Satellite derived trends in NO2 over the major global hotspot regions during the past decade and their inter-comparison

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Ghude, Sachin D.; Van der A, R.J.; Beig, G.; Fadnavis, S.; Polade, S.D.

2009-01-01

We assessed satellite derived tropospheric NO 2 distribution on a global scale and identified the major NO 2 hotspot regions. Combined GOME and SCIAMACHY measurements for the period 1996-2006 have been used to compute the trends over these regions. Our analysis shows that tropospheric NO 2 column amounts have increased over the newly and rapidly developing regions like China (11 ± 2.6%/year), south Asia (1.76 ± 1.1%/year), Middle East (2.3 ± 1%/year) and South Africa (2.4 ± 2.2%/year). Tropospheric NO 2 column amounts show some decrease over the eastern US (-2 ± 1.5%/year) and Europe (0.9 ± 2.1%/year). We found that although tropospheric NO 2 column amounts decreased over the major developed regions in the past decade, the present tropospheric NO 2 column amounts over these regions are still significantly higher than those observed over newly and rapidly developing regions (except China). Tropospheric NO 2 column amounts show some decrease over South America and Central Africa, which are major biomass burning regions in the Southern Hemisphere. - Trends in tropospheric column NO 2 over newly developing regions.

Global carbon monoxide as retrieved from SCIAMACHY by WFM-DOAS

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M. Buchwitz

2004-01-01

Full Text Available First results concerning the retrieval of tropospheric carbon monoxide (CO from satellite solar backscatter radiance measurements in the near-infrared spectral region (~2.3µm are presented. The Weighting Function Modified (WFM DOAS retrieval algorithm has been used to retrieve vertical columns of CO from SCIAMACHY/ENVISAT nadir spectra. We present detailed results for three days from the time periode January to October 2003 selected to have good overlap with the daytime CO measurements of MOPITT onboard EOS Terra. Because the WFM-DOAS Version 0.4 CO columns presented in this paper are scaled by a constant factor of 0.5 to compensate for an obvious overestimation we focus on the variability of the retrieved columns rather than on their absolute values. It is shown that plumes of CO resulting from, e.g. biomass burning in Africa, are detectable with single overpass SCIAMACHY data. Globally, the SCIAMACHY CO columns are in reasonable agreement with the Version 3 CO column data product of MOPITT. For example, for measurements over land, where the quality of the data is typically better than over ocean due to higher surface reflectivity, the standard deviation of the difference with respect to MOPITT is in the range 0.4-0.6x1018 molecules/cm2 and the linear correlation coefficient is between 0.4 and 0.7. The level of agreement between the data of both sensors depends on time and location but is typically within 30% for most latitudes. In the southern hemisphere outside Antarctica SCIAMACHY tends to give systematically higher values than MOPITT. More studies are needed to find out what the reasons for the observed differences with respect to MOPITT are and how the algorithm can be modified to improve the quality of the CO columns as retrieved from SCIAMACHY.

Evaluation of SCIAMACHY Level-1 data versions using nadir ozone profile retrievals in the period 2003-2011

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Shah, Sweta; Tuinder, Olaf N. E.; van Peet, Jacob C. A.; de Laat, Adrianus T. J.; Stammes, Piet

2018-04-01

Ozone profile retrieval from nadir-viewing satellite instruments operating in the ultraviolet-visible range requires accurate calibration of Level-1 (L1) radiance data. Here we study the effects of calibration on the derived Level-2 (L2) ozone profiles for three versions of SCanning Imaging Absorption spectroMeter for Atmospheric ChartograpHY (SCIAMACHY) L1 data: version 7 (v7), version 7 with m-factors (v7mfac) and version 8 (v8). We retrieve nadir ozone profiles from the SCIAMACHY instrument that flew on board Envisat using the Ozone ProfilE Retrieval Algorithm (OPERA) developed at KNMI with a focus on stratospheric ozone. We study and assess the quality of these profiles and compare retrieved L2 products from L1 SCIAMACHY data versions from the years 2003 to 2011 without further radiometric correction. From validation of the profiles against ozone sonde measurements, we find that the v8 performs better than v7 and v7mfac due to correction for the scan-angle dependency of the instrument's optical degradation. Validation for the years 2003 and 2009 with ozone sondes shows deviations of SCIAMACHY ozone profiles of 0.8-15 % in the stratosphere (corresponding to pressure range ˜ 100-10 hPa) and 2.5-100 % in the troposphere (corresponding to pressure range ˜ 1000-100 hPa), depending on the latitude and the L1 version used. Using L1 v8 for the years 2003-2011 leads to deviations of ˜ 1-11 % in stratospheric ozone and ˜ 1-45 % in tropospheric ozone. The SCIAMACHY L1 v8 data can still be improved upon in the 265-330 nm range used for ozone profile retrieval. The slit function can be improved with a spectral shift and squeeze, which leads to a few percent residue reduction compared to reference solar irradiance spectra. Furthermore, studies of the ratio of measured to simulated reflectance spectra show that a bias correction in the reflectance for wavelengths below 300 nm appears to be necessary.

Overview of SCIAMACHY validation: 2002-2004

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Piters, A. J. M.; Bramstedt, K.; Lambert, J.-C.; Kirchhoff, B.

2006-01-01

SCIAMACHY, on board Envisat, has been in operation now for almost three years. This UV/visible/NIR spectrometer measures the solar irradiance, the earthshine radiance scattered at nadir and from the limb, and the attenuation of solar radiation by the atmosphere during sunrise and sunset, from 240 to 2380 nm and at moderate spectral resolution. Vertical columns and profiles of a variety of atmospheric constituents are inferred from the SCIAMACHY radiometric measurements by dedicated retrieval algorithms. With the support of ESA and several international partners, a methodical SCIAMACHY validation programme has been developed jointly by Germany, the Netherlands and Belgium (the three instrument providing countries) to face complex requirements in terms of measured species, altitude range, spatial and temporal scales, geophysical states and intended scientific applications. This summary paper describes the approach adopted to address those requirements. Since provisional releases of limited data sets in summer 2002, operational SCIAMACHY processors established at DLR on behalf of ESA were upgraded regularly and some data products - level-1b spectra, level-2 O3, NO2, BrO and clouds data - have improved significantly. Validation results summarised in this paper and also reported in this special issue conclude that for limited periods and geographical domains they can already be used for atmospheric research. Nevertheless, current processor versions still experience known limitations that hamper scientific usability in other periods and domains. Free from the constraints of operational processing, seven scientific institutes (BIRA-IASB, IFE/IUP-Bremen, IUP-Heidelberg, KNMI, MPI, SAO and SRON) have developed their own retrieval algorithms and generated SCIAMACHY data products, together addressing nearly all targeted constituents. Most of the UV-visible data products - O3, NO2, SO2, H2O total columns; BrO, OClO slant columns; O3, NO2, BrO profiles - already have acceptable

Determination of tropospheric vertical columns of NO2 and aerosol optical properties in a rural setting using MAX-DOAS

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M. O. Wenig

2011-12-01

Full Text Available Multi-AXis Differential Optical Absorption Spectroscopy (MAX-DOAS measurements were performed in a rural location of southwestern Ontario during the Border Air Quality and Meteorology Study. Slant column densities (SCDs of NO2 and O4 were determined using the standard DOAS technique. Using a radiative transfer model and the O4 SCDs, aerosol optical depths were determined for clear sky conditions and compared to OMI, MODIS, AERONET, and local PM2.5 measurements. This aerosol information was input to a radiative transfer model to calculate NO2 air mass factors, which were fit to the measured NO2 SCDs to determine tropospheric vertical column densities (VCDs of NO2. The method of determining NO2 VCDs in this way was validated for the first time by comparison to composite VCDs derived from aircraft and ground-based measurements of NO2. The new VCDs were compared to VCDs of NO2 determined via retrievals from the satellite instruments SCIAMACHY and OMI, for overlapping time periods. The satellite-derived VCDs were higher, with a mean bias of +0.5–0.9×1015 molec cm−2. This last finding is different from previous studies whereby MAX-DOAS geometric VCDs were higher than satellite determinations, albeit for urban areas with higher VCDs. An effective boundary layer height, BLHeff, is defined as the ratio of the tropospheric VCD and the ground level concentration of NO2. Variations of BLHeff can be linked to time of day, source region, stability of the atmosphere, and the presence or absence of elevated NOx sources. In particular, a case study is shown where a high VCD and BLHeff were observed when an elevated industrial plume of NOx and SO2 was fumigated to the surface as a lake breeze impacted the measurement site. High BLHeff values (~1.9 km were observed during a regional smog event when high winds from the SW and high convection promoted mixing throughout the boundary layer. During this event, the regional line flux of NO2 through the region was

Overview of SCIAMACHY validation: 2002–2004

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A. J. M. Piters

2006-01-01

Full Text Available SCIAMACHY, on board Envisat, has been in operation now for almost three years. This UV/visible/NIR spectrometer measures the solar irradiance, the earthshine radiance scattered at nadir and from the limb, and the attenuation of solar radiation by the atmosphere during sunrise and sunset, from 240 to 2380 nm and at moderate spectral resolution. Vertical columns and profiles of a variety of atmospheric constituents are inferred from the SCIAMACHY radiometric measurements by dedicated retrieval algorithms. With the support of ESA and several international partners, a methodical SCIAMACHY validation programme has been developed jointly by Germany, the Netherlands and Belgium (the three instrument providing countries to face complex requirements in terms of measured species, altitude range, spatial and temporal scales, geophysical states and intended scientific applications. This summary paper describes the approach adopted to address those requirements. Since provisional releases of limited data sets in summer 2002, operational SCIAMACHY processors established at DLR on behalf of ESA were upgraded regularly and some data products – level-1b spectra, level-2 O3, NO2, BrO and clouds data – have improved significantly. Validation results summarised in this paper and also reported in this special issue conclude that for limited periods and geographical domains they can already be used for atmospheric research. Nevertheless, current processor versions still experience known limitations that hamper scientific usability in other periods and domains. Free from the constraints of operational processing, seven scientific institutes (BIRA-IASB, IFE/IUP-Bremen, IUP-Heidelberg, KNMI, MPI, SAO and SRON have developed their own retrieval algorithms and generated SCIAMACHY data products, together addressing nearly all targeted constituents. Most of the UV-visible data products – O3, NO2, SO2, H2O total columns; BrO, OClO slant columns; O3, NO2, BrO profiles

SCIAMACHY formaldehyde observations: constraint for isoprene emission estimates over Europe?

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G. Dufour

2009-03-01

Full Text Available Formaldehyde (HCHO is an important intermediate compound in the degradation of volatile organic compounds (VOCs in the troposphere. Sources of HCHO are largely dominated by its secondary production from VOC oxidation, methane and isoprene being the main precursors in unpolluted areas. As a result of the moderate lifetime of HCHO, its spatial distribution is determined by reactive hydrocarbon emissions. We focus here on Europe and investigate the influence of the different emissions on HCHO tropospheric columns with the CHIMERE chemical transport model in order to interpret the comparisons between SCIAMACHY and simulated HCHO columns. Europe was never specifically studied before for these purposes using satellite observations. The bias between measurements and model is less than 20% on average. The differences are discussed according to the errors on the model and the observations and remaining discrepancies are attributed to a misrepresentation of biogenic emissions. This study requires the characterisation of: (1 the model errors and performances concerning formaldehyde. The errors on the HCHO columns, mainly related to chemistry and mixed emission types, are evaluated to 2×10¹⁵ molecule/cm² and the model performances evaluated using surface measurements are satisfactory (~13%; (2 the observation errors that define the needs in spatial and temporal averaging for meaningful comparisons. Using SCIAMACHY observations as constraint for biogenic isoprene emissions in an inverse modelling scheme reduces their uncertainties by about a factor of two in region of intense emissions. The retrieved correction factors for the isoprene emissions range from a factor of 0.15 (North Africa to a factor of 2 (Poland, the United Kingdom depending on the regions.

UTLS water vapour from SCIAMACHY limb measurementsV3.01 (2002-2012).

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Weigel, K; Rozanov, A; Azam, F; Bramstedt, K; Damadeo, R; Eichmann, K-U; Gebhardt, C; Hurst, D; Kraemer, M; Lossow, S; Read, W; Spelten, N; Stiller, G P; Walker, K A; Weber, M; Bovensmann, H; Burrows, J P

2016-01-01

The SCanning Imaging Absorption spectroMeter for Atmospheric CHartographY (SCIAMACHY) aboard the Envisat satellite provided measurements from August 2002 until April 2012. SCIAMACHY measured the scattered or direct sunlight using different observation geometries. The limb viewing geometry allows the retrieval of water vapour at about 10-25 km height from the near-infrared spectral range (1353-1410 nm). These data cover the upper troposphere and lower stratosphere (UTLS), a region in the atmosphere which is of special interest for a variety of dynamical and chemical processes as well as for the radiative forcing. Here, the latest data version of water vapour (V3.01) from SCIAMACHY limb measurements is presented and validated by comparisons with data sets from other satellite and in situ measurements. Considering retrieval tests and the results of these comparisons, the V3.01 data are reliable from about 11 to 23 km and the best results are found in the middle of the profiles between about 14 and 20 km. Above 20 km in the extra tropics V3.01 is drier than all other data sets. Additionally, for altitudes above about 19 km, the vertical resolution of the retrieved profile is not sufficient to resolve signals with a short vertical structure like the tape recorder. Below 14 km, SCIAMACHY water vapour V3.01 is wetter than most collocated data sets, but the high variability of water vapour in the troposphere complicates the comparison. For 14-20 km height, the expected errors from the retrieval and simulations and the mean differences to collocated data sets are usually smaller than 10 % when the resolution of the SCIAMACHY data is taken into account. In general, the temporal changes agree well with collocated data sets except for the Northern Hemisphere extratropical stratosphere, where larger differences are observed. This indicates a possible drift in V3.01 most probably caused by the incomplete treatment of volcanic aerosols in the retrieval. In all other regions a

A GIS-based assessment of the suitability of SCIAMACHY satellite sensor measurements for estimating reliable CO concentrations in a low-latitude climate.

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Fagbeja, Mofoluso A; Hill, Jennifer L; Chatterton, Tim J; Longhurst, James W S

2015-02-01

An assessment of the reliability of the Scanning Imaging Absorption Spectrometer for Atmospheric Cartography (SCIAMACHY) satellite sensor measurements to interpolate tropospheric concentrations of carbon monoxide considering the low-latitude climate of the Niger Delta region in Nigeria was conducted. Monthly SCIAMACHY carbon monoxide (CO) column measurements from January 2,003 to December 2005 were interpolated using ordinary kriging technique. The spatio-temporal variations observed in the reliability were based on proximity to the Atlantic Ocean, seasonal variations in the intensities of rainfall and relative humidity, the presence of dust particles from the Sahara desert, industrialization in Southwest Nigeria and biomass burning during the dry season in Northern Nigeria. Spatial reliabilities of 74 and 42 % are observed for the inland and coastal areas, respectively. Temporally, average reliability of 61 and 55 % occur during the dry and wet seasons, respectively. Reliability in the inland and coastal areas was 72 and 38 % during the wet season, and 75 and 46 % during the dry season, respectively. Based on the results, the WFM-DOAS SCIAMACHY CO data product used for this study is therefore relevant in the assessment of CO concentrations in developing countries within the low latitudes that could not afford monitoring infrastructure due to the required high costs. Although the SCIAMACHY sensor is no longer available, it provided cost-effective, reliable and accessible data that could support air quality assessment in developing countries.

Comparison of GOME tropospheric NO2 columns with NO2 profiles deduced from ground-based in situ measurements

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Schaub, D.; Boersma, K. F.; Kaiser, J. W.; Weiss, A. K.; Folini, D.; Eskes, H. J.; Buchmann, B.

2006-08-01

Nitrogen dioxide (NO2) vertical tropospheric column densities (VTCs) retrieved from the Global Ozone Monitoring Experiment (GOME) are compared to coincident ground-based tropospheric NO2 columns. The ground-based columns are deduced from in situ measurements at different altitudes in the Alps for 1997 to June 2003, yielding a unique long-term comparison of GOME NO2 VTC data retrieved by a collaboration of KNMI (Royal Netherlands Meteorological Institute) and BIRA/IASB (Belgian Institute for Space Aeronomy) with independently derived tropospheric NO2 profiles. A first comparison relates the GOME retrieved tropospheric columns to the tropospheric columns obtained by integrating the ground-based NO2 measurements. For a second comparison, the tropospheric profiles constructed from the ground-based measurements are first multiplied with the averaging kernel (AK) of the GOME retrieval. The second approach makes the comparison independent from the a priori NO2 profile used in the GOME retrieval. This allows splitting the total difference between the column data sets into two contributions: one that is due to differences between the a priori and the ground-based NO2 profile shapes, and another that can be attributed to uncertainties in both the remaining retrieval parameters (such as, e.g., surface albedo or aerosol concentration) and the ground-based in situ NO2 profiles. For anticyclonic clear sky conditions the comparison indicates a good agreement between the columns (n=157, R=0.70/0.74 for the first/second comparison approach, respectively). The mean relative difference (with respect to the ground-based columns) is -7% with a standard deviation of 40% and GOME on average slightly underestimating the ground-based columns. Both data sets show a similar seasonal behaviour with a distinct maximum of spring NO2 VTCs. Further analysis indicates small GOME columns being systematically smaller than the ground-based ones. The influence of different shapes in the a priori and

Validation of NO2 and NO from the Atmospheric Chemistry Experiment (ACE

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M. Schneider

2008-10-01

Full Text Available Vertical profiles of NO2 and NO have been obtained from solar occultation measurements by the Atmospheric Chemistry Experiment (ACE, using an infrared Fourier Transform Spectrometer (ACE-FTS and (for NO2 an ultraviolet-visible-near-infrared spectrometer, MAESTRO (Measurement of Aerosol Extinction in the Stratosphere and Troposphere Retrieved by Occultation. In this paper, the quality of the ACE-FTS version 2.2 NO2 and NO and the MAESTRO version 1.2 NO2 data are assessed using other solar occultation measurements (HALOE, SAGE II, SAGE III, POAM III, SCIAMACHY, stellar occultation measurements (GOMOS, limb measurements (MIPAS, OSIRIS, nadir measurements (SCIAMACHY, balloon-borne measurements (SPIRALE, SAOZ and ground-based measurements (UV-VIS, FTIR. Time differences between the comparison measurements were reduced using either a tight coincidence criterion, or where possible, chemical box models. ACE-FTS NO2 and NO and the MAESTRO NO2 are generally consistent with the correlative data. The ACE-FTS and MAESTRO NO2 volume mixing ratio (VMR profiles agree with the profiles from other satellite data sets to within about 20% between 25 and 40 km, with the exception of MIPAS ESA (for ACE-FTS and SAGE II (for ACE-FTS (sunrise and MAESTRO and suggest a negative bias between 23 and 40 km of about 10%. MAESTRO reports larger VMR values than the ACE-FTS. In comparisons with HALOE, ACE-FTS NO VMRs typically (on average agree to ±8% from 22 to 64 km and to +10% from 93 to 105 km, with maxima of 21% and 36%, respectively. Partial column comparisons for NO2 show that there is quite good agreement between the ACE instruments and the FTIRs, with a mean difference of +7.3% for ACE-FTS and +12.8% for MAESTRO.

