolved quite differently in the two foggy periods. The first foggy period in late April saw a larger LWCfp and a lower Ox concentration and the OA was made up of ~ 20% semi

  7. Evaluating Global Aerosol Models and Aerosol and Water Vapor Properties Near Clouds

    Energy Technology Data Exchange (ETDEWEB)

    Turner, David, D.; Ferrare, Richard, A.

    2011-07-06

    The 'Evaluating Global Aerosol Models and Aerosol and Water Vapor Properties Near Clouds' project focused extensively on the analysis and utilization of water vapor and aerosol profiles derived from the ARM Raman lidar at the Southern Great Plains ARM site. A wide range of different tasks were performed during this project, all of which improved quality of the data products derived from the lidar or advanced the understanding of atmospheric processes over the site. These activities included: upgrading the Raman lidar to improve its sensitivity; participating in field experiments to validate the lidar aerosol and water vapor retrievals; using the lidar aerosol profiles to evaluate the accuracy of the vertical distribution of aerosols in global aerosol model simulations; examining the correlation between relative humidity and aerosol extinction, and how these change, due to horizontal distance away from cumulus clouds; inferring boundary layer turbulence structure in convective boundary layers from the high-time-resolution lidar water vapor measurements; retrieving cumulus entrainment rates in boundary layer cumulus clouds; and participating in a field experiment that provided data to help validate both the entrainment rate retrievals and the turbulent profiles derived from lidar observations.

  8. Evaluation of applicability of high-resolution multiangle imaging photo-polarimetric observations for aerosol atmospheric correction

    Science.gov (United States)

    Kalashnikova, Olga; Garay, Michael; Xu, Feng; Diner, David; Seidel, Felix

    2016-07-01

    Multiangle spectro-polarimetric measurements have been advocated as an additional tool for better understanding and quantifying the aerosol properties needed for atmospheric correction for ocean color retrievals. The central concern of this work is the assessment of the effects of absorbing aerosol properties on remote sensing reflectance measurement uncertainty caused by neglecting UV-enhanced absorption of carbonaceous particles and by not accounting for dust nonsphericity. In addition, we evaluate the polarimetric sensitivity of absorbing aerosol properties in light of measurement uncertainties achievable for the next generation of multi-angle polarimetric imaging instruments, and demonstrate advantages and disadvantages of wavelength selection in the UV/VNIR range. In this work a vector Markov Chain radiative transfer code including bio-optical models was used to quantitatively evaluate in water leaving radiances between atmospheres containing realistic UV-enhanced and non-spherical aerosols and the SEADAS carbonaceous and dust-like aerosol models. The phase matrices for the spherical smoke particles were calculated using a standard Mie code, while those for non-spherical dust particles were calculated using the numerical approach developed for modeling dust for the AERONET network of ground-based sunphotometers. As a next step, we have developed a retrieval code that employs a coupled Markov Chain (MC) and adding/doubling radiative transfer method for joint retrieval of aerosol properties and water leaving radiance from Airborne Multiangle SpectroPolarimetric Imager-1 (AirMSPI-1) polarimetric observations. The AirMSPI-1 instrument has been flying aboard the NASA ER-2 high altitude aircraft since October 2010. AirMSPI typically acquires observations of a target area at 9 view angles between ±67° at 10 m resolution. AirMSPI spectral channels are centered at 355, 380, 445, 470, 555, 660, and 865 nm, with 470, 660, and 865 reporting linear polarization. We

  9. Molecular genetics and diversity of primary biogenic aerosol particles in urban, rural, and high-alpine air

    Directory of Open Access Journals (Sweden)

    V. Després

    2007-02-01

    Full Text Available This study explores the applicability of molecular methods for the characterization of primary biogenic aerosol (PBA particles in the atmosphere. Samples of fine particulate matter (PM2.5 and total suspended particulates (TSP have been collected on different types of filter materials at urban, rural, and high-alpine locations along an altitude transect in the south of Germany (Munich, Hohenpeissenberg, Mt. Zugspitze.

    From filter aliquots loaded with about one milligram of air particulate matter, DNA could be extracted and DNA sequences could be determined for bacteria, fungi, plants and animals. Sequence analyses were used to determine the identity of biological organisms, and terminal restriction length polymorphism analyses (T-RFLP were applied to estimate diversities and relative abundances of bacteria. Investigations of blank and background samples showed that filter materials have to be decontaminated prior to use, and that the sampling and handling procedures have to be carefully controlled to avoid artifacts in the analyses.

    Mass fractions of DNA in PM2.5 were found to be around 0.05% in urban, rural, and high alpine aerosols. The average concentration of DNA determined for urban air was on the order of ~7 ng m−3, indicating that human adults may inhale about one microgram of DNA per day (corresponding to ~105 haploid human genomes.

    Most of the bacterial sequences found in PM2.5 were from Proteobacteria (42 and some from Actinobacteria (10 and Firmicutes (1. The fungal sequences were characteristic for Ascomycota (3 and Basidiomycetes (1, which are known to actively discharge spores into the atmosphere. The plant sequences could be attributed to green plants (2 and moss spores (2, while animal DNA was found only for one unicellular eukaryote (protist.

    Over 80% of the 53 bacterial sequences could be matched with about 40% of the 19 T-RF peaks (58

  10. Observations of the spectral dependence of linear particle depolarization ratio of aerosols using NASA Langley airborne High Spectral Resolution Lidar

    Science.gov (United States)

    Burton, S. P.; Hair, J. W.; Kahnert, M.; Ferrare, R. A.; Hostetler, C. A.; Cook, A. L.; Harper, D. B.; Berkoff, T. A.; Seaman, S. T.; Collins, J. E.; Fenn, M. A.; Rogers, R. R.

    2015-12-01

    Linear particle depolarization ratio is presented for three case studies from the NASA Langley airborne High Spectral Resolution Lidar-2 HSRL-2). Particle depolarization ratio from lidar is an indicator of non-spherical particles and is sensitive to the fraction of non-spherical particles and their size. The HSRL-2 instrument measures depolarization at three wavelengths: 355, 532, and 1064 nm. The three measurement cases presented here include two cases of dust-dominated aerosol and one case of smoke aerosol. These cases have partial analogs in earlier HSRL-1 depolarization measurements at 532 and 1064 nm and in literature, but the availability of three wavelengths gives additional insight into different scenarios for non-spherical particles in the atmosphere. A case of transported Saharan dust has a spectral dependence with a peak of 0.30 at 532 nm with smaller particle depolarization ratios of 0.27 and 0.25 at 1064 and 355 nm, respectively. A case of aerosol containing locally generated wind-blown North American dust has a maximum of 0.38 at 1064 nm, decreasing to 0.37 and 0.24 at 532 and 355 nm, respectively. The cause of the maximum at 1064 nm is inferred to be very large particles that have not settled out of the dust layer. The smoke layer has the opposite spectral dependence, with the peak of 0.24 at 355 nm, decreasing to 0.09 and 0.02 at 532 and 1064 nm, respectively. The depolarization in the smoke case may be explained by the presence of coated soot aggregates. We note that in these specific case studies, the linear particle depolarization ratio for smoke and dust-dominated aerosol are more similar at 355 nm than at 532 nm, having possible implications for using the particle depolarization ratio at a single wavelength for aerosol typing.

  11. Glacier evolution in high-mountain Asia under stratospheric sulfate aerosol injection geoengineering

    Science.gov (United States)

    Zhao, Liyun; Yang, Yi; Cheng, Wei; Ji, Duoying; Moore, John C.

    2017-06-01

    Geoengineering by stratospheric sulfate aerosol injection may help preserve mountain glaciers by reducing summer temperatures. We examine this hypothesis for the glaciers in high-mountain Asia using a glacier mass balance model driven by climate simulations from the Geoengineering Model Intercomparison Project (GeoMIP). The G3 and G4 schemes specify use of stratospheric sulfate aerosols to reduce the radiative forcing under the Representative Concentration Pathway (RCP) 4.5 scenario for the 50 years between 2020 and 2069, and for a further 20 years after termination of geoengineering. We estimate and compare glacier volume loss for every glacier in the region using a glacier model based on surface mass balance parameterization under climate projections from three Earth system models under G3, five models under G4, and six models under RCP4.5 and RCP8.5. The ensemble projections suggest that glacier shrinkage over the period 2010-2069 is equivalent to sea-level rise of 9.0 ± 1.6 mm (G3), 9.8 ± 4.3 mm (G4), 15.5 ± 2.3 mm (RCP4.5), and 18.5 ± 1.7 mm (RCP8.5). Although G3 keeps the average temperature from increasing in the geoengineering period, G3 only slows glacier shrinkage by about 50 % relative to losses from RCP8.5. Approximately 72 % of glaciated area remains at 2069 under G3, as compared with about 30 % for RCP8.5. The widely reported reduction in mean precipitation expected for solar geoengineering is unlikely to be as important as the temperature-driven shift from solid to liquid precipitation for forcing Himalayan glacier change. The termination of geoengineering at 2069 under G3 leads to temperature rise of about 1.3 °C over the period 2070-2089 relative to the period 2050-2069 and corresponding increase in annual mean glacier volume loss rate from 0.17 to 1.1 % yr-1, which is higher than the 0.66 % yr-1 under RCP8.5 during 2070-2089.

  12. Glacier evolution in high-mountain Asia under stratospheric sulfate aerosol injection geoengineering

    Directory of Open Access Journals (Sweden)

    L. Zhao

    2017-06-01

    Full Text Available Geoengineering by stratospheric sulfate aerosol injection may help preserve mountain glaciers by reducing summer temperatures. We examine this hypothesis for the glaciers in high-mountain Asia using a glacier mass balance model driven by climate simulations from the Geoengineering Model Intercomparison Project (GeoMIP. The G3 and G4 schemes specify use of stratospheric sulfate aerosols to reduce the radiative forcing under the Representative Concentration Pathway (RCP 4.5 scenario for the 50 years between 2020 and 2069, and for a further 20 years after termination of geoengineering. We estimate and compare glacier volume loss for every glacier in the region using a glacier model based on surface mass balance parameterization under climate projections from three Earth system models under G3, five models under G4, and six models under RCP4.5 and RCP8.5. The ensemble projections suggest that glacier shrinkage over the period 2010–2069 is equivalent to sea-level rise of 9.0 ± 1.6 mm (G3, 9.8 ± 4.3 mm (G4, 15.5 ± 2.3 mm (RCP4.5, and 18.5 ± 1.7 mm (RCP8.5. Although G3 keeps the average temperature from increasing in the geoengineering period, G3 only slows glacier shrinkage by about 50 % relative to losses from RCP8.5. Approximately 72 % of glaciated area remains at 2069 under G3, as compared with about 30 % for RCP8.5. The widely reported reduction in mean precipitation expected for solar geoengineering is unlikely to be as important as the temperature-driven shift from solid to liquid precipitation for forcing Himalayan glacier change. The termination of geoengineering at 2069 under G3 leads to temperature rise of about 1.3 °C over the period 2070–2089 relative to the period 2050-2069 and corresponding increase in annual mean glacier volume loss rate from 0.17 to 1.1 % yr−1, which is higher than the 0.66 % yr−1 under RCP8.5 during 2070–2089.

  13. Aerosol Organic Matter-Trace Metal Relationships Revealed by Ultra-High Resolution Mass Spectrometry

    Science.gov (United States)

    Wozniak, A. S.; Sleighter, R. L.; Morton, P. L.; Landing, W. M.; Shelley, R. U.; Hatcher, P. G.

    2011-12-01

    Atmospheric delivery of aerosols is important for the biogeochemical cycling of organic matter (OM) and trace elements in marine environments. Aerosols over marine environments can be derived from marine sources or transported from continental regions of variable vegetative cover and anthropogenic influence. These different sources are key determinants of aerosol OM composition, as well as trace metal amounts and characteristics. Dust-influenced aerosols typically contain higher amounts of Fe than anthropogenic-influenced aerosols but have lesser % of soluble Fe (%FeS), believed to be the bioavailable form of Fe for marine phytoplankton. Four samples from the 2008 GEOTRACES intercalibration experiments (Miami, FL, USA) were analyzed by electrospray ionization Fourier transform ion cyclotron resonance mass spectrometry (FT-ICR MS) and related to both air mass back trajectories and %FeS. Three samples showed aerosol sources from the east consistent with Saharan dust inputs, while the fourth sample was derived in part from air masses to the north, influenced by the North American continent. This North American-influenced sample was collected following the 3 day period with the highest %FeS (1.3-1.7%) of the 11 day intercalibration experiment (mean = 0.4-1.1%). FT-ICR mass spectra showed 795 peaks common to the dust-influenced samples but absent from the North American-influenced sample. These peaks were assigned molecular formulas characterized by CHO and CHON compounds with lower H/C and O/C ratios than the 1257 formulas common to all 4 samples, suggesting that the dust-influenced aerosols carry OM that is less oxygenated and more condensed in structure along with Fe of lesser solubility. Air mass trajectory analyses revealed samples collected during a 2010 cruise in the North Atlantic Ocean to be characterized by European-influenced (anthropogenic), African-influenced (dust), and primarily marine air masses, making them ideal for further exploration of the

  14. Highly time-resolved chemical characterization of atmospheric submicron particles during 2008 Beijing Olympic Games using an Aerodyne High-Resolution Aerosol Mass Spectrometer

    Directory of Open Access Journals (Sweden)

    X.-F. Huang

    2010-05-01

    Full Text Available As part of Campaigns of Air Quality Research in Beijing and Surrounding Region–2008 (CAREBeijing-2008, an Aerodyne High-Resolution Time-of-Flight Aerosol Mass Spectrometer (HR-ToF-AMS was deployed in urban Beijing to characterize submicron aerosol particles during the time of 2008 Beijing Olympic Games and Paralytic Games (24 July to 20 September 2008. The campaign mean PM1 mass concentration was 63.1±39.8 μg m−3; the mean composition consisted of organics (37.9%, sulfate (26.7%, ammonium (15.9%, nitrate (15.8%, black carbon (3.1%, and chloride (0.87%. The average size distributions of the species (except BC were all dominated by an accumulation mode peaking at about 600 nm in vacuum aerodynamic diameter, and organics was characterized by an additional smaller mode extending below 100 nm. Positive Matrix Factorization (PMF analysis of the high resolution organic mass spectral dataset differentiated the organic aerosol into four components, i.e., hydrocarbon-like (HOA, cooking-related (COA, and two oxygenated organic aerosols (OOA-1 and OOA-2, which on average accounted for 18.1, 24.4, 33.7 and 23.7% of the total organic mass, respectively. The HOA was identified to be closely associated with primary combustion sources, while the COA mass spectrum showed high similarity to that measured from cooking aerosol emissions. The OOA components correspond to aged secondary organic aerosol. Although the two OOA components have similar elemental (O/C, H/C compositions, they display differences in mass spectra and time series which appear to correlate with the different source regions sampled during the campaign. Back trajectory clustering analysis indicated that the southerly air flows were associated with the highest PM1 pollution during the campaign. This result is similar to observations made in the summer of 2006, although the average PM1 concentration level for the southerly air flows is 31% lower than

  15. Elemental analysis of aerosol organic nitrates with electron ionization high-resolution mass spectrometry

    Directory of Open Access Journals (Sweden)

    A. W. Rollins

    2009-10-01

    Full Text Available Four hydroxynitrates (R(OHR'ONO2 representative of atmospheric volatile organic compound (VOC oxidation products were synthesized, nebulized and sampled into an Aerodyne High Resolution Time of Flight Aerosol Mass Spectrometer (HR-ToF-AMS. The resulting mass spectrum was used to evaluate calibration factors for elemental analysis of organic nitrates by AMS, and to determine the distribution of nitrogen in the detected fragments in a search for an AMS signature of organic nitrates. We find that 30% of the detected nitrogen mass is in the NO+ and NO2+ fragments, 12% at NHx+ fragments, 5% at CxHyOzN+ fragments, and 53% at various CxHyN+ fragments. Elemental analysis indicated that nitrogen was detected with higher efficiency than carbon and hydrogen, but oxygen was detected with reduced efficiency compared to previously reported results for a suite of organics which did not include organic nitrates. The results are used to suggest the maximum corrections to ambient O:C and N:C ratios based on AMS measurements.

  16. High-performance energy harvester fabricated with aerosol deposited PMN-PT material

    Science.gov (United States)

    Chen, C. T.; Lin, S. C.; Lin, T. K.; Wu, W. J.

    2016-11-01

    This paper reports a high-performance piezoelectric energy harvester (EH) fabricated with xPb(Mg1/3Nb2/3)-(l-x)PbTiO3 (PMN-PT) by aerosol deposition method. The result indicates that PMN-PT based EH owns 1.8 times output power which is higher than traditional PbZrxTi1- xO3 (PZT) based EH. In order to compare the output performance of EH fabricated with PMN- PT compared with PZT, the similar thickness of PMN-PT and PZT thin film is deposited on stainless steel subtracted. The experimental results show that PZT-based EH had a maximum output power of 4.65 μW with 1.11 Vp-p output voltage excited at 94.4 Hz under 0.5g base excitation, while the PMN-PT based device has a maximum output power of 8.42 μW with 1.49 Vp-p output voltage at a vibration frequency of 94.8 Hz and the same base excitation level. The volumetric power density was 82.95 μW/mm3 and 48.05 μW/mm3 for the device based on PMN- PT and PZT materials, respectively. All the results demonstrate that PMN-PT has better output performance than PZT.

  17. Validation of high-resolution aerosol optical thickness simulated by a global non-hydrostatic model against remote sensing measurements

    Science.gov (United States)

    Goto, Daisuke; Sato, Yousuke; Yashiro, Hisashi; Suzuki, Kentaroh; Nakajima, Teruyuki

    2017-02-01

    A high-performance computing resource allows us to conduct numerical simulations with a horizontal grid spacing that is sufficiently high to resolve cloud systems. The cutting-edge computational capability, which was provided by the K computer at RIKEN in Japan, enabled the authors to perform long-term, global simulations of air pollutions and clouds with unprecedentedly high horizontal resolutions. In this study, a next generation model capable of simulating global air pollutions with O(10 km) grid spacing by coupling an atmospheric chemistry model to the Non-hydrostatic Icosahedral Atmospheric Model (NICAM) was performed. Using the newly developed model, month-long simulations for July were conducted with 14 km grid spacing on the K computer. Regarding the global distributions of aerosol optical thickness (AOT), it was found that the correlation coefficient (CC) between the simulation and AERONET measurements was approximately 0.7, and the normalized mean bias was -10%. The simulated AOT was also compared with satellite-retrieved values; the CC was approximately 0.6. The radiative effects due to each chemical species (dust, sea salt, organics, and sulfate) were also calculated and compared with multiple measurements. As a result, the simulated fluxes of upward shortwave radiation at the top of atmosphere and the surface compared well with the observed values, whereas those of downward shortwave radiation at the surface were underestimated, even if all aerosol components were considered. However, the aerosol radiative effects on the downward shortwave flux at the surface were found to be as high as 10 W/m2 in a global scale; thus, simulated aerosol distributions can strongly affect the simulated air temperature and dynamic circulation.

  18. Assessment of Atmospheric heavy metal deposition in North Egypt aerosols using neutron activation analysis and optical emission inductively coupled plasma

    Energy Technology Data Exchange (ETDEWEB)

    El-Araby, E.H., E-mail: elaraby_20032000@yahoo.com [Faculty of Science, Physics Department, Jezan University, KSA (Saudi Arabia); Abd El-Wahab, M., E-mail: wahab_magda@yahoo.com [Faculty of women for Arts, Science and Education, Physics Department, Ain Shams University, PO11757 Cairo (Egypt); Diab, H.M., E-mail: hnndiab@yahoo.co.uk [National Center of Nuclear Safety and Radiation Control, Atomic Energy Authority Cairo (Egypt); El-Desouky, T.M., E-mail: trkhegazy@yahoo.com [Faculty of women for Arts, Science and Education, Physics Department, Ain Shams University, PO11757 Cairo (Egypt); Mohsen, M., E-mail: m1mohsen@yahoo.com [Faculty of Science. Physics Department, Ain-Shams University, PO 11566 Cairo (Egypt)

    2011-10-15

    The aim of the present study is to assess the current level of atmospheric heavy metal pollution of aerosols in different cities of North Egypt using the neutron activation analysis and optical emission inductively coupled plasma techniques. The results revealed that the highest concentrations of particulate matter PM{sub 10} and total suspended particulate matter were close to industrial areas. From the results of the enrichment factor calculations, the most significant elements of anthropogenic origin are Ba, Sb, Ce and Zn. - Highlights: > Average concentration of Cd using OE-ICP is below detection limit for all the samples. > Maximum average concentration of Pb in PM10 and TSP is 5425 and 570.3, respectively. > Concentration of 20 elements in PM{sub 10} and TSP aerosols are determined using the NAA. > EF revealed that Pb, Ba, Br, Ce, Hf, La Sb and Zn are of anthropogenic origin.

  19. High aerosol acidity despite declining atmospheric sulfate concentrations over the past 15 years

    Science.gov (United States)

    Weber, Rodney J.; Guo, Hongyu; Russell, Armistead G.; Nenes, Athanasios

    2016-04-01

    Particle acidity affects aerosol concentrations, chemical composition and toxicity. Sulfate is often the main acid component of aerosols, and largely determines the acidity of fine particles under 2.5 μm in diameter, PM2.5. Over the past 15 years, atmospheric sulfate concentrations in the southeastern United States have decreased by 70%, whereas ammonia concentrations have been steady. Similar trends are occurring in many regions globally. Aerosol ammonium nitrate concentrations were assumed to increase to compensate for decreasing sulfate, which would result from increasing neutrality. Here we use observed gas and aerosol composition, humidity, and temperature data collected at a rural southeastern US site in June and July 2013 (ref. ), and a thermodynamic model that predicts pH and the gas-particle equilibrium concentrations of inorganic species from the observations to show that PM2.5 at the site is acidic. pH buffering by partitioning of ammonia between the gas and particle phases produced a relatively constant particle pH of 0-2 throughout the 15 years of decreasing atmospheric sulfate concentrations, and little change in particle ammonium nitrate concentrations. We conclude that the reductions in aerosol acidity widely anticipated from sulfur reductions, and expected acidity-related health and climate benefits, are unlikely to occur until atmospheric sulfate concentrations reach near pre-anthropogenic levels.

  20. Molecular composition of rainwater and aerosol during rain events in León, Spain, using high resolution mass spectrometry.

    Science.gov (United States)

    Fee, Anna

    2017-04-01

    Anna Fee (1), Markus Kalberer (1), Roberto Fraile (2), Amaya Castro (2), Ana. I. Calvo (2), Carlos Blanco-Alegre (2), Fernanda Oduber (2) and Mário Cerqueira (3). 1 Department of Chemistry, University of Cambridge, UK. 2 Department of Applied Chemistry and Physics, IMARENAB, University of León, Spain. 3 Department of Environmental Planning, University of Aveiro, Portugal. A wide range of atmospheric compounds which are present in rainwater are often also present in aerosol. They can be taken up during cloud droplet formation (in-cloud scavenging) or washed out during precipitation (below-cloud scavenging). Such compounds including aromatic hydrocarbons and organic nitrogen containing compounds are hazardous to health. In this study, the organic chemical composition of rainwater and aerosol from rain events in León, Spain, is being analysed using high resolution mass spectrometry. Collected rainwater along with high volume and low volume filters from rain events which occurred during spring, summer and winter of 2016 have been selected for analysis. Rainwater samples were prepared using Polymeric Reversed Phase Solid Phase Extraction (SPE) and filters have been extracted in water with and without SPE. Three different SPE polymer based sorbents were tested; one for extracting neutral compounds and two which are more suitable for extracting organic compounds containing sulphate and other polar functional groups. The sorbent for extracting neutral compounds was found to yield a higher number of compounds from the sample extraction than the other two varieties. Kendrick masses, Van Krevelen plots and carbon oxidation states have been investigated to identify compounds and patterns. Preliminary results show a predominance in peaks with O/C ratios between 0.2 and 0.7 and H/C ratios between 1 and 2 in both rain and aerosol samples which indicates substituted aromatic compounds. Cellulose material and fatty acids may also be present. The rain samples also have a

  1. Aerosols: unexpected disequilibrium phenomena between airborne radio activities of lead-210 and its progenies bismuth-210 and polonium-210.

    Science.gov (United States)

    Wallner, Gabriele; Berner, Axel; Irlweck, Karl

    2002-12-01

    For the first time, concentrations of the long lived radon progenies (210)Pb, (210)Bi and (210)Po were measured in the mine atmosphere of the so called "healing gallery" in Badgastein, Austria, a region famous for its radioactive springs. These investigations were performed in order to study the radioactive equilibrium between the (210)Pb-(210)Bi and the (210)Pb-(210)Po pairs so as to gain more information about the aerosol-forming processes in the mine. The particle size distribution of the aerosols was determined under different ventilation conditions. Six-stage and eight-stage cascade impactors with working ranges from 0.15 to 5 micro m and from 0.063 to 8 micro m, respectively, were used to collect the mine aerosols. These samples were analysed in the laboratory and measured by liquid scintillation spectrometry. The most surprising results were found under full ventilation, when the total activity concentrations of (210)Pb, (210)Bi and (210)Po were 4.6, 2.0 and 16.5 mBq/m(3), respectively. In this case (210)Po/(210)Pb activity ratios ranged between 1.8+/-0.3 and 4.3+/-0.3. These unexpected results were confirmed by the eight-stage impactor samples. For the smallest particles, between 0.062 and 0.125 micro m, an even higher value of 7.5 was observed. As outside sources could be excluded, such (210)Po enrichments must occur during the aerosol-forming process itself inside the mine.

  2. A missing source of aerosols in Antarctica - beyond long-range transport, phytoplankton, and photochemistry

    Science.gov (United States)

    Giordano, Michael R.; Kalnajs, Lars E.; Avery, Anita; Goetz, J. Douglas; Davis, Sean M.; DeCarlo, Peter F.

    2017-01-01

    Understanding the sources and evolution of aerosols is crucial for constraining the impacts that aerosols have on a global scale. An unanswered question in atmospheric science is the source and evolution of the Antarctic aerosol population. Previous work over the continent has primarily utilized low temporal resolution aerosol filters to answer questions about the chemical composition of Antarctic aerosols. Bulk aerosol sampling has been useful in identifying seasonal cycles in the aerosol populations, especially in populations that have been attributed to Southern Ocean phytoplankton emissions. However, real-time, high-resolution chemical composition data are necessary to identify the mechanisms and exact timing of changes in the Antarctic aerosol. The recent 2ODIAC (2-Season Ozone Depletion and Interaction with Aerosols Campaign) field campaign saw the first ever deployment of a real-time, high-resolution aerosol mass spectrometer (SP-AMS - soot particle aerosol mass spectrometer - or AMS) to the continent. Data obtained from the AMS, and a suite of other aerosol, gas-phase, and meteorological instruments, are presented here. In particular, this paper focuses on the aerosol population over coastal Antarctica and the evolution of that population in austral spring. Results indicate that there exists a sulfate mode in Antarctica that is externally mixed with a mass mode vacuum aerodynamic diameter of 250 nm. Springtime increases in sulfate aerosol are observed and attributed to biogenic sources, in agreement with previous research identifying phytoplankton activity as the source of the aerosol. Furthermore, the total Antarctic aerosol population is shown to undergo three distinct phases during the winter to summer transition. The first phase is dominated by highly aged sulfate particles comprising the majority of the aerosol mass at low wind speed. The second phase, previously unidentified, is the generation of a sub-250 nm aerosol population of unknown composition

  3. High-Resolution Electrospray Ionization Mass Spectrometry Analysis of Water- Soluble Organic Aerosols Collected with a Particle into Liquid Sampler

    Energy Technology Data Exchange (ETDEWEB)

    Bateman, Adam P.; Nizkorodov, Serguei; Laskin, Julia; Laskin, Alexander

    2010-10-01

    This work demonstrates the utility of a particle-into-liquid sampler (PILS) a technique traditionally used for identification of inorganic ions present in ambient or laboratory aerosols for the analysis of water soluble organic aerosol (OA) using high resolution electrospray ionization mass spectrometry (HR ESI-MS). Secondary organic aerosol (SOA) was produced from 0.5 ppm mixing ratios of limonene and ozone in a 5 m3 Teflon chamber. SOA was collected simultaneously using a traditional filter sampler and a PILS. The filter samples were later extracted with either water or acetonitrile, while the aqueous PILS samples were analyzed directly. In terms of peak intensities, types of detectable compounds, average O:C ratios, and organic mass to organic carbon ratios, the resulting high resolution mass spectra were essentially identical for the PILS and filter based samples. SOA compounds extracted from both filter/acetonitrile extraction and PILS/water extraction accounted for >95% of the total ion current in ESI mass spectra. This similarity was attributed to high solubility of limonene SOA in water. In contrast, significant differences in detected ions and peak abundances were observed for pine needle biomass burning organic aerosol (BBOA) collected with PILS and filter sampling. The water soluble fraction of BBOA is considerably smaller than for SOA, and a number of unique peaks were detectable only by the filter/acetonitrile method. The combination of PILS collection with HR-ESI-MS analysis offers a new approach for molecular analysis of the water-soluble organic fraction in biogenic SOA, aged photochemical smog, and BBOA.

  4. High Resolution Mass Spectrometry of Seasonal Aerosol Samples From an Urban Location in the Italian Po Valley

    Science.gov (United States)

    Mahon, Brendan; Giorio, Chiara; Gallimore, Peter J.; Zielinski, Arthur T.; Tapparo, Andrea; Kalberer, Markus

    2016-04-01

    The Po Valley in Northern Italy represents one of the most polluted environments in Europe, with PM2.5 and ozone concentrations regularly exceeding 100μg/m3 and 50ppb respectively. Particularly during winter, prolonged inversion conditions together with biomass burning and anthropogenic emissions regularly lead to severe air pollution events. Over the course of several months in 2013-14, we carried out a sampling program at a city-centre site in Padova, Italy, collecting 24-hour high-volume aerosol filter samples, 18 in winter (mid December - mid March) and 20 in summer (late May - late July). Utilising high-resolution Orbitrap mass spectrometry techniques, we have characterised these sample sets to examine the long-term variation in aerosol composition over the sampling campaign and to determine the effect of anthropogenic gaseous pollutants such as NOx and SO2 on the composition of organic particle components. The results showed that between ca. 450-700 ions were measured in each sample in both the summer and winter sample sets, however the majority (90%) of ions in the winter samples were below 300m/z and below 380m/z in the summer samples. A much higher percentage of CHO-only ions were found in winter (ca. 27%) compared to the summer samples (ca. 6%), indicating a higher degree of photochemical reactions taking place involving pollutants such as NOx and SO2 in summer. Our results represent the first long term data set of high-resolution measurements of aerosol composition and demonstrate that this technique is an important tool in evaluating the composition of aerosol particles in complex polluted urban areas.

  5. Iodine isotopes (127I and 129I) in aerosols at high altitude Alp stations.

    Science.gov (United States)

    Jabbar, Tania; Steier, Peter; Wallner, Gabriele; Priller, Alfred; Kandler, Norbert; Kaiser, August

    2012-08-21

    Concentrations of gases and particulate matter have been proven to be affected by meteorological and geographical variables from urban locations to high mountain clean air sites. Following our previous research in Vienna, we summarize here new findings about concentration levels of iodine isotopes in aerosols collected at two Alpine meteorological stations, Sonnblick (Austria) and Zugspitze (Germany) during 2001. The present study mainly focuses on the effect of altitude on the anthropogenic concentration of (129)I and on the isotopic ratio (129)I/(127)I. Iodine was separated from matrix elements by using either an anion exchange method or solvent extraction, and was analyzed by ICP-MS and AMS. Over the altitude change from Vienna to Zugspitze and Sonnblick (202 m to 2962 m and 3106 m above sea level), stable iodine level decreased from an average of 0.94 ng m(-3) to 0.52 ng m(-3) and 0.62 ng m(-3), respectively. Similarly, (129)I concentrations at both Alpine stations were about 1 order of magnitude lower (10(4) atoms m(-3)) than values obtained for Vienna (10(5) atoms m(-3)) and reveal a strong vertical concentration gradient of (129)I. A high degree of variability is observed, which is due to wide variation in the origin of air masses. Furthermore, air trajectory analysis demonstrates the importance of large scale air transport mostly from southeast Europe for influencing Sonnblick whereas influence from northwest Europe is strong at Zugspitze. In contrast to (129)I, a higher concentration of (7)Be was found at higher altitude stations compared to Vienna which probably results from its production in the upper atmosphere.

  6. Competing effects of viscosity and surface-tension depression on the hygroscopicity and CCN activity of laboratory surrogates for oligomers in atmospheric aerosol

    Science.gov (United States)

    Hodas, N.; Zuend, A.; Shiraiwa, M.; Flagan, R. C.; Seinfeld, J.; Schilling, K.; Berkemeier, T.

    2015-12-01

    The presence of oligomers in biomass burning aerosol, as well as secondary organic aerosol derived from other sources, influences particle viscosity and can introduce kinetic limitations to water uptake. This, in turn, impacts aerosol optical properties and the efficiency with which these particles serve as cloud condensation nuclei (CCN). To explore the influence of organic-component viscosity on aerosol hygroscopicity, the water-uptake behavior of aerosol systems comprised of polyethylene glycol (PEG) and mixtures of PEG and ammonium sulfate (AS) was measured under sub- and supersaturated relative humidity (RH) conditions. Experiments were conducted with systems containing PEG with average molecular weights ranging from 200 to 10,000 g/mol, corresponding to a range in viscosity of 0.004 - 4.5 Pa s under dry conditions. While evidence suggests that viscous aerosol components can suppress water uptake at RH activity with increasing PEG molecular weight was observed. We attribute this to an increase in the efficiency with which PEG serves as a surfactant with increasing molecular weight. This effect is most pronounced for PEG-AS mixtures and, in fact, a modest increase in CCN activity is observed for the PEG 10,000-AS mixture as compared to pure AS, as evidenced by a 4% reduction in critical activation diameter. Experimental results are compared with calculations of hygroscopic growth at thermodynamic equilibrium using the Aerosol Inorganic-Organic Mixtures Functional groups Activity Coefficients model and the potential influence of kinetic limitations to observed water uptake is further explored with the Kinetic Multi-Layer Model of Gas-Particle Interactions. Results suggest the competing effects of organic-component viscosity and surface-tension depression may lead to RH-dependent differences in hygroscopicity for oligomers and other surface-active compounds present in atmospheric aerosols, for which PEG serves as a surrogate in these experiments.

  7. Characterisation of Fluorescent Biological Aerosol Particles during South-West Monsoon from a High Altitude Site in South India

    Science.gov (United States)

    Valsan, A. E.; R, R.; V, B. C.; Huffman, J. A.; Poeschl, U.; Gunthe, S. S.

    2015-12-01

    Biological aerosols (Bioaerosols) constitute a wide range of dead and alive biological materials that are suspended in the atmosphere. Though ubiquitous in earth's atmosphere, bioaerosols are poorly characterized in terms of their atmospheric abundance, sources and physical properties. Here we discuss the number concentration and size distribution of coarse mode (>1µm) biological aerosols measured at a relatively clean high altitude continental site, Munnar (10.09 N, 77.06 E; 1605 m asl) located in the Western Ghats mountain ranges of Southern Tropical India. The fluorescent biological aerosol particles (FBAP) were continuously measured using Ultra Violet Aerodynamic Particle Sizer (UVAPS) from 01 June to 21 August 2014 (South-West Monsoon Period) which showed some interesting patterns. The mean number and mass concentration of coarse FBAP during the campaign was observed to be 1.7 x 10-2cm-3 and 0.24µg m-3 respectively, which corresponds to 2% and 9% of coarse total aerosol particles (TAP) number and mass concentration. FBAP concentration decreased significantly during periods of heavy and continuous rain with constant South-West winds. This may be due to the clean marine influx coming from the ocean and continuous washout. The Relative Humidity (RH) and temperature remained consistent during this period without any strong diurnal pattern. When the wind fluctuated in North-West directions, the FBAP concentration increased to even an order of magnitude higher than the periods of South-West winds which can be attributed to the transported bioaerosols from the nearby vegetated area. In spite of variability in the number concentrations, the size distribution of FBAP exhibited a prominent peak at ~3 μm throughout the campaign, which should be fungal spores. They also exhibited a strong diurnal pattern with high concentrations occuring during the night time which peaks in the early morning hours.Biological aerosols (Bioaerosols) constitute a wide range of dead and

  8. Out of Africa: High aerosol concentrations in the upper troposphere over Africa

    Directory of Open Access Journals (Sweden)

    J. Heintzenberg

    2003-05-01

    Full Text Available In the year 2000, six flights (three southbound and three northbound of the CARIBIC project were conducted between Germany and two destinations in the southern hemisphere (Windhoek, Namibia and Cape Town, South Africa. In the present report, results on particle number concentrations are discussed in three size ranges (>4 nm, >12 nm, and >18 nm particle diameter during the unique transequatorial Africa flights. The flights covered a total of about 80 h in May, July, and December. Thus, no claim can be made for long-term representativeness of the aerosol data. Nevertheless, they are the first upper systematic tropospheric transequatorial aerosol profiles over Africa. The average aerosol results show a broad maximum, roughly symmetrical to the equator, which compares well in latitudinal extent to a maximum of CO concentrations measured on the same flights. This export of continental surface aerosol to the upper troposphere will be dispersed on a global scale both with the easterly flow near the equator and with the westerlies in the adjacent subtropical regions. There was strong evidence of recent new particle formation before aerosol arrival at flight level, in particular during the time periods between 9:00 and 13:00 local time over Africa. Direct and indirect climate effects of the respective particulate matter remain to be investigated by future flights with the ongoing extension of the CARIBIC payload towards size-resolved measurements above 100 nm particle diameter. At the same time global chemical transport models and aerosol dynamics models need to be extended to be able to reproduce the CARIBIC findings over Africa.

  9. Measurements of HNO3, SO2 High Resolution Aerosol SO4 (sup 2-), and Selected Aerosol Species Aboard the NASA DC-8 Aircraft: During the Transport and Chemical Evolution Over the Pacific Airborne Mission (TRACE-P)

    Science.gov (United States)

    Talbot, Robert W.; Dibb, Jack E.

    2004-01-01

    The UNH investigation during TRACE-P provided measurements of selected acidic gases and aerosol species aboard the NASA DC-8 research aircraft. Our investigation focused on measuring HNO3, SO2, and fine (less than 2 microns) aerosol SO4(sup 2-) with two minute time resolution in near-real-time. We also quantified mixing ratios of aerosol ionic species, and aerosol (210)Pb and (7)Be collected onto bulk filters at better than 10 minute resolution. This suite of measurements contributed extensively to achieving the principal objectives of TRACE-P. In the context of the full data set collected by experimental teams on the DC-8, our observations provide a solid basis for assessing decadal changes in the chemical composition and source strength of Asian continental outflow. This region of the Pacific should be impacted profoundly by Asian emissions at this time with significant degradation of air quality over the next few decades. Atmospheric measurements in the western Pacific region will provide a valuable time series to help quantify the impact of Asian anthropogenic activities. Our data also provide important insight into the chemical and physical processes transforming Asian outflow during transport over the Pacific, particularly uptake and reactions of soluble gases on aerosol particles. In addition, the TRACE-P data set provide strong constraints for assessing and improving the chemical fields simulated by chemical transport models.

  10. Physical and optical characteristics of atmospheric aerosols during ICARB at Manora Peak, Nainital: A sparsely inhabited, high-altitude location in the Himalayas

    Indian Academy of Sciences (India)

    U C Dumka; K Krishna Moorthy; P Pant; P Hegde; Ram Sagar; K Pandey

    2008-07-01

    Collocated measurements of the optical and physical properties of columnar and near-surface aerosols were carried out from Manora Peak, Nainital (a sparsely inhabited, high altitude location, ∼2km above mean sea level, in the Himalayas), during the Integrated Campaign for Aerosols, gases and Radiation Budget (ICARB) under the Geosphere Biosphere Programme of the Indian Space Research Organization (ISRO-GBP). Under this, observational data of spectral aerosol optical depths (AOD), mass concentration of aerosol black carbon (B), mass concentration () and number concentration () of composite (total) aerosols near the surface and meteorological parameters were collected during the period February 15 to April 30, 2006. Though very low (> 0.1 at 500 nm) AODs were observed during clear days, as much as a fourfold increase was seen on hazy days. The Ångström exponent (), deduced from the spectral AODs, revealed high values during clear days, while on hazy days was low; with an overall mean value of 0.69 ± 0.06 for the campaign period. BC mass concentration varied between 0.36 and 2.87 g m−3 and contributed in the range 0.7 to 1.8% to the total aerosol mass. Total aerosol number concentration and BC mass concentration showed diurnal variation with a midnight and early morning minimum and a late afternoon maximum; a pattern quite opposite to that seen in low altitude stations. These are attributed to the dynamics of the atmospheric boundary layer.

  11. A Review of Research on Human Activity Induced Climate Change I.Greenhouse Gases and Aerosols

    Institute of Scientific and Technical Information of China (English)

    王明星; 刘强; 杨昕

    2004-01-01

    Extensive research on the sources and sinks of greenhouse gases, carbon cycle modeling, and the characterization of atmospheric aerosols has been carried out in China during the last 10 years or so. This paper presents the major achievements in the fields of emissions of greenhouse gases from agricultural lands,carbon cycle modeling, the characterization of Asian mineral dust, source identification of the precursors of the tropospheric ozone, and observations of the concentrations of atmospheric organic compounds.Special, more detailed information on the emissions of methane from rice fields and the physical and chemical characteristics of mineral aerosols are presented.

  12. High-time resolved measurements of biogenic and anthropogenic secondary organic aerosol precursors and products in urban air

    Science.gov (United States)

    Flores, Rosa M.; Doskey, Paul V.

    2016-04-01

    Volatile organic compounds (VOCs), which are present in the atmosphere entirely in the gas phase are directly emitted by biogenic (~1089 Tg yr-1) and anthropogenic sources (~185 Tg yr-1). However, the sources and molecular speciation of intermediate VOCs (IVOCs), which are for the most part also present almost entirely in the gas phase, are not well characterized. The VOCs and IVOCs participate in reactions that form ozone and semivolatile OC (SVOC) that partition into the aerosol phase. Formation and evolution of secondary organic aerosol (SOA) are part of a complex dynamic process that depends on the molecular speciation and concentration of VOCs, IVOCs, primary organic aerosol (POA), and the level of oxidants (NO3, OH, O3). The current lack of understanding of OA properties and their impact on radiative forcing, ecosystems, and human health is partly due to limitations of models to predict SOA production on local, regional, and global scales. More accurate forecasting of SOA production requires high-temporal resolution measurement and molecular characterization of SOA precursors and products. For the subject study, the IVOCs and aerosol-phase organic matter were collected using the high-volume sampling technique and were analyzed by multidimensional gas chromatography with time-of-flight mass spectrometry (GCxGC-ToFMS). The IVOCs included terpenes, terpenoids, n-alkanes, branched alkanes, isoprenoids, alkylbenzenes, cycloalkylbenzenes, PAH, alkyl PAH, and an unresolved complex mixture (UCM). Diurnal variations of OA species containing multiple oxygenated functionalities and selected SOA tracers of isorprene, α-pinene, toluene, cyclohexene, and n-dodecane oxidation were also quantified. The data for SOA precursor and oxidation products presented here will be useful for evaluating the ability of molecular-specific SOA models to forecast SOA production in and downwind of urban areas.

  13. Primary and Secondary Organic Marine Aerosol and Oceanic Biological Activity: Recent Results and New Perspectives for Future Studies

    OpenAIRE

    Matteo Rinaldi; Stefano Decesari; Emanuela Finessi; Lara Giulianelli; Claudio Carbone; Sandro Fuzzi; Colin D. O'Dowd; Darius Ceburnis; Maria Cristina Facchini

    2010-01-01

    One of the most important natural aerosol systems at the global level is marine aerosol that comprises both organic and inorganic components of primary and secondary origin. The present paper reviews some new results on primary and secondary organic marine aerosol, achieved during the EU project MAP (Marine Aerosol Production), comparing them with those reported in the recent literature. Marine aerosol samples collected at the coastal site of Mace Head, Ireland, show a chemical composition tr...

  14. Anthropogenic sources of aerosol particles in a football stadium: Real-time characterization of emissions from cigarette smoking, cooking, hand flares, and color smoke bombs by high-resolution aerosol mass spectrometry

    Science.gov (United States)

    Faber, Peter; Drewnick, Frank; Veres, Patrick R.; Williams, Jonathan; Borrmann, Stephan

    2013-10-01

    Aerosol particles from several anthropogenic sources associated with football stadia including cooking, cigarette smoking, burning of color smoke bombs and hand flares were analyzed by high-resolution aerosol mass spectrometry. The physical and chemical characteristics of these different aerosols, in particular the organic fraction, were explored in laboratory studies to obtain robust references. These data were compared with field campaign results from a Bundesliga (German football league) match in the Coface Arena (Mainz, Germany) on 20th April 2012. The field measurement revealed a strongly elevated mass concentration of organic aerosols (OA) compared to background levels showing a temporal structure clearly related to the match. PMF analysis established that during the football match event cigarette smoke was the predominant component of submicron organic aerosol (67% of total OA). Cooking emissions from food outlets within the stadium correlated well with the sales figures of the catering stations and were also found to be of relevance (24% of total OA) especially in the period before kickoff. Pyrotechnics were not observed during this football match and no signatures of these sources were found in the mass spectra from the stadium measurements. All species that were elevated during the football match returned to their initial background levels within one hour after the match had finished. This demonstrates a good ventilation capacity of the open-topped Coface Arena.

  15. Highly time-resolved chemical characterization of atmospheric submicron particles during 2008 Beijing Olympic Games using an Aerodyne High-Resolution Aerosol Mass Spectrometer

    Directory of Open Access Journals (Sweden)

    X.-F. Huang

    2010-09-01

    Full Text Available As part of Campaigns of Air Quality Research in Beijing and Surrounding Region-2008 (CAREBeijing-2008, an Aerodyne High-Resolution Time-of-Flight Aerosol Mass Spectrometer (HR-ToF-AMS was deployed in urban Beijing to characterize submicron aerosol particles during the time of 2008 Beijing Olympic Games and Paralympic Games (24 July to 20 September 2008. The campaign mean PM1 mass concentration was 63.1 ± 39.8 μg m−3; the mean composition consisted of organics (37.9%, sulfate (26.7%, ammonium (15.9%, nitrate (15.8%, black carbon (3.1%, and chloride (0.87%. The average size distributions of the species (except BC were all dominated by an accumulation mode peaking at about 600 nm in vacuum aerodynamic diameter, and organics was characterized by an additional smaller mode extending below 100 nm. Positive Matrix Factorization (PMF analysis of the high resolution organic mass spectral dataset differentiated the organic aerosol into four components, i.e., hydrocarbon-like (HOA, cooking-related (COA, and two oxygenated organic aerosols (OOA-1 and OOA-2, which on average accounted for 18.1, 24.4, 33.7 and 23.7% of the total organic mass, respectively. The HOA was identified to be closely associated with primary combustion sources, while the COA mass spectrum and diurnal pattern showed similar characteristics to that measured for cooking emissions. The OOA components correspond to aged secondary organic aerosol. Although the two OOA components have similar elemental (O/C, H/C compositions, they display differences in mass spectra and time series which appear to correlate with the different source regions sampled during the campaign. Back trajectory clustering analysis indicated that the southerly air flows were associated with the highest PM1 pollution during the campaign. Aerosol particles in southern airmasses were especially rich in inorganic and oxidized organic species. Aerosol particles in northern airmasses

  16. Highly functionalized organic nitrates in the southeast United States: Contribution to secondary organic aerosol and reactive nitrogen budgets

    Science.gov (United States)

    Mohr, Claudia; Lopez-Hilfiker, Felipe D.; Lutz, Anna; Hallquist, Mattias; Lee, Lance; Romer, Paul; Cohen, Ronald C.; Iyer, Siddharth; Kurtén, Theo; Hu, Weiwei; Day, Douglas A.; Campuzano-Jost, Pedro; Jimenez, Jose L.; Xu, Lu; Ng, Nga Lee; Guo, Hongyu; Weber, Rodney J.; Wild, Robert J.; Brown, Steven S.; Koss, Abigail; de Gouw, Joost; Olson, Kevin; Goldstein, Allen H.; Seco, Roger; Kim, Saewung; McAvey, Kevin; Shepson, Paul B.; Starn, Tim; Baumann, Karsten; Edgerton, Eric S.; Liu, Jiumeng; Shilling, John E.; Miller, David O.; Brune, William; Schobesberger, Siegfried; D'Ambro, Emma L.; Thornton, Joel A.

    2016-01-01

    Speciated particle-phase organic nitrates (pONs) were quantified using online chemical ionization MS during June and July of 2013 in rural Alabama as part of the Southern Oxidant and Aerosol Study. A large fraction of pONs is highly functionalized, possessing between six and eight oxygen atoms within each carbon number group, and is not the common first generation alkyl nitrates previously reported. Using calibrations for isoprene hydroxynitrates and the measured molecular compositions, we estimate that pONs account for 3% and 8% of total submicrometer organic aerosol mass, on average, during the day and night, respectively. Each of the isoprene- and monoterpenes-derived groups exhibited a strong diel trend consistent with the emission patterns of likely biogenic hydrocarbon precursors. An observationally constrained diel box model can replicate the observed pON assuming that pONs (i) are produced in the gas phase and rapidly establish gas–particle equilibrium and (ii) have a short particle-phase lifetime (∼2–4 h). Such dynamic behavior has significant implications for the production and phase partitioning of pONs, organic aerosol mass, and reactive nitrogen speciation in a forested environment. PMID:26811465

  17. High-sensitivity microchip electrophoresis determination of inorganic anions and oxalate in atmospheric aerosols with adjustable selectivity and conductivity detection.

    Science.gov (United States)

    Noblitt, Scott D; Schwandner, Florian M; Hering, Susanne V; Collett, Jeffrey L; Henry, Charles S

    2009-02-27

    A sensitive and selective separation of common anionic constituents of atmospheric aerosols, sulfate, nitrate, chloride, and oxalate, is presented using microchip electrophoresis. The optimized separation is achieved in under 1 min and at low background electrolyte ionic strength (2.9 mM) by combining a metal-binding electrolyte anion (17 mM picolinic acid), a sulfate-binding electrolyte cation (19 mM HEPBS), a zwitterionic surfactant with affinity towards weakly solvated anions (19 mM N-tetradecyl,N,N-dimethyl-3-ammonio-1-propansulfonate), and operation in counter-electroosmotic flow (EOF) mode. The separation is performed at pH 4.7, permitting pH manipulation of oxalate's mobility. The majority of low-concentration organic acids are not observed at these conditions, allowing for rapid subsequent injections without the presence of interfering peaks. Because the mobilities of sulfate, nitrate, and oxalate are independently controlled, other minor constituents of aerosols can be analyzed, including nitrite, fluoride, and formate if desired using similar separation conditions. Contact conductivity detection is utilized, and the limit of detection for oxalate (S/N=3) is 180 nM without stacking. Sensitivity can be increased with field-amplified sample stacking by injecting from dilute electrolyte with a detection limit of 19 nM achieved. The high-sensitivity, counter-EOF operation, and short analysis time make this separation well-suited to continuous online monitoring of aerosol composition.

  18. Highly functionalized organic nitrates in the southeast United States: Contribution to secondary organic aerosol and reactive nitrogen budgets.

    Science.gov (United States)

    Lee, Ben H; Mohr, Claudia; Lopez-Hilfiker, Felipe D; Lutz, Anna; Hallquist, Mattias; Lee, Lance; Romer, Paul; Cohen, Ronald C; Iyer, Siddharth; Kurtén, Theo; Hu, Weiwei; Day, Douglas A; Campuzano-Jost, Pedro; Jimenez, Jose L; Xu, Lu; Ng, Nga Lee; Guo, Hongyu; Weber, Rodney J; Wild, Robert J; Brown, Steven S; Koss, Abigail; de Gouw, Joost; Olson, Kevin; Goldstein, Allen H; Seco, Roger; Kim, Saewung; McAvey, Kevin; Shepson, Paul B; Starn, Tim; Baumann, Karsten; Edgerton, Eric S; Liu, Jiumeng; Shilling, John E; Miller, David O; Brune, William; Schobesberger, Siegfried; D'Ambro, Emma L; Thornton, Joel A

    2016-02-09

    Speciated particle-phase organic nitrates (pONs) were quantified using online chemical ionization MS during June and July of 2013 in rural Alabama as part of the Southern Oxidant and Aerosol Study. A large fraction of pONs is highly functionalized, possessing between six and eight oxygen atoms within each carbon number group, and is not the common first generation alkyl nitrates previously reported. Using calibrations for isoprene hydroxynitrates and the measured molecular compositions, we estimate that pONs account for 3% and 8% of total submicrometer organic aerosol mass, on average, during the day and night, respectively. Each of the isoprene- and monoterpenes-derived groups exhibited a strong diel trend consistent with the emission patterns of likely biogenic hydrocarbon precursors. An observationally constrained diel box model can replicate the observed pON assuming that pONs (i) are produced in the gas phase and rapidly establish gas-particle equilibrium and (ii) have a short particle-phase lifetime (∼2-4 h). Such dynamic behavior has significant implications for the production and phase partitioning of pONs, organic aerosol mass, and reactive nitrogen speciation in a forested environment.