Inter-comparison of stratospheric O3 and NO2 abundances retrieved from balloon borne direct sun observations and Envisat/SCIAMACHY limb measurements

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A. Butz

2006-01-01

Full Text Available Stratospheric O3 and NO2 abundances measured by different remote sensing instruments are inter-compared: (1 Line-of-sight absorptions and vertical profiles inferred from solar spectra in the ultra-violet (UV, visible and infrared (IR wavelength ranges measured by the LPMA/DOAS (Limb Profile Monitor of the Atmosphere/Differential Optical Absorption Spectroscopy balloon payload during balloon ascent/descent and solar occultation are examined with respect to internal consistency. (2 The balloon borne stratospheric profiles of O3 and NO2 are compared to collocated space-borne skylight limb observations of the Envisat/SCIAMACHY satellite instrument. The trace gas profiles are retrieved from SCIAMACHY spectra using different algorithms developed at the Universities of Bremen and Heidelberg and at the Harvard-Smithsonian Center for Astrophysics. A comparison scheme is used that accounts for the spatial and temporal mismatch as well as differing photochemical conditions between the balloon and satellite borne measurements. It is found that the balloon borne measurements internally agree to within ±10% and ±20% for O3 and NO2, respectively, whereas the agreement with the satellite is ±20% for both gases in the 20 km to 30 km altitude range and in general worse below 20 km.

Comparison of GOME tropospheric NO2 columns with NO2 profiles deduced from ground-based in situ measurements

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D. Schaub

2006-01-01

Full Text Available Nitrogen dioxide (NO2 vertical tropospheric column densities (VTCs retrieved from the Global Ozone Monitoring Experiment (GOME are compared to coincident ground-based tropospheric NO2 columns. The ground-based columns are deduced from in situ measurements at different altitudes in the Alps for 1997 to June 2003, yielding a unique long-term comparison of GOME NO2 VTC data retrieved by a collaboration of KNMI (Royal Netherlands Meteorological Institute and BIRA/IASB (Belgian Institute for Space Aeronomy with independently derived tropospheric NO2 profiles. A first comparison relates the GOME retrieved tropospheric columns to the tropospheric columns obtained by integrating the ground-based NO2 measurements. For a second comparison, the tropospheric profiles constructed from the ground-based measurements are first multiplied with the averaging kernel (AK of the GOME retrieval. The second approach makes the comparison independent from the a priori NO2 profile used in the GOME retrieval. This allows splitting the total difference between the column data sets into two contributions: one that is due to differences between the a priori and the ground-based NO2 profile shapes, and another that can be attributed to uncertainties in both the remaining retrieval parameters (such as, e.g., surface albedo or aerosol concentration and the ground-based in situ NO2 profiles. For anticyclonic clear sky conditions the comparison indicates a good agreement between the columns (n=157, R=0.70/0.74 for the first/second comparison approach, respectively. The mean relative difference (with respect to the ground-based columns is −7% with a standard deviation of 40% and GOME on average slightly underestimating the ground-based columns. Both data sets show a similar seasonal behaviour with a distinct maximum of spring NO2 VTCs. Further analysis indicates small GOME columns being systematically smaller than the ground-based ones. The influence of different shapes in the a

A global single-sensor analysis of 2002-2011 tropospheric nitrogen dioxide trends observed from space

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Schneider, P.; van der A, R. J.

2012-08-01

A global nine-year archive of monthly tropospheric NO2 data acquired by the SCanning Imaging Absorption spectroMeter for Atmospheric CartograpHY (SCIAMACHY) instrument was analyzed with respect to trends between August 2002 and August 2011. In the past, similar studies relied on combining data from multiple sensors; however, the length of the SCIAMACHY data set now for the first time allows utilization of a consistent time series from just a single sensor for mapping NO2 trends at comparatively high horizontal resolution (0.25°). This study provides an updated analysis of global patterns in NO2 trends and finds that previously reported decreases in tropospheric NO2 over Europe and the United States as well as strong increases over China and several megacities in Asia have continued in recent years. Positive trends of up to 4.05 (±0.41) × 1015 molecules cm-2 yr-1 and up to 19.7 (±1.9) % yr-1 were found over China, with the regional mean trend being 7.3 (±3.1) % yr-1. The megacity with the most rapid relative increase was found to be Dhaka in Bangladesh. Subsequently focusing on Europe, the study further analyzes trends by country and finds significantly decreasing trends for seven countries ranging from -3.0 (±1.6) % yr-1 to -4.5 (±2.3) % yr-1. A comparison of the satellite data with station data indicates that the trends derived from both sources show substantial differences on the station scale, i.e., when comparing a station trend directly with the equivalent satellite-derived trend at the same location, but provide quite similar large-scale spatial patterns. Finally, the SCIAMACHY-derived NO2 trends are compared with equivalent trends in NO2concentration computed using the Co-operative Programme for Monitoring and Evaluation of the Long-range Transmission of Air Pollutants in Europe (EMEP) model. The results show that the spatial patterns in trends computed from both data sources mostly agree in Central and Western Europe, whereas substantial differences

Uncertainty in biogenic isoprene emissions and its impacts on tropospheric chemistry in East Asia.

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Han, K M; Park, R S; Kim, H K; Woo, J H; Kim, J; Song, C H

2013-10-01

In this study, the accuracy of biogenic isoprene emission fluxes over East Asia during two summer months (July and August) was examined by comparing two tropospheric HCHO columns (ΩHCHO) obtained from the SCIAMACHY sensor and the Community Multi-scale Air Quality (CMAQ v4.7.1) model simulations, using three available biogenic isoprene emission inventories over East Asia: i) GEIA, ii) MEGAN and iii) MOHYCAN. From this comparative analysis, the tropospheric HCHO columns from the CMAQ model simulations, using the MEGAN and MOHYCAN emission inventories (Ω(CMAQ, MEGAN) and Ω(CMAQ, MOHYCAN)), were found to agree well with the tropospheric HCHO columns from the SCIAMACHY observations (Ω(SCIA)). Secondly, the propagation of such uncertainties in the biogenic isoprene emission fluxes to the levels of atmospheric oxidants (e.g., OH and HO2) and other atmospheric gaseous/particulate species over East Asia during the two summer months was also investigated. As the biogenic isoprene emission fluxes decreased from the GEIA to the MEGAN emission inventories, the levels of OH radicals increased by factors of 1.39 and 1.75 over Central East China (CEC) and South China, respectively. Such increases in the OH radical mixing ratios subsequently influence the partitioning of HO(y) species. For example, the HO2/OH ratios from the CMAQ model simulations with GEIA isoprene emissions were 2.7 times larger than those from the CMAQ model simulations based on MEGAN isoprene emissions. The large HO2/OH ratios from the CMAQ model simulations with the GEIA biogenic emission were possibly due to the overestimation of GEIA biogenic isoprene emissions over East Asia. It was also shown that such large changes in HO(x) radicals created large differences on other tropospheric compounds (e.g., NO(y) chemistry) over East Asia during the summer months. Copyright © 2013 The Authors. Published by Elsevier B.V. All rights reserved.

A New Retrieval Algorithm for OMI NO2: Tropospheric Results and Comparisons with Measurements and Models

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Swartz, W. H.; Bucesla, E. J.; Lamsal, L. N.; Celarier, E. A.; Krotkov, N. A.; Bhartia, P, K,; Strahan, S. E.; Gleason, J. F.; Herman, J.; Pickering, K.

2012-01-01

Nitrogen oxides (NOx =NO+NO2) are important atmospheric trace constituents that impact tropospheric air pollution chemistry and air quality. We have developed a new NASA algorithm for the retrieval of stratospheric and tropospheric NO2 vertical column densities using measurements from the nadir-viewing Ozone Monitoring Instrument (OMI) on NASA's Aura satellite. The new products rely on an improved approach to stratospheric NO2 column estimation and stratosphere-troposphere separation and a new monthly NO2 climatology based on the NASA Global Modeling Initiative chemistry-transport model. The retrieval does not rely on daily model profiles, minimizing the influence of a priori information. We evaluate the retrieved tropospheric NO2 columns using surface in situ (e.g., AQS/EPA), ground-based (e.g., DOAS), and airborne measurements (e.g., DISCOVER-AQ). The new, improved OMI tropospheric NO2 product is available at high spatial resolution for the years 200S-present. We believe that this product is valuable for the evaluation of chemistry-transport models, examining the spatial and temporal patterns of NOx emissions, constraining top-down NOx inventories, and for the estimation of NOx lifetimes.

Synergetic cloud fraction determination for SCIAMACHY using MERIS

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C. Schlundt

2011-02-01

Full Text Available Since clouds play an essential role in the Earth's climate system, it is important to understand the cloud characteristics as well as their distribution on a global scale using satellite observations. The main scientific objective of SCIAMACHY (SCanning Imaging Absorption spectroMeter for Atmospheric CHartographY onboard the ENVISAT satellite is the retrieval of vertical columns of trace gases.

On the one hand, SCIAMACHY has to be sensitive to low variations in trace gas concentrations which means the ground pixel size has to be large enough. On the other hand, such a large pixel size leads to the problem that SCIAMACHY spectra are often contaminated by clouds. SCIAMACHY spectral measurements are not well suitable to derive a reliable sub-pixel cloud fraction that can be used as input parameter for subsequent retrievals of cloud properties or vertical trace gas columns. Therefore, we use MERIS/ENVISAT spectral measurements with its high spatial resolution as sub-pixel information for the determination of MerIs Cloud fRation fOr Sciamachy (MICROS. Since MERIS covers an even broader swath width than SCIAMACHY, no problems in spatial and temporal collocation of measurements occur. This enables the derivation of a SCIAMACHY cloud fraction with an accuracy much higher as compared with other current cloud fractions that are based on SCIAMACHY's PMD (Polarization Measurement Device data.

We present our new developed MICROS algorithm, based on the threshold approach, as well as a qualitative validation of our results with MERIS satellite images for different locations, especially with respect to bright surfaces such as snow/ice and sands. In addition, the SCIAMACHY cloud fractions derived from MICROS are intercompared with other current SCIAMACHY cloud fractions based on different approaches demonstrating a considerable improvement regarding geometric cloud fraction determination using the MICROS algorithm.

Uncertainty in biogenic isoprene emissions and its impacts on tropospheric chemistry in East Asia

International Nuclear Information System (INIS)

Han, K.M.; Park, R.S.; Kim, H.K.; Woo, J.H.; Kim, J.; Song, C.H.

2013-01-01

In this study, the accuracy of biogenic isoprene emission fluxes over East Asia during two summer months (July and August) was examined by comparing two tropospheric HCHO columns (Ω HCHO ) obtained from the SCIAMACHY sensor and the Community Multi-scale Air Quality (CMAQ v4.7.1) model simulations, using three available biogenic isoprene emission inventories over East Asia: i) GEIA, ii) MEGAN and iii) MOHYCAN. From this comparative analysis, the tropospheric HCHO columns from the CMAQ model simulations, using the MEGAN and MOHYCAN emission inventories (Ω CMAQ, MEGAN and Ω CMAQ, MOHYCAN ), were found to agree well with the tropospheric HCHO columns from the SCIAMACHY observations (Ω SCIA ). Secondly, the propagation of such uncertainties in the biogenic isoprene emission fluxes to the levels of atmospheric oxidants (e.g., OH and HO 2 ) and other atmospheric gaseous/particulate species over East Asia during the two summer months was also investigated. As the biogenic isoprene emission fluxes decreased from the GEIA to the MEGAN emission inventories, the levels of OH radicals increased by factors of 1.39 and 1.75 over Central East China (CEC) and South China, respectively. Such increases in the OH radical mixing ratios subsequently influence the partitioning of HO y species. For example, the HO 2 /OH ratios from the CMAQ model simulations with GEIA isoprene emissions were 2.7 times larger than those from the CMAQ model simulations based on MEGAN isoprene emissions. The large HO 2 /OH ratios from the CMAQ model simulations with the GEIA biogenic emission were possibly due to the overestimation of GEIA biogenic isoprene emissions over East Asia. It was also shown that such large changes in HO x radicals created large differences on other tropospheric compounds (e.g., NO y chemistry) over East Asia during the summer months. - Highlights: • GEIA isoprene emissions were possibly overestimated over East Asia. • Using MEGAN or MOHYCAN emissions in CMAQ well captured

Overview of SCIAMACHY validation: 2002 2004

Science.gov (United States)

Piters, A. J. M.; Bramstedt, K.; Lambert, J.-C.; Kirchhoff, B.

2005-08-01

SCIAMACHY, on board Envisat, is now in operation for almost three years. This UV/visible/NIR spectrometer measures the solar irradiance, the earthshine radiance scattered at nadir and from the limb, and the attenuation of solar radiation by the atmosphere during sunrise and sunset, from 240 to 2380 nm and at moderate spectral resolution. Vertical columns and profiles of a variety of atmospheric constituents are inferred from the SCIAMACHY radiometric measurements by dedicated retrieval algorithms. With the support of ESA and several international partners, a methodical SCIAMACHY validation programme has been developed jointly by Germany, the Netherlands and Belgium (the three instrument providing countries) to face complex requirements in terms of measured species, altitude range, spatial and temporal scales, geophysical states and intended scientific applications. This summary paper describes the approach adopted to address those requirements. The actual validation of the operational SCIAMACHY processors established at DLR on behalf of ESA has been hampered by data distribution and processor problems. Since first data releases in summer 2002, operational processors were upgraded regularly and some data products - level-1b spectra, level-2 O3, NO2, BrO and clouds data - have improved significantly. Validation results summarised in this paper conclude that for limited periods and geographical domains they can already be used for atmospheric research. Nevertheless, remaining processor problems cause major errors preventing from scientific usability in other periods and domains. Untied to the constraints of operational processing, seven scientific institutes (BIRA-IASB, IFE, IUP-Heidelberg, KNMI, MPI, SAO and SRON) have developed their own retrieval algorithms and generated SCIAMACHY data products, together addressing nearly all targeted constituents. Most of the UV-visible data products (both columns and profiles) already have acceptable, if not excellent, quality

Comparison of the inversion algorithms applied to the ozone vertical profile retrieval from SCIAMACHY limb measurements

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A. Rozanov

2007-09-01

Full Text Available This paper is devoted to an intercomparison of ozone vertical profiles retrieved from the measurements of scattered solar radiation performed by the SCIAMACHY instrument in the limb viewing geometry. Three different inversion algorithms including the prototype of the operational Level 1 to 2 processor to be operated by the European Space Agency are considered. Unlike usual validation studies, this comparison removes the uncertainties arising when comparing measurements made by different instruments probing slightly different air masses and focuses on the uncertainties specific to the modeling-retrieval problem only. The intercomparison was performed for 5 selected orbits of SCIAMACHY showing a good overall agreement of the results in the middle stratosphere, whereas considerable discrepancies were identified in the lower stratosphere and upper troposphere altitude region. Additionally, comparisons with ground-based lidar measurements are shown for selected profiles demonstrating an overall correctness of the retrievals.

Spectrograph dedicated to measuring tropospheric trace gas constituents from space

NARCIS (Netherlands)

Vries, J. de; Laan, E.C.; Deutz, A.F.; Escudero-Sanz, I.; Bokhove, H.; Hoegee, J.; Aben, I.; Jongma, R.; Landgraf, J.; Hasekamp, O.P.; Houweling, S.; Weele, M. van; Oss, R. van; Oord, G. van den; Levelt, P.

2005-01-01

Several organizations in the Netherlands are cooperating to develop user requirements and instrument concepts in the line of SCIAMACHY and OMI but with an increased focus on measuring tropospheric constituents from space. The concepts use passive spectroscopy in dedicated wavelength sections in the

SCIAMACHY WFM-DOAS XCO2: reduction of scattering related errors

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R. Sussmann

2012-10-01

Full Text Available Global observations of column-averaged dry air mole fractions of carbon dioxide (CO2, denoted by XCO2 , retrieved from SCIAMACHY on-board ENVISAT can provide important and missing global information on the distribution and magnitude of regional CO2 surface fluxes. This application has challenging precision and accuracy requirements. In a previous publication (Heymann et al., 2012, it has been shown by analysing seven years of SCIAMACHY WFM-DOAS XCO2 (WFMDv2.1 that unaccounted thin cirrus clouds can result in significant errors. In order to enhance the quality of the SCIAMACHY XCO2 data product, we have developed a new version of the retrieval algorithm (WFMDv2.2, which is described in this manuscript. It is based on an improved cloud filtering and correction method using the 1.4 μm strong water vapour absorption and 0.76 μm O2-A bands. The new algorithm has been used to generate a SCIAMACHY XCO2 data set covering the years 2003–2009. The new XCO2 data set has been validated using ground-based observations from the Total Carbon Column Observing Network (TCCON. The validation shows a significant improvement of the new product (v2.2 in comparison to the previous product (v2.1. For example, the standard deviation of the difference to TCCON at Darwin, Australia, has been reduced from 4 ppm to 2 ppm. The monthly regional-scale scatter of the data (defined as the mean intra-monthly standard deviation of all quality filtered XCO2 retrievals within a radius of 350 km around various locations has also been reduced, typically by a factor of about 1.5. Overall, the validation of the new WFMDv2.2 XCO2 data product can be summarised by a single measurement precision of 3.8 ppm, an estimated regional-scale (radius of 500 km precision of monthly averages of 1.6 ppm and an estimated regional-scale relative accuracy of 0.8 ppm. In addition to the comparison with the limited number of TCCON sites, we also present a comparison with NOAA's global CO2 modelling

GOME-2A retrievals of tropospheric NO2 in different spectral ranges – influence of penetration depth

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L. K. Behrens

2018-05-01

Full Text Available In this study, we present a novel nitrogen dioxide (NO2 differential optical absorption spectroscopy (DOAS retrieval in the ultraviolet (UV spectral range for observations from the Global Ozone Monitoring Instrument 2 on board EUMETSAT's MetOp-A (GOME-2A satellite. We compare the results to those from an established NO2 retrieval in the visible (vis spectral range from the same instrument and investigate how differences between the two are linked to the NO2 vertical profile shape in the troposphere.As expected, radiative transfer calculations for satellite geometries show that the sensitivity close to the ground is higher in the vis than in the UV spectral range. Consequently, NO2 slant column densities (SCDs in the vis are usually higher than in the UV if the NO2 is close to the surface. Therefore, these differences in NO2 SCDs between the two spectral ranges contain information on the vertical distribution of NO2 in the troposphere. We combine these results with radiative transfer calculations and simulated NO2 fields from the TM5-MP chemistry transport model to evaluate the simulated NO2 vertical distribution.We investigate regions representative of both anthropogenic and biomass burning NO2 pollution. Anthropogenic air pollution is mostly located in the boundary layer close to the surface, which is reflected by large differences between UV and vis SCDs of  ∼  60 %. Biomass burning NO2 in contrast is often uplifted into elevated layers above the boundary layer. This is best seen in tropical Africa south of the Equator, where the biomass burning NO2 is well observed in the UV, and the SCD difference between the two spectral ranges is only  ∼  36 %. In tropical Africa north of the Equator, however, the biomass burning NO2 is located closer to the ground, reducing its visibility in the UV.While not enabling a full retrieval of the vertical NO2 profile shape in the troposphere, our results can help to constrain the vertical

Uncertainty in biogenic isoprene emissions and its impacts on tropospheric chemistry in East Asia

Energy Technology Data Exchange (ETDEWEB)

Han, K.M.; Park, R.S. [School of Environmental Science and Engineering, Gwangju Institute of Science and Technology (GIST), Gwangju, 500-712 (Korea, Republic of); Advanced Environmental Monitoring Research Center (ADEMRC), Gwangju Institute of Science and Technology (GIST), Gwangju, 500-712 (Korea, Republic of); Kim, H.K.; Woo, J.H. [Department of Advanced Technology Fusion, Konkuk University, 1 Hwayang dong, Gwangjin-gu, Seoul, 143-701 (Korea, Republic of); Kim, J. [Department of Atmospheric Sciences, Yonsei University, 134 Sinchon-dong, Seodaemoon-gu, Seoul, 120-749 (Korea, Republic of); Song, C.H., E-mail: chsong@gist.ac.kr [School of Environmental Science and Engineering, Gwangju Institute of Science and Technology (GIST), Gwangju, 500-712 (Korea, Republic of); Advanced Environmental Monitoring Research Center (ADEMRC), Gwangju Institute of Science and Technology (GIST), Gwangju, 500-712 (Korea, Republic of)

2013-10-01

In this study, the accuracy of biogenic isoprene emission fluxes over East Asia during two summer months (July and August) was examined by comparing two tropospheric HCHO columns (Ω{sub HCHO}) obtained from the SCIAMACHY sensor and the Community Multi-scale Air Quality (CMAQ v4.7.1) model simulations, using three available biogenic isoprene emission inventories over East Asia: i) GEIA, ii) MEGAN and iii) MOHYCAN. From this comparative analysis, the tropospheric HCHO columns from the CMAQ model simulations, using the MEGAN and MOHYCAN emission inventories (Ω{sub CMAQ,} {sub MEGAN} and Ω{sub CMAQ,} {sub MOHYCAN}), were found to agree well with the tropospheric HCHO columns from the SCIAMACHY observations (Ω{sub SCIA}). Secondly, the propagation of such uncertainties in the biogenic isoprene emission fluxes to the levels of atmospheric oxidants (e.g., OH and HO{sub 2}) and other atmospheric gaseous/particulate species over East Asia during the two summer months was also investigated. As the biogenic isoprene emission fluxes decreased from the GEIA to the MEGAN emission inventories, the levels of OH radicals increased by factors of 1.39 and 1.75 over Central East China (CEC) and South China, respectively. Such increases in the OH radical mixing ratios subsequently influence the partitioning of HO{sub y} species. For example, the HO{sub 2}/OH ratios from the CMAQ model simulations with GEIA isoprene emissions were 2.7 times larger than those from the CMAQ model simulations based on MEGAN isoprene emissions. The large HO{sub 2}/OH ratios from the CMAQ model simulations with the GEIA biogenic emission were possibly due to the overestimation of GEIA biogenic isoprene emissions over East Asia. It was also shown that such large changes in HO{sub x} radicals created large differences on other tropospheric compounds (e.g., NO{sub y} chemistry) over East Asia during the summer months. - Highlights: • GEIA isoprene emissions were possibly overestimated over East Asia. �

The role of chemistry in under-predictions of NO2 in the upper troposphere

Science.gov (United States)

Henderson, B. H.; Pinder, R. W.; Goliff, W. S.; Stockwell, W. R.; Fahr, A.; Sarwar, G.; Hutzell, W. T.; Mathur, R.; Vizuete, W.; Cohen, R. C.

2009-12-01

Global and regional atmospheric models under-predict upper troposphere NO2 compared to satellite and aircraft observations. The upper tropospheric under-prediction of NO2 could be a function of emissions, transport, chemistry or some combination. Previous researchers have linked poor performance in the model to over-prediction of the OH and under-prediction of the HO2 by chemistry (Olson et al. 2006, Bertram et al. 2007). This study isolates upper tropospheric chemistry to evaluate the chemical contribution to NO2 under-predictions and to diagnose OH and HO2 discrepancies. We use a 0-dimensional time dependent model to evaluate seven chemical mechanisms. Because chamber data representing upper tropospheric conditions does not exist, we evaluate the predictions based against an observation-based aging model. Following Bertram et al (2007), we use the NOx:HNO3 ratio to categorize the chemical age of thousands of 10 second average observations between 8 and 10km. Measurements of 10 inorganics and 32 hydrocarbons are translated to model species for each of seven chemical mechanisms. We chose mechanisms ranging from condensed to semi-explicit. The seven mechanisms' design scopes range from urban to global scale. Results include simulations from Model for OZone And Related chemical Tracers (MOZART), Carbon Bond 05 (CB05), State Air Pollution Research Center (SAPRC) 99, SAPRC 07, GEOS-Chem, Regional Atmospheric Chemical Mechanism version 2, and the LEEDS Master Chemical Mechanism. Results from each chemical mechanism are compared to aircraft observations and to those obtained with other chemical mechanisms. Each mechanism is then further evaluated using integrated reaction rate analysis to identify sources of NO2 bias. We find that the largest contributors to the NO2 bias are over-predictions of PAN and HNO3. The formation of PAN is sensitive to the acetone photolysis rate. The conversion of NOx to HNO3 is most sensitive to hydroxyl radical concentrations. Hydroxyl

A large-scale intercomparison of stratospheric vertical distributions of NO2 and BrO retrieved from the SCIAMACHY limb measurements and ground-based twilight observations

Science.gov (United States)

Rozanov, Alexei; Hendrick, Francois; Lotz, Wolfhardt; van Roozendael, Michel; Bovensmann, Heinrich; Burrows, John P.

This study is devoted to the intercomparison of NO2 and BrO vertical profiles obtained from the satellite and ground-based measurements. Although, the ground-based observations are performed only at selected locations, they have a great potential to be used for the validation of satellite measurements since continuous long-term measurement series performed with the same instruments are available. Thus, long-term trends in the observed species can be analyzed and intercompared. Previous intercomparisons of the vertical distributions of NO2 and BrO retrieved from SCIAMACHY limb measurements at the University of Bremen and obtained at IASB-BIRA by applying a profiling technique to ground-based zenith-sky DOAS observations have shown a good agreement between the results of completely different measurement techniques. However, only a relatively short time period of one year was analyzed so far which do not allow investigating seasonal variations and trends. Furthermore, some minor discrepancies are still to be analyzed. In the current study, several years datasets obtained at Observatoire de Haute-Provence (OHP) in France and in Harestua in Norway will be compared to the retrievals of SCIAMACHY limb measurements. Seasonal and annual variations will be analyzed and possible reasons for the remaining discrepancies will be discussed.

Atmospheric methane and carbon dioxide from SCIAMACHY satellite data: initial comparison with chemistry and transport models

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M. Buchwitz

2005-01-01

Full Text Available The remote sensing of the atmospheric greenhouse gases methane (CH4 and carbon dioxide (CO2 in the troposphere from instrumentation aboard satellites is a new area of research. In this manuscript, results obtained from observations of the up-welling radiation in the near-infrared by SCIAMACHY on board ENVISAT are presented. Vertical columns of CH4, CO2 and oxygen (O2 have been retrieved and the (air or O2-normalised CH4 and CO2 column amounts, the dry air column averaged mixing ratios XCH4 and XCO2 derived. In this manuscript the first results, obtained by using the version 0.4 of the Weighting Function Modified (WFM DOAS retrieval algorithm applied to SCIAMACHY data, are described and compared with global models. For the set of individual cloud free measurements over land the standard deviation of the difference with respect to the models is in the range ~100–200 ppbv (5–10% for XCH4 and ~14–32 ppmv (4–9% for XCO2. The inter-hemispheric difference of the methane mixing ratio, as determined from single day data, is in the range 30–110 ppbv and in reasonable agreement with the corresponding model data (48–71 ppbv. The weak inter-hemispheric difference of the CO2 mixing ratio can also be detected with single day data. The spatiotemporal pattern of the measured and the modelled XCO2 are in reasonable agreement. However, the amplitude of the difference between the maximum and the minimum for SCIAMACHY XCO2 is about ±20 ppmv which is about a factor of four larger than the variability of the model data which is about ±5 ppmv. More studies are needed to explain the observed differences. The XCO2 model field shows low CO2 concentrations beginning of January 2003 over a spatially extended CO2 sink region located in southern tropical/sub-tropical Africa. The SCIAMACHY data also show low CO2 mixing ratios over this area. According to the model the sink region becomes a source region about six months later and exhibits higher mixing ratios

Retrieval of tropospheric NO2 using the MAX-DOAS method combined with relative intensity measurements for aerosol correction

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P. F. Levelt

2010-10-01

Full Text Available Multi-Axis Differential Optical Absorption Spectroscopy (MAX-DOAS is a technique to measure trace gas amounts in the lower troposphere from ground-based scattered sunlight observations. MAX-DOAS observations are especially suitable for validation of tropospheric trace gas observations from satellite, since they have a representative range of several kilometers, both in the horizontal and in the vertical dimension. A two-step retrieval scheme is presented here, to derive aerosol corrected tropospheric NO2 columns from MAX-DOAS observations. In a first step, boundary layer aerosols, characterized in terms of aerosol optical thickness (AOT, are estimated from relative intensity observations, which are defined as the ratio of the sky radiance at elevation α and the sky radiance in the zenith. Relative intensity measurements have the advantage of a strong dependence on boundary layer AOT and almost no dependence on boundary layer height. In a second step, tropospheric NO2 columns are derived from differential slant columns, based on AOT-dependent air mass factors. This two-step retrieval scheme was applied to cloud free periods in a twelve month data set of observations in De Bilt, The Netherlands. In a comparison with AERONET (Cabauw site a mean difference in AOT (AERONET minus MAX-DOAS of −0.01±0.08 was found, and a correlation of 0.85. Tropospheric-NO2 columns were compared with OMI-satellite tropospheric NO2. For ground-based observations restricted to uncertainties below 10%, no significant difference was found, and a correlation of 0.88.

Trends of tropospheric NO2 over the Yangtze River Delta region and the possible linkage to rapid urbanization

Science.gov (United States)

Ma, Mingliang; Zhang, Deying; Liu, Qiyang; Song, Yue; Zhou, Jiayuan; Shi, Runhe; Gao, Wei

2017-09-01

Over the past decade, China has experienced a rapid increase in urbanization. The urban built-up areas (population) of Shanghai increased by 16.1% (22.9%) from 2006 to 2015. This study aims to analyze the variations of tropospheric NO2 over Yangtze River Delta region and the impacts of rapid urbanization during 2006-2015. The results indicate that tropospheric NO2 vertical column density (VCD) of all cities in the study area showed an increasing trend during 2006-2011 whereas a decreasing trend during 2011-2015. Most cities showed a lower tropospheric NO2 VCD value in 2015 compared to that in 2006, except for Changzhou and Nantong. Shanghai and Ningbo are two hotspots where the tropospheric NO2 VCD decreased most significantly, at a rate of 22% and 19%, respectively. This effect could be ascribed to the implementation of harsh emission control policies therein. Similar seasonal variability was observed over all cities, with larger values observed in the summer and smaller values shown in the winter. Further investigations show that the observed increasing trend of tropospheric NO2 during 2006-2011 could be largely explained by rapid urbanization linked to car ownership, GDP, power consumption, population and total industrial output. Such effect was not prominent after 2011, mainly due to the implementation of emission control strategies.

Exploring mechanisms of a tropospheric archetype: CH{sub 3}O{sub 2} + NO

Energy Technology Data Exchange (ETDEWEB)

Launder, Andrew M.; Agarwal, Jay; Schaefer, Henry F., E-mail: ccq@uga.edu [Center for Computational Quantum Chemistry, University of Georgia, Athens, Georgia 30602 (United States)

2015-12-21

Methylperoxy radical (CH{sub 3}O{sub 2}) and nitric oxide (NO) contribute to the propagation of photochemical smog in the troposphere via the production of methoxy radical (CH{sub 3}O) and nitrogen dioxide (NO{sub 2}). This reaction system also furnishes trace quantities of methyl nitrate (CH{sub 3}ONO{sub 2}), a sink for reactive NO{sub x} species. Here, the CH{sub 3}O{sub 2} + NO reaction is examined with highly reliable coupled-cluster methods. Specifically, equilibrium geometries for the reactants, products, intermediates, and transition states of the ground-state potential energy surface are characterized. Relative reaction enthalpies at 0 K (ΔH{sub 0K}) are reported; these values are comprised of electronic energies extrapolated to the complete basis set limit of CCSDT(Q) and zero-point vibrational energies computed at CCSD(T)/cc-pVTZ. A two-part mechanism involving CH{sub 3}O and NO{sub 2} production followed by radical recombination to CH{sub 3}ONO{sub 2} is determined to be the primary channel for formation of CH{sub 3}ONO{sub 2} under tropospheric conditions. Constrained optimizations of the reaction paths at CCSD(T)/cc-pVTZ suggest that the homolytic bond dissociations involved in this reaction path are barrierless.

Top-down NOX Emissions of European Cities Derived from Modelled and Spaceborne Tropospheric NO2 Columns

Science.gov (United States)

Verstraeten, W. W.; Boersma, K. F.; Douros, J.; Williams, J. E.; Eskes, H.; Delcloo, A. W.