  19. What's Up in the Atmosphere? Exploring How Aerosols Impact Sky Color Through Hands-on Activities with Elementary GLOBE

    Science.gov (United States)

    Damadeo, K.; Taylor, J.

    2015-12-01

    What color is the sky today? The GLOBE Kids - Anita, Simon, and Dennis want to know why the sky isn't always the same shade of blue and sometimes isn't even blue. Through the new Elementary GLOBE Aerosols Storybook and Learning Activities, the GLOBE Kids learn that there's a lot more than air in the atmosphere, which can affect the colors we see in the sky. There are four hands-on activities in this unit: 1) Sky Observers - Students make observations of the sky, record their findings and share their observation reports with their peers. The activity promotes active observation and recording skills to help students observe sky color, and recognize that sky color changes; 2) Why (Not) So Blue? - Students make predictions about how drops of milk will affect color and visibility in cups of water representing the atmosphere to help them understand that aerosols in the atmosphere have an effect on sky conditions, including sky color and visibility. The activity also introduces the classification categories for daytime sky color and visibility; 3) See the Light - Students use prisms and glue sticks to explore the properties of light. The activity demonstrates that white light is made up of seven colors that represent different wavelengths, and illustrates why the sky is blue during the day and red at sunset; 4) Up in the Air - Students work in groups to make an aerosol sampler, a simple adhesive tool that allows students to collect data and estimate the extent of aerosols present at their school, understanding that, in fact, there are particles in the air we breathe. NGSS Alignment includes: Disciplinary Core Ideas- ESS2.D: Weather and Climate, ESS3.C: Human Impacts on Earth Systems, PS4.B: Electromagnetic Radiation, ESS3.A: Natural Resources; Science and Engineering Practices- Asking Questions and Defining Problems, Planning and Carrying Out an Investigation, Analyzing and Interpreting Data, Engaging in Argument from Evidence, Obtaining, Evaluating, and Communicating

  20. Cloud Condensation Nuclei Activity, Droplet Growth Kinetics and Hygroscopicity of Biogenic and Anthropogenic Secondary Organic Aerosol (SOA)

    Science.gov (United States)

    Zhao, Defeng; Buchholz, Angela; Kortner, Birthe; Schlag, Patrick; Rubach, Florian; Hendrik, Fucks; Kiendler-Scharr, Astrid; Tillmann, Ralf; Wahner, Andreas; Hallquist, Mattias; Flores, Michel; Rudich, Yinon; Glasius, Marianne; Kourtchev, Ivan; Kalberer, Markus; Mentel, Thomas

    2015-04-01

    Recent field data and model analysis show that secondary organic aerosol (SOA) formation is enhanced under anthropogenic influences (de Gouw et al. 2005, Spracklen et al. 2011). The interaction of biogenic VOCs (BVOCs) with anthropogenic emissions such as anthropogenic VOCs (AVOCs) could change the particle formation yields and the aerosol properties, as was recently demonstrated (Emanuelsson et al., 2013; Flores et al., 2014). However, the effect of the interaction of BVOCs with AVOCs on cloud condensation nuclei (CCN) activity and hygroscopicity of SOA remains elusive. Characterizing such changes is necessary in order to assess the indirect radiative forcing of biogenic aerosols that form under anthropogenic influence. In this study, we investigated the influence of AVOCs on CCN activation and hygroscopic growth of BSOA. SOA was formed from photooxidation of monoterpenes and aromatics as representatives of BVOCs and AVOCs, respectively. The hygroscopicity and CCN activation of BSOA were studied and compared with that of anthropogenic SOA (ASOA) and the mixture of ASOA and BSOA (ABSOA). We found that ASOA had a significantly higher hygroscopicity than BSOA at similar OH dose, which is attributed to a higher oxidation level of ASOA. While the ASOA fraction had an enhancing effect on the hygroscopicity of ABSOA compared to BSOA, the hygroscopicity of ABSOA cannot be explained by a linear combination of the pure ASOA and BSOA systems, indicating potentially additional non-linear effects such as oligomerization. However, in contrast to hygroscopicity, ASOA showed similar CCN activity as BSOA, in spite of its higher oxidation level. The ASOA fraction did not enhance the CCN activity of ABSOA. The discrepancy between hygroscopicity and CCN activity is discussed. In addition, BSOA, ABSOA and ASOA formed similar droplet size with ammonium sulfate in CCN at a given supersaturation, indicating none of these aerosols had a delay in the water uptake in the supersaturated

  1. Aerosol Effect on the Phase of Low-Level Clouds in the Arctic

    Science.gov (United States)

    Filioglou, M.; Mielonen, T.; Giannakaki, E.; Arola, A. T.; Komppula, M.; Romakkaniemi, S.

    2016-12-01

    Cloud phase (liquid or ice) affects the cloud's persistence and optical properties, and thus the atmospheric radiation balance. In the warming Arctic, the transition from ice to liquid clouds has a potential to enhance the warming rate, however, changes in aerosol properties can affect the cloud phase even more substantially. Here, a characterization of low level clouds and their dependence on dust aerosols, which are assumed to be the most important ice nuclei (IN) over the Arctic area, is presented based on measurements from the Cloud-Aerosol Lidar and Infrared Pathfinder Satellite Observations (CALIPSO). The level 2 aerosol and cloud layer products with 5 km horizontal resolution from the CALIOP lidar (Cloud-Aerosol Lidar with Orthogonal Polarization) were employed for the period June 2006 to December 2015. The three available cloud phases (ice, water, unknown) were linked with the coinciding aerosol type characterization (dust, polluted dust, smoke and background aerosols). Based on the ice cloud fraction calculations done in this study, clouds freeze in warmer temperatures in the presence of dust particles than with other aerosol types. A difference in the cloud freezing temperature as high as 7o C was observed. Thus, dust aerosols have a high potential to affect the properties of Arctic clouds. Furthermore, possible increments in efficient IN due to long-range transported aerosols or new local aerosol sources due to anthropogenic activities may lead to optically thinner clouds modifying the radiation balance over Arctic.

  2. Direct Radiative Effect and Heating Rate of black carbon aerosol: high time resolution measurements and source-identified forcing effects

    Science.gov (United States)

    Ferrero, Luca; Mocnik, Grisa; Cogliati, Sergio; Comi, Alberto; Degni, Francesca; Di Mauro, Biagio; Colombo, Roberto; Bolzacchini, Ezio

    2016-04-01

    Black carbon (BC) absorbs sunlight in the atmosphere heating it. However, up to now, heating rate (HR) calculations from the divergence of the net radiative flux with altitude or from the modelling activity are too sparse. This work fills the aforementioned gap presenting a new methodology based on a full set of physical equations to experimentally determine both the radiative power density absorbed into a ground-based atmospheric layer (ADRE), and the consequent HR induced by the absorptive component of aerosol. In urban context, it is essentially related to the BC. The methodology is also applicable to natural components (i.e. dust) and is obtained solving the first derivative of the main radiative transfer equations. The ADRE and the consequent HR can be determined coupling spectral aerosol absorption measurements with the spectrally resolved measurements of the direct, diffuse downward radiation and the surface reflected radiance components. Moreover, the spectral absorption of BC aerosol allows its source apportionment (traffic and biomass burning (BB)) allowing the same apportionment on HR. This work reports one year of high-time resolution measurements (5 min) of sunlight absorption and HR induced by BC aerosol over Milan. A unique sampling site was set up from March 2015 with: 1) Aethalometer (AE-31, Magee Scientific, 7-λ), 2) the Multiplexer-Radiometer-Irradiometer which detects downward and reflected radiance (350-1000 nm in 3648 spectral bands) coupled with a rotating shadow-band to measure spectrally-resolved global and diffuse radiation (thus direct), 3) a meteorological station (LSI-Lastem) equipped with 3 pyranometers (global, diffuse and refrected radiation; 300-3000 nm), a thermohygrometer, a barometer, an anemometer, 4) condensation and optical particle counters (TSI 3775 and Grimm 1.107), 5) low volume sampler (FAI Hydra dual sampler, PM2.5 and PM10) for sample collection and chemistry determination. Results concerning the radiative power

  3. Activation of the Solid Silica Layer of Aerosol-Based C/SiO₂ Particles for Preparation of Various Functional Multishelled Hollow Microspheres.

    Science.gov (United States)

    Li, Xiangcun; Luo, Fan; He, Gaohong

    2015-05-12

    Double-shelled C/SiO2 hollow microspheres with an outer nanosheet-like silica shell and an inner carbon shell were reported. C/SiO2 aerosol particles were synthesized first by a one-step rapid aerosol process. Then the solid silica layer of the aerosol particles was dissolved and regrown on the carbon surface to obtain novel C/SiO2 double-shelled hollow microspheres. The new microspheres prepared by the facile approach possess high surface area and pore volume (226.3 m(2) g(-1), 0.51 cm(3) g(-1)) compared with the original aerosol particles (64.3 m(2) g(-1), 0.176 cm(3) g(-1)), providing its enhanced enzyme loading capacity. The nanosheet-like silica shell of the hollow microspheres favors the fixation of Au NPs (C/SiO2/Au) and prevents them from growing and migrating at 500 °C. Novel C/C and C/Au/C (C/Pt/C) hollow microspheres were also prepared based on the hollow nanostructure. C/C microspheres (482.0 m(2) g(-1), 0.92 cm(3) g(-1)) were ideal electrode materials. In particular, the Au NPs embedded into the two carbon layers (C/Au/C, 431.2 m(2) g(-1), 0.774 cm(3) g(-1)) show a high catalytic activity and extremely chemical stability even at 850 °C. Moreover, C/SiO2/Au, C/Au/C microspheres can be easily recycled and reused by an external magnetic field because of the presence of Fe3O4 species in the inner carbon shell. The synthetic route reported here is expected to simplify the fabrication process of double-shelled or yolk-shell microspheres, which usually entails multiple steps and a previously synthesized hard template. Such a capability can facilitate the preparation of various functional hollow microspheres by interfacial design.

  4. Glass shards, pumice fragments and volcanic aerosol particles - diagenesis a recorder of volcanic activity?

    Science.gov (United States)

    Obenholzner, J. H.; Schroettner, H.; Poelt, P.; Delgado, H.

    2003-04-01

    Detailed SEM/EDS studies of Triassic (Southern Alps, A, I, Sl) and Miocene (Mixteca Alta, Mexico) tuffs revealed that volcanic glass shards can be replaced by zeolites (analcite), chlorites and smectites preserving the shape of primary shards (1). The Triassic pyroclastic deposits have been incorporated in the pre-Alpine burial diagenesis, the Miocene pyroclastic deposits are bentonites. The volcanologist is impressed by the circumstances that million years old pyroclast relict textures can be sized. Shape parameters obtained by image analysis can be compared with much younger pyroclastic deposits (2). Both deposits have not been effected by shearing. The alteration of pumice fragments of Triassic age is not a simple replacement process. Intergrowth of different illites and chlorites and probably vesicle filling by SiO2 and subsequent overgrowth make a reconstruction sometimes difficult. These processes are accompanied by the formation of REE-, Y- and Zr-bearing minerals as well as with the alteration of zircons. Studies of recently erupted ash from Popocatepetl volcano reveal the presence of a variety of µm-sized contact-metamorphosed clasts being a part of the volcanic ash (3). Such clasts should be present in many older pyroclastic deposits, especially where volcanoes had been situated on massive sedimentary units providing contact metamorphism in the realm of a magma chamber or during magma ascent. Volcanic aerosol particles collected in 1997 from the passively degassing plume of Popocatepetl volcano revealed in FESEM/EDS analysis (H. Schroettner and P. Poelt) a wide spectrum of fluffy, spherical and coagulated spherical particles (µm-sized). Under pre-vacuum conditions they remained stable for ca. 3 years (3). In nature the fate of these particles in the atmosphere is unknown. Are there relicts in marine, lacustrine sediments and ice cores, which could be used as proxies of volcanic activity? (1) Obenholzner &Heiken,1999. Ann.Naturhist.Mus.Wien, 100 A, 13

  5. Efficacy of High-volume Evacuator in Aerosol Reduction: Truth or Myth? A Clinical and Microbiological Study

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    Hitesh Desarda

    2014-09-01

    Full Text Available Background and aims. Basic periodontal treatment aims at eliminating supra- and sub-gingival plaque and establishing conditions which will allow effective self-performed plaque control. This aim is primarily achieved with sonic and ultrasonic scalers. However, generation of bacterial aerosols during these procedures is of great concern to patients, the dentist and the dental assistant. The aim of this study was to compare the reduction in aerosol with and without high-volume evacuator through a microbiological study. Materials and methods. For this clinical study a fumigated closed operatory was selected. Maxillary incisors and canines were selected as an area for scaling. Piezoelectric ultrasonic scaling was performed in the absence and in the presence of a high-volume evacuator at 12 and 20 inches from the patient's oral cavity. In both groups scaling was carried out for 10 minutes. Nutrient agar plates were exposed for a total of 20 minutes. After this procedure, nutrient agar plates were incubated in an incubator at 37°C for 24 hours. The next day the nutrient agar plates were examined for colony forming units by a single microbiologist. Results. The results showed no statistically significant differences in colony forming units (CFU with and without the use of a high-volume evacuator either at 12 or 20 inches from the patient’s oral cavity. Conclusion. It was concluded that high-volume evacuator, when used as a separate unit without any modification, is not effective in reducing aerosol counts and environmental contamination.

  6. Molecular composition and volatility of isoprene photochemical oxidation secondary organic aerosol under low and high NOx conditions

    Energy Technology Data Exchange (ETDEWEB)

    D' Ambro, Emma; Lee, Ben H.; Liu, Jiumeng; Shilling, John E.; Gaston, Cassandra J.; Lopez-Hilfiker, Felipe D.; Schobesberger, Siegfried; Zaveri, Rahul A.; Mohr, Claudia; Lutz, Anna; Zhang, Zhenfa; Gold, Avram; Surratt, Jason D.; Rivera-Rios, Jean; Keutsch, Frank N.; Thornton, Joel A.

    2017-01-04

    We present measurements of secondary organic aerosol (SOA) formation from isoprene photochemical oxidation formed in an environmental simulation chamber using dry neutral seed particles, thereby suppressing the role of acid catalyzed multiphase chemistry, at a variety of oxidant conditions. A high-resolution time-of-flight chemical ionization mass spectrometer (HRToF-CIMS) utilizing iodide-adduct ionization coupled to the Filter Inlet for Gases and AEROsols (FIGAERO) allowed for the simultaneous online sampling of the gas and particle composition. Under high HO2 and low NO conditions, highly oxygenated (O:C ≥ 1) C5 compounds were major components (~50%) of the SOA. The overall composition of the SOA evolved both as a function of time and as a function of input NO concentrations. As the level of input NO increased, organic nitrates increased in both the gas- and particle-phases, but the dominant non-nitrate particle-phase components monotonically decreased. We use comparisons of measured and predicted gas-particle partitioning of individual components to assess the validity of literature-based group-contribution methods for estimating saturation vapor concentrations. While there is evidence for equilibrium partitioning being achieved on the chamber residence time scale (5.2 hours) for some individual components, significant errors in group-contribution methods are revealed. In addition, >30% of the SOA mass, detected as low-molecular weight compounds, cannot be reconciled with equilibrium partitioning. These compounds desorb from the FIGAERO at unexpectedly high temperatures given their molecular composition, indicative of thermal decomposition of effectively lower volatility components, likely larger molecular weight oligomers. We use these insights from the laboratory and observations of the same SOA components made during the Southern Oxidant and Aerosol Study (SOAS) to assess the importance of isoprene photooxidation as a local SOA source.

  7. Aerosol radiative effect in UV, VIS, NIR, and SW spectra under haze and high-humidity urban conditions

    Science.gov (United States)

    Zhang, Ming; Ma, Yingying; Gong, Wei; Wang, Lunche; Xia, Xiangao; Che, Huizheng; Hu, Bo; Liu, Boming

    2017-10-01

    Aerosol properties derived from sun-photometric observations at Wuhan during a haze period were analyzed and used as input in a radiative transfer model to calculate the aerosol radiative effect (ARE) in ultraviolet (UV), visible (VIS), near-infrared (NIR), and shortwave (SW) spectra. The results showed that the aerosol optical depth (AOD) at 440 nm increased from 0.32 under clear-air conditions to 0.85 during common haze and 1.39 during severe haze. An unusual inverse relationship was found between the Ångström exponent (AE) and AOD during the haze period at Wuhan. Under high-humidity conditions, the fine-mode median radius of aerosols increased from 0.113 μm to approximately 0.2-0.5 μm as a result of hygroscopic growth, which led to increases in the AOD and decreases in the AE simultaneously. These changes were responsible for the inverse relationship between AE and AOD at Wuhan. The surface ARE in the UV (AREUV), VIS (AREVIS), NIR (ARENIR), and SW (ARESW) spectra changed from -4.46, -25.37, -12.15, and -41.99 W/m2 under clear-air conditions to -9.48, -53.96, -29.81, and -93.25 W/m2 during common hazy days and -12.89, -80.16, -55.17, and -148.22 W/m2 during severe hazy days, respectively, and the percentages of AREUV, AREVIS, and ARENIR in ARESW changed from 11%, 61%, and 28%-9%, 54%, and 37%, respectively. Meanwhile, the ARE efficiencies (REE) in SW varied from -206.5 W/m2 under clear-air conditions to -152.94 W/m2 during the common haze period and -131.47 W/m2 during the severe haze period. The smallest decreasing rate of the REE in NIR was associated with the increase of ARENIR. The weakened REE values were related to the strong forward scattering and weak backward scattering of fine aerosol particles with increasing size resulting from hygroscopic growth, while the variation of the single scattering albedo showed less impact. Source region analysis by back trajectories and the concentration weighted trajectory (CWT) method showed that black carbon came

  8. Synchronised Aerosol Mass Spectrometer Measurements across Europe

    Science.gov (United States)

    Nemitz, Eiko

    2010-05-01

    Up to twelve Aerodyne Aerosol Mass Spectrometers (AMSs) were operated simultaneously at rural and background stations (EMEP and EUSAAR sites) across Europe. Measurements took place during three intensive periods, in collaboration between the European EUCAARI IP and the EMEP monitoring activities under the UNECE Convention for Long-Range Transboundary Air Pollution (CLRTAP) during three contrasting months (May 2008, Sep/Oct 2008, Feb/Mar 2009). These measurements were conducted, analysed and quality controlled carefully using a unified protocol, providing the largest spatial database of aerosol chemical composition measured with a unified online technique to date, and a unique snapshots of the European non-refractory submicron aerosol climatology. As campaign averages over all active monitoring sites, organics represent 28 to 43%, sulphate 18 to 25%, ammonium 13 to 15% and nitrate 15 to 36% of the resolved aerosol mass, with the highest relative nitrate contribution during the Feb/Mar campaign. The measurements demonstrate that in NW Europe (e.g. Ireland, UK, The Netherlands, Germany, Switzerland) the regional submicron aerosol tends to be neutralised and here nitrates make a major contribution to the aerosol mass. By contrast, periods with low nitrate and acidic aerosol were observed at sites in S and E Europe (e.g. Greece, Finland), presumably due to a combination of larger SO2 point sources in Easter Europe, smaller local NH3 sources and, in the case of Greece, higher temperatures. While at the more marine and remote sites (Ireland, Scotland, Finland) nitrate concentrations were dominated by episodic transport phenomena, at continental sites (Switzerland, Germany, Hungary) nitrate followed a clear diurnal cycle, reflecting the thermodynamic behaviour of ammonium nitrate. The datasets clearly shows spatially co-ordinated, large-scale pollution episodes of organics, sulphate and nitrate, the latter being most pronounced during the Feb/Mar campaign. At selected

  9. Novel method of generation of Ca(HCO32 and CaCO3 aerosols and first determination of hygroscopic and cloud condensation nuclei activation properties

    Directory of Open Access Journals (Sweden)

    A. Trimborn

    2010-09-01

    Full Text Available Atmospheric mineral aerosols contain CaCO3 as a reactive component. A novel method to produce CaCO3 aerosol was developed by spraying Ca(HCO32 solution, which was generated from a CaCO3 suspension and CO2. By aerosol mass spectrometry the freshly sprayed and dried aerosol was characterized to consist of pure Ca(HCO32 which under annealing in a tube furnace transformed into CaCO3. Transmission Electron Microscopy demonstrated that the particles produced were spherical. The method was able to generate aerosol of sufficient concentration and proper size for the study of physiochemical properties and investigations of heterogeneous reactions of mineral aerosol. The dried Ca(HCO32 particles were somewhat more hygroscopic than CaCO3 particles. However, during humidification a restructuring took place and ∼2/3 of the Ca(HCO32 was transformed to CaCO3. The mixed Ca(HCO32/CaCO3(s particles were insoluble with a growth factor of 1.03 at 95% (hygroscopicity parameter κ=0.011±0.007 relative humidity. This compares to a corresponding growth factor of 1.01 for CaCO3(s (κ=0.0016±0.0004. Mass spectrometric composition analysis, restructuring, and insolubility of the mixed particles suggested that solid Ca(HCO32(s was observed. This would be in contrast to the current belief that Ca(HCO32(s is thermodynamically instable. The CCN activity of Ca(HCO32(s aerosol (κ≈0.15 is remarkably higher than that of CaCO3 aerosol (κ=0.0019±0.0007 and less than that of Ca(NO32. The noticeable but limited solubility of Ca(HCO32 of ≈0.01 mol/l explains limited hygroscopic growth and good CCN activity. Experiments in the Large Jülich Aerosol Chamber indicated that Ca(HCO32(s could exist for several hours under dry atmospheric conditions. However, it was likely buried in a protective layer of CaCO3(s. We conclude that Ca(HCO32 may be formed in the atmosphere in cloud droplets of activated mineral dust by reaction of CaCO3 with CO2 and H2O. The presence of Ca(HCO32 and

  10. Aerosol-assisted plasma deposition of hydrophobic polycations makes surfaces highly antimicrobial.

    Science.gov (United States)

    Liu, Harris; Kim, Yoojeong; Mello, Kerrianne; Lovaasen, John; Shah, Apoorva; Rice, Norman; Yim, Jacqueline H; Pappas, Daphne; Klibanov, Alexander M

    2014-02-01

    The currently used multistep chemical synthesis for making surfaces antimicrobial by attaching to them hydrophobic polycations is replaced herein by an aerosol-assisted plasma deposition procedure. To this end, N,N-hexyl,methyl-PEI (HMPEI) is directly plasma-coated onto a glass surface. The resultant immobilized HMPEI coating has been thoroughly characterized and shown to be robust, bactericidal against Escherichia coli, and virucidal against human influenza virus.

  11. Preliminary results of the aerosol optical depth retrieval in Johor, Malaysia

    Science.gov (United States)

    Lim, H. Q.; Kanniah, K. D.; Lau, A. M. S.

    2014-02-01

    Monitoring of atmospheric aerosols over the urban area is important as tremendous amounts of pollutants are released by industrial activities and heavy traffic flow. Air quality monitoring by satellite observation provides better spatial coverage, however, detailed aerosol properties retrieval remains a challenge. This is due to the limitation of aerosol retrieval algorithm on high reflectance (bright surface) areas. The aim of this study is to retrieve aerosol optical depth over urban areas of Iskandar Malaysia; the main southern development zone in Johor state, using Moderate Resolution Imaging Spectroradiometer (MODIS) 500 m resolution data. One of the important steps is the aerosol optical depth retrieval is to characterise different types of aerosols in the study area. This information will be used to construct a Look Up Table containing the simulated aerosol reflectance and corresponding aerosol optical depth. Thus, in this study we have characterised different aerosol types in the study area using Aerosol Robotic Network (AERONET) data. These data were processed using cluster analysis and the preliminary results show that the area is consisting of coastal urban (65%), polluted urban (27.5%), dust particles (6%) and heavy pollution (1.5%) aerosols.

  12. Aerosol hygroscopicity and cloud droplet activation of extracts of filters from biomass burning experiments

    Science.gov (United States)

    Carrico, Christian M.; Petters, Markus D.; Kreidenweis, Sonia M.; Collett, Jeffrey L.; Engling, Guenter; Malm, William C.

    2008-04-01

    In this laboratory closure study, we compare sub- and supersaturated water uptake properties for aerosol particles possessing a range of hygroscopicity. Measurements for water sub-saturated conditions used a hygroscopic tandem differential mobility analyzer (HTDMA). Simultaneously, measurements of particle critical supersaturation were conducted on the same sample stream with a continuous flow cloud condensation nuclei (CCN) counter. For these experiments, we used filter-collected samples of biomass smoke generated in the combustion of two common wildland fire fuels, western sagebrush and Alaskan duff core. Extractions of separate sections of the filter were performed using two solvents, ultrapure water and methanol. The extracts were subsequently atomized, producing aerosols having a range of hygroscopic responses. HTDMA and CCN measurements were fit to a single-parameter model of water uptake, in which the fit parameter is denoted κ, the hygroscopicity parameter. Here, for the four extracts we observed mean values of the hygroscopicity parameter of 0.06 CCN-derived values of κ for each experiment agreed within approximately 20%. Applicability of the κ-parameterization to other multicomponent aerosols relevant to the atmosphere remains to be tested.