2017-12-01

High nitrogen oxides (NOX = NO + NO2) concentrations near the surface impact humans and ecosystems badly and play a key role in tropospheric chemistry. NO2 is an important precursor of tropospheric ozone (O3) which in turn affects the production of the hydroxyl radical controlling the chemical lifetime of key atmospheric pollutants and reactive greenhouse gases. Combustion from industrial, traffic and household activities in large and densely populated urban areas result in high NOX emissions. Accurate mapping of these emissions is essential but hard to do since reported emissions factors may differ from real-time emissions in order of magnitude. Modelled NO2 levels and lifetimes also have large associated uncertainties and overestimation in the chemical lifetime which may mask missing NOX chemistry in current chemistry transport models (CTM's). The simultaneously estimation of both the NO2 lifetime and as well as the concentrations by applying the Exponentially Modified Gaussian (EMG) method on tropospheric NO2 columns lines densities should improve the surface NOX emission estimates. Here we evaluate if the EMG methodology applied on the tropospheric NO2 columns simulated by the LOTOS-EUROS (Long Term Ozone Simulation-European Ozone Simulation) CTM can reproduce the NOX emissions used as model input. First we process both the modelled tropospheric NO2 columns for the period April-September 2013 for 21 selected European urban areas under windy conditions (averaged vertical wind speeds between surface and 500 m from ECMWF > 2 m s-1) as well as the accompanying OMI (Ozone Monitoring Instrument) data providing us with real-time observation-based estimates of midday NO2 columns. Then we compare the top-down derived surface NOX emissions with the 2011 MACC-III emission inventory, used in the CTM as input to simulate the NO2 columns. For cities where NOX emissions can be assumed as originating from one large source good agreement is found between the top-down derived

Estimates of Free-tropospheric NO2 Abundance from the Aura Ozone Monitoring Instrument (OMI) Using Cloud Slicing Technique

Science.gov (United States)

Choi, S.; Joiner, J.; Krotkov, N. A.; Choi, Y.; Duncan, B. N.; Celarier, E. A.; Bucsela, E. J.; Vasilkov, A. P.; Strahan, S. E.; Veefkind, J. P.; Cohen, R. C.; Weinheimer, A. J.; Pickering, K. E.

2013-12-01

Total column measurements of NO2 from space-based sensors are of interest to the atmospheric chemistry and air quality communities; the relatively short lifetime of near-surface NO2 produces satellite-observed hot-spots near pollution sources including power plants and urban areas. However, estimates of NO2 concentrations in the free-troposphere, where lifetimes are longer and the radiative impact through ozone formation is larger, are severely lacking. Such information is critical to evaluate chemistry-climate and air quality models that are used for prediction of the evolution of tropospheric ozone and its impact of climate and air quality. Here, we retrieve free-tropospheric NO2 volume mixing ratio (VMR) using the cloud slicing technique. We use cloud optical centroid pressures (OCPs) as well as collocated above-cloud vertical NO2 columns (defined as the NO2 column from top of the atmosphere to the cloud OCP) from the Ozone Monitoring Instrument (OMI). The above-cloud NO2 vertical columns used in our study are retrieved independent of a priori NO2 profile information. In the cloud-slicing approach, the slope of the above-cloud NO2 column versus the cloud optical centroid pressure is proportional to the NO2 volume mixing ratio (VMR) for a given pressure (altitude) range. We retrieve NO2 volume mixing ratios and compare the obtained NO2 VMRs with in-situ aircraft profiles measured during the NASA Intercontinental Chemical Transport Experiment Phase B (INTEX-B) campaign in 2006. The agreement is good when proper data screening is applied. In addition, the OMI cloud slicing reports a high NO2 VMR where the aircraft reported lightning NOx during the Deep Convection Clouds and Chemistry (DC3) campaign in 2012. We also provide a global seasonal climatology of free-tropospheric NO2 VMR in cloudy conditions. Enhanced NO2 in free troposphere commonly appears near polluted urban locations where NO2 produced in the boundary layer may be transported vertically out of the

Ship-based MAX-DOAS measurements of tropospheric NO2, SO2, and HCHO distribution along the Yangtze River

Science.gov (United States)

Hong, Qianqian; Liu, Cheng; Chan, Ka Lok; Hu, Qihou; Xie, Zhouqing; Liu, Haoran; Si, Fuqi; Liu, Jianguo

2018-04-01

In this paper, we present ship-based Multi-Axis Differential Optical Absorption Spectroscopy (MAX-DOAS) measurements of tropospheric trace gases' distribution along the Yangtze River during winter 2015. The measurements were performed along the Yangtze River between Shanghai and Wuhan, covering major industrial areas in eastern China. Tropospheric vertical column densities (VCDs) of nitrogen dioxide (NO2), sulfur dioxide (SO2), and formaldehyde (HCHO) were retrieved using the air mass factor calculated by the radiative transfer model. Enhanced tropospheric NO2 and SO2 VCDs were detected over downwind areas of industrial zones over the Yangtze River. In addition, spatial distributions of atmospheric pollutants are strongly affected by meteorological conditions; i.e., positive correlations were found between concentration of pollutants and wind speed over these areas, indicating strong influence of transportation of pollutants from high-emission upwind areas along the Yangtze River. Comparison of tropospheric NO2 VCDs between ship-based MAX-DOAS and Ozone Monitoring Instrument (OMI) satellite observations shows good agreement with each other, with a Pearson correlation coefficient (R) of 0.82. In this study, the NO2 / SO2 ratio was used to estimate the relative contributions of industrial sources and vehicle emissions to ambient NO2 levels. Analysis results of the NO2 / SO2 ratio show a higher contribution of industrial NO2 emissions in Jiangsu Province, while NO2 levels in Jiangxi and Hubei provinces are mainly related to vehicle emissions. These results indicate that different pollution control strategies should be applied in different provinces. In addition, multiple linear regression analysis of ambient carbon monoxide (CO) and odd oxygen (Ox) indicated that the primary emission and secondary formation of HCHO contribute 54.4 ± 3.7 % and 39.3 ± 4.3 % to the ambient HCHO, respectively. The largest contribution from primary emissions in winter suggested that

CO emission and export from Asia: an analysis combining complementary satellite measurements (MOPITT, SCIAMACHY and ACE-FTS with global modeling

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P. F. Bernath

2008-09-01

Full Text Available This study presents the complementary picture of the pollution outflow provided by several satellite observations of carbon monoxide (CO, based on different observation techniques. This is illustrated by an analysis of the Asian outflow during the spring of 2005, through comparisons with simulations by the LMDz-INCA global chemistry transport model. The CO observations from the MOPITT and SCIAMACHY nadir sounders, which provide vertically integrated information with excellent horizontal sampling, and from the ACE-FTS solar occultation instrument, which has limited spatial coverage but allows the retrieval of vertical profiles, are used. Combining observations from MOPITT (mainly sensitive to the free troposphere and SCIAMACHY (sensitive to the full column allows a qualitative evaluation of the boundary layer CO. The model tends to underestimate this residual compared to the observations, suggesting underestimated emissions, especially in eastern Asia. However, a better understanding of the consistency and possible biases between the MOPITT and SCIAMACHY CO is necessary for a quantitative evaluation. Underestimated emissions, and possibly too low lofting and underestimated chemical production in the model, lead to an underestimate of the export to the free troposphere, as highlighted by comparisons with MOPITT and ACE-FTS. Both instruments observe large trans-Pacific transport extending from ~20° N to ~60° N, with high upper tropospheric CO observed by ACE-FTS above the eastern Pacific (with values of up to 300 ppbv around 50° N at 500 hPa and up to ~200 ppbv around 30° N at 300 hPa. The low vertical and horizontal resolutions of the global model do not allow the simulation of the strong enhancements in the observed plumes. However, the transport patterns are well captured, and are mainly attributed to export from eastern Asia, with increasing contributions from South Asia and Indonesia towards the tropics. Additional measurements of C₂

SCIAMACHY WFM-DOAS XCO2: comparison with CarbonTracker XCO2 focusing on aerosols and thin clouds

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J. P. Burrows

2012-08-01

Full Text Available Carbon dioxide (CO2 is the most important greenhouse gas whose atmospheric loading has been significantly increased by anthropogenic activity leading to global warming. Accurate measurements and models are needed in order to reliably predict our future climate. This, however, has challenging requirements. Errors in measurements and models need to be identified and minimised. In this context, we present a comparison between satellite-derived column-averaged dry air mole fractions of CO2, denoted XCO2, retrieved from SCIAMACHY/ENVISAT using the WFM-DOAS (weighting function modified differential optical absorption spectroscopy algorithm, and output from NOAA's global CO2 modelling and assimilation system CarbonTracker. We investigate to what extent differences between these two data sets are influenced by systematic retrieval errors due to aerosols and unaccounted clouds. We analyse seven years of SCIAMACHY WFM-DOAS version 2.1 retrievals (WFMDv2.1 using CarbonTracker version 2010. We investigate to what extent the difference between SCIAMACHY and CarbonTracker XCO2 are temporally and spatially correlated with global aerosol and cloud data sets. For this purpose, we use a global aerosol data set generated within the European GEMS project, which is based on assimilated MODIS satellite data. For clouds, we use a data set derived from CALIOP/CALIPSO. We find significant correlations of the SCIAMACHY minus CarbonTracker XCO2 difference with thin clouds over the Southern Hemisphere. The maximum temporal correlation we find for Darwin, Australia (r2 = 54%. Large temporal correlations with thin clouds are also observed over other regions of the Southern Hemisphere (e.g. 43% for South America and 31% for South Africa. Over the Northern Hemisphere the temporal correlations are typically much lower. An exception is India, where large temporal correlations with clouds and aerosols have also been found. For all other regions the temporal correlations with

Geophysical validation of SCIAMACHY Limb Ozone Profiles

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E. J. Brinksma

2006-01-01

Full Text Available We discuss the quality of the two available SCIAMACHY limb ozone profile products. They were retrieved with the University of Bremen IFE's algorithm version 1.61 (hereafter IFE, and the official ESA offline algorithm (hereafter OL versions 2.4 and 2.5. The ozone profiles were compared to a suite of correlative measurements from ground-based lidar and microwave, sondes, SAGE II and SAGE III (Stratospheric Aerosol and Gas Experiment. To correct for the expected Envisat pointing errors, which have not been corrected implicitly in either of the algorithms, we applied a constant altitude shift of -1.5 km to the SCIAMACHY ozone profiles. The IFE ozone profile data between 16 and 40 km are biased low by 3-6%. The average difference profiles have a typical standard deviation of 10% between 20 and 35 km. We show that more than 20% of the SCIAMACHY official ESA offline (OL ozone profiles version 2.4 and 2.5 have unrealistic ozone values, most of these are north of 15° S. The remaining OL profiles compare well to correlative instruments above 24 km. Between 20 and 24 km, they underestimate ozone by 15±5%.

Rapid economic growth leads to boost in NO2 pollution over India, as seen from space

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Hilboll, Andreas; Richter, Andreas; Burrows, John P.

2016-04-01

Over the past decades, the Indian economy has been growing at an exceptional pace. This growth was induced and accompanied by a strong increase of the Indian population. Consequently, traffic, electricity consumption, and industrial production have soared over the past decades, leading to a strong increase in fuel consumption and thus pollutant emissions. Nitrogen oxides (NO+NO2) are a major component of anthropogenic air pollution, playing key part in reaction cycles leading to the formation of tropospheric ozone. They are mainly emitted by the combustion of fossil fuels; other sources include production by lightning, biomass burning, and microbial activity in soils. Since the mid-1990s, space-borne measurements of tropospheric nitrogen dioxide (NO2) have been conducted by the GOME, SCIAMACHY, GOME-2, and OMI instruments. These instruments perform hyperspectral measurements of scattered and reflected sunlight. Their measurements are then analyzed using differential optical absorption spectroscopy (DOAS) to yield vertically integrated columnar trace gas abundances. Here, we will present the results of 20 years of NO2 measurements over the Indian subcontinent. After showing the spatial distribution of NO2 pollution over India, we will present time series for individual states and urban agglomerations. These time series will then be related to various indicators of economic development. Finally, we will highlight several instances where single industrial pollution sources and their development can clearly be identified from the NO2 maps and estimate their NO2 emissions.

Improved water vapour spectroscopy in the 4174–4300 cm−1 region and its impact on SCIAMACHY HDO/H2O measurements

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R. A. Scheepmaker

2013-04-01

Full Text Available The relative abundance of the heavy water isotopologue HDO provides a deeper insight into the atmospheric hydrological cycle. The SCanning Imaging Absorption spectroMeter for Atmospheric CartograpHY (SCIAMACHY allows for global retrievals of the ratio HDO/H2O in the 2.3 micron wavelength range. However, the spectroscopy of water lines in this region remains a large source of uncertainty for these retrievals. We therefore evaluate and improve the water spectroscopy in the range 4174–4300 cm−1 and test if this reduces systematic uncertainties in the SCIAMACHY retrievals of HDO/H2O. We use a laboratory spectrum of water vapour to fit line intensity, air broadening and wavelength shift parameters. The improved spectroscopy is tested on a series of ground-based high resolution FTS spectra as well as on SCIAMACHY retrievals of H2O and the ratio HDO/H2O. We find that the improved spectroscopy leads to lower residuals in the FTS spectra compared to HITRAN 2008 and Jenouvrier et al. (2007 spectroscopy, and the retrievals become more robust against changes in the retrieval window. For both the FTS and SCIAMACHY measurements, the retrieved total H2O columns decrease by 2–4% and we find a negative shift of the HDO/H2O ratio, which for SCIAMACHY is partly compensated by changes in the retrieval setup and calibration software. The updated SCIAMACHY HDO/H2O product shows somewhat steeper latitudinal and temporal gradients and a steeper Rayleigh distillation curve, strengthening previous conclusions that current isotope-enabled general circulation models underestimate the variability in the near-surface HDO/H2O ratio.

SO2 Emissions and Lifetimes: Estimates from Inverse Modeling Using In Situ and Global, Space-Based (SCIAMACHY and OMI) Observations

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Lee, Chulkyu; Martin Randall V.; vanDonkelaar, Aaron; Lee, Hanlim; Dickerson, RUssell R.; Hains, Jennifer C.; Krotkov, Nickolay; Richter, Andreas; Vinnikov, Konstantine; Schwab, James J.

2011-01-01

Top-down constraints on global sulfur dioxide (SO2) emissions are inferred through inverse modeling using SO2 column observations from two satellite instruments (SCIAMACHY and OMI). We first evaluated the S02 column observations with surface SO2 measurements by applying local scaling factors from a global chemical transport model (GEOS-Chem) to SO2 columns retrieved from the satellite instruments. The resulting annual mean surface SO2 mixing ratios for 2006 exhibit a significant spatial correlation (r=0.86, slope=0.91 for SCIAMACHY and r=0.80, slope = 0.79 for OMI) with coincident in situ measurements from monitoring networks throughout the United States and Canada. We evaluate the GEOS-Chem simulation of the SO2 lifetime with that inferred from in situ measurements to verity the applicability of GEOS-Chem for inversion of SO2 columns to emissions. The seasonal mean SO2 lifetime calculated with the GEOS-Chem model over the eastern United States is 13 h in summer and 48 h in winter, compared to lifetimes inferred from in situ measurements of 19 +/- 7 h in summer and 58 +/- 20 h in winter. We apply SO2 columns from SCIAMACHY and OMI to derive a top-down anthropogenic SO2 emission inventory over land by using the local GEOS-Chem relationship between SO2 columns and emissions. There is little seasonal variation in the top-down emissions (SO2 emissions (52.4 Tg S/yr from SCIAMACHY and 49.9 Tg S / yr from OMI) closely agrees with the bottom-up emissions (54.6 Tg S/yr) in the GEOS-Chem model and exhibits consistency in global distributions with the bottom-up emissions (r = 0.78 for SCIAMACHY, and r = 0.77 for OMI). However, there are significant regional differences.

Application of OMI tropospheric NO2 for air quality monitoring in Northern Europe: shipping and land-based case studies

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Ialongo, Iolanda; Hakkarainen, Janne; Jalkanen, Jukka-Pekka; Johansson, Lasse; Boersma, Folkert; Krotkov, Nickolay; Tamminen, Johanna

2014-05-01

Satellite-based data are very important for air quality applications in the Baltic Sea area, because they provide information on air pollution over sea and there where ground-based network and aircraft measurements are not available. Both the emissions from urban sites over land and ships over sea, contribute to the tropospheric NO2 levels. The tropospheric NO2 monitoring at high latitudes using satellite data is challenging because of the reduced light hours in winter and the snow-covered surface, which make the retrieval complex, and because of the reduced signal due to low Sun. This work presents a detailed characterization of the tropospheric NO2 columns focused on part of the Baltic Sea region using the Ozone Monitoring Instrument (OMI) tropospheric NO2 standard product. Previous works have focused on larger seas and lower latitudes. The results showed that, despite the regional area of interest, it is possible to distinguish the signal from the main coastal cities and from the ships by averaging the data over a seasonal time range. The summertime NO2 emission and lifetime values (E = (1.0 ± 0.1)x1028 molec. and τ = (3.0 ± 0.5) h, respectively) in Helsinki were estimated from the decay of the signal with distance from the city center. The method developed for megacities was successfully applied to a smaller scale source, in both size and intensity (i.e., the city of Helsinki), which is located at high latitudes (~ 60oN). The same methodology could be applied to similar scale cities elsewhere, as far as they are relatively isolated from other sources. The transport by the wind plays an important role in the Baltic Sea area. The NO2 spatial distribution is mainly determined by the contribution of strong westerly winds, which dominate the wind patterns during summer. The comparison between the emissions from model calculations and OMI NO2 tropospheric columns confirmed the applicability of satellite data for ship emission monitoring. In particular, both the

The ESA GOME-Evolution "Climate" water vapor product: a homogenized time series of H2O columns from GOME, SCIAMACHY, and GOME-2

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Beirle, Steffen; Lampel, Johannes; Wang, Yang; Mies, Kornelia; Dörner, Steffen; Grossi, Margherita; Loyola, Diego; Dehn, Angelika; Danielczok, Anja; Schröder, Marc; Wagner, Thomas

2018-03-01

We present time series of the global distribution of water vapor columns over more than 2 decades based on measurements from the satellite instruments GOME, SCIAMACHY, and GOME-2 in the red spectral range. A particular focus is the consistency amongst the different sensors to avoid jumps from one instrument to another. This is reached by applying robust and simple retrieval settings consistently. Potentially systematic effects due to differences in ground pixel size are avoided by merging SCIAMACHY and GOME-2 observations to GOME spatial resolution, which also allows for a consistent treatment of cloud effects. In addition, the GOME-2 swath is reduced to that of GOME and SCIAMACHY to have consistent viewing geometries.Remaining systematic differences between the different sensors are investigated during overlap periods and are corrected for in the homogenized time series. The resulting Climate product v2.2 (https://doi.org/10.1594/WDCC/GOME-EVL_water_vapor_clim_v2.2" target="_blank">https://doi.org/10.1594/WDCC/GOME-EVL_water_vapor_clim_v2.2) allows the study of the temporal evolution of water vapor over the last 20 years on a global scale.

Comparison of stratospheric NO2 profiles above Kiruna, Sweden retrieved from ground-based zenith sky DOAS measurements, SAOZ balloon measurements and SCIAMACHY limb observations

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Gu, Myojeong; Enell, Carl-Fredrik; Hendrick, François; Pukite, Janis; Van Roozendael, Michel; Platt, Ulrich; Raffalski, Uwe; Wagner, Thomas

2015-04-01

Stratospheric NO2 not only destroys ozone but acts as a buffer against halogen catalyzed ozone loss by converting halogen species into stable nitrates. These two roles of stratospheric NO2 depend on the altitude. Hence, the objective of this study is to investigate the vertical distribution of stratospheric NO2. We compare the NO2 profiles derived from the zenith sky DOAS with those obtained from, SAOZ balloon measurements and satellite limb observations. Vertical profiles of stratospheric NO2 are retrieved from ground-based zenith sky DOAS observations operated at Kiruna, Sweden (68.84°N, 20.41°E) since 1996. To determine the profile of stratospheric NO2 measured from ground-based zenith sky DOAS, we apply the Optimal Estimation Method (OEM) to retrieval of vertical profiles of stratospheric NO2 which has been developed by IASB-BIRA. The basic principle behind this profiling approach is the dependence of the mean scattering height on solar zenith angle (SZA). We compare the retrieved profiles to two additional datasets of stratospheric NO2 profile. The first one is derived from satellite limb observations by SCIAMACHY (Scanning Imaging Absorption spectrometer for Atmospheric CHartographY) on EnviSAT. The second is derived from the SAOZ balloon measurements (using a UV/Visible spectrometer) performed at Kiruna in Sweden.

Six years of total ozone column measurements from SCIAMACHY nadir observations

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Lerot, C.; van Roozendael, M.; van Geffen, J.; van Gent, J.; Fayt, C.; Spurr, R.; Lichtenberg, G.; von Bargen, A.

2009-04-01

Total O3 columns have been retrieved from six years of SCIAMACHY nadir UV radiance measurements using SDOAS, an adaptation of the GDOAS algorithm previously developed at BIRA-IASB for the GOME instrument. GDOAS and SDOAS have been implemented by the German Aerospace Center (DLR) in the version 4 of the GOME Data Processor (GDP) and in version 3 of the SCIAMACHY Ground Processor (SGP), respectively. The processors are being run at the DLR processing centre on behalf of the European Space Agency (ESA). We first focus on the description of the SDOAS algorithm with particular attention to the impact of uncertainties on the reference O3 absorption cross-sections. Second, the resulting SCIAMACHY total ozone data set is globally evaluated through large-scale comparisons with results from GOME and OMI as well as with ground-based correlative measurements. The various total ozone data sets are found to agree within 2% on average. However, a negative trend of 0.2-0.4%/year has been identified in the SCIAMACHY O3 columns; this probably originates from instrumental degradation effects that have not yet been fully characterized.

Six years of total ozone column measurements from SCIAMACHY nadir observations

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G. Lichtenberg

2009-04-01

Full Text Available Total O₃ columns have been retrieved from six years of SCIAMACHY nadir UV radiance measurements using SDOAS, an adaptation of the GDOAS algorithm previously developed at BIRA-IASB for the GOME instrument. GDOAS and SDOAS have been implemented by the German Aerospace Center (DLR in the version 4 of the GOME Data Processor (GDP and in version 3 of the SCIAMACHY Ground Processor (SGP, respectively. The processors are being run at the DLR processing centre on behalf of the European Space Agency (ESA. We first focus on the description of the SDOAS algorithm with particular attention to the impact of uncertainties on the reference O₃ absorption cross-sections. Second, the resulting SCIAMACHY total ozone data set is globally evaluated through large-scale comparisons with results from GOME and OMI as well as with ground-based correlative measurements. The various total ozone data sets are found to agree within 2% on average. However, a negative trend of 0.2–0.4%/year has been identified in the SCIAMACHY O₃ columns; this probably originates from instrumental degradation effects that have not yet been fully characterized.

Rate Constants for the Reactions of OH with CO, NO and NO2, and of HO2 with NO2 in the Presence of Water Vapour at Lower-Tropospheric Conditions

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Rolletter, Michael; Fuchs, Hendrik; Novelli, Anna; Ehlers, Christian; Hofzumahaus, Andreas

2016-04-01

Recent studies have shown that the chemistry of gaseous nitrous acid (HONO) in the lower troposphere is not fully understood. Aside from heterogenous reactions, the daytime HONO formation in the gas-phase is not well understood (Li et al., Science, 2014). For a better understanding of HONO in the gas-phase, we have reinvestigated the reaction rate constants of important tropospheric reactions of the HOx radical family (OH and HO2) with nitrogen oxides at realistic conditions of the lower troposphere (at ambient temperature/pressure and in humid air). In this study we apply a direct pump and probe technique with high accuracy, using small radical concentrations to avoid secondary chemistry. Pulsed laser photolysis/laser-induced fluorescence (LP/LIF) was used to investigate the reaction rate constants of OH with CO, NO, NO2, and HO2 with NO2 in synthetic air at different water vapor concentrations (up to 5 x 1017 molecules cm-3). Photolysis of ozone in the presence of gaseous water was the source of OH. The reactions took place in a flow-tube at room temperature and atmospheric pressure. The chemical decay of the radicals was monitored by laser-induced fluorescence detection in a low-pressure cell, which sampled air continuously from the end of the flow-tube. Knowing the reactant concentrations subsequently allowed to calculate the bimolecular reaction rate constants at 1 atm from the pseudo-first-order decays. In order to observe HO2 reactions, OH was converted into HO2 with an excess of CO in the flow-tube. The newly measured rate constants for OH with CO, NO and NO2 agree very well with current recommendations by NASA/JPL and IUPAC and have an improved accuracy (uncertainty < 5%). These rate coefficients are independent of the presence of water vapour. The measured rate constant of HO2 with NO2 was found to depend significantly on the water-vapour concentration (probably due to formation of HO2*H2O complexes) and to exceed current recommendations by NASA/JPL and

Impact of the new HNO3-forming channel of the HO2+NO reaction on tropospheric HNO3, NOx, HOx and ozone

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A. Kukui

2008-07-01

Full Text Available We have studied the impact of the recently observed reaction NO+HO2→HNO3 on atmospheric chemistry. A pressure and temperature-dependent parameterisation of this minor channel of the NO+HO2→NO2+OH reaction has been included in both a 2-D stratosphere-troposphere model and a 3-D tropospheric chemical transport model (CTM. Significant effects on the nitrogen species and hydroxyl radical concentrations are found throughout the troposphere, with the largest percentage changes occurring in the tropical upper troposphere (UT. Including the reaction leads to a reduction in NOx everywhere in the troposphere, with the largest decrease of 25% in the tropical and Southern Hemisphere UT. The tropical UT also has a corresponding large increase in HNO3 of 25%. OH decreases throughout the troposphere with the largest reduction of over 20% in the tropical UT. The mean global decrease in OH is around 13%, which is very large compared to the impact that typical photochemical revisions have on this modelled quantity. This OH decrease leads to an increase in CH4 lifetime of 5%. Due to the impact of decreased NOx on the OH:HO2 partitioning, modelled HO2 actually increases in the tropical UT on including the new reaction. The impact on tropospheric ozone is a decrease in the range 5 to 12%, with the largest impact in the tropics and Southern Hemisphere. Comparison with observations shows that in the region of largest changes, i.e. the tropical UT, the inclusion of the new reaction tends to degrade the model agreement. Elsewhere the model comparisons are not able to critically assess the impact of including this reaction. Only small changes are calculated in the minor species distributions in the stratosphere.

On the role of visible radiation in ozone profile retrieval from nadir UV/VIS satellite measurements: An experiment with neural network algorithms inverting SCIAMACHY data

International Nuclear Information System (INIS)

Sellitto, P.; Di Noia, A.; Del Frate, F.; Burini, A.; Casadio, S.; Solimini, D.

2012-01-01

Theoretical evidence has been given on the role of visible (VIS) radiation in enhancing the accuracy of ozone retrievals from satellite data, especially in the troposphere. However, at present, VIS is not being systematically used together with ultraviolet (UV) measurements, even when possible with one single instrument, e.g., the SCanning Imaging Absorption spectroMeter for Atmospheric CartograpHY (SCIAMACHY). Reasons mainly reside in the defective performance of optimal estimation and regularization algorithms caused by inaccurate modeling of VIS interaction with aerosols or clouds, as well as in inconsistent intercalibration between UV and VIS measurements. Here we intend to discuss the role of VIS radiation when it feeds a retrieval algorithm based on Neural Networks (NNs) that does not need a forward radiative transfer model and is robust with respect to calibration errors. The NN we designed was trained with a set of ozonesondes (OSs) data and tested over an independent set of OS measurements. We compared the ozone concentration profiles retrieved from UV-only with those retrieved from UV plus VIS nadir data taken by SCIAMACHY. We found that VIS radiation was able to yield more than 10% increase of accuracy and to substantially reduce biases of retrieved profiles at tropospheric levels.

Geophysical validation and long-term consistency between GOME-2/MetOp-A total ozone column and measurements from the sensors GOME/ERS-2, SCIAMACHY/ENVISAT and OMI/Aura

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M. E. Koukouli

2012-09-01

Full Text Available The main aim of the paper is to assess the consistency of five years of Global Ozone Monitoring Experiment-2/Metop-A [GOME-2] total ozone columns and the long-term total ozone satellite monitoring database already in existence through an extensive inter-comparison and validation exercise using as reference Brewer and Dobson ground-based measurements. The behaviour of the GOME-2 measurements is being weighed against that of GOME (1995–2011, Ozone Monitoring Experiment [OMI] (since 2004 and the Scanning Imaging Absorption spectroMeter for Atmospheric CartograpHY [SCIAMACHY] (since 2002 total ozone column products. Over the background truth of the ground-based measurements, the total ozone columns are inter-evaluated using a suite of established validation techniques; the GOME-2 time series follow the same patterns as those observed by the other satellite sensors. In particular, on average, GOME-2 data underestimate GOME data by about 0.80%, and underestimate SCIAMACHY data by 0.37% with no seasonal dependence of the differences between GOME-2, GOME and SCIAMACHY. The latter is expected since the three datasets are based on similar DOAS algorithms. This underestimation of GOME-2 is within the uncertainty of the reference data used in the comparisons. Compared to the OMI sensor, on average GOME-2 data underestimate OMI_DOAS (collection 3 data by 1.28%, without any significant seasonal dependence of the differences between them. The lack of seasonality might be expected since both the GOME data processor [GDP] 4.4 and OMI_DOAS are DOAS-type algorithms and both consider the variability of the stratospheric temperatures in their retrievals. Compared to the OMI_TOMS (collection 3 data, no bias was found. We hence conclude that the GOME-2 total ozone columns are well suitable to continue the long-term global total ozone record with the accuracy needed for climate monitoring studies.

Aerosols correction of the OMI tropospheric NO2 retrievals over cloud-free scenes: Different methodologies based on the O2-O2 477 nm band

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Chimot, Julien; Vlemmix, Tim; Veefkind, Pepijn; Levelt, Pieternel

2016-04-01

Numerous studies have drawn attention to the complexities related to the retrievals of tropospheric NO2 columns derived from satellite UltraViolet-Visible (UV-Vis) measurements in the presence of aerosols. Correction for aerosol effects will remain a challenge for the next generation of air quality satellite instruments such as TROPOMI on Sentinel-5 Precursor, Sentinel-4 and Sentinel-5. The Ozone Monitoring Instrument (OMI) instrument has provided daily global measurements of tropospheric NO2 for more than a decade. However, aerosols are not explicitly taken into account in the current operational OMI tropospheric NO2 retrieval chain (DOMINO v2 [Boersma et al., 2011]). Our study analyses 2 approaches for an operational aerosol correction, based on the use of the O2-O2 477 nm band. The 1st approach is the cloud-model based aerosol correction, also named "implicit aerosol correction", and already used in the operational chain. The OMI O2-O2 cloud retrieval algorithm, based on the Differential Optical Absorption Spectroscopy (DOAS) approach, is applied both to cloudy and to cloud-free scenes with aerosols present. Perturbation of the OMI cloud retrievals over scenes dominated by aerosols has been observed in recent studies led by [Castellanos et al., 2015; Lin et al., 2015; Lin et al., 2014]. We investigated the causes of these perturbations by: (1) confronting the OMI tropospheric NO2, clouds and MODIS AQUA aerosol products; (2) characterizing the key drivers of the aerosol net effects, compared to a signal from clouds, in the UV-Vis spectra. This study has focused on large industrialised areas like East-China, over cloud-free scenes. One of the key findings is the limitation due to the coarse sampling of the employed cloud Look-Up Table (LUT) to convert the results of the applied DOAS fit into effective cloud fraction and pressure. This leads to an underestimation of tropospheric NO2 amount in cases of particles located at elevated altitude. A higher sampling of the

Surface pressure retrieval from SCIAMACHY measurements in the O2 A Band: validation of the measurements and sensitivity on aerosols

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B. van Diedenhoven

2005-01-01

Full Text Available We perform surface pressure retrievals from cloud-free Oxygen A band measurements of SCIAMACHY. These retrievals can be well validated because surface pressure is a quantity that is, in general, accurately known from meteorological models. Therefore, surface pressure retrievals and their validation provide important insight into the quality of the instrument calibration. Furthermore, they can provide insight into retrievals which are affected by similar radiation transport processes, for example the retrieval of total columns of H2O, CO, CO2 and CH4. In our retrieval aerosols are neglected. Using synthetic measurements, it is shown that for low to moderate surface albedos this leads to an underestimation of the retrieved surface pressures. For high surface albedos this generally leads to an overestimation of the retrieved surface pressures. The surface pressures retrieved from the SCIAMACHY measurements indeed show this dependence on surface albedo, when compared to the corresponding pressures from a meteorological database. However, an offset of about 20 hPa was found, which can not be caused by neglecting aerosols in the retrieval. The same offset was found when comparing the retrieved surface pressures to those retrieved from co-located GOME Oxygen A band measurements. This implies a calibration error in the SCIAMACHY measurements. By adding an offset of 0.86% of the continuum reflectance at 756 nm to the SCIAMACHY reflectance measurements, this systematic bias vanishes.

A method for evaluating spatially-resolved NOx emissions using Kalman filter inversion, direct sensitivities, and space-based NO2 observations

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R. V. Martin

2008-09-01

Full Text Available An inverse modeling method was developed and tested for identifying possible biases in emission inventories using satellite observations. The relationships between emission inputs and modeled ambient concentrations were estimated using sensitivities calculated with the decoupled direct method in three dimensions (DDM-3D implemented within the framework of the Community Multiscale Air Quality (CMAQ regional model. As a case study to test the approach, the method was applied to regional ground-level NOx emissions in the southeastern United States as constrained by observations of NO2 column densities derived from the Scanning Imaging Absorption Spectrometer for Atmospheric Chartography (SCIAMACHY satellite instrument. A controlled "pseudodata" scenario with a known solution was used to establish that the methodology can achieve the correct solution, and the approach was then applied to a summer 2004 period where the satellite data are available. The results indicate that emissions biases differ in urban and rural areas of the southeast. The method suggested slight downward (less than 10% adjustment to urban emissions, while rural region results were found to be highly sensitive to NOx processes in the upper troposphere. As such, the bias in the rural areas is likely not solely due to biases in the ground-level emissions. It was found that CMAQ was unable to predict the significant level of NO2 in the upper troposphere that was observed during the NASA Intercontinental Chemical Transport Experiment (INTEX measurement campaign. The best correlation between satellite observations and modeled NO2 column densities, as well as comparison to ground-level observations of NO2, was obtained by performing the inverse while accounting for the significant presence of NO2 in the upper troposphere not captured by the regional model.

U.S. Participation in the GOME and SCIAMACHY Projects

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Chance, K. V.

1996-01-01

This report summarizes research done under NASA Grant NAGW-2541 from April 1, 1996 through March 31, 1997. The research performed during this reporting period includes development and maintenance of scientific software for the GOME retrieval algorithms, consultation on operational software development for GOME, consultation and development for SCIAMACHY near-real-time (NRT) and off-line (OL) data products, and development of infrared line-by-line atmospheric modeling and retrieval capability for SCIAMACHY. SAO also continues to participate in GOME validation studies, to the limit that can be accomplished at the present level of funding. The Global Ozone Monitoring Experiment was successfully launched on the ERS-2 satellite on April 20, 1995, and remains working in normal fashion. SCIAMACHY is currently in instrument characterization. The first two European ozone monitoring instruments (OMI), to fly on the Metop series of operational meteorological satellites being planned by Eumetsat, have been selected to be GOME-type instruments (the first, in fact, will be the refurbished GOME flight spare). K. Chance is the U.S. member of the OMI Users Advisory Group.