  13. Deriving aerosol hygroscopic mixing state from size-resolved CCN activity and HR-ToF-AMS measurements

    Science.gov (United States)

    Bhattu, Deepika; Tripathi, S. N.; Chakraborty, Abhishek

    2016-10-01

    The ability of a particle to uptake water and form a cloud droplet depends on its hygroscopicity. To understand its impact on cloud properties and ultimately radiative forcing, knowledge of chemically-resolved mixing state information or the one based on hygroscopic growth is crucial. Typically, global models assume either pure internal or external mixing state which might not be true for all conditions and sampling locations. To investigate into this, the current study employed an indirect approach to infer the probable mixing state. The hygroscopic parameters derived from κ-Kohler theory using size-resolved CCN measurements (κCCN) and bulk/size-resolved aerosol mass spectrometer (AMS) measurements (κAMS) were compared. The accumulation mode particles were found to be more hygroscopic (κCCN = 0.24) than Aitken mode (κCCN = 0.13), perhaps due to increased ratio of inorganic to organic mass fraction. The activation diameter calculated from size-resolved CCN activity measurements at 5 different supersaturation (SS) levels varied in the range of 115 nm-42 nm with κCCN = 0.13-0.23 (avg = 0.18 ± 0.10 (±1σ)). Further, κAMS>κCCN was observed possibly due to the fact that organic and inorganic mass present in the Aitken mode was not correctly represented by bulk chemical composition and size-resolved fractional contribution of oxidized OA was not accurately accounted. Better correlation of organic fraction (forg) and κCCN at lower SS explained this behaviour. The decrease in κCCN with the time of the day was more pronounced at lower SS because of the relative mass reduction of soluble inorganic species by ∼17%. Despite the large differences between κ measured from two approaches, less over-prediction (up to 18%) between measured and predicted CCN concentration suggested lower impact of chemical composition and mixing state at higher SS. However, at lower SS, presences of externally mixed CCN-inactive aerosols lead to CCN over-prediction reflecting the

  14. A molecular-level approach for characterizing water-insoluble components of ambient organic aerosol particulates using ultra-high resolution mass spectrometry

    Directory of Open Access Journals (Sweden)

    A. S. Willoughby

    2014-04-01

    Full Text Available The chemical composition of organic aerosols in the atmosphere is strongly influenced by human emissions, and the effect these have on the environment, human health, and climate change is determined by the molecular nature of these chemical species. The complexity of organic aerosol samples limits the ability to study the chemical composition, and, therefore, the associated properties and the impacts they have. Many studies address the water-soluble fraction of organic aerosols, and have had much success in identifying specific molecular formulas for thousands of compounds present. However, little attention is given to the water-insoluble portion, which can contain most of the fossil material that is emitted through human activity. Here we compare the organic aerosols present in water extracts and organic solvent extracts (pyridine and acetonitrile of an ambient aerosol sample collected in a rural location that is impacted by natural and anthropogenic emission sources. A semi-quantitative method was developed using proton nuclear magnetic resonance spectroscopy to determine that the amount of organic matter extracted by pyridine is comparable to that of water. Electrospray ionization Fourier transform ion cyclotron resonance mass spectra show that pyridine extracts a molecularly unique fraction of organic matter compared to water or acetonitrile, which extract chemically similar organic matter components. The molecular formulas unique to pyridine were less polar, more aliphatic, and reveal formulas containing sulfur to be an important component of insoluble aerosol organic matter.

  15. Aerosol-cirrus interactions: a number based phenomenon at all?

    Directory of Open Access Journals (Sweden)

    M. Seifert

    2004-01-01

    Full Text Available In situ measurements of the partitioning of aerosol particles within cirrus clouds were used to investigate aerosol-cloud interactions in ice clouds. The number density of interstitial aerosol particles (non-activated particles in between the cirrus crystals was compared to the number density of cirrus crystal residuals. The data was obtained during the two INCA (Interhemispheric Differences in Cirrus Properties from Anthropogenic Emissions campaigns, performed in the Southern Hemisphere (SH and Northern Hemisphere (NH midlatitudes. Different aerosol-cirrus interactions can be linked to the different stages of the cirrus lifecycle. Cloud formation is linked to positive correlations between the number density of interstitial aerosol (Nint and crystal residuals (Ncvi, whereas the correlations are smaller or even negative in a dissolving cloud. Unlike warm clouds, where the number density of cloud droplets is positively related to the aerosol number density, we observed a rather complex relationship when expressing Ncvi as a function of Nint for forming clouds. The data sets are similar in that they both show local maxima in the Nint range 100 to 200cm, where the SH- maximum is shifted towards the higher value. For lower number densities Nint and Ncvi are positively related. The slopes emerging from the data suggest that a tenfold increase in the aerosol number density corresponds to a 3 to 4 times increase in the crystal number density. As Nint increases beyond the ca. 100 to 200cm, the mean crystal number density decreases at about the same rate for both data sets. For much higher aerosol number densities, only present in the NH data set, the mean Ncvi remains low. The situation for dissolving clouds allows us to offer two possible, but at this point only speculative, alternative interactions between aerosols and cirrus: evaporating clouds might be associated with a source of aerosol particles, or air pollution (high aerosol number density might

  16. Observed high-altitude warming and snow cover retreat over Tibet and the Himalayas enhanced by black carbon aerosols

    Science.gov (United States)

    Xu, Y.; Ramanathan, V.; Washington, W. M.

    2016-02-01

    Himalayan mountain glaciers and the snowpack over the Tibetan Plateau provide the headwater of several major rivers in Asia. In situ observations of snow cover extent since the 1960s suggest that the snowpack in the region have retreated significantly, accompanied by a surface warming of 2-2.5 °C observed over the peak altitudes (5000 m). Using a high-resolution ocean-atmosphere global climate model and an observationally constrained black carbon (BC) aerosol forcing, we attribute the observed altitude dependence of the warming trends as well as the spatial pattern of reductions in snow depths and snow cover extent to various anthropogenic factors. At the Tibetan Plateau altitudes, the increase in atmospheric CO2 concentration exerted a warming of 1.7 °C, BC 1.3 °C where as cooling aerosols cause about 0.7 °C cooling, bringing the net simulated warming consistent with the anomalously large observed warming. We therefore conclude that BC together with CO2 has contributed to the snow retreat trends. In particular, BC increase is the major factor in the strong elevation dependence of the observed surface warming. The atmospheric warming by BC as well as its surface darkening of snow is coupled with the positive snow albedo feedbacks to account for the disproportionately large role of BC in high-elevation regions. These findings reveal that BC impact needs to be properly accounted for in future regional climate projections, in particular on high-altitude cryosphere.

  17. Study of a complex environmental mixture by electrospray ionization and laser desorption ionization high resolution mass spectrometry: the cigarette smoke aerosol

    Directory of Open Access Journals (Sweden)

    Vincent Carré

    2015-06-01

    Full Text Available Aerosols from the mainstream cigarette smoke have been analyzed by electrospray ionization (ESI coupled to Fourier transform ion cyclotron resonance mass spectrometry (FTICRMS. Measurements have been conducted in positive ion mode. The chemical composition of cigarette smoke aerosol is significant because it gives insights of one complex indoor environmental mixture. Almost 1300 chemical compositions relative to nitrogen species were successfully determined through the accurate mass measurement and the good ion production of the used technique. The most abundant class of compounds corresponds to N2 one (hydrocarbons with two nitrogen atoms. For other classes, the van Krevelen diagrams ensured to define that other nitrogen and oxygen-nitrogen compounds adopted similar behavior in terms of unsaturation and alkylation range. The detailed composition of cigarette smoke aerosol provided a typical chemical fingerprint from the biomass pyrolysis with tobacco-specific compounds. We examined also the contribution of laser desorption ionization (LDI technique coupled to FTICRMS for the acute analysis of cigarette smoke aerosol. While a part of the chemical composition were found similar to ESI results, LDI achieved a broader range of poly-aromatic compounds and highlight new class compounds as pure hydrocarbon and oxygen-containing species. The combination of ESI and LDI with high resolution mass spectrometry clearly increased significantly the coverage of the “whole composition” of environmental aerosols such as cigarette smoke aerosol.

  18. Aerosol Interactions with Extensive Stratus Cloud During VOCALS

    Science.gov (United States)

    Clarke, A. D.; McNaughton, C. S.; Freitag, S.; Howell, S.; Kapustin, V.; Snider, J.; Campos, T. L.; Leon, D.; Shank, L.; Wood, R.

    2009-12-01

    The 2008 VOCALS experiment over the Pacific and off the north coast of Chile provided numerous opportunities to examine aerosol-stratus interactions over 1000km flight legs and processes associated with their breakup into pockets of open cells (POC’s). Our HiGEAR (Hawaii Group for Environmental Aerosol Research) measurements on the NCAR C-130 aircraft included the aerosol size-distribution, size-resolved volatile and non-volatile components, ionic and organic chemistry (AMS), black carbon (BC, as measured by Single Particle Soot Photometer - SP2) and associated optical properties. We are exploring these observations in conjunction with meteorological data, trace gas data (eg. O3, CO) and cloud condensation nuclei (CCN) to resolve features related to the source, removal and evolution of aerosol active as CCN. Stratus clouds decks along the coast were heavily impacted by anthropogenic combustion sources along the coast. Offshore in the marine boundary layer (MBL) below cloud these influences diminished and transitioned to clean central Pacific aerosol west of about 75W. Periods with smallest aerosol sizes tended to show subsidence around the South Pacific high pressure system while larger sizes had spent more time in the MBL. However, at various altitudes in the free troposphere (FT) above cloud, relatively low concentrations of biomass burning (BB) aerosol occurred in patches and “rivers” of flow. These BB aerosol were often near cloud top or within a day of subsiding to cloud top for estimated rates of about 0.4 cm/s. The BB aerosol was generally associated with elevated CO, organic, non-volatile aerosol, and BC. POC’s were lowest in CO compared to both adjacent cloudy air and FT air, indicating less prior influence from combustion aerosol than cloudy regions. POC regions manifested dramatic aerosol reduction through precipitation and drizzle resulting in low concentrations with diameters often less than about 40nm. Offshore, drizzling cloudy regions

  19. Radiocarbon-based Source Apportionment of Organic, Elemental and Water-soluble Organic Carbon Aerosols and the Light Absorption of Water-soluble Organic Carbon Aerosols in the East Asia High-intensity Winter Campaigns in 2014

    Science.gov (United States)

    Fang, W.; Andersson, A.; Zheng, M.; Lee, M.; Kim, S. W.; Du, K.; Gustafsson, O.

    2016-12-01

    Improved understanding of anthropogenic aerosol effects on atmospheric chemistry and climate as well as efficient mitigation actions are hampered by the limited comprehension of the relative contributions of different sources of carbonaceous aerosols and of their subsequent atmospheric processing. Here, we present dual carbon isotope constrained source apportionment and optical properties of carbonaceous aerosols simultaneously both at urban and rural receptor sites, includes North China Plain (NCP, Beijing and Tianjin), Yangtze River Delta (YRD, Shanghai, Zhejiang), and Jeju Island (Korea Climate Observatory at Gosan) during January 2014 field campaigns. The radiocarbon (∆14C) data show that fossil combustions contribute equally ˜80 ± 5% to elemental carbon (EC) aerosol in Beijing, Tianjin, and Shanghai, and 66 ± 9% to Gosan-EC aerosol, while the specific sources of the dominant fossil fuel component were dramatically different among these sites. The mean fraction coal combustion of Beijing-EC, Tianjin-EC, and Gosan-EC is double that of Shanghai-EC. The other large fraction (72―92%) of carbonaceous aerosol is organic carbon (OC) aerosol which contains water soluble and water insoluble organic carbon (WSOC and WISOC). OC, WISOC, and WSOC in Beijing and Gosan sites were still observed largely from fossil sources (53―75%). The more 13C-enriched signature of Gosan-WSOC (-22.8 ± 0.2‰) compared to Gosan-EC (-23.9 ± 0.4‰) and Beijing-WSOC (-23.5 ± 0.7‰) reflects that WSOC is likely more affected by atmospheric aging during long-rang transport than is EC. The high light absorption coefficients of PM2.5, PM1, and TSP were observed at Gosan during this study and was frequently reaching 20―60 Mm-1 by aethalometer and continuous light absorption photometer. The mass absorption cross section of WSOC (MAC365) for above sites is high (1.5 ± 0.8 m2/g), accounted for ˜14 ± 5% of the total direct absorbance relative to EC, which is significantly higher than

  20. Investigating primary marine aerosol properties: CCN activity of sea salt and mixed particles

    Science.gov (United States)

    King, S. M.; Butcher, A. C.; Rosenoern, T.; Coz, E.; Lieke, K. I.; de Leeuw, G.; Nilsson, E. D.; Bilde, M.

    2012-04-01

    Sea salt particles ejected as a result of bubbles bursting from artificial seawater in a closed stainless steel tank were sampled for size distribution, morphology, and cloud condensation nucleus (CCN) activity. The two-component artificial seawater consisted of salt, either NaCl or sea salt, and one organic compound in deionized water. Several organic molecules representative of oceanic organic matter were investigated. Bubbles were generated either by aeration through a porous diffuser or by water jet impingement on the surface of the artificial seawater. The effect of bubble lifetime, which was controlled by varying the depth of the diffuser in the water column, on particle size and CCN activity was investigated and was found to be insignificant for the organic compounds studied. The CCN activities of particles produced from diffuser-generated bubbles were generally governed by the high hygroscopicity of salt, such that activation was indistinguishable from that of salt, except in the case of very low mass ratio of salt to organic matter in the seawater solution. There was, however, a considerable decrease in CCN activity for particles produced from jet impingement on seawater that had a salinity of 10‰ and contained 0.45 mM of sodium laurate, an organic surfactant. The production of a thick foam layer from impingement may explain the difference in activation and supports hypotheses that particle production from the two methods of generating bubbles is not similar. Accurate conclusions from observed CCN activities of particles from artificial seawater containing organic matter require knowledge of the CCN activity of the inorganic component, especially as a small amount of the inorganic can heavily influence activation. Therefore, the CCN activity of both artificial sea salt and NaCl were measured and compared. Part of the discrepancy observed between the CCN activities of the two salts may be due to morphological differences, which were investigated using

  1. Seasonal variations in high time-resolved chemical compositions, sources, and evolution of atmospheric submicron aerosols in the megacity Beijing

    Science.gov (United States)

    Hu, Wei; Hu, Min; Hu, Wei-Wei; Zheng, Jing; Chen, Chen; Wu, Yusheng; Guo, Song

    2017-08-01

    A severe regional haze problem in the megacity Beijing and surrounding areas, caused by fast formation and growth of fine particles, has attracted much attention in recent years. In order to investigate the secondary formation and aging process of urban aerosols, four intensive campaigns were conducted in four seasons between March 2012 and March 2013 at an urban site in Beijing (116.31° E, 37.99° N). An Aerodyne high-resolution time-of-flight aerosol mass spectrometry (HR-ToF-AMS) was deployed to measure non-refractory chemical components of submicron particulate matter (NR-PM1). The average mass concentrations of PM1 (NR-PM1+black carbon) were 45.1 ± 45.8, 37.5 ± 31.0, 41.3 ± 42.7, and 81.7 ± 72.4 µg m-3 in spring, summer, autumn, and winter, respectively. Organic aerosol (OA) was the most abundant component in PM1, accounting for 31, 33, 44, and 36 % seasonally, and secondary inorganic aerosol (SNA, sum of sulfate, nitrate, and ammonium) accounted for 59, 57, 43, and 55 % of PM1 correspondingly. Based on the application of positive matrix factorization (PMF), the sources of OA were obtained, including the primary ones of hydrocarbon-like (HOA), cooking (COA), biomass burning OA (BBOA) and coal combustion OA (CCOA), and secondary component oxygenated OA (OOA). OOA, which can be split into more-oxidized (MO-OOA) and less-oxidized OOA (LO-OOA), accounted for 49, 69, 47, and 50 % in four seasons, respectively. Totally, the fraction of secondary components (OOA+SNA) contributed about 60-80 % to PM1, suggesting that secondary formation played an important role in the PM pollution in Beijing, and primary sources were also non-negligible. The evolution process of OA in different seasons was investigated with multiple metrics and tools. The average carbon oxidation states and other metrics show that the oxidation state of OA was the highest in summer, probably due to both strong photochemical and aqueous-phase oxidations. It was indicated by the good correlations

  2. Hygroscopicity of the submicrometer aerosol at the high-alpine site Jungfraujoch, 3580 m a.s.l., Switzerland

    Directory of Open Access Journals (Sweden)

    S. Sjogren

    2008-09-01

    Full Text Available Data from measurements of hygroscopic growth of submicrometer aerosol with a hygroscopicity tandem differential mobility analyzer (HTDMA during four campaigns at the high alpine research station Jungfraujoch, Switzerland, are presented. The campaigns took place during the years 2000, 2002, 2004 and 2005, each lasting approximately one month. Hygroscopic growth factors (GF, i.e. the relative change in particle diameter from dry diameter, D0, to diameter measured at higher relative humidity, RH are presented for three distinct air mass types, namely for: 1 free tropospheric winter conditions, 2 planetary boundary layer influenced air masses (during a summer period and 3 Saharan dust events (SDE. The GF values at 85% RH (D0=100 nm were 1.40±0.11 and 1.29±0.08 for the first two situations while for SDE a bimodal GF distribution was often found. No phase changes were observed when the RH was varied between 10–90%, and the continuous water uptake could be well described with a single-parameter empirical model. The frequency distributions of the average hygroscopic growth factors and the width of the retrieved growth factor distributions (indicating whether the aerosol is internally or externally mixed are presented, which can be used for modeling purposes.

    Measurements of size resolved chemical composition were performed with an aerosol mass spectrometer in parallel to the GF measurements. This made it possible to estimate the apparent ensemble mean GF of the organics (GForg using inverse ZSR (Zdanovskii-Stokes-Robinson modeling. GForg was found to be ~1.20 at aw=0.85, which is at the upper end of previous laboratory and field data though still in agreement with the highly aged and oxidized nature of the Jungfraujoch aerosol.

  3. In situ fabrication of depth-type hierarchical CNT/quartz fiber filters for high efficiency filtration of sub-micron aerosols and high water repellency

    Science.gov (United States)

    Li, Peng; Zong, Yichen; Zhang, Yingying; Yang, Mengmeng; Zhang, Rufan; Li, Shuiqing; Wei, Fei

    2013-03-01

    We fabricated depth-type hierarchical CNT/quartz fiber (QF) filters through in situ growth of CNTs upon quartz fiber (QF) filters using a floating catalyst chemical vapor deposition (CVD) method. The filter specific area of the CNT/QF filters is more than 12 times higher than that of the pristine QF filters. As a result, the penetration of sub-micron aerosols for CNT/QF filters is reduced by two orders of magnitude, which reaches the standard of high-efficiency particulate air (HEPA) filters. Simultaneously, due to the fluffy brush-like hierarchical structure of CNTs on QFs, the pore size of the hybrid filters only has a small increment. The pressure drop across the CNT/QF filters only increases about 50% with respect to that of the pristine QF filters, leading to an obvious increased quality factor of the CNT/QF filters. Scanning electron microscope images reveal that CNTs are very efficient in capturing sub-micron aerosols. Moreover, the CNT/QF filters show high water repellency, implying their superiority for applications in humid conditions.We fabricated depth-type hierarchical CNT/quartz fiber (QF) filters through in situ growth of CNTs upon quartz fiber (QF) filters using a floating catalyst chemical vapor deposition (CVD) method. The filter specific area of the CNT/QF filters is more than 12 times higher than that of the pristine QF filters. As a result, the penetration of sub-micron aerosols for CNT/QF filters is reduced by two orders of magnitude, which reaches the standard of high-efficiency particulate air (HEPA) filters. Simultaneously, due to the fluffy brush-like hierarchical structure of CNTs on QFs, the pore size of the hybrid filters only has a small increment. The pressure drop across the CNT/QF filters only increases about 50% with respect to that of the pristine QF filters, leading to an obvious increased quality factor of the CNT/QF filters. Scanning electron microscope images reveal that CNTs are very efficient in capturing sub-micron aerosols

  4. Size-dependent activation of aerosols into cloud droplets at a subarctic background site during the second Pallas Cloud Experiment (2nd PaCE: method development and data evaluation

    Directory of Open Access Journals (Sweden)

    T. Anttila

    2008-07-01

    Full Text Available In situ measurements of aerosol water uptake and activation of aerosols into cloud droplets provide information on how aerosols influence the microphysical properties of clouds. Here we present a computational scheme that can be used in connection with such measurements to assess the influence of the particle chemical composition and mixing state (in terms of the water uptake on the cloud nucleating ability of particles. Additionally, it provides an estimate for the peak supersaturation of water vapour reached during the formation of the observed cloud(s. The method was applied in interpreting results of a measurement campaign that focused on aerosol-cloud interactions taking place at a subarctic background site located in northern Finland (second Pallas Cloud Experiment, 2nd PaCE. A set of case studies was conducted, and the observed activation behavior could be successfully explained by a maximum supersaturation that varied between 0.18 and 0.26% depending on the case. In these cases, the diameter corresponding to the activated fraction of 50% was in the range of 110–140 nm, and the particles were only moderately water soluble with hygroscopic growth factors varying between 1.1 and 1.4. The conducted analysis showed that the activated fractions and the total number of particles acting as CCN are expected to be highly sensitive to the particle hygroscopicity. For example, the latter quantity varied over a factor between 1.8 and 3.1, depending on the case, when the mean hygroscopic growth factors were varied by 10%. Another important conclusion is that size-dependent activation profiles carries information on the mixing state of particles.

  5. Aerosol optical depths at Mohal-Kullu in the northwestern Indian Himalayan high altitude station during ICARB

    Indian Academy of Sciences (India)

    Jagdish C Kuniyal; Alpana Thakur; Harinder K Thakur; Sanjeev Sharma; P Pant; Pan S Rawat; K Krishna Moorthy

    2009-02-01

    First time observations of spectral aerosol optical depths (AODs) at Mohal (31.9°N, 77.11°E; altitude 1154m amsl) in the Kullu valley, located in the northwestern Indian Himalayan region, have been carried out during Integrated Campaign for Aerosols, gases and Radiation Budget (ICARB), as a part of the Indian Space Research Organisation–Geosphere Biosphere Program (ISRO–GBP). AODs at six wavelengths are obtained using Microtops-II Sunphotometer and Ozonometer. The monthly mean values of AOD at 500 nm are found to be 0.27 ± 0.04 and 0.24 ± 0.02 during March and April, 2006 respectively. However, their monthly mean values are 0.33 ± 0.04 at 380 nm and 0.20 ± 0.03 nm at 870 nm during March 2006 and 0.31 ± 0.3 at 380 nm and 0.17 ± 0.2 at 870 nm during April 2006, showing a gradual decrease in AOD with wavelength. The Ångstrom wavelength exponent '' had a mean value of 0.72 ± 0.05, implying reduced dominance of fine particles. Further, the afternoon AOD values are higher as compared to forenoon values by ∼33.0% during March and by ∼9.0% during April 2006 and are attributed to the pollutant lifted up from the valley by the evolving boundary layer. Besides the long-range transportation of aerosol particles by airmass from the Great Sahara and the Thar Desert regions to the observing site, the high values of AODs have also been influenced by biomass burning and frequent incidents of forest fire at local levels.

  6. Examination of parameterizations for CCN number concentrations based on in-situ aerosol activation property measurements in the North China Plain

    Directory of Open Access Journals (Sweden)

    Z. Z. Deng

    2013-01-01

    Full Text Available Precise quantification of cloud condensation nuclei (CCN number concentrations is crucial for understanding aerosol indirect effect and characterizing this effect in models. An evaluation of various methods for CCN parameterization is carried out in this paper based on in-situ measurements of aerosol activation properties within HaChi (Haze in China project. Comparisons are made by closure studies between methods using CCN spectra, bulk activation ratios, cut-off diameters and size-resolved activation ratios. The estimation of CCN number concentrations by the method using aerosol activation curves, either averaged over a day or with diurnal variation, is found to be most satisfying and straightforward. This could be well expected since size-resolved activation ratios include information regarding the effects of size-resolved chemical composition and mixing state on aerosol activation properties. The method using the averages of critical diameters, which are inferred from measured CCN number concentrations and particle number size distribution, also provides a good prediction of CCN number concentrations. Based on comparisons of all these methods in this paper, it is recommended that CCN number concentrations be predicted using particle number size distribution with inferred critical diameters or size-resolved activation ratios.

  7. Mosquito knock-down and adulticidal activities of essential oils by vaporizer, impregnated filter paper and aerosol methods

    Directory of Open Access Journals (Sweden)

    M. Ramar

    2014-09-01

    Full Text Available Essential oils from 12 medicinal plants were evaluated by three different bioassay methods (Vaporizer, Filter paper and Aerosol for Knock-down and adulticidal efficacy on the filarial vector mosquito, Culex quinquefasciatus. Based on screening results the effective plants were selected for investigating Knock-down and adulticidal potential against adult female of the laboratory-reared mosquito species, Cx. quinquefasciatus. In vaporizer bioassay method four different doses (1.25, 2.5, 5 and 10% were used. Four different doses (0.625, 1.25, 2.5 and 10% were used both filter paper (cm2 and aerosol (cm3 bioassay methods. Five essential oils (calamus, camphor, citronella, clove and eucalyptus were identified as potential treatments in vaporizer bioassay. The result showed that the knock down time decreased with increased concentration in clove oil treatment; the Knock-down time (KT 50 = 46.1 ± 0.1, 38.5 ± 0.1, 30.7 ± 0.2, and 20.1 ± 0.1 minutes was recorded at 1.25, 2.5, 5 and 10% /cm3 respectively. In filter paper method nine essential oils were identified as potential treatments. After 1 hr exposure period clove oil recorded the lowest median Knock-down time (KT50 which was calculated as 9.15 ± 0.1min/cm2. Followed by citronella (KT50 =11.4 ± 0.1 min and eucalyptus (KT50 =11.4 ±0.1min oils since they recorded lower median Knock-down time. All the twelve essential oils were identified as potential treatments in aerosol activity. The lethal time decreased when the concentration increased. At 5 % concentration the median lethal time (LT50 for clove oil was calculated as (LT50=3.80 ± 0.1minutes. The Cinnamon oil was effective which recorded (LT50 = 1.99 mins as median lethal time. Camphor (LT50 =19.6± 0.1 min oil were found to be less toxic by aerosol method. These results suggest that clove oil and cinnamon oil have the potential to be used as a eco-friendly approach for the control of the major important filaria vector Cx. quinquefasciatus

  8. The Seasonal Variations of Aerosols over East Asia as Jointly Inferred from MODIS and OMI

    Institute of Scientific and Technical Information of China (English)

    LIU Qi; DING Wei-Dong; FU Yun-Fei

    2011-01-01

    Data on aerosol optical thickness (AOT) and single scattering albedo (SSA) derived from Moderate Resolution Imaging Spectrometer (MODIS) and Ozone Monitoring Instrument (OMI) measurements, respectively, are used jointly to examine the seasonal variations of aerosols over East Asia. The seasonal signals of the total AOT are well defined and nearly similar over the land and over the ocean. These findings indicate a natural cycle of aerosols that originate primarily from natural emissions. In contrast, the small-sized aerosols represented by the fine-mode AOT, which are primarily generated over the land by human activities, do not have evident seasonalscale fluctuations. A persistent maximum of aerosol load- ings centered over the Sichuan basin is associated with considerable amounts of fine-mode aerosols throughout the year. Most regions exhibit a general spring maximum. During the summer, however, the aerosol loadings are the most marked over north central China. This occurrence may result from anthropogenic fine particles, such as sulfate and nitrate. Four typical regions were selected to perform a covariation analysis of the monthly gridded AOT and SSA. Over southwestern and southeastern China, if the aerosol loadings are small to moderate they are composed primarily of the highly absorptive aerosols. However, more substantial aerosol loadings probably represent less-absorptive aerosols. The opposite covaria- tion pattern occurring over the coastal-adjacent oceans suggests that the polluted oceanic atmosphere is closely correlated with the windward terrestrial aerosols. North central China is strongly affected by dust aerosols that show moderate absorption. This finding may explain the lower variability in the SSA that accompanies increasing aerosol loadings in this region.