On the impact of aircraft emitted NO{sub x} on upper troposphere photochemistry

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Wahner, A.; Rohrer, F.; Ehhalt, D.H. [Forschungszentrum Juelich GmbH (Germany). Inst. fuer Atmosphaerische Chemie

1997-12-31

The enhanced nitrogen oxide concentrations influence the photochemical production of ozone as well as the steady state concentrations of hydroxyl radicals, OH, in the upper troposphere. That increase is small compared to the impact of NO{sub x} from fossil fuel combustion on boundary layer ozone. A simple quasi 2-D model was used for the latitude band 40 deg - 50 deg N to analyze the reasons for that. The model includes a simplified CH{sub 4} - CO chemistry and the salient sources of upper tropospheric NO{sub x}, namely lightning, stratospheric input, aircraft emissions and fast upward transport of surface emissions. It is shown that the maximum of net O{sub 3} production and OH concentrations occur at much lower NO{sub x} mixing ratios than in the lower troposphere. (author)

On the impact of aircraft emitted NO{sub x} on upper troposphere photochemistry

Energy Technology Data Exchange (ETDEWEB)

Wahner, A; Rohrer, F; Ehhalt, D H [Forschungszentrum Juelich GmbH (Germany). Inst. fuer Atmosphaerische Chemie

1998-12-31

The enhanced nitrogen oxide concentrations influence the photochemical production of ozone as well as the steady state concentrations of hydroxyl radicals, OH, in the upper troposphere. That increase is small compared to the impact of NO{sub x} from fossil fuel combustion on boundary layer ozone. A simple quasi 2-D model was used for the latitude band 40 deg - 50 deg N to analyze the reasons for that. The model includes a simplified CH{sub 4} - CO chemistry and the salient sources of upper tropospheric NO{sub x}, namely lightning, stratospheric input, aircraft emissions and fast upward transport of surface emissions. It is shown that the maximum of net O{sub 3} production and OH concentrations occur at much lower NO{sub x} mixing ratios than in the lower troposphere. (author)

Identification of tropospheric emissions sources from satellite observations: Synergistic use of HCHO, NO2, and SO2 trace gas measurements

Science.gov (United States)

Marbach, T.; Beirle, S.; Khokhar, F.; Platt, U.

2005-12-01

We present case studies for combined HCHO, NO2, and SO2 satellite observations, derived from GOME measurements. Launched on the ERS-2 satellite in April 1995, GOME has already performed continuous operations over 8 years providing global observations of the different trace gases. In this way, satellite observations provide unique opportunities for the identifications of trace gas sources. The satellite HCHO observations provide information concerning the localization of biomass burning (intense source of HCHO). The principal biomass burning areas can be observed in the Amazon basin region and in central Africa Weaker HCHO sources (south east of the United States, northern part of the Amazon basin, and over the African tropical forest), not correlated with biomass burning, could be due to biogenic isoprene emissions. The HCHO data can be compared with NO2 and SO2 results to identify more precisely the tropospheric sources (biomass burning events, human activities, additional sources like volcanic emissions). Biomass burning are important tropospheric sources for both HCHO and NO2. Nevertheless HCHO reflects more precisely the biomass burning as it appears in all biomass burning events. NO2 correlate with HCHO over Africa (grassland fires) but not over Indonesia (forest fires). In south America, an augmentation of the NO2 concentrations can be observed with the fire shift from the forest to grassland vegetation. So there seems to be a dependence between the NO2 emissions during biomass burning and the vegetation type. Other high HCHO, SO2, and NO2 emissions can be correlated with climatic events like the El Nino in 1997, which induced dry conditions in Indonesia causing many forest fires.

Atmospheric greenhouse gases retrieved from SCIAMACHY: comparison to ground-based FTS measurements and model results

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O. Schneising

2012-02-01

Full Text Available SCIAMACHY onboard ENVISAT (launched in 2002 enables the retrieval of global long-term column-averaged dry air mole fractions of the two most important anthropogenic greenhouse gases carbon dioxide and methane (denoted XCO₂ and XCH₄. In order to assess the quality of the greenhouse gas data obtained with the recently introduced v2 of the scientific retrieval algorithm WFM-DOAS, we present validations with ground-based Fourier Transform Spectrometer (FTS measurements and comparisons with model results at eight Total Carbon Column Observing Network (TCCON sites providing realistic error estimates of the satellite data. Such validation is a prerequisite to assess the suitability of data sets for their use in inverse modelling.

It is shown that there are generally no significant differences between the carbon dioxide annual increases of SCIAMACHY and the assimilation system CarbonTracker (2.00 ± 0.16 ppm yr⁻¹ compared to 1.94 ± 0.03 ppm yr⁻¹ on global average. The XCO₂ seasonal cycle amplitudes derived from SCIAMACHY are typically larger than those from TCCON which are in turn larger than those from CarbonTracker. The absolute values of the northern hemispheric TCCON seasonal cycle amplitudes are closer to SCIAMACHY than to CarbonTracker and the corresponding differences are not significant when compared with SCIAMACHY, whereas they can be significant for a subset of the analysed TCCON sites when compared with CarbonTracker. At Darwin we find discrepancies of the seasonal cycle derived from SCIAMACHY compared to the other data sets which can probably be ascribed to occurrences of undetected thin clouds. Based on the comparison with the reference data, we conclude that the carbon dioxide data set can be characterised by a regional relative precision (mean standard deviation of the differences of about 2.2 ppm and a relative accuracy (standard deviation of the mean differences

Toward Quantitative Estimation of the Effect of Aerosol Particles in the Global Climate Model and Cloud Resolving Model

Science.gov (United States)

Eskes, H.; Boersma, F.; Dirksen, R.; van der A, R.; Veefkind, P.; Levelt, P.; Brinksma, E.; van Roozendael, M.; de Smedt, I.; Gleason, J.

2005-05-01

Based on measurements of GOME on ESA ERS-2, SCIAMACHY on ESA-ENVISAT, and Ozone Monitoring Instrument (OMI) on the NASA EOS-Aura satellite there is now a unique 11-year dataset of global tropospheric nitrogen dioxide measurements from space. The retrieval approach consists of two steps. The first step is an application of the DOAS (Differential Optical Absorption Spectroscopy) approach which delivers the total absorption optical thickness along the light path (the slant column). For GOME and SCIAMACHY this is based on the DOAS implementation developed by BIRA/IASB. For OMI the DOAS implementation was developed in a collaboration between KNMI and NASA. The second retrieval step, developed at KNMI, estimates the tropospheric vertical column of NO2 based on the slant column, cloud fraction and cloud top height retrieval, stratospheric column estimates derived from a data assimilation approach and vertical profile estimates from space-time collocated profiles from the TM chemistry-transport model. The second step was applied with only minor modifications to all three instruments to generate a uniform 11-year data set. In our talk we will address the following topics: - A short summary of the retrieval approach and results - Comparisons with other retrievals - Comparisons with global and regional-scale models - OMI-SCIAMACHY and SCIAMACHY-GOME comparisons - Validation with independent measurements - Trend studies of NO2 for the past 11 years

Total ozone column derived from GOME and SCIAMACHY using KNMI retrieval algorithms: Validation against Brewer measurements at the Iberian Peninsula

Science.gov (United States)

Antón, M.; Kroon, M.; López, M.; Vilaplana, J. M.; Bañón, M.; van der A, R.; Veefkind, J. P.; Stammes, P.; Alados-Arboledas, L.

2011-11-01

This article focuses on the validation of the total ozone column (TOC) data set acquired by the Global Ozone Monitoring Experiment (GOME) and the Scanning Imaging Absorption Spectrometer for Atmospheric Chartography (SCIAMACHY) satellite remote sensing instruments using the Total Ozone Retrieval Scheme for the GOME Instrument Based on the Ozone Monitoring Instrument (TOGOMI) and Total Ozone Retrieval Scheme for the SCIAMACHY Instrument Based on the Ozone Monitoring Instrument (TOSOMI) retrieval algorithms developed by the Royal Netherlands Meteorological Institute. In this analysis, spatially colocated, daily averaged ground-based observations performed by five well-calibrated Brewer spectrophotometers at the Iberian Peninsula are used. The period of study runs from January 2004 to December 2009. The agreement between satellite and ground-based TOC data is excellent (R2 higher than 0.94). Nevertheless, the TOC data derived from both satellite instruments underestimate the ground-based data. On average, this underestimation is 1.1% for GOME and 1.3% for SCIAMACHY. The SCIAMACHY-Brewer TOC differences show a significant solar zenith angle (SZA) dependence which causes a systematic seasonal dependence. By contrast, GOME-Brewer TOC differences show no significant SZA dependence and hence no seasonality although processed with exactly the same algorithm. The satellite-Brewer TOC differences for the two satellite instruments show a clear and similar dependence on the viewing zenith angle under cloudy conditions. In addition, both the GOME-Brewer and SCIAMACHY-Brewer TOC differences reveal a very similar behavior with respect to the satellite cloud properties, being cloud fraction and cloud top pressure, which originate from the same cloud algorithm (Fast Retrieval Scheme for Clouds from the Oxygen A-Band (FRESCO+)) in both the TOSOMI and TOGOMI retrieval algorithms.

Quasi-biennial (QBO), annual (AO), and semi-annual oscillation (SAO) in stratospheric SCIAMACHY O3, NO2, and BrO limb data using a multivariate least squares approach

Science.gov (United States)

Dikty, Sebastian; von Savigny, Christian; Sinnhuber, Bjoern-Martin; Rozanov, Alexej; Weber, Mark; Burrows, John P.

We use SCIAMACHY (SCanning Imaging Absorption spectroMeter for Atmospheric CHartog-raphY) ozone, nitrogen dioxide and bromine oxide profiles (20-50 km altitude, 2003-2008) to quantify the amplitudes of QBO, AO, and SAO signals with the help of a simple multivariate regression model. The analysis is being carried out with SCIAMACHY data covering all lat-itudes with the exception of polar nights, when measurements are not available. The overall global yield is approximately 10,000 profiles per month, which are binned into 10-steps with one zonal mean profile being calculated per day and per latitude bin.

Aerosol optical thickness retrieval over land and water using SCIAMACHY/GOME data

NARCIS (Netherlands)

Kusmierczyk-Michulec, J.; Leeuw, G. de

2005-01-01

An algorithm for the retrieval of the aerosol optical thickness over land and over water from SCIAMACHY (SCanning Imaging Absorption SpectroMeter for Atmospheric ChartographY) is presented. Because calibrated data are not yet available for the SCIAMACHY channels used by the algorithm, the concepts

The global distribution of tropospheric NO{sub x} estimated by a 3-D chemical tracer model

Energy Technology Data Exchange (ETDEWEB)

Kraus, A.B.; Rohrer, F.; Ehhalt, D.H. [Forschungszentrum Juelich GmbH (Germany). Inst. fuer Atmosphaerische Chemie

1997-12-31

The global distribution of NO{sub x} in the troposphere is calculated using a three-dimensional chemical tracer model with a simplified chemistry scheme for the tracers NO{sub x} {identical_to} NO + NO{sub 2} and HNO{sub 3}. At northern mid- and high latitudes, the calculated tropospheric NO{sub x} content is dominated by the surface source fossil fuel combustion. In the tropical free troposphere lightning discharges provide about 80% of the total NO{sub x} throughout the year. The zonally averaged fractional contribution of aircraft emissions strongly depends on season. The NO mixing ratios determined by the model show good overall agreement with corresponding zonal mean values observed during the STRATOZ III aircraft campaign in June. Over Canada, mixing ratios as high as 0.5-1.0 ppbv NO were measured during TROPOZ II, the origin of which is not yet understood. (author) 8 refs.

The global distribution of tropospheric NO{sub x} estimated by a 3-D chemical tracer model

Energy Technology Data Exchange (ETDEWEB)

Kraus, A B; Rohrer, F; Ehhalt, D H [Forschungszentrum Juelich GmbH (Germany). Inst. fuer Atmosphaerische Chemie

1998-12-31

The global distribution of NO{sub x} in the troposphere is calculated using a three-dimensional chemical tracer model with a simplified chemistry scheme for the tracers NO{sub x} {identical_to} NO + NO{sub 2} and HNO{sub 3}. At northern mid- and high latitudes, the calculated tropospheric NO{sub x} content is dominated by the surface source fossil fuel combustion. In the tropical free troposphere lightning discharges provide about 80% of the total NO{sub x} throughout the year. The zonally averaged fractional contribution of aircraft emissions strongly depends on season. The NO mixing ratios determined by the model show good overall agreement with corresponding zonal mean values observed during the STRATOZ III aircraft campaign in June. Over Canada, mixing ratios as high as 0.5-1.0 ppbv NO were measured during TROPOZ II, the origin of which is not yet understood. (author) 8 refs.

Long-Term Changes of Tropospheric Trace Gases over Pakistan Derived From Multiple Satellite Instruments

Science.gov (United States)

Zeb, Naila; Fahim Khokhar, Muhammad; Murtaza, Rabbia; Noreen, Asma; Khalid, Tameem

2016-07-01

Air pollution is the expected key environmental issue of Pakistan in coming years due to its ongoing rapid economic growth and this trend suggests only worst air quality over time. In 2014, World bank reported the Pakistan's urban air quality among the most severe in the world and intimated the government to make improvement in air quality as a priority policy agenda. In addition it is recommended to strengthen the institutional and technical capacity of organizations responsible for air quality management. Therefore, the study is designed to put efforts in highlighting air quality issues. The study will provide first database for tropospheric trace gases over Pakistan. The study aims to analyse tropospheric concentrations of CO, TOC, NO2 and HCHO over Pakistan using multisensory data from January 2005 to January 2014. Spatio-temporal and seasonal variability of tropospheric trace gases is observed over the decade to explore long term trend. Hotspots are identified to see variation of species with latitude and to highlight possible sources of trace gases over the Pakistan. High concentrations of trace gases are mainly observed over the Punjab region, which may be attributed to its metropolitan importance. It is the major agricultural, industrialized and urbanized (nearly 60% of the Pakistan's population) sector of the country. Overall significant decreasing trend of CO is identified by MOPITT with relative change of 12.4%. Tropospheric ozone column (TOC) showed insignificant increasing trend with temporal increase of 10.4% whereas NO2 exhibited a significant temporal increase of about 28%. For formaldehyde (HCHO), an increase of about 3.8% is calculated for SCIAMACHY data. Well defined seasonal cycles for these trace gases are observed over the whole study period. CO concentrations showed peak in winter months (November/December/January/February) and dip in the months of Summer/Monsoon (June/July/August). In spite of CO, TCO increases gradually in March and peaks

Observations of HO{sub x}, NO{sub x}, NO{sub y}, and CO. NO{sub x} control of the photochemical production and removal of ozone in the upper troposphere

Energy Technology Data Exchange (ETDEWEB)

Wennberg, P O; Hanisco, T F; Lanzendorf, E L; Jaegle, L Y; Jacob, D J; Cohen, R C; Anderson, J G [Harvard Univ., Cambridge, MA (United States). Dept. of Chemistry; [Dept. of Earth and Planetary Sciences; Fahey, D W; Gao, R S; Keim, E R [National Oceanic and Atmospheric Administration, Boulder, CO (United States). Aeronomy Lab.; others, and

1998-12-31

In-situ measurements from the NASA ER2 aircraft provide the first observations of the odd-hydrogen radicals in the upper troposphere. A new photochemical model was constructed to explain the observations. Based on the model, the way of NO{sub x} influence on the photochemistry of ozone was determined. The measurements also explain why high NO{sub x}/NO{sub y} ratios are sustained in the upper troposphere. (R.P.)

Observations of HO{sub x}, NO{sub x}, NO{sub y}, and CO. NO{sub x} control of the photochemical production and removal of ozone in the upper troposphere

Energy Technology Data Exchange (ETDEWEB)

Wennberg, P.O.; Hanisco, T.F.; Lanzendorf, E.L.; Jaegle, L.Y.; Jacob, D.J.; Cohen, R.C.; Anderson, J.G. [Harvard Univ., Cambridge, MA (United States). Dept. of Chemistry]|[Dept. of Earth and Planetary Sciences; Fahey, D.W.; Gao, R.S.; Keim, E.R. [National Oceanic and Atmospheric Administration, Boulder, CO (United States). Aeronomy Lab.; and others

1997-12-31

In-situ measurements from the NASA ER2 aircraft provide the first observations of the odd-hydrogen radicals in the upper troposphere. A new photochemical model was constructed to explain the observations. Based on the model, the way of NO{sub x} influence on the photochemistry of ozone was determined. The measurements also explain why high NO{sub x}/NO{sub y} ratios are sustained in the upper troposphere. (R.P.)

A new cavity ring-down instrument for airborne monitoring of N2O5, NO3, NO2 and O3 in the upper troposphere lower stratosphere

Science.gov (United States)

Ruth, Albert A.; Brown, Steven S.; Dinesan, Hemanth; Dubé, William P.; Goulette, Marc; Hübler, Gerhard; Orphal, Johannes; Zahn, Andreas

2016-04-01

The chemistry of NO3 and N2O5 is important to the regulation of both tropospheric and stratospheric ozone. In situ detection of NO3 and N2O5 in the upper troposphere lower stratosphere (UTLS) represents a new scientific direction as the only previous measurements of these species in this region of the atmosphere has been via remote sensing techniques. Because both the sources and the sinks for NO3 and N2O5 are potentially stratified spatially, their mixing ratios, and their influence on nitrogen oxide and ozone transport and loss at night can show large variability as a function of altitude. Aircraft-based measurements of heterogeneous N2O5 uptake in the lower troposphere have uncovered a surprising degree of variability in the uptake coefficient [1], but there are no corresponding high altitude measurements.The UTLS is routinely sampled by the IAGOS-CARIBIC program (Civil Aircraft for the Regular Investigation of the atmosphere Based on an Instrument Container, www.caribic-atmospheric.com), a European infrastructural program with the aim of studying the chemistry and transport across this part of the atmosphere. An airfreight container with 15 different automated instruments from 8 European research partners is utilized on board a commercial Lufthansa airbus 340-600 to monitor ~ 100 atmospheric species (trace gases and aerosol parameters) in the UTLS. The instrumentation in the CARIBIC container is now to be supplemented by a new cavity ring-down device for monitoring nitrogen oxides, jointly developed by researchers from Cork (Ireland), Boulder (USA) and Karlsruhe (Germany). The compact and light-weight instrument is designed to monitor not only NO3 and N2O5, but also NO2 and O3. The detection is based on 4 high-finesse optical cavities (cavity length ~ 44 cm). Two cavities are operated at 662 nm (maximum absorption of NO3), the other two at 405 nm (maximum absorption of NO2). The inlet to one of the (662)-cavities is heated in order to thermally decompose N2O5

Global Investigation of the Mg Atom and ion Layers using SCIAMACHY/Envisat Observations between 70 km and 150 km Altitude and WACCM-MG Model Results

Science.gov (United States)

Langowski, M.; vonSavigny, C.; Burrows, J. P.; Feng, W.; Plane, J. M. C.; Marsh, D. R.; Janches, Diego; Sinnhuber, M.; Aikin, A. C.

2014-01-01

Mg and Mg+ concentration fields in the upper mesosphere/lower thermosphere (UMLT) region are retrieved from SCIAMACHY/Envisat limb measurements of Mg and Mg+ dayglow emissions using a 2-D tomographic retrieval approach. The time series of monthly means of Mg and Mg+ for number density as well as vertical column density in different latitudinal regions are shown. Data from the limb mesosphere-thermosphere mode of SCIAMACHY/Envisat are used, which covers the 50 km to 150 km altitude region with a vertical sampling of 3.3 km and a highest latitude of 82 deg. The high latitudes are not covered in the winter months, because there is no dayglow emission during polar night. The measurements were performed every 14 days from mid-2008 until April 2012. Mg profiles show a peak at around 90 km altitude with a density between 750 cm(exp-3) and 2000 cm(exp-3). Mg does not show strong seasonal variation at mid-latitudes. The Mg+ peak occurs 5-15 km above the neutral Mg peak at 95-105 km. Furthermore, the ions show a significant seasonal cycle with a summer maximum in both hemispheres at mid- and high-latitudes. The strongest seasonal variations of the ions are observed at mid-latitudes between 20-40 deg and densities at the peak altitude range from 500 cm(exp-3) to 6000 cm(exp-3). The peak altitude of the ions shows a latitudinal dependence with a maximum at mid-latitudes that is up to 10 km higher than the peak altitude at the equator. The SCIAMACHY measurements are compared to other measurements and WACCM model results. In contrast to the SCIAMACHY results, the WACCM results show a strong seasonal variability for Mg with a winter maximum, which is not observable by SCIAMACHY, and globally higher peak densities. Although the peak densities do not agree the vertical column densities agree, since SCIAMACHY results show a wider vertical profile. The agreement of SCIAMACHY and WACCM results is much better for Mg+, showing the same seasonality and similar peak densities. However

Estimating daily surface NO2 concentrations from satellite data - a case study over Hong Kong using land use regression models

Science.gov (United States)

Anand, Jasdeep S.; Monks, Paul S.

2017-07-01

Land use regression (LUR) models have been used in epidemiology to determine the fine-scale spatial variation in air pollutants such as nitrogen dioxide (NO2) in cities and larger regions. However, they are often limited in their temporal resolution, which may potentially be rectified by employing the synoptic coverage provided by satellite measurements. In this work a mixed-effects LUR model is developed to model daily surface NO2 concentrations over the Hong Kong SAR during the period 2005-2015. In situ measurements from the Hong Kong Air Quality Monitoring Network, along with tropospheric vertical column density (VCD) data from the OMI, GOME-2A, and SCIAMACHY satellite instruments were combined with fine-scale land use parameters to provide the spatiotemporal information necessary to predict daily surface concentrations. Cross-validation with the in situ data shows that the mixed-effects LUR model using OMI data has a high predictive power (adj. R2 = 0. 84), especially when compared with surface concentrations derived using the MACC-II reanalysis model dataset (adj. R2 = 0. 11). Time series analysis shows no statistically significant trend in NO2 concentrations during 2005-2015, despite a reported decline in NOx emissions. This study demonstrates the utility in combining satellite data with LUR models to derive daily maps of ambient surface NO2 for use in exposure studies.

Spectral wave analysis at the mesopause from SCIAMACHY airglow data compared to SABER temperature spectra

Directory of Open Access Journals (Sweden)

M. Ern

2009-01-01

Full Text Available Space-time spectral analysis of satellite data is an important method to derive a synoptic picture of the atmosphere from measurements sampled asynoptically by satellite instruments. In addition, it serves as a powerful tool to identify and separate different wave modes in the atmospheric data. In our work we present space-time spectral analyses of chemical heating rates derived from Scanning Imaging Absorption SpectroMeter for Atmospheric CHartographY (SCIAMACHY hydroxyl nightglow emission measurements onboard Envisat for the years 2002–2006 at mesopause heights. Since SCIAMACHY nightglow hydroxyl emission measurements are restricted to the ascending (nighttime part of the satellite orbit, our analysis also includes temperature spectra derived from 15 μm CO2 emissions measured by the Sounding of the Atmosphere using Broadband Emission Radiometry (SABER instrument. SABER offers better temporal and spatial coverage (daytime and night-time values of temperature and a more regular sampling grid. Therefore SABER spectra also contain information about higher frequency waves. Comparison of SCIAMACHY and SABER results shows that SCIAMACHY, in spite of its observational restrictions, provides valuable information on most of the wave modes present in the mesopause region. The main differences between wave spectra obtained from these sensors can be attributed to the differences in their sampling patterns.

Long-term analysis of carbon dioxide and methane column-averaged mole fractions retrieved from SCIAMACHY

Directory of Open Access Journals (Sweden)

O. Schneising

2011-03-01

Full Text Available Carbon dioxide (CO₂ and methane (CH₄ are the two most important anthropogenic greenhouse gases contributing to global climate change. SCIAMACHY onboard ENVISAT (launch 2002 was the first and is now with TANSO onboard GOSAT (launch 2009 one of only two satellite instruments currently in space whose measurements are sensitive to CO₂ and CH₄ concentration changes in the lowest atmospheric layers where the variability due to sources and sinks is largest.

We present long-term SCIAMACHY retrievals (2003–2009 of column-averaged dry air mole fractions of both gases (denoted XCO₂ and XCH₄ derived from absorption bands in the near-infrared/shortwave-infrared (NIR/SWIR spectral region focusing on large-scale features. The results are obtained using an upgraded version (v2 of the retrieval algorithm WFM-DOAS including several improvements, while simultaneously maintaining its high processing speed. The retrieved mole fractions are compared to global model simulations (CarbonTracker XCO₂ and TM5 XCH₄ being optimised by assimilating highly accurate surface measurements from the NOAA/ESRL network and taking the SCIAMACHY averaging kernels into account. The comparisons address seasonal variations and long-term characteristics.

The steady increase of atmospheric carbon dioxide primarily caused by the burning of fossil fuels can be clearly observed with SCIAMACHY globally. The retrieved global annual mean XCO₂ increase agrees with CarbonTracker within the error bars (1.80±0.13 ppm yr⁻¹ compared to 1.81±0.09 ppm yr⁻¹. The amplitude of the XCO₂ seasonal cycle as retrieved by SCIAMACHY, which is 4.3±0.2 ppm for the Northern Hemisphere and 1.4±0.2 ppm for the Southern Hemisphere, is on average about 1 ppm larger than for CarbonTracker.

An investigation of the boreal forest carbon uptake during the

Explicit and Observation-based Aerosol Treatment in Tropospheric NO2 Retrieval over China from the Ozone Monitoring Instrument

Science.gov (United States)

Liu, M.; Lin, J.; Boersma, F.; Pinardi, G.; Wang, Y.; Chimot, J.; Wagner, T.; Xie, P.; Eskes, H.; Van Roozendael, M.; Hendrick, F.

2017-12-01

Satellite retrieval of vertical column densities (VCDs) of tropospheric nitrogen dioxide (NO2) is influenced by aerosols substantially. Aerosols affect the retrieval of "effective cloud fraction (CF)" and "effective cloud top pressure (CP)" that are used in the subsequent NO2 retrieval to account for the presentence of clouds. And aerosol properties and vertical distributions directly affect the NO2 air mass factor (AMF) calculations. Our published POMINO algorithm uses a parallelized LIDORT-driven AMFv6 code to derive CF, CP and NO2 VCD. Daily information on aerosol optical properties are taken from GEOS-Chem simulations, with aerosol optical depth (AOD) further constrained by monthly MODIS AOD. However, the published algorithm does not include an observation-based constraint of aerosol vertical distribution. Here we construct a monthly climatological observation dataset of aerosol extinction profiles, based on Level-2 CALIOP data over 2007-2015, to further constrain aerosol vertical distributions. GEOS-Chem captures the temporal variations of CALIOP aerosol layer heights (ALH) but has an overall underestimate by about 0.3 km. It tends to overestimate the aerosol extinction by 10% below 2 km but with an underestimate by 30% above 2 km, leading to a low bias by 10-30% in the retrieved tropospheric NO2 VCD. After adjusting GEOS-Chem aerosol extinction profiles by the CALIOP monthly ALH climatology, the retrieved NO2 VCDs increase by 4-16% over China on a monthly basis in 2012. The improved NO2 VCDs are better correlated to independent MAX-DOAS observations at three sites than POMINO and DOMINO are - especially for the polluted cases, R2 reaches 0.76 for the adjusted POMINO, much higher than that for the published POMINO (0.68) and DOMINO (0.38). The newly retrieved CP increases by 60 hPa on average, because of a stronger aerosol screening effect. Compared to the CF used in DOMINO, which implicitly includes aerosol information, our improved CF is much lower and can

Intra-pixel variability in satellite tropospheric NO2 column densities derived from simultaneous space-borne and airborne observations over the South African Highveld

Science.gov (United States)

Broccardo, Stephen; Heue, Klaus-Peter; Walter, David; Meyer, Christian; Kokhanovsky, Alexander; van der A, Ronald; Piketh, Stuart; Langerman, Kristy; Platt, Ulrich

2018-05-01

Aircraft measurements of NO2 using an imaging differential optical absorption spectrometer (iDOAS) instrument over the South African Highveld region in August 2007 are presented and compared to satellite measurements from OMI and SCIAMACHY. In situ aerosol and trace-gas vertical profile measurements, along with aerosol optical thickness and single-scattering albedo measurements from the Aerosol Robotic Network (AERONET), are used to devise scenarios for a radiative transfer modelling sensitivity study. Uncertainty in the air-mass factor due to variations in the aerosol and NO2 profile shape is constrained and used to calculate vertical column densities (VCDs), which are compared to co-located satellite measurements. The lower spatial resolution of the satellites cannot resolve the detailed plume structures revealed in the aircraft measurements. The airborne DOAS in general measured steeper horizontal gradients and higher peak NO2 vertical column density. Aircraft measurements close to major sources, spatially averaged to the satellite resolution, indicate NO2 column densities more than twice those measured by the satellite. The agreement between the high-resolution aircraft instrument and the satellite instrument improves with distance from the source, this is attributed to horizontal and vertical dispersion of NO2 in the boundary layer. Despite the low spatial resolution, satellite images reveal point sources and plumes that retain their structure for several hundred kilometres downwind.

Spectral wave analysis at the mesopause from SCIAMACHY airglow data compared to SABER temperature spectra

Directory of Open Access Journals (Sweden)

M. Ern

2009-01-01

Full Text Available Space-time spectral analysis of satellite data is an important method to derive a synoptic picture of the atmosphere from measurements sampled asynoptically by satellite instruments. In addition, it serves as a powerful tool to identify and separate different wave modes in the atmospheric data. In our work we present space-time spectral analyses of chemical heating rates derived from Scanning Imaging Absorption SpectroMeter for Atmospheric CHartographY (SCIAMACHY hydroxyl nightglow emission measurements onboard Envisat for the years 2002–2006 at mesopause heights.

Since SCIAMACHY nightglow hydroxyl emission measurements are restricted to the ascending (nighttime part of the satellite orbit, our analysis also includes temperature spectra derived from 15 μm CO₂ emissions measured by the Sounding of the Atmosphere using Broadband Emission Radiometry (SABER instrument. SABER offers better temporal and spatial coverage (daytime and night-time values of temperature and a more regular sampling grid. Therefore SABER spectra also contain information about higher frequency waves.

Comparison of SCIAMACHY and SABER results shows that SCIAMACHY, in spite of its observational restrictions, provides valuable information on most of the wave modes present in the mesopause region. The main differences between wave spectra obtained from these sensors can be attributed to the differences in their sampling patterns.

Towards Improving Satellite Tropospheric NO2 Retrieval Products: Impacts of the spatial resolution and lighting NOx production from the a priori chemical transport model

Science.gov (United States)

Smeltzer, C. D.; Wang, Y.; Zhao, C.; Boersma, F.

2009-12-01

Polar orbiting satellite retrievals of tropospheric nitrogen dioxide (NO2) columns are important to a variety of scientific applications. These NO2 retrievals rely on a priori profiles from chemical transport models and radiative transfer models to derive the vertical columns (VCs) from slant columns measurements. In this work, we compare the retrieval results using a priori profiles from a global model (TM4) and a higher resolution regional model (REAM) at the OMI overpass hour of 1330 local time, implementing the Dutch OMI NO2 (DOMINO) retrieval. We also compare the retrieval results using a priori profiles from REAM model simulations with and without lightning NOx (NO + NO2) production. A priori model resolution and lightning NOx production are both found to have large impact on satellite retrievals by altering the satellite sensitivity to a particular observation by shifting the NO2 vertical distribution interpreted by the radiation model. The retrieved tropospheric NO2 VCs may increase by 25-100% in urban regions and be reduced by 50% in rural regions if the a priori profiles from REAM simulations are used during the retrievals instead of the profiles from TM4 simulations. The a priori profiles with lightning NOx may result in a 25-50% reduction of the retrieved tropospheric NO2 VCs compared to the a priori profiles without lightning. As first priority, a priori vertical NO2 profiles from a chemical transport model with a high resolution, which can better simulate urban-rural NO2 gradients in the boundary layer and make use of observation-based parameterizations of lightning NOx production, should be first implemented to obtain more accurate NO2 retrievals over the United States, where NOx source regions are spatially separated and lightning NOx production is significant. Then as consequence of a priori NO2 profile variabilities resulting from lightning and model resolution dynamics, geostationary satellite, daylight observations would further promote the next

Characterization of wildfire NOx emissions using MODIS fire radiative power and OMI tropospheric NO2 columns

Directory of Open Access Journals (Sweden)

R. C. Cohen

2011-06-01

Full Text Available We use observations of fire radiative power (FRP from the Moderate Resolution Imaging Spectroradiometer~(MODIS and tropospheric NO2 column measurements from the Ozone Monitoring Instrument (OMI to derive NO2 wildfire emission coefficients (g MJ−1 for three land types over California and Nevada. Retrieved emission coefficients were 0.279±0.077, 0.342±0.053, and 0.696±0.088 g MJ−1 NO2 for forest, grass and shrub fuels, respectively. These emission coefficients reproduce ratios of emissions with fuel type reported previously using independent methods. However, the magnitude of these coefficients is lower than prior estimates. While it is possible that a negative bias in the OMI NO2 retrieval over regions of active fire emissions is partly responsible, comparison with several other studies of fire emissions using satellite platforms indicates that current emission factors may overestimate the contributions of flaming combustion and underestimate the contributions of smoldering combustion to total fire emissions. Our results indicate that satellite data can provide an extensive characterization of the variability in fire NOx emissions; 67 % of the variability in emissions in this region can be accounted for using an FRP-based parameterization.

Comparison of the HadGEM2 climate-chemistry model against in situ and SCIAMACHY atmospheric methane data

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G. D. Hayman

2014-12-01

Full Text Available Wetlands are a major emission source of methane (CH4 globally. In this study, we evaluate wetland emission estimates derived using the UK community land surface model (JULES, the Joint UK Land Earth Simulator against atmospheric observations of methane, including, for the first time, total methane columns derived from the SCIAMACHY instrument on board the ENVISAT satellite. Two JULES wetland emission estimates are investigated: (a from an offline run driven with Climatic Research Unit–National Centers for Environmental Prediction (CRU-NCEP meteorological data and (b from the same offline run in which the modelled wetland fractions are replaced with those derived from the Global Inundation Extent from Multi-Satellites (GIEMS remote sensing product. The mean annual emission assumed for each inventory (181 Tg CH4 per annum over the period 1999–2007 is in line with other recently published estimates. There are regional differences as the unconstrained JULES inventory gives significantly higher emissions in the Amazon (by ~36 Tg CH4 yr−1 and lower emissions in other regions (by up to 10 Tg CH4 yr−1 compared to the JULES estimates constrained with the GIEMS product. Using the UK Hadley Centre's Earth System model with atmospheric chemistry (HadGEM2, we evaluate these JULES wetland emissions against atmospheric observations of methane. We obtain improved agreement with the surface concentration measurements, especially at high northern latitudes, compared to previous HadGEM2 runs using the wetland emission data set of Fung et al. (1991. Although the modelled monthly atmospheric methane columns reproduce the large-scale patterns in the SCIAMACHY observations, they are biased low by 50 part per billion by volume (ppb. Replacing the HadGEM2 modelled concentrations above 300 hPa with HALOE–ACE assimilated TOMCAT output results in a significantly better agreement with the SCIAMACHY observations. The use of the GIEMS product to constrain the JULES

Observation of Atmospheric Constituents From Space

Science.gov (United States)

Burrows, J. P.