  9. Pre-activation of aerosol particles by ice preserved in pores

    Science.gov (United States)

    Marcolli, Claudia

    2017-02-01

    Pre-activation denotes the capability of particles or materials to nucleate ice at lower relative humidities or higher temperatures compared to their intrinsic ice nucleation efficiency after having experienced an ice nucleation event or low temperature before. This review presumes that ice preserved in pores is responsible for pre-activation and analyses pre-activation under this presumption. Idealized trajectories of air parcels are used to discuss the pore characteristics needed for ice to persist in pores and to induce macroscopic ice growth out of the pores. The pore width needed to keep pores filled with water decreases with decreasing relative humidity as described by the inverse Kelvin equation. Thus, narrow pores remain filled with ice well below ice saturation. However, the smaller the pore width, the larger the melting and freezing point depressions within the pores. Therefore, pre-activation due to pore ice is constrained by the melting of ice in narrow pores and the sublimation of ice from wide pores imposing restrictions on the temperature and relative humidity range of pre-activation for cylindrical pores. Ice is better protected in ink-bottle-shaped pores with a narrow opening leading to a large cavity. However, whether pre-activation is efficient also depends on the capability of ice to grow macroscopically, i.e. out of the pore. A strong effect of pre-activation is expected for swelling pores, because at low relative humidity (RH) their openings narrow and protect the ice within them against sublimation. At high relative humidities, they open up and the ice can grow to macroscopic size and form an ice crystal. Similarly, ice protected in pockets is perfectly sheltered against sublimation but needs the dissolution of the surrounding matrix to be effective. Pores partially filled with condensable material may also show pre-activation. In this case, complete filling occurs at lower RH than for empty pores and freezing shifts to lower temperatures.Pre-activation

  10. Hygroscopic properties of aerosol particles at high relative humidity and their diurnal variations in the North China Plain

    Directory of Open Access Journals (Sweden)

    P. F. Liu

    2011-01-01

    Full Text Available The hygroscopic properties of submicron aerosol particles were determined at a suburban site (Wuqing in the North China Plain among a cluster of cities during the period 17 July to 12 August 2009. A High Humidity Tandem Differential Mobility Analyser (HH-TDMA instrument was applied to measure the hygroscopic growth factor (GF at 90%, 95% and 98.5% relative humidity (RH for particles with dry diameter between 50–250 nm. The probability distribution of GF (GF-PDF averaged over the period shows a distinct bimodal pattern, namely, a dominant more-hygroscopic (MH group and a smaller nearly-hydrophobic (NH group. The MH group particles were highly hygroscopic, and their GF was relatively constant during the period with average values of 1.54±0.02, 1.81±0.04 and 2.45±0.07 at 90%, 95% and 98.5% RH (D0=100 nm, respectively. The NH group particles grew very slightly when exposed to high RH, with GF values of 1.08±0.02, 1.13±0.06 and 1.24±0.13, respectively at 90%, 95% and 98.5% RH (D0=100 nm. The hygroscopic growth behaviours at different RHs were well represented by the hygroscopicity parameter κ with a single-parameter Köhler model. Thus, the calculation of GF as a function of RH and dry diameter could be facilitated by an empirical parameterization of κ as function of dry diameter. A strong diurnal pattern in number fraction of different hygroscopic groups was observed, indicating a diurnal variation of aerosol mixing state and/or chemical composition. The average number fraction of NH particles during the day was about 8%, while during the nighttime fractions up to 20% were reached. Correspondingly, the state of mixing in terms of water uptake varied significantly during a day. The high fraction of NH particles measured during the night denotes a high degree of external mixing of ambient aerosols, while during the day the degree of external mixing decreased. Simulations using a particle-resolved aerosol

  11. Sensitivity of remote aerosol distributions to representation of cloud-aerosol interactions in a global climate model

    Directory of Open Access Journals (Sweden)

    H. Wang

    2013-01-01

    Full Text Available Many global aerosol and climate models, including the widely used Community Atmosphere Model version 5 (CAM5, have large biases in predicting aerosols in remote regions such as upper troposphere and high latitudes. In this study, we conduct CAM5 sensitivity simulations to understand the role of key processes associated with aerosol transformation and wet removal affecting the vertical and horizontal long-range transport of aerosols to the remote regions. Improvements are made to processes that are currently not well represented in CAM5, which are guided by surface and aircraft measurements together with results from a multi-scale aerosol-climate model (PNNL-MMF that explicitly represents convection and aerosol-cloud interactions at cloud-resolving scales. We pay particular attention to black carbon (BC due to its importance in the Earth system and the availability of measurements. We introduce into CAM5 a new unified scheme for convective transport and aerosol wet removal with explicit aerosol activation above convective cloud base. This new implementation reduces the excessive BC aloft to better simulate observed BC profiles that show decreasing mixing ratios in the mid- to upper-troposphere. After implementing this new unified convective scheme, we examine wet removal of submicron aerosols that occurs primarily through cloud processes. The wet removal depends strongly on the sub-grid scale liquid cloud fraction and the rate of conversion of liquid water to precipitation. These processes lead to very strong wet removal of BC and other aerosols over mid- to high latitudes during winter months. With our improvements, the Arctic BC burden has a10-fold (5-fold increase in the winter (summer months, resulting in a much better simulation of the BC seasonal cycle as well. Arctic sulphate and other aerosol species also increase but to a lesser extent. An explicit treatment of BC aging with slower aging assumptions produces an additional 30-fold (5-fold

  12. Aerosol plume transport and transformation in high spectral resolution lidar measurements and WRF-Flexpart simulations during the MILAGRO Field Campaign

    Directory of Open Access Journals (Sweden)

    B. de Foy

    2010-11-01

    Full Text Available The Mexico City Metropolitan Area (MCMA experiences high loadings of atmospheric aerosols from anthropogenic sources, biomass burning and wind-blown dust. This paper uses a combination of measurements and numerical simulations to identify different plumes affecting the basin and to characterize transformation inside the plumes. The airborne High Spectral Resolution Lidar measures extinction coefficients and extinction to backscatter ratio at 532 nm, and backscatter coefficients and depolarization ratios at 532 and 1064 nm. These can be used to identify aerosol types. The measurement curtains are compared with particle trajectory simulations using WRF-Flexpart for different source groups. The good correspondence between measurements and simulations suggests that the aerosol transport is sufficiently well characterized by the models to estimate aerosol types and ages. Plumes in the basin undergo complex transport, and are frequently mixed together. Urban aerosols are readily identifiable by their low depolarization ratios and high lidar ratios, and dust by the opposite properties. Fresh biomass burning plumes have very low depolarization ratios which increase rapidly with age. This rapid transformation is consistent with the presence of atmospheric tar balls in the fresh plumes.

  13. Aerosol plume transport and transformation in high spectral resolution lidar measurements and WRF-Flexpart simulations during the MILAGRO Field Campaign

    Science.gov (United States)

    de Foy, B.; Burton, S. P.; Ferrare, R. A.; Hostetler, C. A.; Hair, J. W.; Wiedinmyer, C.; Molina, L. T.

    2011-04-01

    The Mexico City Metropolitan Area (MCMA) experiences high loadings of atmospheric aerosols from anthropogenic sources, biomass burning and wind-blown dust. This paper uses a combination of measurements and numerical simulations to identify different plumes affecting the basin and to characterize transformation inside the plumes. The High Spectral Resolution Lidar on board the NASA LaRC B-200 King Air aircraft measured extinction coefficients and extinction to backscatter ratio at 532 nm, and backscatter coefficients and depolarization ratios at 532 and 1064 nm. These can be used to identify aerosol types. The measurement curtains are compared with particle trajectory simulations using WRF-Flexpart for different source groups. The good correspondence between measurements and simulations suggests that the aerosol transport is sufficiently well characterized by the models to estimate aerosol types and ages. Plumes in the basin undergo complex transport, and are frequently mixed together. Urban aerosols are readily identifiable by their low depolarization ratios and high lidar ratios, and dust by the opposite properties. Fresh biomass burning plumes have very low depolarization ratios which increase rapidly with age. This rapid transformation is consistent with the presence of atmospheric tar balls in the fresh plumes.

  14. Aerosol plume transport and transformation in high spectral resolution lidar measurements and WRF-Flexpart simulations during the MILAGRO Field Campaign

    Directory of Open Access Journals (Sweden)

    B. de Foy

    2011-04-01

    Full Text Available The Mexico City Metropolitan Area (MCMA experiences high loadings of atmospheric aerosols from anthropogenic sources, biomass burning and wind-blown dust. This paper uses a combination of measurements and numerical simulations to identify different plumes affecting the basin and to characterize transformation inside the plumes. The High Spectral Resolution Lidar on board the NASA LaRC B-200 King Air aircraft measured extinction coefficients and extinction to backscatter ratio at 532 nm, and backscatter coefficients and depolarization ratios at 532 and 1064 nm. These can be used to identify aerosol types. The measurement curtains are compared with particle trajectory simulations using WRF-Flexpart for different source groups. The good correspondence between measurements and simulations suggests that the aerosol transport is sufficiently well characterized by the models to estimate aerosol types and ages. Plumes in the basin undergo complex transport, and are frequently mixed together. Urban aerosols are readily identifiable by their low depolarization ratios and high lidar ratios, and dust by the opposite properties. Fresh biomass burning plumes have very low depolarization ratios which increase rapidly with age. This rapid transformation is consistent with the presence of atmospheric tar balls in the fresh plumes.

  15. Evaluating the skill of high-resolution WRF-Chem simulations in describing drivers of aerosol direct climate forcing on the regional scale

    Science.gov (United States)

    Crippa, P.; Sullivan, R. C.; Thota, A.; Pryor, S. C.

    2016-01-01

    Assessing the ability of global and regional models to describe aerosol optical properties is essential to reducing uncertainty in aerosol direct radiative forcing in the contemporary climate and to improving confidence in future projections. Here we evaluate the performance of high-resolution simulations conducted using the Weather Research and Forecasting model with coupled with Chemistry (WRF-Chem) in capturing spatiotemporal variability of aerosol optical depth (AOD) and the Ångström exponent (AE) by comparison with ground- and space-based remotely sensed observations. WRF-Chem is run over eastern North America at a resolution of 12 km for a representative year (2008). A systematic positive bias in simulated AOD relative to observations is found (annual mean fractional bias (MFB) is 0.15 and 0.50 relative to MODIS (MODerate resolution Imaging Spectroradiometer) and AERONET, respectively), whereas the spatial variability is well captured during most months. The spatial correlation of observed and simulated AOD shows a clear seasonal cycle with highest correlation during summer months (r = 0.5-0.7) when the aerosol loading is large and more observations are available. The model is biased towards the simulation of coarse-mode aerosols (annual MFB for AE = -0.10 relative to MODIS and -0.59 for AERONET), but the spatial correlation for AE with observations is 0.3-0.5 during most months, despite the fact that AE is retrieved with higher uncertainty from the remote-sensing observations. WRF-Chem also exhibits high skill in identifying areas of extreme and non-extreme aerosol loading, and its ability to correctly simulate the location and relative intensity of extreme aerosol events (i.e., AOD > 75th percentile) varies between 30 and 70 % during winter and summer months, respectively.

  16. Satellite-based 3D structure of cloud and aerosols over the Indian Monsoon region: implications for aerosol-cloud interaction

    Science.gov (United States)

    Dey, Sagnik; Sengupta, Kamalaika; Basil, George; Das, Sushant; Nidhi, Nidhi; Dash, S. K.; Sarkar, Arjya; Srivastava, Parul; Singh, Ajit; Agarwal, P.

    2012-11-01

    Accurate knowledge of vertical distributions of aerosol and cloud fields and their space-time variations are required to reduce the uncertainty in estimated climate forcing. Here, multi-sensor (both passive and active) data were used to construct the climatology of 3-D cloud and aerosol fields over the Indian monsoon region. Multilayer clouds are found to persist throughout the year, among which cumulus and stratocumulus dominate the low clouds and cirrus dominates the high clouds. A combination of passive stereo-technique (MISR) and radiometric technique (ISCPP) captures the multilayer cloud structure as revealed by active sensor CALIOP. Coexistence of low clouds throughout the year with high aerosol concentration beneath and above leads to a transition from increasing to decreasing cloud fraction with an increase in aerosol optical depth. Such transition is rapid in the monsoon season due to convergence of low clouds to form high clouds facilitated by high aerosol loading. Further, the regional climate model RegCM 4.1 has been used to examine aerosol-cloud interaction. The aerosol-induced changes of low cloud amount are under-estimated by the model. The observation-based seasonal climatology of aerosol and cloud fields presented here may help in improving the model simulations of cloud variability and associated rainfall.

  17. Climate Implications of the Heterogeneity of Anthropogenic Aerosol Forcing

    Science.gov (United States)

    Persad, Geeta Gayatri

    Short-lived anthropogenic aerosols are concentrated in regions of high human activity, where they interact with radiation and clouds, causing horizontally heterogeneous radiative forcing between polluted and unpolluted regions. Aerosols can absorb shortwave energy in the atmosphere, but deplete it at the surface, producing opposite radiative perturbations between the surface and atmosphere. This thesis investigates climate and policy implications of this horizontal and vertical heterogeneity of anthropogenic aerosol forcing, employing the Geophysical Fluid Dynamics Laboratory's AM2.1 and AM3 models, both at a global scale and using East Asia as a regional case study. The degree of difference between spatial patterns of climate change due to heterogeneous aerosol forcing versus homogeneous greenhouse gas forcing deeply impacts the detection, attribution, and prediction of regional climate change. This dissertation addresses a gap in current understanding of these two forcings' response pattern development, using AM2.1 historical forcing simulations. The results indicate that fast atmospheric and land-surface processes alone substantially homogenize the global pattern of surface energy flux response to heterogeneous aerosol forcing. Aerosols' vertical redistribution of energy significantly impacts regional climate, but is incompletely understood. It is newly identified here, via observations and historical and idealized forcing simulations, that increased aerosol-driven atmospheric absorption may explain half of East Asia's recent surface insolation decline. Further, aerosols' surface and atmospheric effects counteract each other regionally---atmospheric heating enhances summer monsoon circulation, while surface dimming suppresses it---but absorbing aerosols' combined effects reduce summer monsoon rainfall. This thesis constitutes the first vertical decomposition of aerosols' impacts in this high-emissions region and elucidates the monsoonal response to aerosols

  18. Source regions for atmospheric aerosol measured at Barrow, Alaska.

    Science.gov (United States)

    Polissar, A V; Hopke, P K; Harris, J M

    2001-11-01

    Aerosol data consisting of condensation nuclei (CN) counts, black carbon (BC) mass concentration, and aerosol light scattering coefficient at the wavelength of 450 nm (SC) measured at Barrow, AK, from 1986 to 1997 have been analyzed. BC and SC show an annual cycle with the Arctic haze maxima in the winter and spring and the minima in the summer. The CN time series shows two maxima in March and August. Potential source contribution function (PSCF) that combines the aerosol data with air parcel backward trajectories was applied to identify potential source areas and the preferred pathways that give rise to the observed high aerosol concentrations at Barrow. Ten-day isentropic back trajectories arriving twice daily at 500 and 1500 m above sea level were calculated for the period from 1986 to 1997. The PSCF analyses were performed based on the 80th percentile criterion values for the 2- and 24-h averages of the measured aerosol parameters. There was a good correspondence between PSCF maps for the 2- and 24-h averages, indicating that 1-day aerosol sampling in the Arctic adequately represents the aerosol source areas. In winter, the high PSCF values for BC and SC are related to industrial source areas in Eurasia. The trajectory domain in winter and spring is larger than in summer, reflecting weaker transport in summer. No high PSCF areas for BC and SC can be observed in summer. The result is related to the poor transport into the Arctic plus the strong removal of aerosol by precipitation in summer. In contrast to the BC and SC maps, the CN plot for summer shows high PSCF areas in the North Pacific Ocean. High CN values appearto be mostly connected with the long-range transport from Eurasia in winter and spring and with the reduced sulfur compound emission from biogenic activities in the ocean in the summer. PSCF analysis was found to be effective in identifying potential aerosol source areas.

  19. Aerosol optical properties relevant to regional remote sensing of CCN activity and links to their organic mass fraction: airborne observations over Central Mexico and the US West Coast during MILAGRO/INTEX-B

    Directory of Open Access Journals (Sweden)

    Y. Shinozuka

    2009-05-01

    Full Text Available Remote sensing of cloud condensation nuclei (CCN would help evaluate the indirect effects of tropospheric aerosols on clouds and climate. To assess its feasibility, we examined relationships of submicron aerosol composition to CCN activity and optical properties observed during the MILAGRO/INTEX-B aircraft campaigns. An indicator of CCN activity, κ, was calculated from hygroscopicity measured under saturation. κ for dry 100-nm particles decreased with the organic fraction of non-refractory mass of submicron particles (OMF as 10(−0.43−0.44*OMF over Central Mexico and 10(−0.29−0.70*OMF over the US West Coast. These fits represent the critical dry diameter, centered near 100 nm for 0.2% supersaturation but varied as κ(−1/3, within measurement uncertainty (~20%. The decreasing trends of CCN activity with the organic content, evident also in our direct CCN counts, were consistent with previous ground and laboratory observations of highly organic particles. The wider range of OMF, 0–0.8, for our research areas means that aerosol composition will be more critical for estimation of CCN concentration than at the fixed sites previously studied. Furthermore, the wavelength dependence of extinction was anti-correlated with OMF as −0.70*OMF+2.0 for Central Mexico's urban and industrial pollution air masses, for unclear reasons. The Angstrom exponent of absorption increased with OMF, more rapidly under higher single scattering albedo, as expected for the interplay between soot and colored weak absorbers (some organic species and dust. Because remote sensing products currently use the wavelength dependence of extinction albeit in the column integral form and may potentially include that of absorption, these regional spectral dependencies are expected to facilitate retrievals of aerosol bulk chemistry and CCN activity over Central Mexico.

  20. Aerosol optical properties relevant to regional remote sensing of CCN activity and links to their organic mass fraction: airborne observations over Central Mexico and the US West Coast during MILAGRO/INTEX-B

    Directory of Open Access Journals (Sweden)

    Y. Shinozuka

    2009-09-01

    Full Text Available Remote sensing of cloud condensation nuclei (CCN would help evaluate the indirect effects of tropospheric aerosols on clouds and climate. To assess its feasibility, we examined relationships of submicron aerosol composition to CCN activity and optical properties observed during the MILAGRO/INTEX-B aircraft campaigns. An indicator of CCN activity, κ, was calculated from hygroscopicity measured under saturation. κ for dry 100 nm particles decreased with increasing organic fraction of non-refractory mass of submicron particles (OMF as 0.34–0.20×OMF over Central Mexico and 0.47–0.43×OMF over the US West Coast. These fits represent the critical dry diameter, centered near 100 nm for 0.2% supersaturation but varied as κ(−1/3, within measurement uncertainty (~20%. The decreasing trends of CCN activity with the organic content, evident also in our direct CCN counts, were consistent with previous ground and laboratory observations of highly organic particles. The wider range of OMF, 0–0.8, for our research areas means that aerosol composition will be more critical for estimation of CCN concentration than at the fixed sites previously studied. Furthermore, the wavelength dependence of extinction was anti-correlated with OMF as −0.70×OMF+2.0 for Central Mexico's urban and industrial pollution air masses, for unclear reasons. The Angstrom exponent of absorption increased with OMF, more rapidly under higher single scattering albedo, as expected for the interplay between soot and colored weak absorbers (some organic species and dust. Because remote sensing products currently use the wavelength dependence of extinction albeit in the column integral form and may potentially include that of absorption, these regional spectral dependencies are expected to facilitate retrievals of aerosol bulk chemical composition and CCN activity over Central Mexico.

  1. Organic functional groups in aerosol particles from burning and non-burning forest emissions at a high-elevation mountain site

    Directory of Open Access Journals (Sweden)

    S. Takahama

    2011-07-01

    Full Text Available Ambient particles collected on teflon filters at the Peak of Whistler Mountain, British Columbia (2182 m a.s.l. during spring and summer 2009 were measured by Fourier transform infrared (FTIR spectroscopy for organic functional groups (OFG. The project mean and standard deviation of organic aerosol mass concentrations (OM for all samples was 3.2±3.3 (μg m−3. Measurements of aerosol mass fragments, size, and number concentrations were used to separate fossil-fuel combustion and burning and non-burning forest sources of the measured organic aerosol. The OM was composed of the same anthropogenic and non-burning forest components observed at Whistler mid-valley in the spring of 2008; during the 2009 campaign, biomass burning aerosol was additionally observed from fire episodes occurring between June and September. On average, organic hydroxyl, alkane, carboxylic acid, ketone, and primary amine groups represented 31 %±11 %, 34 %±9 %, 23 %±6 %, 6 %±7 %, and 6 %±3 % of OM, respectively. Ketones in aerosols were associated with burning and non-burning forest origins, and represented up to 27 % of the OM. The organic aerosol fraction resided almost entirely in the submicron fraction without significant diurnal variations. OM/OC mass ratios ranged mostly between 2.0 and 2.2 and O/C atomic ratios between 0.57 and 0.76, indicating that the organic aerosol reaching the site was highly aged and possibly formed through secondary formation processes.

  2. Modeling of metallic aerosol formation in a multicomponent system at high temperatures using a discrete-sectional model. Appendix 7

    Energy Technology Data Exchange (ETDEWEB)

    NONE

    1997-02-01

    A multicomponent discrete-sectional model was used to simulate the fate of lead in a high temperature system. The results show the ability of the developed model to simulate metallic aerosol systems at high temperatures. The PbO reaction and nucleation rate can be determined by comparing the simulations and the experimental data. Condensation on SiO{sub 2} particle surfaces is found important for removing the PbO vapor. The value of the accommodation factor that is applied to account for nonidealities in the condensation process are determined. The differences between the nanosized particles and the bulk particles are elucidated. The use of such a model helped to understand the effects of various mechanisms in determining the metal oxide vapor concentration profile and in establishing the ultimate particle size distribution.

  3. Do atmospheric aerosols form glasses?

    Science.gov (United States)

    Zobrist, B.; Marcolli, C.; Pedernera, D. A.; Koop, T.

    2008-09-01

    A new process is presented by which water soluble organics might influence ice nucleation, ice growth, chemical reactions and water uptake of aerosols in the upper troposphere: the formation of glassy aerosol particles. Glasses are disordered amorphous (non-crystalline) solids that form when a liquid is cooled without crystallization until the viscosity increases exponentially and molecular diffusion practically ceases. The glass transition temperatures, Tg, homogeneous ice nucleation temperatures, Thom, and ice melting temperatures, Tm, of various aqueous inorganic, organic and multi-component solutions are investigated with a differential scanning calorimeter. The investigated solutes are: various polyols, glucose, raffinose, levoglucosan, an aromatic compound, sulfuric acid, ammonium bisulfate and mixtures of dicarboxylic acids (M5), of dicarboxylic acids and ammonium sulfate (M5AS), of two polyols, of glucose and ammonium nitrate, and of raffinose and M5AS. The results indicate that aqueous solutions of the investigated inorganic solutes show Tg values that are too low to be of atmospheric importance. In contrast, aqueous organic and multi-component solutions readily form glasses at low but atmospherically relevant temperatures (≤230 K). To apply the laboratory data to the atmospheric situation, the measured phase transition temperatures were transformed from a concentration to a water activity scale by extrapolating water activities determined between 252 K and 313 K to lower temperatures. The obtained state diagrams reveal that the higher the molar mass of the aqueous organic or multi-component solutes, the higher Tg of their respective solutions at a given water activity. To a lesser extent, Tg also depends on the hydrophilicity of the organic solutes. Therefore, aerosol particles containing larger (≳150 g mol-1) and more hydrophobic organic molecules are more likely to form glasses at intermediate to high relative humidities in the upper troposphere

  4. Do atmospheric aerosols form glasses?

    Directory of Open Access Journals (Sweden)

    D. A. Pedernera

    2008-09-01

    Full Text Available A new process is presented by which water soluble organics might influence ice nucleation, ice growth, chemical reactions and water uptake of aerosols in the upper troposphere: the formation of glassy aerosol particles. Glasses are disordered amorphous (non-crystalline solids that form when a liquid is cooled without crystallization until the viscosity increases exponentially and molecular diffusion practically ceases. The glass transition temperatures, Tg, homogeneous ice nucleation temperatures, Thom, and ice melting temperatures, Tm, of various aqueous inorganic, organic and multi-component solutions are investigated with a differential scanning calorimeter. The investigated solutes are: various polyols, glucose, raffinose, levoglucosan, an aromatic compound, sulfuric acid, ammonium bisulfate and mixtures of dicarboxylic acids (M5, of dicarboxylic acids and ammonium sulfate (M5AS, of two polyols, of glucose and ammonium nitrate, and of raffinose and M5AS. The results indicate that aqueous solutions of the investigated inorganic solutes show Tg values that are too low to be of atmospheric importance. In contrast, aqueous organic and multi-component solutions readily form glasses at low but atmospherically relevant temperatures (≤230 K. To apply the laboratory data to the atmospheric situation, the measured phase transition temperatures were transformed from a concentration to a water activity scale by extrapolating water activities determined between 252 K and 313 K to lower temperatures. The obtained state diagrams reveal that the higher the molar mass of the aqueous organic or multi-component solutes, the higher Tg of their respective solutions at a given water activity. To a lesser extent, Tg also depends on the hydrophilicity of the organic solutes. Therefore, aerosol particles containing larger (≳150 g mol−1 and

  5. Do atmospheric aerosols form glasses?

    Directory of Open Access Journals (Sweden)

    B. Zobrist

    2008-05-01

    Full Text Available A new process is presented by which water-soluble organics might influence ice nucleation, ice growth, chemical reactions and water uptake of aerosols in the upper troposphere: the formation of glassy aerosol particles. Glasses are disordered amorphous (non-crystalline solids that form when a liquid is cooled without crystallization until the viscosity increases exponentially and molecular diffusion practically ceases. The glass transition temperatures, Tg, homogeneous ice nucleation temperatures, Thom, and ice melting temperatures, Tm, of various aqueous inorganic, organic and multi-component solutions are investigated with a differential scanning calorimeter. The investigated solutes are: various polyols, glucose, raffinose, levoglucosan, an aromatic compound, sulfuric acid, ammonium bisulphate and mixtures of dicarboxylic acids (M5, of dicarboxylic acids and ammonium sulphate (M5AS, of two polyols, of glucose and ammonium nitrate, and of raffinose and M5AS. The results indicate that aqueous solutions of the investigated inorganic solutes show Tg-values that are too low to be of atmospheric importance. In contrast, aqueous organic and multi-component solutions readily form glasses at low but atmospherically relevant temperatures (≤230 K. To apply the laboratory data to the atmospheric situation, the measured phase transition temperatures were transformed from a concentration to a water activity scale by extrapolating water activities determined between 252 K and 313 K to lower temperatures. The obtained state diagrams reveal that the higher the molar mass of the aqueous organic or multi-component solutes, the higher Tg of their respective solutions at a given water activity. To a lesser extent, Tg also depends on the hydrophilicity of the organic solutes. Therefore, aerosol particles containing larger and more hydrophobic organic

  6. High-Activity Dealloyed Catalysts

    Energy Technology Data Exchange (ETDEWEB)

    Kongkanand, Anusorn [General Motors LLC, Pontiac, MI (United States)

    2014-09-30

    Reduction of costly Pt usage in proton exchange membrane fuel cell electrodes is one of the major challenges towards development and commercialization of fuel cell vehicles. Although few have met the initial-kinetic activity requirements in a realistic fuel cell device, no catalyst material has ever met the demanding fuel cell durability targets set by DOE. In this project, a team of 4 universities and 2 companies came together to investigate a concept that appeared promising in preliminary non-fuel cell tests then to further develop the catalyst to a mature level ready for vehicle implementation. The team consists of academia with technical leadership in their respective areas, a catalyst supplier, and a fuel cell system integrator.The tightly collaborative project enabled development of a highly active and durable catalyst with performance that significantly exceeds that of previous catalysts and meets the DOE targets for the first time (Figure 1A). The catalyst was then further evaluated in full-active-area stack in a realistic vehicle operating condition (Figure 1B). This is the first public demonstration that one can realize the performance benefit and Pt cost reduction over a conventional pure Pt catalyst in a long-term realistic PEMFC system. Furthermore, systematic analyses of a range of catalysts with different performance after fuel cell testing allowed for correlation between catalyst microstructure and its electrocatalytic activity and durability. This will in turn aid future catalyst development.

  7. Molecular composition and volatility of isoprene photochemical oxidation secondary organic aerosol under low- and high-NOx conditions

    Science.gov (United States)

    D'Ambro, Emma L.; Lee, Ben H.; Liu, Jiumeng; Shilling, John E.; Gaston, Cassandra J.; Lopez-Hilfiker, Felipe D.; Schobesberger, Siegfried; Zaveri, Rahul A.; Mohr, Claudia; Lutz, Anna; Zhang, Zhenfa; Gold, Avram; Surratt, Jason D.; Rivera-Rios, Jean C.; Keutsch, Frank N.; Thornton, Joel A.

    2017-01-01

    We present measurements of secondary organic aerosol (SOA) formation from isoprene photochemical oxidation in an environmental simulation chamber at a variety of oxidant conditions and using dry neutral seed particles to suppress acid-catalyzed multiphase chemistry. A high-resolution time-of-flight chemical ionization mass spectrometer (HR-ToF-CIMS) utilizing iodide-adduct ionization coupled to the Filter Inlet for Gases and Aerosols (FIGAERO) allowed for simultaneous online sampling of the gas and particle composition. Under high-HO2 and low-NO conditions, highly oxygenated (O : C ≥ 1) C5 compounds were major components (˜ 50 %) of SOA. The SOA composition and effective volatility evolved both as a function of time and as a function of input NO concentrations. Organic nitrates increased in both the gas and particle phases as input NO increased, but the dominant non-nitrate particle-phase components monotonically decreased. We use comparisons of measured and predicted gas-particle partitioning of individual components to assess the validity of literature-based group-contribution methods for estimating saturation vapor concentrations. While there is evidence for equilibrium partitioning being achieved on the chamber residence timescale (5.2 h) for some individual components, significant errors in group-contribution methods are revealed. In addition, > 30 % of the SOA mass, detected as low-molecular-weight semivolatile compounds, cannot be reconciled with equilibrium partitioning. These compounds desorb from the FIGAERO at unexpectedly high temperatures given their molecular composition, which is indicative of thermal decomposition of effectively lower-volatility components such as larger molecular weight oligomers.

  8. Characterisation of episodic aerosol types over the Australian continent

    Directory of Open Access Journals (Sweden)

    Y. Qin

    2009-03-01

    Full Text Available Classification of Australian continental aerosol types resulting from episodes of enhanced source activity, such as smoke plumes and dust outbreaks, is carried out via cluster analysis of optical properties obtained from inversion of sky radiance distributions at Australian aerosol ground stations using data obtained over the last decade. The cluster analysis distinguishes four significant classes, which are identified on the basis of their optical properties and provenance as determined by satellite imagery and back-trajectory analysis. The four classes are identified respectively as aged smoke, fresh smoke, coarse dust and a super-absorptive aerosol. While the first three classes show similarities with comparable aerosol types identified elsewhere, the super-absorptive aerosol has no obvious foreign prototype. The class identified as coarse dust shows a prominent depression in single scattering albedo in the blue spectral region due to absorption by hematite, which is shown to be more abundant in central Australian dust relative to the "dust belt"of the Northern Hemisphere. The super-absorptive class is distinctive in view of its very low single scattering albedo (~0.7 at 500 nm and variable enhanced absorption at 440 nm. The strong absorption by this aerosol requires a high black carbon content while the enhanced blue-band absorption may derive from organic compounds emitted during the burning of specific vegetation types. This aerosol exerts a positive radiative forcing at the top of atmosphere (TOA, with a large deposition of energy in the atmosphere per unit aerosol optical depth. This contrasts to the other three classes where the TOA forcing is negative. Optical properties of the four types will be used to improve the representation of Australian continental aerosol in climate models, and to enhance the accuracy of satellite-based aerosol retrievals over Australia.

  9. Characterisation of episodic aerosol types over the Australian continent

    Directory of Open Access Journals (Sweden)

    Y. Qin

    2008-11-01

    Full Text Available Classification of Australian continental aerosol types resulting from episodes of enhanced source activity, such as smoke plumes and dust outbreaks, is carried out via cluster analysis of microphysical properties obtained from inversion of sky radiance distributions at Australian aerosol ground stations using data obtained over the last decade. The cluster analysis distinguishes four significant classes, which are identified on the basis of their optical properties and provenance as determined by satellite imagery and back-trajectory analysis. The four classes are identified respectively as aged smoke, fresh smoke, coarse dust and a super-absorptive aerosol. While the first three classes show similarities with comparable aerosol types identified elsewhere, the super-absorptive aerosol has no obvious foreign prototype. The class identified as coarse dust shows a prominent depression in single scattering albedo in the blue spectral region due to absorption by hematite, which is shown to be more abundant in central Australian dust relative to the "dust belt" of the Northern Hemisphere. The super-absorptive class is distinctive in view of its very low single scattering albedo (~0.7 at 500 nm and variable enhanced absorption at 440 nm. The strong absorption by this aerosol requires a high black carbon content while the enhanced blue-band absorption may derive from organic compounds emitted during the burning of specific vegetation types. This aerosol exerts a positive radiative forcing at the top of atmosphere (TOA, with a large deposition of energy in the atmosphere per unit aerosol optical depth. This contrasts to the other three classes where the TOA forcing is negative. Optical properties of the four types will be used to improve the representation of Australian continental aerosol in climate models, and to enhance the accuracy of satellite-based aerosol retrievals over Australia.

  10. Seasonal and spatial variability of the organic matter-to-organic carbon mass ratios in Chinese urban organic aerosols and a first report of high correlations between aerosol oxalic acid and zinc

    Science.gov (United States)

    Xing, L.; Fu, T.-M.; Cao, J. J.; Lee, S. C.; Wang, G. H.; Ho, K. F.; Cheng, M.-C.; You, C.-F.; Wang, T. J.

    2013-01-01

    We calculated the organic matter to organic carbon mass ratios (OM/OC mass ratios) in PM2.5 collected from 14 Chinese cities during summer and winter of 2003 and analyzed the causes for their seasonal and spatial variability. The OM/OC mass ratios were calculated two ways. Using a mass balance method, the calculated OM/OC mass ratios averaged 1.92 ± 0.39 yr-round, with no significant seasonal or spatial variation. The second calculation was based on chemical species analyses of the organic compounds extracted from the PM2.5 samples using dichloromethane/methanol and water. The calculated OM/OC mass ratio in summer was relatively high (1.75 ± 0.13) and spatially-invariant, due to vigorous photochemistry and secondary OA production throughout the country. The calculated OM/OC mass ratio in winter (1.59 ± 0.18) was significantly lower than that in summer, with lower values in northern cities (1.51 ± 0.07) than in southern cities (1.65 ± 0.15). This likely reflects the wider usage of coal for heating purposes in northern China in winter, in contrast to the larger contributions from biofuel and biomass burning in southern China in winter. On average, organic matters constituted 36% and 34% of Chinese urban PM2.5 mass in summer and winter, respectively. We reported, for the first time, high correlations between Zn and oxalic acid in Chinese urban aerosols in summer. This is consistent with the formation of stable Zn oxalate complex in the aerosol phase previously proposed by Furukawa and Takahashi (2011). We found that many other dicarboxylic acids were also highly correlated with Zn in the summer Chinese urban aerosol samples, suggesting that they may also form stable organic complexes with Zn. Such formation may have profound implications for the atmospheric abundance and hygroscopic property of aerosol dicarboxylic acids.

  11. Recent Improvements to CALIOP Level 3 Aerosol Profile Product for Global 3-D Aerosol Extinction Characterization

    Science.gov (United States)

    Tackett, J. L.; Getzewich, B. J.; Winker, D. M.; Vaughan, M. A.

    2015-12-01

    With nine years of retrievals, the CALIOP level 3 aerosol profile product provides an unprecedented synopsis of aerosol extinction in three dimensions and the potential to quantify changes in aerosol distributions over time. The CALIOP level 3 aerosol profile product, initially released as a beta product in 2011, reports monthly averages of quality-screened aerosol extinction profiles on a uniform latitude/longitude grid for different cloud-cover scenarios, called "sky conditions". This presentation demonstrates improvements to the second version of the product which will be released in September 2015. The largest improvements are the new sky condition definitions which parse the atmosphere into "cloud-free" views accessible to passive remote sensors, "all-sky" views accessible to active remote sensors and "cloudy-sky" views for opaque and transparent clouds which were previously inaccessible to passive remote sensors. Taken together, the new sky conditions comprehensively summarize CALIOP aerosol extinction profiles for a broad range of scientific queries. In addition to dust-only extinction profiles, the new version will include polluted-dust and smoke-only extinction averages. A new method is adopted for averaging dust-only extinction profiles to reduce high biases which exist in the beta version of the level 3 aerosol profile product. This presentation justifies the new averaging methodology and demonstrates vertical profiles of dust and smoke extinction over Africa during the biomass burning season. Another crucial advancement demonstrated in this presentation is a new approach for computing monthly mean aerosol optical depth which removes low biases reported in the beta version - a scenario unique to lidar datasets.

  12. Climate implications of carbonaceous aerosols: An aerosol microphysical study using the GISS/MATRIX climate model

    Energy Technology Data Exchange (ETDEWEB)

    Bauer, Susanne E.; Menon, Surabi; Koch, Dorothy; Bond, Tami; Tsigaridis, Kostas

    2010-04-09

    Recently, attention has been drawn towards black carbon aerosols as a likely short-term climate warming mitigation candidate. However the global and regional impacts of the direct, cloud-indirect and semi-direct forcing effects are highly uncertain, due to the complex nature of aerosol evolution and its climate interactions. Black carbon is directly released as particle into the atmosphere, but then interacts with other gases and particles through condensation and coagulation processes leading to further aerosol growth, aging and internal mixing. A detailed aerosol microphysical scheme, MATRIX, embedded within the global GISS modelE includes the above processes that determine the lifecycle and climate impact of aerosols. This study presents a quantitative assessment of the impact of microphysical processes involving black carbon, such as emission size distributions and optical properties on aerosol cloud activation and radiative forcing. Our best estimate for net direct and indirect aerosol radiative forcing change is -0.56 W/m{sup 2} between 1750 and 2000. However, the direct and indirect aerosol effects are very sensitive to the black and organic carbon size distribution and consequential mixing state. The net radiative forcing change can vary between -0.32 to -0.75 W/m{sup 2} depending on these carbonaceous particle properties. Assuming that sulfates, nitrates and secondary organics form a coating shell around a black carbon core, rather than forming a uniformly mixed particles, changes the overall net radiative forcing from a negative to a positive number. Black carbon mitigation scenarios showed generally a benefit when mainly black carbon sources such as diesel emissions are reduced, reducing organic and black carbon sources such as bio-fuels, does not lead to reduced warming.

  13. Fluorescent biological aerosol particle measurements at a tropical high-altitude site in southern India during the southwest monsoon season

    Science.gov (United States)

    Valsan, A. E.; Ravikrishna, R.; Biju, C. V.; Pöhlker, C.; Després, V. R.; Huffman, J. A.; Pöschl, U.; Gunthe, S. S.

    2016-08-01

    An ultraviolet aerodynamic particle sizer (UV-APS) was continuously operated for the first time during two seasons to sample the contrasting winds during monsoon and winter to characterize the properties of fluorescent biological aerosol particles (FBAPs), at a high-altitude site in India. Averaged over the entire monsoon campaign (1 June-21 August 2014), the arithmetic mean number and mass concentrations of coarse-mode (> 1 µm) FBAPs were 0.02 cm-3 and 0.24 µg m-3, respectively, which corresponded to ˜ 2 and 6 % of total aerosol loading, respectively. Average FBAP number size distribution exhibited a peak at ˜ 3 µm, which is attributed to the fungal spores, as supported by scanning electron microscope (SEM) images, and these results are consistent with previous studies made for FBAPs. During 11 weeks of measurements the variability of the total coarse-mode particle number (TAP) concentration was high compared to that observed in FBAP number concentrations. The TAP and FBAP number concentrations measured at this site were strongly dependent on changes in wind direction and rainfall. During periods of westerly/southwesterly winds with heavy persistent rainfall, the TAP and FBAP concentrations exhibited very low values (1.3 and 0.005 cm-3, respectively) with no significant diurnal variations, whereas during periods of northerly winds with scattered rainfall FBAPs exhibited relatively high concentration values (0.05 cm-3) with pronounced diurnal variations, which were strongly coupled with diurnal variations in meteorological parameters. The campaign-averaged FBAP number concentrations were shown to correlate with daily patterns of meteorological parameters and were positively correlated with relative humidity (RH; R2 = 0.58) and negatively with temperature (R2 = 0.60) and wind speed (R2 = 0.60). We did not observe any significant positive correlation with precipitation as reported by previous researchers from selected areas. These measurement results confirm the

  14. Buildup of aerosol precursor gases and sulfur-induced activation of soot in nascent jet aircraft exhaust plumes

    Energy Technology Data Exchange (ETDEWEB)

    Kaercher, B.; Hirschberg, M.M.; Fabian, P. [Muenchen Univ. (Germany). Lehrstuhl fuer Bioklimatologie und Immissionsforschung; Gerz, T. [Deutsche Forschungsanstalt fuer Luft- und Raumfahrt e.V. (DLR), Oberpfaffenhofen (Germany). Inst. fuer Physik der Atmosphaere

    1997-12-31

    Research issues concerning the chemical transformation of exhaust trace gases are summarized. The photochemical evolution of NO{sub x} early in the plume is strongly coupled to plume mixing. Substantial amounts of HNO{sub 3} are generated in nascent plumes even if no NO{sub 2} is emitted. The production of H{sub 2}SO{sub 4} becomes very efficient if part of the fuel sulfur is emitted as SO{sub 3}. Each emitted soot particle can acquire 1-10% by mass fully oxidized sulfur molecules prior to binary homogeneous nucleation, if a few percent of the exhaust SO{sub x} are emitted as SO{sub 3}, indicating an important activation pathway for soot, and leading to a marked enhancement of new aerosol formation and growth rates. (author) 11 refs.

  15. Activity measurement of gamma-ray emitters in aerosol filters exposed in Lithuania, in March-April 2011.

    Science.gov (United States)

    Gudelis, A; Gorina, I; Nedveckaitė, T; Kovař, P; Dryak, P; Suran, J

    2013-11-01

    Two aerosol sampling stations in Lithuania were simultaneously used for assessing consequences of the accident at the Fukushima Dai-ichi nuclear power plant. The maximum activity concentrations of (129 m)Te, (131)I, (134)Cs and (137)Cs were 0.59 ± 0.06, 3.5 ± 0.3, 0.90 ± 0.08, 0.90 ± 0.07 mBq m(-3) at station #1 in Vilnius, and 0.29 ± 0.03, 1.0 ± 0.1, 0.41 ± 0.04, 0.41 ± 0.0 4 mBq m(-3) at station #2 in northeastern part of Lithuania, respectively.

  16. Fontan patient with plastic bronchitis treated successfully using aerosolized tissue plasminogen activator: a case report and review of the literature.

    Science.gov (United States)

    Do, Thomas B; Chu, James M; Berdjis, Farhouch; Anas, Nick G

    2009-04-01

    Plastic bronchitis is an uncommon condition characterized by the production of large pale bronchial casts that obstruct the tracheobronchial tree. The cellular content, cohesiveness, and often rubber-like consistency distinguish bronchial casts from the usual mucus plugs found with such disease states as asthma. Plastic bronchitis can be found secondary to many conditions, and a simplified classification scheme organizes it into two groups: an inflammatory type consisting of casts with an eosinophilic inflammatory infiltrate and an acellular type with a predominance of fibrin distinguished by its relative lack of cellular infiltrate, its mucin predominance, and its appearance only in children with congenital cyanotic heart disease. This report describes a 5-year-old girl who experienced plastic bronchitis 3 months after a Fontan procedure for hypoplastic left heart syndrome that was treated successfully with aerosolized tissue plasminogen activator.

  17. Systematic aerosol characterization by combining GOME-2 UV Aerosol Indices with trace gas concentrations

    Science.gov (United States)

    Penning de Vries, M.; Stammes, P.; Wagner, T.

    2012-04-01

    The task of determining aerosol type using passive remote sensing instruments is a daunting one. First, because the variety in aerosol (optical) properties is very large; and second, because the effect of aerosols on the detected top-of-atmosphere reflectance spectrum is smooth and mostly featureless. In addition, spectrometers like GOME-2 have a coarse spatial resolution, which makes aerosol characterization even more difficult due to interferences with clouds. On account of these problems, we do not attempt to derive aerosol properties from single measurements: instead, we combine time series of UV Aerosol Index and trace gas concentrations to derive the dominating aerosol type for each season. Aside from the Index values and trace gas concentrations themselves, the correlation between UV Aerosol Indices (which are indicative of aerosol absorption) with NO2, HCHO, and CHOCHO columns - or absence of it - provides clues to the (main) source of the aerosols in the investigated region and time range. For example: a high correlation of HCHO and Absorbing Aerosol Index points to aerosols from biomass burning, highly correlated CHOCHO, HCHO, and SCattering Index indicate biogenic secondary organic aerosols, and coinciding high NO2 concentrations with high SCattering Index values are associated with industrial and urban aerosols. We here present case studies for several regions to demonstrate the suitability of our approach. Then, we introduce a method to systematically derive the dominating aerosol type on a global scale on time scales varying from monthly to yearly.

  18. Type-segregated aerosol effects on regional monsoon activity: A study using ground-based experiments and model simulations

    Science.gov (United States)

    Vijayakumar, K.; Devara, P. C. S.; Sonbawne, S. M.

    2014-12-01

    Classification of observed aerosols into key types [e.g., clean-maritime (CM), desert-dust (DD), urban-industrial/biomass-burning (UI/BB), black carbon (BC), organic carbon (OC) and mixed-type aerosols (MA)] would facilitate to infer aerosol sources, effects, and feedback mechanisms, not only to improve the accuracy of satellite retrievals but also to quantify the assessment of aerosol radiative impacts on climate. In this paper, we report the results of a study conducted in this direction, employing a Cimel Sun-sky radiometer at the Indian Institute of Tropical Meteorology (IITM), Pune, India during 2008 and 2009, which represent two successive contrasting monsoon years. The study provided an observational evidence to show that the local sources are subject to heavy loading of absorbing aerosols (dust and black carbon), with strong seasonality closely linked to the monsoon annual rainfall cycle over Pune, a tropical urban station in India. The results revealed the absence of CM aerosols in the pre-monsoon as well as in the monsoon seasons of 2009 as opposed to 2008. Higher loading of dust aerosols is observed in the pre-monsoon and monsoon seasons of 2009; majority may be coated with fine BC aerosols from local emissions, leading to reduction in regional rainfall. Further, significant decrease in coarse-mode AOD and presence of carbonaceous aerosols, affecting the aerosol-cloud interaction and monsoon-rain processes via microphysics and dynamics, is considered responsible for the reduction in rainfall during 2009. Additionally, we discuss how optical depth, contributed by different types of aerosols, influences the distribution of monsoon rainfall over an urban region using the Monitoring Atmospheric Composition and Climate (MACC) aerosol reanalysis. Furthermore, predictions of the Dust REgional Atmospheric Model (DREAM) simulations combined with HYSPLIT (HYbrid Single Particle Lagrangian Integrated Trajectory) cluster model are also discussed in support of the

  19. Coagulation effect on the activity size distributions of long lived radon progeny aerosols and its application to atmospheric residence time estimation techniques.

    Science.gov (United States)

    Anand, S; Mayya, Y S

    2015-03-01

    The long lived naturally occurring radon progeny species in the atmosphere, namely (210)Pb, (210)Bi and (210)Po, have been used as important tracers for understanding the atmospheric mixing processes and estimating aerosol residence times. Several observations in the past have shown that the activity size distribution of these species peaks at larger particle sizes as compared to the short lived radon progeny species - an effect that has been attributed to the process of coagulation of the background aerosols to which they are attached. To address this issue, a mathematical equation is derived for the activity-size distribution of tracer species by formulating a generalized distribution function for the number of tracer atoms present in coagulating background particles in the presence of radioactive decay and removal. A set of these equations is numerically solved for the progeny chain using Fuchs coagulation kernel combined with a realistic steady-state aerosol size spectrum that includes nucleation, accumulation and coarse mode components. The important findings are: (i) larger shifts in the modal sizes of (210)Pb and (210)Po at higher aerosol concentrations such as that found in certain Asian urban regions (ii) enrichment of tracer specific activity on particles as compared to that predicted by pure attachment laws (iii) sharp decline of daughter-to-parent activity ratios for decreasing particle sizes. The implication of the results to size-fractionated residence time estimation techniques is highlighted. A coagulation corrected graphical approach is presented for estimating the residence times from the size-segregated activity ratios of (210)Bi and (210)Po with respect to (210)Pb. The discrepancy between the residence times predicted by conventional formula and the coagulation corrected approach for specified activity ratios increases at higher atmospheric aerosol number concentrations (>10(10) #/m(3)) for smaller sizes (<1 μm). The results are further

  20. Supersaturation of Calcipotriene and Betamethasone Dipropionate in a Novel Aerosol Foam Formulation for Topical Treatment of Psoriasis Provides Enhanced Bioavailability of the Active Ingredients.

    Science.gov (United States)

    Lind, Marianne; Nielsen, Kim Troensegaard; Schefe, Line Hollesen; Nørremark, Kasper; Eriksson, André Huss; Norsgaard, Hanne; Pedersen, Brian Thoning; Petersson, Karsten

    2016-09-01

    Previous studies have demonstrated the superior efficacy of a novel aerosol foam formulation of fixed combination calcipotriene 0.005% (Cal) and betamethasone dipropionate 0.064% (BD), compared with the ointment formulation. The aim of this study is to ascertain whether enhanced bioavailability of the active ingredients due to supersaturation and/or occlusive properties can explain the observed greater clinical efficacy. Solubility and evaporation experiments were conducted to examine the abilities of Cal/BD aerosol foam ingredients to create a supersaturated environment. Optical microscopy, Raman imaging and X-ray powder diffraction were used to examine the physical state of Cal and BD in the formulations after application, and determine whether a supersaturated state remained stable for clinically relevant time periods. In vitro skin penetration and ex vivo biomarker assays were conducted to compare the skin penetration and bioavailability of Cal and BD from the aerosol foam and ointment formulations, respectively. Occlusive properties were examined via transepidermal water loss. Solubility studies showed that Cal and BD solubility increased with increasing dimethyl ether (DME) content. Both active ingredients are completely dissolved in the final aerosol foam formulation. DME rapidly evaporates after spraying, and the amount was reduced to 0.5% of the initial amount after 2 min. This led to the formation of a supersaturated environment, where Cal and BD crystals were absent for at least 26 h after application. Cal/BD aerosol foam had significantly greater in vitro skin penetration and had increased bioavailability compared with Cal/BD ointment. Both formulations effectively occluded the skin. A stable supersaturated solution of Cal/BD in the aerosol foam leads to increased bioavailability and explains the improved clinical effect when compared to the Cal/BD ointment. The studies included in the paper are all conducted by LEO Pharma A/S or CROs on behalf of LEO

  1. Applications of High-Resolution Electrospray Ionization Mass Spectrometry to Measurements of Average Oxygen to Carbon Ratios in Secondary Organic Aerosols

    Energy Technology Data Exchange (ETDEWEB)

    Bateman, Adam P.; Laskin, Julia; Laskin, Alexander; Nizkorodov, Sergey

    2012-07-02

    The applicability of high resolution electrospray ionization mass spectrometry (HR ESI-MS) to measurements of the average oxygen to carbon ratio (O/C) in organic aerosols was investigated. Solutions with known average O/C containing up to 10 standard compounds representative of secondary organic aerosol (SOA) were analyzed and corresponding electrospray ionization efficiencies were quantified. The assumption of equal ionization efficiency commonly used in estimating O/C ratios of organic aerosols was found to be reasonably accurate. We found that the accuracy of the measured O/C ratios increases by averaging the values obtained from both (+) and (-) modes. A correlation was found between the ratio of the ionization efficiencies in the positive and negative ESI modes with the octanol-water partition constant, and more importantly, with the compound's O/C. To demonstrate the utility of this correlation for estimating average O/C values of unknown mixtures, we analyzed the ESI (+) and ESI (-) data for SOA produced by oxidation of limonene and isoprene and compared to online O/C measurements using an aerosol mass spectrometer (AMS). This work demonstrates that the accuracy of the HR ESI-MS methods is comparable to that of the AMS, with the added benefit of molecular identification of the aerosol constituents.

  2. Ferrets develop fatal influenza after inhaling small particle aerosols of highly pathogenic avian influenza virus A/Vietnam/1203/2004 (H5N1

    Directory of Open Access Journals (Sweden)

    Sosna William A

    2010-09-01

    Full Text Available Abstract Background There is limited knowledge about the potential routes for H5N1 influenza virus transmission to and between humans, and it is not clear whether humans can be infected through inhalation of aerosolized H5N1 virus particles. Ferrets are often used as a animal model for humans in influenza pathogenicity and transmissibility studies. In this manuscript, a nose-only bioaerosol inhalation exposure system that was recently developed and validated was used in an inhalation exposure study of aerosolized A/Vietnam/1203/2004 (H5N1 virus in ferrets. The clinical spectrum of influenza resulting from exposure to A/Vietnam/1203/2004 (H5N1 through intranasal verses inhalation routes was analyzed. Results Ferrets were successfully infected through intranasal instillation or through inhalation of small particle aerosols with four different doses of Influenza virus A/Vietnam/1203/2004 (H5N1. The animals developed severe influenza encephalomyelitis following intranasal or inhalation exposure to 101, 102, 103, or 104 infectious virus particles per ferret. Conclusions Aerosolized Influenza virus A/Vietnam/1203/2004 (H5N1 is highly infectious and lethal in ferrets. Clinical signs appeared earlier in animals infected through inhalation of aerosolized virus compared to those infected through intranasal instillation.

  3. Single particle characterization of biomass burning organic aerosol (BBOA: evidence for non-uniform mixing of high molecular weight organics and potassium

    Directory of Open Access Journals (Sweden)

    A. K. Y. Lee

    2015-11-01

    Full Text Available Biomass burning is a major source of black carbon (BC and primary organic aerosol globally. In particular, biomass burning organic aerosol (BBOA is strongly associated with atmospheric brown carbon (BrC that absorbs near ultraviolet and visible light, resulting in significant impacts on regional visibility degradation and radiative forcing. The mixing state of BBOA can play a critical role in the prediction of aerosol optical properties. In this work, single particle measurements from a soot-particle aerosol mass spectrometer coupled with a light scattering module (LS-SP-AMS were performed to examine the mixing state of BBOA, refractory black carbon (rBC and potassium (K+, a tracer for biomass burning aerosol in an air mass influenced by aged biomass burning. Cluster analysis of single particle measurements identified five BBOA-related particle types. rBC accounted for 3–14 w.t. % of these particle types on average. Only one particle type exhibited a strong ion signal for K+, with mass spectra characterized by low molecular weight organic species. The remaining four particle types were classified based on the apparent molecular weight of the BBOA constituents. Two particle types were associated with low potassium content and significant amounts of high molecular weight (HMW organic compounds. Our observations indicate non-uniform mixing of particles within a biomass burning plume in terms of molecular weight and illustrate that HMW BBOA can be a key contributor to low-volatility BrC observed in BBOA particles.

  4. Atmospheric aerosols parameters behavior and its association with meteorological activities variables over western Indian tropical semi-urban site i.e., Udaipur

    Science.gov (United States)

    Vyas, B. M.; Saxenna, Abhishek; Panwar, Chhagan

    2016-05-01

    The present study has been focused to the identify the role of meteorological processes on changing the monthly variation of AOD at 550nm, Angstrom Exponent Coefficient (AEC, 440/670nm) and Cloud Effective Radius (CER, μm) measured during January, 2005 to December 2013 over western Indian location i.e., Udaipur (24.6° N, 73.7° E, 560 m amsl). The monthly variation of AOD 550nm, AEC and during entire study period have shown the strong combined influence of different local surface meteorological parameters in varying amplitude with different nature. The higher values of wind speed, ambient surface temperature, planetary boundary layer, and favorable wind direction coming from desert and oceanic region (W and SW) may be recognize as some of possible factor to exhibit the higher aerosols loading of bigger aerosol size particles in pre-monsoon. These meteorological factors seem also to be plausible responsible factors for drastically reducing the cloud effective radius in pre-monsoon season. In contrary to this, in winter, lower atmospheric aerosols burden and more abundance of fine size particles along with increasing the CER sizes also seem to be influenced and governed by the adverse nature of meteorological conditions such lowering the PBL, T, WS as well as with air pollutants transportation by wind from the N and NE region, of high aerosols loading of fine size particles as anthropogenic aerosols located far away to the observing site.

  5. CALIPSO Observations of Aerosol Properties Near Clouds

    Science.gov (United States)

    Marshak, Alexander; Varnai, Tamas; Yang, Weidong

    2010-01-01

    Clouds are surrounded by a transition zone of rapidly changing aerosol properties. Characterizing this zone is important for better understanding aerosol-cloud interactions and aerosol radiative effects as well as for improving satellite measurements of aerosol properties. We present a statistical analysis of a global dataset of CALIPSO (Cloud-Aerosol Lidar and infrared Pathfinder Satellite Observation) Lidar observations over oceans. The results show that the transition zone extends as far as 15 km away from clouds and it is ubiquitous over all oceans. The use of only high confidence level cloud-aerosol discrimination (CAD) data confirms the findings. However, the results underline the need for caution to avoid biases in studies of satellite aerosol products, aerosol-cloud interactions, and aerosol direct radiative effects.

  6. Sensitivity of Remote Aerosol Distributions to Representation of Cloud-Aerosol Interactions in a Global Climate Model

    Energy Technology Data Exchange (ETDEWEB)

    Wang, Hailong; Easter, Richard C.; Rasch, Philip J.; Wang, Minghuai; Liu, Xiaohong; Ghan, Steven J.; Qian, Yun; Yoon, Jin-Ho; Ma, Po-Lun; Vinoj, V.

    2013-06-05

    Many global aerosol and climate models, including the widely used Community Atmosphere Model version 5 (CAM5), have large biases in predicting aerosols in remote regions such as upper troposphere and high latitudes. In this study, we conduct CAM5 sensitivity simulations to understand the role of key processes associated with aerosol transformation and wet removal affecting the vertical and horizontal long-range transport of aerosols to the remote regions. Improvements are made to processes that are currently not well represented in CAM5, which are guided by surface and aircraft measurements together with results from a multi-scale aerosol-climate model (PNNL-MMF) that explicitly represents convection and aerosol-cloud interactions at cloud-resolving scales. We pay particular attention to black carbon (BC) due to its importance in the Earth system and the availability of measurements. We introduce into CAM5 a new unified scheme for convective transport and aerosol wet removal with explicit aerosol activation above convective cloud base. This new implementation reduces the excessive BC aloft to better simulate observed BC profiles that show decreasing mixing ratios in the mid- to upper-troposphere. After implementing this new unified convective scheme, we examine wet removal of submicron aerosols that occurs primarily through cloud processes. The wet removal depends strongly on the sub-grid scale liquid cloud fraction and the rate of conversion of liquid water to precipitation. These processes lead to very strong wet removal of BC and other aerosols over mid- to high latitudes during winter months. With our improvements, the Arctic BC burden has a10-fold (5-fold) increase in the winter (summer) months, resulting in a much better simulation of the BC seasonal cycle as well. Arctic sulphate and other aerosol species also increase but to a lesser extent. An explicit treatment of BC aging with slower aging assumptions produces an additional 30-fold (5-fold) increase in

  7. On the impacts of phytoplankton-derived organic matter on the properties of the primary marine aerosol – Part 2: Composition, hygroscopicity and cloud condensation activity

    Directory of Open Access Journals (Sweden)

    E. Fuentes

    2010-11-01

    Full Text Available The effect of colloidal and dissolved organic matter <0.2 μm, secreted by marine biota, on the hygroscopic growth and droplet activation behaviour of the primary marine aerosol was studied. Seawater proxies were prepared by the combination of artificial seawater devoid of marine organics and natural seawater enriched in organic exudate released by laboratory-grown phytoplankton cultures, as described in a companion paper. The primary aerosol was produced by bubble bursting, using a plunging multijet system as an aerosol generator.

    The aerosol generated from seawater proxies enriched with marine exudate presented organic volume fractions on the order of 5–37%, as derived by applying a simple mixing rule. The hygroscopic growth and cloud condensation nuclei (CCN activity of the marine organics-enriched particles where 9–17% and 5–24% lower, respectively, than those of the aerosol produced from artificial seawater devoid of exudate. Experiments in a companion paper indicated that the cloud nuclei formation could be enhanced in diatom bloom areas because of the increase in the primary particle production induced by marine organics. The experiments in the present study, however, indicate that the impacts of such an enhancement would be counteracted by the reduction in the CCN activity of the primary particles enriched in marine organics.

    The extent of the effect of the biogenic matter on the particle behaviour was dependent on the seawater organic concentration and type of algal exudate. Aerosol produced from seawater proxies containing diatomaceous exudate presented higher hydrophobicity and lower CCN activity than those enriched with nanoplankton exudate. The organic fraction of the particles increased with increasing seawater organic concentration, with the highest organic enrichment found for the diatomaceous exudate. These findings are indicative that, besides the differences induced by the aerosol generator employed

  8. Time-Resolved Molecular Characterization of Limonene/Ozone Aerosol using High-Resolution Electrospray Ionization Mass Spectrometry

    Energy Technology Data Exchange (ETDEWEB)

    Bateman, Adam P.; Nizkorodov, Serguei; Laskin, Julia; Laskin, Alexander

    2009-09-09

    Molecular composition of limonene/O3 secondary organic aerosol (SOA) was investigated using high-resolution electrospray ionization mass spectrometry (HR-ESI-MS) as a function of reaction time. SOA was generated by ozonation of D-limonene in a reaction chamber and sampled at different time intervals using a cascade impactor. The SOA samples were extracted into acetonitrile and analyzed using a HR-ESI-MS instrument with a resolving power of 100,000 (m/Δm). The resulting mass spectra provided detailed information about the extent of oxidation inferred from the O:C ratios, double bond equivalency (DBE) factors, and aromaticity indexes (AI) in hundreds of identified individual SOA species.

  9. Highly time-resolved urban aerosol characteristics during springtime in Yangtze River Delta, China: insights from soot particle aerosol mass spectrometry

    Science.gov (United States)

    Wang, Junfeng; Ge, Xinlei; Chen, Yanfang; Shen, Yafei; Zhang, Qi; Sun, Yele; Xu, Jianzhong; Ge, Shun; Yu, Huan; Chen, Mindong

    2016-07-01

    In this work, the Aerodyne soot particle - aerosol mass spectrometer (SP-AMS) was deployed for the first time during the spring of 2015 in urban Nanjing, a megacity in the Yangtze River Delta (YRD) of China, for online characterization of the submicron aerosols (PM1). The SP-AMS enables real-time and fast quantification of refractory black carbon (rBC) simultaneously with other non-refractory species (ammonium, sulfate, nitrate, chloride, and organics). The average PM1 concentration was found to be 28.2 µg m-3, with organics (45 %) as the most abundant component, following by sulfate (19.3 %), nitrate (13.6 %), ammonium (11.1 %), rBC (9.7 %), and chloride (1.3 %). These PM1 species together can reconstruct ˜ 44 % of the light extinction during this campaign based on the IMPROVE method. Chemically resolved mass-based size distributions revealed that small particles especially ultrafine ones (cycles of nitrate, chloride, and SV-OOA both showed good anti-correlations with air temperatures, suggesting their variations were likely driven by thermodynamic equilibria and gas-to-particle partitioning. On the other hand, in contrast to other species, sulfate, and LV-OOA concentrations increased in the afternoon, and showed no positive correlations with relative humidity (RH), likely indicating the contribution from photochemical oxidation is dominant over that of aqueous-phase processing for their formations. The bivariate polar plots show that the SV-OOA was formed locally, and the variations of hydrogen-to-carbon (H / C) and oxygen-to-carbon (O / C) ratios in the Van Krevelen space further suggests an evolution pathway of SV-OOA to LV-OOA. Our findings regarding springtime aerosol chemistry in Nanjing may have important implications for the air quality remediation in the densely populated regions.

  10. Aerosol size distributions measured in urban, rural and high-alpine air with an electrical low pressure impactor (ELPI)

    Science.gov (United States)

    Held, A.; Zerrath, A.; McKeon, U.; Fehrenbach, T.; Niessner, R.; Plass-Dülmer, C.; Kaminski, U.; Berresheim, H.; Pöschl, U.

    An electrical low pressure impactor (ELPI) was used to study atmospheric aerosol particle number, surface, and mass concentrations and size distributions over a diameter range of 7 nm-10 μm at urban, rural and high-alpine locations along an alpine altitude transect across Southern Germany. The measurements were performed in the city of Munich and at the global atmosphere watch (GAW) stations Hohenpeißenberg and Zugspitze in the years 2001-2004. To minimize particle bounce effects and enable chemical analysis of the collected particles without disturbance by grease on the impaction substrates, the sample flow was conditioned to about 75% relative humidity. The performance of the ELPI instrument was evaluated by comparison with well-established aerosol measurement techniques including condensation particle counters, scanning and differential mobility particle sizers, filter sampling, and gravimetric determination of particulate mass. In general, particle number concentrations, size distributions, and PM2.5 concentrations determined with the ELPI were in good agreement with alternative techniques (rank correlation coefficients ρ = 0.70-0.95). The ELPI filter stage data for the particle diameter range of 7-30 nm, however, appeared to be strongly biased towards high values. Long-term measurements at the rural site (Hohenpeißenberg) revealed distinct seasonal patterns with the highest number concentrations in summer (median daily average: 3100 cm -3) and the highest mass concentrations in spring and fall (median daily average PM2.5 and PM10: 21-25 and 27-35 μg m -3, respectively). In spring and fall we also observed pronounced maxima of particle surface and mass concentration in the coarse mode (peak at ˜3 μm), which are most likely due to primary biological material. Relatively clean air (PM10 urban air from Munich (NE) clearly contributed to elevated particle mass loadings (PM10 > = 10 μg m -3).

  11. Retrieval of Maps of PM2.5 Aerosol in the Problematic California Valleys: Bright, Speckled Reflectances, Thin AOT, but High Pollution

    Science.gov (United States)

    Chatfield, R. B.

    2015-12-01

    The San Joaquin Valley suffers from severe episodes of respirable aerosol (PM2.5) in wintertime. We provide maps of aerosol episodes using daily snapshots of PM2.5 and its changing features despite numerous difficulties inherent to sampling the region, with special focus on the DISCOVER-AQ period, Jan-Feb 2013, which had many supporting measurements. Both high pollution and retrieval difficulties tend to occur in many Mediterranean agricultural regions. One difficulty is the relatively bright surfaces with considerable exposed soil. NASA's MAIAC and MODIS Deep Blue retrieval techniques are shown to have considerable skill even at low aerosol optical thickness (AOT) values, as evaluated by concurrent AERONET sunphotometer measurements. More significantly, these AOT values can correspond to high daytime PM2.5 since aerosol mixed layer depth is thin and variable, 200m - 600 m. The thin layers derive from typical subsidence of dry air between more stormy periods. This situation provides an advantage: water vapor column is also almost completely limited to a similar mixed layer depth, and can thus serve as a measure of aerosol dilution. The ratio of AOT to column-water-vapor from MODIS products provides two advantages: (1) it can provide a measure related to particle density, via a mixed-layer proxy, and (2) it can ratio out some errors that crop up in the retrieval of very low AOT, e.g. bidirectional reflectance and other angular dependences. These effects are combined, so we disentangle them using AERONET data. Data from the NASA Langley HSRL-2 lidar and in-situ measurements from DISCOVER-AQ are also helpful. At the time of abstract submission, sporadic errors in the column water estimates provide the greatest limitation. Looking to the near future, we suggest why the use of geostationary TEMPO data will allow multiple sampling opportunities per day, supplementary or alternative information for AOT, aerosol absorption, and even column water.

  12. Aerosol-cloud-precipitation interactions: A challenging problem in regional environment and climate research

    Institute of Scientific and Technical Information of China (English)

    P.C.S.Devara; M.G.Manoj

    2013-01-01

    Aerosols affect clouds in two broad ways:(i) presence of more number of aerosols leads to formation of more smaller droplets,and reduces coalescence,resulting in brighter clouds that reflect more solar energy back to space,hence they contribute to cooling of the Earth's surface and (ii) numerous smaller cloud droplets tend to reduce precipitation and change the extent of cloud cover and increase cloud lifetime and albedo.One of our recent studies on aerosols over the Indo-Gangetic Plains (IGP) relative to the pristine oceans to the south of Indian Ocean showed that highly absorbing aerosols could potentially lead to the revival of active condition preceded by long break.The absorption of solar radiation by aerosols such as black carbon and desert dust produces surface cooling and local stabilization of lower atmosphere.This stability effect is overcome by the enhanced moisture convergence due to the meridional gradient of aerosol-induced heating.In some other studies,we showed association between cloud thickness and cloud to sub-cloud ratio (SCR),aerosol variability (in terms of aerosol optical depth and aerosol index) and monsoon precipitation and climate over regional scale.This paper provides an overview of some salient results that have been obtained from the studies conducted,using the ground-and space-based active and passive remote sensing techniques,at the Indian Institute of Tropical Meteorology (IITM),Pune,India in the recent decade.

  13. New representation of water activity based on a single solute specific constant to parameterize the hygroscopic growth of aerosols in atmospheric models

    Directory of Open Access Journals (Sweden)

    S. Metzger

    2012-06-01

    Full Text Available Water activity is a key factor in aerosol thermodynamics and hygroscopic growth. We introduce a new representation of water activity (aw, which is empirically related to the solute molality (μs through a single solute specific constant, νi. Our approach is widely applicable, considers the Kelvin effect and covers ideal solutions at high relative humidity (RH, including cloud condensation nuclei (CCN activation. It also encompasses concentrated solutions with high ionic strength at low RH such as the relative humidity of deliquescence (RHD. The constant νi can thus be used to parameterize the aerosol hygroscopic growth over a wide range of particle sizes, from nanometer nucleation mode to micrometer coarse mode particles. In contrast to other aw-representations, our νi factor corrects the solute molality both linearly and in exponent form x · ax. We present four representations of our basic aw-parameterization at different levels of complexity for different aw-ranges, e.g. up to 0.95, 0.98 or 1. νi is constant over the selected aw-range, and in its most comprehensive form, the parameterization describes the entire aw range (0–1. In this work we focus on single solute solutions. νi can be pre-determined with a root-finding method from our water activity representation using an aw−μs data pair, e.g. at solute saturation using RHD and solubility measurements. Our aw and supersaturation (Köhler-theory results compare well with the thermodynamic reference model E-AIM for the key compounds NaCl and (NH42SO4 relevant for CCN modeling and calibration studies. Envisaged applications include regional and global atmospheric chemistry and

  14. Topics in current aerosol research

    CERN Document Server

    Hidy, G M

    1971-01-01

    Topics in Current Aerosol Research deals with the fundamental aspects of aerosol science, with emphasis on experiment and theory describing highly dispersed aerosols (HDAs) as well as the dynamics of charged suspensions. Topics covered range from the basic properties of HDAs to their formation and methods of generation; sources of electric charges; interactions between fluid and aerosol particles; and one-dimensional motion of charged cloud of particles. This volume is comprised of 13 chapters and begins with an introduction to the basic properties of HDAs, followed by a discussion on the form

  15. Characterization of Organic Nitrate Formation in Limonene Secondary Organic Aerosol using High-Resolution Chemical Ionization Mass Spectrometry

    Science.gov (United States)

    Faxon, Cameron; Hammes, Julia; Peng, Jianfei; Hallquist, Mattias; Pathak, Ravi

    2016-04-01

    Previous work has shown that organic nitrates (RONO2) are prevalent in the boundary layer, and can contribute significantly to secondary organic aerosol formation. Monoterpenes, including limonene, have been shown to be precursors for the formation of these organic nitrates. Limonene has two double bonds, either of which may be oxidized by NO3 or O3. This leads to the generation of products that can subsequently condense or partition into the particle phase, producing secondary organic aerosol. In order to further elucidate the particle and gas phase product distribution of organic nitrates forming from the reactions of limonene and the nitrate radical (NO3), a series of experiments were performed in the Gothenburg Flow Reactor for Oxidation Studies at Low Temperatures (G-FROST), described by previous work. N2O5 was used as the source for NO3 and NO2, and a characterized diffusion source was used to introduce limonene into the flow reactor. All experiments were conducted in the absence of light, and the concentration of limonene was increased step-wise throughout each experiment to modify the ratio of N2O5to limonene. The experiments were conducted such that both limonene- and N2O5-limited regimes were present. Gas and particle phase products were measured using an iodide High-Resolution Time-of-Flight Mass Spectrometer (HR-ToF-CIMS) coupled to a Filter Inlet for Gases and AEROsols (FIGAERO, and particle size and SOA mass concentrations were derived using a Scanning Mobility Particle Sizer (SMPS). CIMS measurement techniques have previously been employed for the measurement of organic nitrate products of such compounds using multiple reagent ions. The use of this instrumentation allowed for the identification of chemical formulas for gas and particle phase species. The findings from the experiments will be presented in terms of the relative gas-particle partitioning of major products and the effects of N2O5/limonene ratios on product distributions. Additionally, a

  16. The Two-Column Aerosol Project (TCAP) Science Plan

    Energy Technology Data Exchange (ETDEWEB)

    Berkowitz, CM; Berg, LK; Cziczo, DJ; Flynn, CJ; Kassianov, EI; Fast, JD; Rasch, PJ; Shilling, JE; Zaveri, RA; Zelenyuk, A; Ferrare, RA; Hostetler, CA; Cairns, B; Russell, PB; Ervens, B

    2011-07-27

    The Two-Column Aerosol Project (TCAP) field campaign will provide a detailed set of observations with which to (1) perform radiative and cloud condensation nuclei (CCN) closure studies, (2) evaluate a new retrieval algorithm for aerosol optical depth (AOD) in the presence of clouds using passive remote sensing, (3) extend a previously developed technique to investigate aerosol indirect effects, and (4) evaluate the performance of a detailed regional-scale model and a more parameterized global-scale model in simulating particle activation and AOD associated with the aging of anthropogenic aerosols. To meet these science objectives, the Atmospheric Radiation Measurement (ARM) Climate Research Facility will deploy the ARM Mobile Facility (AMF) and the Mobile Aerosol Observing System (MAOS) on Cape Cod, Massachusetts, for a 12-month period starting in the summer of 2012 in order to quantify aerosol properties, radiation, and cloud characteristics at a location subject to both clear and cloudy conditions, and clean and polluted conditions. These observations will be supplemented by two aircraft intensive observation periods (IOPs), one in the summer and a second in the winter. Each IOP will deploy one, and possibly two, aircraft depending on available resources. The first aircraft will be equipped with a suite of in situ instrumentation to provide measurements of aerosol optical properties, particle composition and direct-beam irradiance. The second aircraft will fly directly over the first and use a multi-wavelength high spectral resolution lidar (HSRL) and scanning polarimeter to provide continuous optical and cloud properties in the column below.

  17. Evaluation of the sectional aerosol microphysics module SALSA implementation in ECHAM5-HAM aerosol-climate model

    Directory of Open Access Journals (Sweden)

    T. Bergman

    2011-12-01

    Full Text Available We present the implementation and evaluation of a sectional aerosol microphysics model SALSA within the aerosol-climate model ECHAM5-HAM. This aerosol microphysics module has been designed to be flexible and computationally efficient so that it can be implemented in regional or global scale models. The computational efficiency has been achieved by keeping the number of variables needed to describe the size and composition distribution to the minimum. The aerosol size distribution is described using 20 size sections with 10 size sections in size space which cover diameters ranging from 3 nm to 10 μm divided to three subranges each having distinct optimised process and compound selection.

    The ability of the module to describe the global aerosol properties was evaluated by comparison against (1 measured continental and marine size distributions, (2 observed variability of continental modal number concentrations, (3 measured sulphate, organic carbon, black carbon and sea salt mass concentrations, (4 observations of AOD and other aerosol optical properties from satellites and AERONET network, (5 global aerosol budgets and concentrations from previous model studies, and (6 model results using M7 which is the default aerosol microphysics module in ECHAM5-HAM.

    The evaluation shows that the global aerosol properties can be reproduced reasonably well using the coarse resolution of 10 size sections in size space. The simulated global aerosol budgets are within the range of previous studies. Surface concentrations of sea salt, sulphate and carbonaceous species have an annual mean within a factor of five of the observations, while the simulated sea salt concentrations reproduce the observations less accurately and show high variability. Regionally, AOD is in relatively good agreement with the observations (within a factor of two. At mid-latitudes the observed AOD is captured well, while at high-latitudes as well as in some polluted and

  18. Natural Aerosols Explain Seasonal and Spatial Patterns of Southern Ocean Cloud Albedo

    Energy Technology Data Exchange (ETDEWEB)

    McCoy, Daniel; Burrows, Susannah M.; Wood, R.; Grosvenor, Daniel P.; Elliott, Scott; Ma, Po-Lun; Rasch, Philip J.; Hartmann, Dennis L.

    2015-07-17

    Small particles called aerosols act as nucleation sites for cloud drop formation, affecting clouds and cloud properties – ultimately influencing the cloud dynamics, lifetime, water path and areal extent that determine the reflectivity (albedo) of clouds. The concentration Nd of droplets in clouds that influences planetary albedo is sensitive to the availability of aerosol particles on which the droplets form. Natural aerosol concentrations not only affect cloud properties themselves, but also modulate the sensitivity of clouds to changes in anthropogenic aerosols. Here, it is shown that modeled natural aerosols, principally marine biogenic primary and secondary aerosol sources, explain more than half of the spatiotemporal variability in satellite-observed Nd. Enhanced Nd over regions of high biological activity is found to be driven primarily by high concentrations of sulfate aerosol at lower Southern Ocean latitudes (35-45°S) and by organic matter in sea spray aerosol at higher latitudes (45-55°S). Biogenic sources are estimated to increase the summertime mean reflected solar radiation in excess of 10 W m-2 over parts of the Southern Ocean, which is comparable to the annual mean increases expected from anthropogenic aerosols over heavily polluted regions of the Northern Hemisphere.

  19. High Resolution Aerosol Optical Depth Mapping of Beijing Using LANSAT8 Imagery

    Science.gov (United States)

    Li, Yan; Liu, Yuanliang; Wu, Jianliang

    2016-06-01

    Aerosol Optical Depth (AOD) is one of the most important parameters in the atmospheric correction of remote sensing images. We present a new method of per pixel AOD retrieval using the imagery of Landsat8. It is based on Second Simulation of the Satellite Signal in the Solar Spectrum (6S). General dark target method takes dense vegetation pixels as dark targets and derives their 550nm AODs directly from the LUT, and interpolates the AODs of other pixels according to spatial neighbourhood using those of dark target pixels. This method will down estimate the AOD levels for urban areas. We propose an innovative method to retrieval the AODs using multiple temporal data. For a pixel which has nothing change between the associated time, there must exists an intersection of surface albedo. When there are enough data to find the intersection it ought to be a value that meet the error tolerance. In this paper, we present an example of using three temporal Landsat ETM+ image to retrieve AOD taking Beijing as the testing area. The result is compared to the commonly employed dark target algorithm to show the effectiveness of the methods.

  20. Global volcanic aerosol properties derived from emissions, 1990-2014, using CESM1(WACCM): VOLCANIC AEROSOLS DERIVED FROM EMISSIONS

    Energy Technology Data Exchange (ETDEWEB)

    Mills, Michael J. [Atmospheric Chemistry Observations and Modeling Laboratory, National Center for Atmospheric Research, Boulder Colorado USA; Schmidt, Anja [School of Earth and Environment, University of Leeds, Leeds UK; Easter, Richard [Atmospheric Sciences and Global Change Division, Pacific Northwest National Laboratory, Richland Washington USA; Solomon, Susan [Department of Earth, Atmospheric, and Planetary Sciences, Massachusetts Institute of Technology, Cambridge Massachusetts USA; Kinnison, Douglas E. [Atmospheric Chemistry Observations and Modeling Laboratory, National Center for Atmospheric Research, Boulder Colorado USA; Ghan, Steven J. [Atmospheric Sciences and Global Change Division, Pacific Northwest National Laboratory, Richland Washington USA; Neely, Ryan R. [School of Earth and Environment, University of Leeds, Leeds UK; National Centre for Atmospheric Science, University of Leeds, Leeds UK; Marsh, Daniel R. [Atmospheric Chemistry Observations and Modeling Laboratory, National Center for Atmospheric Research, Boulder Colorado USA; Conley, Andrew [Atmospheric Chemistry Observations and Modeling Laboratory, National Center for Atmospheric Research, Boulder Colorado USA; Bardeen, Charles G. [Atmospheric Chemistry Observations and Modeling Laboratory, National Center for Atmospheric Research, Boulder Colorado USA; Gettelman, Andrew [Atmospheric Chemistry Observations and Modeling Laboratory, National Center for Atmospheric Research, Boulder Colorado USA

    2016-03-06

    Accurate representation of global stratospheric aerosol properties from volcanic and non-volcanic sulfur emissions is key to understanding the cooling effects and ozone-loss enhancements of recent volcanic activity. Attribution of climate and ozone variability to volcanic activity is of particular interest in relation to the post-2000 slowing in the apparent rate of global average temperature increases, and variable recovery of the Antarctic ozone hole. We have developed a climatology of global aerosol properties from 1990 to 2014 calculated based on volcanic and non-volcanic emissions of sulfur sources. We have complied a database of volcanic SO2 emissions and plume altitudes for eruptions between 1990 and 2014, and a new prognostic capability for simulating stratospheric sulfate aerosols in version 5 of the Whole Atmosphere Community Climate Model, a component of the Community Earth System Model. Our climatology shows remarkable agreement with ground-based lidar observations of stratospheric aerosol optical depth (SAOD), and with in situ measurements of aerosol surface area density (SAD). These properties are key parameters in calculating the radiative and chemical effects of stratospheric aerosols. Our SAOD climatology represents a significant improvement over satellite-based analyses, which ignore aerosol extinction below 15 km, a region that can contain the vast majority of stratospheric aerosol extinction at mid- and high-latitudes. Our SAD climatology significantly improves on that provided for the Chemistry-Climate Model Initiative, which misses 60% of the SAD measured in situ. Our climatology of aerosol properties is publicly available on the Earth System Grid.

  1. In situ fabrication of depth-type hierarchical CNT/quartz fiber filters for high efficiency filtration of sub-micron aerosols and high water repellency.

    Science.gov (United States)

    Li, Peng; Zong, Yichen; Zhang, Yingying; Yang, Mengmeng; Zhang, Rufan; Li, Shuiqing; Wei, Fei

    2013-04-21

    We fabricated depth-type hierarchical CNT/quartz fiber (QF) filters through in situ growth of CNTs upon quartz fiber (QF) filters using a floating catalyst chemical vapor deposition (CVD) method. The filter specific area of the CNT/QF filters is more than 12 times higher than that of the pristine QF filters. As a result, the penetration of sub-micron aerosols for CNT/QF filters is reduced by two orders of magnitude, which reaches the standard of high-efficiency particulate air (HEPA) filters. Simultaneously, due to the fluffy brush-like hierarchical structure of CNTs on QFs, the pore size of the hybrid filters only has a small increment. The pressure drop across the CNT/QF filters only increases about 50% with respect to that of the pristine QF filters, leading to an obvious increased quality factor of the CNT/QF filters. Scanning electron microscope images reveal that CNTs are very efficient in capturing sub-micron aerosols. Moreover, the CNT/QF filters show high water repellency, implying their superiority for applications in humid conditions.

  2. Aerosol properties over south india during different seasons

    Science.gov (United States)

    Sivaprasad, P.; Babu, C. A.; Jayakrishnan, P. R.

    Aerosols play an important role in the radiation balance and cloud properties, thereby affect the entire climatology of the earth-atmosphere system. Besides natural sources like dust, seasalt and natural sulphates, anthropogenic activities also inject aerosols like soot and industrial sulphates. Of these sea-salt and sulphates scatter the solar radiation. Soot is an absorbing aerosol while soil dust and organic matters are partly absorbing aerosols. Wind and rainfall are major factors affecting the transportation and deposition of the aerosols. India is a country blessed with plenty of monsoon rains. Winter (December to February), summer (March to May), monsoon (June to September) and post monsoon (October to November) are the four seasons over the region. Aerosol properties vary according to the season. Natural aerosols blown from the deserts have a major role in the aerosol optical depth over India. Of this, dust from Arabian desert that is carried by the winds are most important. The aerosol optical depth of south India is entirely different from that of north India. Maximum aerosol concentration is found over Gangetic plane in most of the seasons, whereas entire south India shows less aerosol optical depth. In the present study the aerosol properties of south India is analysed in general. Particular analysis is carried out for the four regions in the east and west coasts around Chennai, Kolkotha, Mumbai and Cochin. Chennai and Kolkotha are situated in the east coast whereas Cochin and Mumbai are in the west coast. These are industrial cities in India. Chennai region does not get monsoon rainfall since it is situated in the leeward side of Western ghats. But in the post monsoon season Chennai gets good amount of rainfall. Other three regions get good amount of rainfall during monsoon season. The study uses Terra MODIS, TOMS, NCEP/NCAR and TRMM data. Aerosol properties are analysed using Terra MODIS and Nimbus TOMS data. The variations of the aerosol optical

  3. Assessment of nocturnal aerosol optical depth from lunar photometry at the Izaña high mountain observatory

    Science.gov (United States)

    Barreto, África; Román, Roberto; Cuevas, Emilio; Berjón, Alberto J.; Almansa, A. Fernando; Toledano, Carlos; González, Ramiro; Hernández, Yballa; Blarel, Luc; Goloub, Philippe; Guirado, Carmen; Yela, Margarita

    2017-08-01

    This work is a first approach to correct the systematic errors observed in the aerosol optical depth (AOD) retrieved at nighttime using lunar photometry and calibration techniques dependent on the lunar irradiance model. To this end, nocturnal AOD measurements were performed in 2014 using the CE318-T master Sun-sky-lunar photometer (lunar Langley calibrated) at the Izaña high mountain observatory. This information has been restricted to 59 nights characterized as clean and stable according to lidar vertical profiles. A phase angle dependence as well as an asymmetry within the Moon's cycle of the Robotic Lunar Observatory (ROLO) model could be deduced from the comparison in this 59-night period of the CE318-T calibration performed by means of the lunar Langley calibration and the calibration performed every single night by means of the common Langley technique. Nocturnal AOD has also been compared in the same period with a reference AOD based on daylight AOD extracted from the AErosol RObotic NETwork (AERONET) at the same station. Considering stable conditions, the difference ΔAODfit, between AOD from lunar observations and the linearly interpolated AOD (the reference) from daylight data, has been calculated. The results show that ΔAODfit values are strongly affected by the Moon phase and zenith angles. This dependency has been parameterized using an empirical model with two independent variables (Moon phase and zenith angles) in order to correct the AOD for these residual dependencies. The correction of this parameterized dependency has been checked at four stations with quite different environmental conditions (Izaña, Lille, Carpentras and Dakar) showing a significant reduction of the AOD dependence on phase and zenith angles and an improved agreement with daylight reference data. After the correction, absolute AOD differences for day-night-day clean and stable transitions remain below 0.01 for all wavelengths.

  4. Technical Note: A new global database of trace gases and aerosols from multiple sources of high vertical resolution measurements

    Directory of Open Access Journals (Sweden)

    G. E. Bodeker

    2008-09-01

    Full Text Available A new database of trace gases and aerosols with global coverage, derived from high vertical resolution profile measurements, has been assembled as a collection of binary data files; hereafter referred to as the "Binary DataBase of Profiles" (BDBP. Version 1.0 of the BDBP, described here, includes measurements from different satellite- (HALOE, POAM II and III, SAGE I and II and ground-based measurement systems (ozonesondes. In addition to the primary product of ozone, secondary measurements of other trace gases, aerosol extinction, and temperature are included. All data are subjected to very strict quality control and for every measurement a percentage error on the measurement is included. To facilitate analyses, each measurement is added to 3 different instances (3 different grids of the database where measurements are indexed by: (1 geographic latitude, longitude, altitude (in 1 km steps and time, (2 geographic latitude, longitude, pressure (at levels ~1 km apart and time, (3 equivalent latitude, potential temperature (8 levels from 300 K to 650 K and time.

    In contrast to existing zonal mean databases, by including a wider range of measurement sources (both satellite and ozonesondes, the BDBP is sufficiently dense to permit calculation of changes in ozone by latitude, longitude and altitude. In addition, by including other trace gases such as water vapour, this database can be used for comprehensive radiative transfer calculations. By providing the original measurements rather than derived monthly means, the BDBP is applicable to a wider range of applications than databases containing only monthly mean data. Monthly mean zonal mean ozone concentrations calculated from the BDBP are compared with the database of Randel and Wu, which has been used in many earlier analyses. As opposed to that database which is generated from regression model fits, the BDBP uses the original (quality controlled measurements with no smoothing applied in any

  5. Assessment of nocturnal aerosol optical depth from lunar photometry at the Izaña high mountain observatory

    Directory of Open Access Journals (Sweden)

    Á. Barreto

    2017-08-01

    Full Text Available This work is a first approach to correct the systematic errors observed in the aerosol optical depth (AOD retrieved at nighttime using lunar photometry and calibration techniques dependent on the lunar irradiance model. To this end, nocturnal AOD measurements were performed in 2014 using the CE318-T master Sun–sky–lunar photometer (lunar Langley calibrated at the Izaña high mountain observatory. This information has been restricted to 59 nights characterized as clean and stable according to lidar vertical profiles. A phase angle dependence as well as an asymmetry within the Moon's cycle of the Robotic Lunar Observatory (ROLO model could be deduced from the comparison in this 59-night period of the CE318-T calibration performed by means of the lunar Langley calibration and the calibration performed every single night by means of the common Langley technique. Nocturnal AOD has also been compared in the same period with a reference AOD based on daylight AOD extracted from the AErosol RObotic NETwork (AERONET at the same station. Considering stable conditions, the difference ΔAODfit, between AOD from lunar observations and the linearly interpolated AOD (the reference from daylight data, has been calculated. The results show that ΔAODfit values are strongly affected by the Moon phase and zenith angles. This dependency has been parameterized using an empirical model with two independent variables (Moon phase and zenith angles in order to correct the AOD for these residual dependencies. The correction of this parameterized dependency has been checked at four stations with quite different environmental conditions (Izaña, Lille, Carpentras and Dakar showing a significant reduction of the AOD dependence on phase and zenith angles and an improved agreement with daylight reference data. After the correction, absolute AOD differences for day–night–day clean and stable transitions remain below 0.01 for all wavelengths.

  6. Lab-scale development of a high temperature aerosol particle sampling probe system for field measurements in thermochemical conversion of biomass

    Energy Technology Data Exchange (ETDEWEB)

    Lindskog, M.; Malik, A.; Pagels, J.; Sanati, M. [Lund Univ., Lund (Sweden). Div. of Ergonomics and Aerosol Technology

    2010-07-01

    Thermochemical conversion of biomass requires both combustion in an oxygen rich environment and gasification in an oxygen deficient environment. Therefore, the mass concentration of fly ash from combustion processes is dominated by inorganic compounds, and the particulate matter obtained from gasification is dominated by carbonaceous compounds. The fine fly ash particles can initiate corrosion and fouling and also increases emissions of fine particulates to the atmosphere. This study involved the design of a laboratory scale setup consisting of a high temperature sampling probe and an aerosol generation system to study the formation of fine particle from biomass gasification processes. An aerosol model system using potassium chloride (KCl) as the ash compound and Di Octyl Sebacate oil (DOS) as the volatile organic part was used to test the high temperature sampling probe. Tests conducted at 200 degrees C showed good reproducibility of the aerosol generator. The tests also demonstrated suitable dilution ratios which enabled the denuder to absorb all of the gaseous organic compounds in the set up, thus enabling measurement of only the particle phase. Condensable organic concentrations of 1-68 mg/m{sup 3} were easily handled by the high temperature sampling probe system, indicating that the denuder worked well. Additional tests will be performed using an Aerosol Mass Spectrometer (AMST) to verify that the denuder can capture all of the gaseous organic compounds also when condensed onto agglomerated soot particles. 6 refs., 1 tab., 9 figs.

  7. ATI TDA 5A aerosol generator evaluation

    Energy Technology Data Exchange (ETDEWEB)

    Gilles, D.A.

    1998-07-27

    Oil based aerosol ``Smoke`` commonly used for testing the efficiency and penetration of High Efficiency Particulate Air filters (HEPA) and HEPA systems can produce flammability hazards that may not have been previously considered. A combustion incident involving an aerosol generator has caused an investigation into the hazards of the aerosol used to test HEPA systems at Hanford.

  8. Sensitivity of remote aerosol distributions to representation of cloud–aerosol interactions in a global climate model

    Directory of Open Access Journals (Sweden)

    H. Wang

    2013-06-01

    Full Text Available Many global aerosol and climate models, including the widely used Community Atmosphere Model version 5 (CAM5, have large biases in predicting aerosols in remote regions such as the upper troposphere and high latitudes. In this study, we conduct CAM5 sensitivity simulations to understand the role of key processes associated with aerosol transformation and wet removal affecting the vertical and horizontal long-range transport of aerosols to the remote regions. Improvements are made to processes that are currently not well represented in CAM5, which are guided by surface and aircraft measurements together with results from a multi-scale aerosol–climate model that explicitly represents convection and aerosol–cloud interactions at cloud-resolving scales. We pay particular attention to black carbon (BC due to its importance in the Earth system and the availability of measurements. We introduce into CAM5 a new unified scheme for convective transport and aerosol wet removal with explicit aerosol activation above convective cloud base. This new implementation reduces the excessive BC aloft to better simulate observed BC profiles that show decreasing mixing ratios in the mid- to upper-troposphere. After implementing this new unified convective scheme, we examine wet removal of submicron aerosols that occurs primarily through cloud processes. The wet removal depends strongly on the subgrid-scale liquid cloud fraction and the rate of conversion of liquid water to precipitation. These processes lead to very strong wet removal of BC and other aerosols over mid- to high latitudes during winter months. With our improvements, the Arctic BC burden has a 10-fold (5-fold increase in the winter (summer months, resulting in a much-better simulation of the BC seasonal cycle as well. Arctic sulphate and other aerosol species also increase but to a lesser extent. An explicit treatment of BC aging with slower aging assumptions produces an additional 30-fold (5-fold

  9. Atmosphere aerosol satellite project Aerosol-UA

    Science.gov (United States)

    Milinevsky, Gennadi; Yatskiv, Yaroslav; Syniavskyi, Ivan; Bovchaliuk, Andrii; Degtyaryov, Oleksandr; Sosonkin, Mikhail; Mishchenko, Michael; Danylevsky, Vassyl; Ivanov, Yury; Oberemok, Yevgeny; Masley, Volodymyr; Rosenbush, Vera; Moskalev, Sergii

    2017-04-01

    The experiment Aerosol-UA is Ukrainian space mission aimed to the terrestrial atmospheric aerosol spatial distribution and microphysics investigations. The experiment concept is based on idea of Glory/APS mission of precise orbital measurements of polarization and intensity of the sunlight scattered by the atmosphere, aerosol and the surface the multichannel Scanning Polarimeter (ScanPol) with narrow field-of-view. ScanPol measurements will be accompanied by the wide-angle MultiSpectral Imager-Polarimeter (MSIP). The ScanPol is designed to measure Stokes parameters I, Q, U within the spectral range from the UV to the SWIR in a wide range of phase angles along satellite ground path. Expected ScanPol polarimetric accuracy is 0.15%. A high accuracy measurement of the degree of linear polarization is provided by on-board calibration of the ScanPol polarimeter. On-board calibration is performed for each scan of the mirror scanning system. A set of calibrators is viewed during the part of the scan range when the ScanPol polarimeter looks in the direction opposite to the Earth's surface. These reference assemblies provide calibration of the zero of the polarimetric scale (unpolarized reference assembly) and the scale factor for the polarimetric scale (polarized reference assembly). The zero of the radiometric scale is provided by the dark reference assembly.The spectral channels of the ScanPol are used to estimate the tropospheric aerosol absorption, the aerosol over the ocean and the land surface, the signals from cirrus clouds, stratospheric aerosols caused by major volcanic eruptions, and the contribution of the Earth's surface. The imager-polarimeter MSIP will collect 60°x60° field-of-view images on the state of the atmosphere and surface in the area, where the ScanPol polarimeter will measure, to retrieve aerosol optical depth and polarization properties of aerosol by registration of three Stokes parameters simultaneously in three spectral channels. The two more

  10. Film Growth Rates and Activation Energies for Core-Shell Nanoparticles Derived from a CVD Based Aerosol Process

    Directory of Open Access Journals (Sweden)

    Frederik Weis

    2015-03-01

    Full Text Available Silica core-shell nanoparticles of about 60–120 nm with a closed outer layer of bismuth or molybdenum oxide of 1–10 nm were synthesized by an integrated chemical vapor synthesis/chemical vapor deposition process at atmospheric pressure. Film growth rates and activation energies were derived from transmission electron microscopy (TEM images for a deposition process based on molybdenum hexacarbonyl and triphenyl bismuth as respective coating precursors. Respective activation energies of 123 ± 10 and 155 ± 10 kJ/mol are in good agreement with the literature and support a deposition mechanism based on surface-induced removal of the precursor ligands. Clean substrate surfaces are thus prerequisite for conformal coatings. Integrated aerosol processes are solvent-free and intrinsically clean. In contrast, commercial silica substrate particles were found to suffer from organic residues which hinder shell formation, and require an additional calcination step to clean the surface prior to coating. Dual layer core-shell structures with molybdenum oxide on bismuth oxide were synthesized with two coating reactors in series and showed similar film growth rates.

  11. Measurements in a highly polluted Asian mega city: observations of aerosol number size distribution, modal parameters and nucleation events

    Directory of Open Access Journals (Sweden)

    P. Mönkkönen

    2004-09-01

    Full Text Available Diurnal variation of number size distribution (particle size 3–800 nm and modal parameters (geometric standard deviation, geometric mean diameter and modal aerosol particle concentration in a highly polluted urban environment was investigated during October and November 2002 in New Delhi, India. Continuous monitoring for more than two weeks with the time resolution of 10 min was conducted using a Differential Mobility Particle Sizer (twin DMPS. The results indicated clear increase in Aitken mode (25–100 nm particles during traffic peak hours, but towards the evenings there were more Aitken mode particles compared to the mornings. Also high concentrations of accumulation mode particles (>100 nm were detected in the evenings only. In the evenings, biomass/refuse burning and cooking are possible sources beside the traffic. We have also shown that nucleation events are possible in this kind of atmosphere even though as clear nucleation events as observed in rural sites could not be detected. The formation rate of 3 nm particles (J3 of the observed events varied from 3.3 to 13.9 cm−3s−1 and the growth rate varied from 11.6 to 18.1 nmh−1 showing rapid growth and high formation rate, which seems to be typical in urban areas.

  12. Measurements in a highly polluted Asian mega city: observations of aerosol number size distribution, modal parameters and nucleation events

    Directory of Open Access Journals (Sweden)

    P. Mönkkönen

    2005-01-01

    Full Text Available Diurnal variation of number size distribution (particle size 3-800nm and modal parameters (geometric standard deviation, geometric mean diameter and modal aerosol particle concentration in a highly polluted urban environment was investigated during October and November 2002 in New Delhi, India. Continuous monitoring for more than two weeks with the time resolution of 10min was conducted using a Differential Mobility Particle Sizer (twin DMPS. The results indicated clear increase in Aitken mode (25-100nm particles during traffic peak hours, but towards the evenings there were more Aitken mode particles compared to the mornings. Also high concentrations of accumulation mode particles (>100nm were detected in the evenings only. In the evenings, biomass/refuse burning and cooking are possible sources beside the traffic. We have also shown that nucleation events are possible in this kind of atmosphere even though as clear nucleation events as observed in rural sites could not be detected. The formation rate of 3nm particles (J3 of the observed events varied from 3.3 to 13.9cm-3s-1 and the growth rate varied from 11.6 to 18.1nmh-1 showing rapid growth and high formation rate, which seems to be typical in urban areas.

  13. Highly functionalized organic nitrates in the southeast United States: Contribution to secondary organic aerosol and reactive nitrogen budgets

    Energy Technology Data Exchange (ETDEWEB)

    Lee, Ben H.; Mohr, Claudia; Lopez-Hilfiker, Felipe D.; Lutz, Anna; Hallquist, Mattias; Lee, Lance; Romer, Paul; Cohen, Ronald C.; Iyer, Siddharth; Kurtén, Theo; Hu, Weiwei; Day, Douglas A.; Campuzano-Jost, Pedro; Jimenez, Jose L.; Xu, Lu; Ng, Nga Lee; Guo, Hongyu; Weber, Rodney J.; Wild, Robert J.; Brown, Steven S.; Koss, Abigail; de Gouw, Joost; Olson, Kevin; Goldstein, Allen H.; Seco, Roger; Kim, Saewung; McAvey, Kevin; Shepson, Paul B.; Starn, Tim; Baumann, Karsten; Edgerton, Eric S.; Liu, Jiumeng; Shilling, John E.; Miller, David O.; Brune, William; Schobesberger, Siegfried; D' Ambro, Emma L.; Thornton, Joel A.

    2016-01-25

    Organic nitrates (ON = RONO2 + RO2NO2) are an important reservoir, if not sink, of atmospheric nitrogen oxides (NOx=NO+NO2). ON formed from isoprene oxidation alone are responsible for the export of 8 to 30% of anthropogenic NOx out of the U.S. continental boundary layer [Horowitz et al., 1998; Liang et al., 1998]. Regional NOx budgets and tropospheric ozone (O3) production, are therefore particularly sensitive to uncertainties in the yields and fates of ON [Beaver et al., 2012; Browne et al., 2013]. The yields implemented in modeling studies are determined from laboratory experiments in which only a few of the first generation gaseous ON or the total gas and particle-phase ON have been quantified [Perring et al., 2013 and references therein], while production of highly functionalized ON capable of strongly partitioning to the particle-phase have been inferred [Farmer et al., 2010; Ng et al., 2007; Nguyen et al., 2011; Perraud et al., 2012; Rollins et al., 2012], or directly measured [Ehn et al., 2014]. Addition of a nitrate (–ONO2) functional group to a hydrocarbon is estimated to lower the equilibrium saturation vapor pressure by 2.5 to 3 orders of magnitude [e.g. Capouet and Muller, 2006]. Thus, organic nitrate formation can potentially enhance particle-phase partitioning of hydrocarbons in regions with elevated levels of nitrogen oxides, contributing to secondary organic aerosol (SOA) formation [Ng et al., 2007]. There has, however, been no high time-resolved measurements of speciated ON in the particle-phase. We utilize a newly developed high-resolution time-of-flight chemical ionization mass spectrometer (HR-ToF-CIMS) using Iodide-adduct ionization [B H Lee et al., 2014a] with a filter inlet for gases and aerosols (FIGAERO) [Lopez-Hilfiker et al., 2014] that allows alternating in situ measurement of the molecular composition of gas and particle phases. We present obs