Remote sensing of the atmosphere from space is a growing research field. Surprisingly but for good physical reasons, the mesosphere and stratosphere are easier to probe from space than the troposphere. GOME (Global Ozone Monitoring Experiment) and SCIAMACHY (Scanning Imaging absorption spectroMeter for Atmospheric CHartographY) are related European instruments, which were proposed and been designed to measure atmospheric constituents (gases, aerosols and clouds) by passive remote sensing of the up-welling solar radiation leaving atmosphere. GOME is a smaller version of SCIAMACHY and was launched as part of the core payload of the second European research satellite (ERS-2) on the 20th April 1995. GOME comprises four spectral channels and measures simultaneously the earthshine radiance or solar extra terrestrial irradiance between 240 and 790 nm. Inversion of GOME measurements using the DOAS (Differential Optical Absorption Spectroscopy) yields the total column of trace gases (e.g. O3, NO2, HCHO, BrO and OClO). Application of the FURM (Full Retrieval Method) enables the profiles of O3 to be retrieved. One of the important achievements of GOME has been the separation of tropopsheirc columns of trace gases using TEM (Tropospheric Excess Method). SCIAMACHY has been developed as Germa n, Dutch and Belgian contribution to ENVISAT. It has significantly enhanced capability compared to GOME, measuring a larger spectral range, 220-2380 nm, and observing in alternate nadir and limb modes as well as solar and lunar occultation. ENVISAT is to be launched into a sun synchronous polar orbit, having an equator crossing time of 10.00 a.m. at the beginning of March 2002. SCIAMACHY is thereby able to measure many more species and vertical profiles than GOME. This facilitates improved tropospheric retrievals. Finally GeoTROPE (Geostationary TROPospheric Explorer) is a new mission, which is proposed for launch within the ESA Earth Explorer Opportunity Mission. It comprises two national

Tropospheric VOC measurements by PTR-MS

International Nuclear Information System (INIS)

Hansel, A.; Wisthaler, A.; Graus, M.; Grabmer, W.

2002-01-01

Full text: O 3 is formed photochemically from the photolysis of NO 2 , and because O 3 reacts rapidly with NO these reactions result in a photoequilibrium between NO, NO 2 with no net formation or loss of O 3 , However, in the presence of volatile organic compounds (VOCs), the degradation reactions of VOCs lead to the formation of intermediate peroxy radicals which react with NO, converting NO to NO 2 , which then photolyze to form O 3 . Thus, in order to understand quantitatively tropospheric ozone chemistry, it is necessary to know the VOC distribution within the troposphere as well as VOC fluxes from individual sources. Examples will be presented how the use of Proton Transfer Reaction Mass Spectrometry (PTR-MS) has enhanced our understanding of anthropogenic VOC emissions, biosphere-atmosphere exchange processes, and photochemical processing of both anthropogenic and biogenic VOCs in the troposphere. (author)

Precise pointing knowledge for SCIAMACHY solar occultation measurements

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K. Bramstedt

2012-11-01

Full Text Available We present a method to precisely determine the viewing direction for solar occultation instruments from scans over the solar disk. Basic idea is the fit of the maximum intensity during the scan, which corresponds to the center of the solar disk in the scanning direction. We apply this method to the solar occultation measurements of the satellite instrument SCIAMACHY, which scans the Sun in elevation direction. The achieved mean precision is 0.46 mdeg, which corresponds to an tangent height error of about 26 m for individual occultation sequences. The deviation of the derived elevation angle from the geolocation information given along with the product has a seasonal cycle with an amplitude of 2.26 mdeg, which is in tangent height an amplitude of about 127 m. The mean elevation angle offset is −4.41 mdeg (249 m. SCIAMACHY's sun follower device controls the azimuth viewing direction during the occultation measurements. The derived mean azimuth direction has an standard error of 0.65 mdeg, which is about 36 m in horizontal direction at the tangent point. We observe also a seasonal cycle of the azimuth mispointing with an amplitude of 2.3 mdeg, which is slightly increasing with time. The almost constant mean offset is 88 mdeg, which is about 5.0 km horizontal offset at the tangent point.

Validation of six years of SCIAMACHY carbon monoxide observations using MOZAIC CO profile measurements

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A. T. J. de Laat

2012-09-01

Full Text Available This paper presents a validation study of SCanning Imaging Absorption SpectroMeter for Atmospheric CartograpHY (SCIAMACHY carbon monoxide (CO total column measurements from the Iterative Maximum Likelihood Method (IMLM algorithm using vertically integrated profile aircraft measurements obtained within the MOZAIC project for the six year time period of 2003–2008.

Overall we find a good agreement between SCIAMACHY and airborne measurements for both mean values – also on a year-to-year basis – as well as seasonal variations. Several locations show large biases that are attributed to local effects like orography and proximity of large emission sources. Differences were detected for individual years: 2003, 2004 and 2006 have larger biases than 2005, 2007 and 2008, which appear to be related to SCIAMACHY instrumental issues but require more research. Results from this study are consistent with, and complementary to, findings from a previous validation study using ground-based measurements (de Laat et al., 2010b. According to this study, the SCIAMACHY data, if individual measurements are of sufficient quality – good signal-to-noise, can be used to determine the spatial distribution and seasonal cycles of CO total columns over clean areas. Biases found over areas with strong emissions (Africa, China could be explained by low sensitivity of the instrument in the boundary layer and users are recommended to avoid using the SCIAMACHY data while trying to quantify CO burden and/or retrieve CO emissions in such areas.

Improved pointing information for SCIAMACHY from in-flight measurements of the viewing directions towards sun and moon

Science.gov (United States)

Bramstedt, Klaus; Stone, Thomas C.; Gottwald, Manfred; Noël, Stefan; Bovensmann, Heinrich; Burrows, John P.

2017-07-01

measurements are changed in the range of 0 to +130 m and the limb measurements are changed in the range of -50 to +60 m (depending on season, altitude and azimuth angle). The horizontal location of the tangent point is changed by about 5 km for all measurements. These updates are implemented in version 9 of the SCIAMACHY Level 1b products and Level 2 version 7 (based on L1b version 9).

Improved pointing information for SCIAMACHY from in-flight measurements of the viewing directions towards sun and moon

Directory of Open Access Journals (Sweden)

K. Bramstedt

2017-07-01

occultation measurements are changed in the range of 0 to +130 m and the limb measurements are changed in the range of −50 to +60 m (depending on season, altitude and azimuth angle. The horizontal location of the tangent point is changed by about 5 km for all measurements. These updates are implemented in version 9 of the SCIAMACHY Level 1b products and Level 2 version 7 (based on L1b version 9.

Global investigation of the Mg atom and ion layers using SCIAMACHY/Envisat observations between 70 and 150 km altitude and WACCM-Mg model results

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M. P. Langowski

2015-01-01

Full Text Available Mg and Mg+ concentration fields in the upper mesosphere/lower thermosphere (UMLT region are retrieved from SCIAMACHY/Envisat limb measurements of Mg and Mg+ dayglow emissions using a 2-D tomographic retrieval approach. The time series of monthly mean Mg and Mg+ number density and vertical column density in different latitudinal regions are presented. Data from the limb mesosphere–thermosphere mode of SCIAMACHY/Envisat are used, which cover the 50 to 150 km altitude region with a vertical sampling of ≈3.3 km and latitudes up to 82°. The high latitudes are not observed in the winter months, because there is no dayglow emission during polar night. The measurements were performed every 14 days from mid-2008 until April 2012. Mg profiles show a peak at around 90 km altitude with a density between 750 cm−3 and 1500 cm−3. Mg does not show strong seasonal variation at latitudes below 40°. For higher latitudes the density is lower and only in the Northern Hemisphere a seasonal cycle with a summer minimum is observed. The Mg+ peak occurs 5–15 km above the neutral Mg peak altitude. These ions have a significant seasonal cycle with a summer maximum in both hemispheres at mid and high latitudes. The strongest seasonal variations of Mg+ are observed at latitudes between 20 and 40° and the density at the peak altitude ranges from 500 cm−3 to 4000 cm−3. The peak altitude of the ions shows a latitudinal dependence with a maximum at mid latitudes that is up to 10 km higher than the peak altitude at the equator. The SCIAMACHY measurements are compared to other measurements and WACCM model results. The WACCM results show a significant seasonal variability for Mg with a summer minimum, which is more clearly pronounced than for SCIAMACHY, and globally a higher peak density than the SCIAMACHY results. Although the peak density of both is not in agreement, the vertical column density agrees well, because SCIAMACHY and WACCM profiles have different

Detection of carbon monoxide pollution from cities and wildfires on regional and urban scales: the benefit of CO column retrievals from SCIAMACHY 2.3 µm measurements under cloudy conditions

Science.gov (United States)

Borsdorff, Tobias; Andrasec, Josip; aan de Brugh, Joost; Hu, Haili; Aben, Ilse; Landgraf, Jochen

2018-05-01

In the perspective of the upcoming TROPOMI Sentinel-5 Precursor carbon monoxide data product, we discuss the benefit of using CO total column retrievals from cloud-contaminated SCIAMACHY 2.3 µm shortwave infrared spectra to detect atmospheric CO enhancements on regional and urban scales due to emissions from cities and wildfires. The study uses the operational Sentinel-5 Precursor algorithm SICOR, which infers the vertically integrated CO column together with effective cloud parameters. We investigate its capability to detect localized CO enhancements distinguishing between clear-sky observations and observations with low (Paris, Los Angeles and Tehran as well as the wildfire events in Mexico-Guatemala 2005 and Alaska-Canada 2004. The CO average of the SCIAMACHY full-mission data set of clear-sky observations can detect weak CO enhancements of less than 10 ppb due to air pollution in these cities. For low-cloud conditions, the CO data product performs similarly well. For medium-high clouds, the observations show a reduced CO signal both over Tehran and Los Angeles, while for Paris no significant CO enhancement can be detected. This indicates that information about the vertical distribution of CO can be obtained from the SCIAMACHY measurements. Moreover, for the Mexico-Guatemala fires, the low-cloud CO data captures a strong outflow of CO over the Gulf of Mexico and the Pacific Ocean and so provides complementary information to clear-sky retrievals, which can only be obtained over land. For both burning events, enhanced CO values are even detectable with medium-high-cloud retrievals, confirming a distinct vertical extension of the pollution. The larger number of additional measurements, and hence the better spatial coverage, significantly improve the detection of wildfire pollution using both the clear-sky and cloudy CO retrievals. Due to the improved instrument performance of the TROPOMI instrument with respect to its precursor SCIAMACHY, the upcoming Sentinel-5

SCIAMACHY Level 1 data: calibration concept and in-flight calibration

Science.gov (United States)

Lichtenberg, G.; Kleipool, Q.; Krijger, J. M.; van Soest, G.; van Hees, R.; Tilstra, L. G.; Acarreta, J. R.; Aben, I.; Ahlers, B.; Bovensmann, H.; Chance, K.; Gloudemans, A. M. S.; Hoogeveen, R. W. M.; Jongma, R. T. N.; Noël, S.; Piters, A.; Schrijver, H.; Schrijvers, C.; Sioris, C. E.; Skupin, J.; Slijkhuis, S.; Stammes, P.; Wuttke, M.

2006-11-01

The calibration of SCIAMACHY was thoroughly checked since the instrument was launched on-board ENVISAT in February 2002. While SCIAMACHY's functional performance is excellent since launch, a number of technical difficulties have appeared, that required adjustments to the calibration. The problems can be separated into three types: (1) Those caused by the instrument and/or platform environment. Among these are the high water content in the satellite structure and/or MLI layer. This results in the deposition of ice on the detectors in channels 7 and 8 which seriously affects the retrievals in the IR, mostly because of the continuous change of the slit function caused by scattering of the light through the ice layer. Additionally a light leak in channel 7 severely hampers any retrieval from this channel. (2) Problems due to errors in the on-ground calibration and/or data processing affecting for example the radiometric calibration. A new approach based on a mixture of on-ground and in-flight data is shortly described here. (3) Problems caused by principal limitations of the calibration concept, e.g. the possible appearance of spectral structures after the polarisation correction due to unavoidable errors in the determination of atmospheric polarisation. In this paper we give a complete overview of the calibration and problems that still have to be solved. We will also give an indication of the effect of calibration problems on retrievals where possible. Since the operational processing chain is currently being updated and no newly processed data are available at this point in time, for some calibration issues only a rough estimate of the effect on Level 2 products can be given. However, it is the intention of this paper to serve as a future reference for detailed studies into specific calibration issues.

Satellite-Based Stratospheric and Tropospheric Measurements: Determination of Global Ozone and Other Trace Species

Science.gov (United States)

Chance, Kelly

2003-02-01

This grant is an extension to our previous NASA Grant NAG5-3461, providing incremental funding to continue GOME (Global Ozone Monitoring Experiment) and SCIAMACHY (SCanning Imaging Absorption SpectroMeter for Atmospheric CHartographY) studies. This report summarizes research done under these grants through December 31, 2002. The research performed during this reporting period includes development and maintenance of scientific software for the GOME retrieval algorithms, consultation on operational software development for GOME, consultation and development for SCIAMACHY near-real-time (NRT) and off-line (OL) data products, and participation in initial SCIAMACHY validation studies. The Global Ozone Monitoring Experiment was successfully launched on the ERS-2 satellite on April 20, 1995, and remains working in normal fashion. SCIAMACHY was launched March 1, 2002 on the ESA Envisat satellite. Three GOME-2 instruments are now scheduled to fly on the Metop series of operational meteorological satellites (Eumetsat). K. Chance is a member of the reconstituted GOME Scientific Advisory Group, which will guide the GOME-2 program as well as the continuing ERS-2 GOME program.

Aerosol particle size distribution in the stratosphere retrieved from SCIAMACHY limb measurements

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E. Malinina

2018-04-01

Full Text Available w can be retrieved with an uncertainty of less than 20 %. The algorithm was successfully applied to the tropical region (20° N–20° S for 10 years (2002–2012 of SCIAMACHY observations in limb-viewing geometry, establishing a unique data set. Analysis of this new climatology for the particle size distribution parameters showed clear increases in the mode radius after the tropical volcanic eruptions, whereas no distinct behaviour of the absolute distribution width could be identified. A tape recorder, which describes the time lag as the perturbation propagates to higher altitudes, was identified for both parameters after the volcanic eruptions. A quasi-biannual oscillation (QBO pattern at upper altitudes (28–32 km is prominent in the anomalies of the analysed parameters. A comparison of the aerosol effective radii derived from SCIAMACHY and SAGE II data was performed. The average difference is found to be around 30 % at the lower altitudes, decreasing with increasing height to almost zero around 30 km. The data sample available for the comparison is, however, relatively small.

Multiannual tropical tropospheric ozone columns and the case of the 2015 el Niño event

Science.gov (United States)

Leventidou, Elpida; Eichmann, Kai-Uwe; Weber, Mark; Burrows, John P.

2016-04-01

Stratospheric ozone is well known for protecting the surface from harmful ultraviolet solar radiation whereas ozone in the troposphere plays a more complex role. In the lower troposphere ozone can be extremely harmful for human health as it can oxidize biological tissues and causes respiratory problems. Several studies have shown that the tropospheric ozone burden (300±30Tg (IPCC, 2007)) increases by 1-7% per decade in the tropics (Beig and Singh, 2007; Cooper et al., 2014) which makes the need to monitor it on a global scale crucial. Remote sensing from satellites has been proven to be very useful in providing consistent information of tropospheric ozone concentrations over large areas. Tropical tropospheric ozone columns can be retrieved with the Convective Cloud Differential (CCD) technique (Ziemke et al. 1998) using retrieved total ozone columns and cloud parameters from space-borne observations. We have developed a CCD-IUP algorithm which was applied to GOME/ ERS-2 (1995-2003), SCIAMACHY/ Envisat (2002-2012), and GOME-2/ MetOpA (2007-2012) weighting function DOAS (Coldewey-Egbers et al., 2005, Weber et al., 2005) total ozone data. A unique long-term record of monthly averaged tropical tropospheric ozone columns (20°S - 20°N) was created starting in 1996. This dataset has been extensively validated by comparisons with SHADOZ (Thompson et al., 2003) ozonesonde data and limb-nadir Matching (Ebojie et al. 2014) tropospheric ozone data. The comparison shows good agreement with respect to range, inter-annual variation, and variance. Biases where found to be within 5DU and the RMS errors less than 10 DU. This 17-years dataset has been harmonized into one consistent time series, taking into account the three instruments' difference in ground pixel size. The harmonised dataset is used to determine tropical tropospheric ozone trends and climatological values. The 2015 el Niño event has been characterised as one of the top three strongest el Niños since 1950. El Ni

Spectral studies of ocean water with space-borne sensor SCIAMACHY using Differential Optical Absorption Spectroscopy (DOAS

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M. Vountas

2007-09-01

Full Text Available Methods enabling the retrieval of oceanic parameter from the space borne instrumentation Scanning Imaging Absorption Spectrometer for Atmospheric ChartographY (SCIAMACHY using Differential Optical Absorption Spectroscopy (DOAS are presented. SCIAMACHY onboard ENVISAT measures back scattered solar radiation at a spectral resolution (0.2 to 1.5 nm. The DOAS method was used for the first time to fit modelled Vibrational Raman Scattering (VRS in liquid water and in situ measured phytoplankton absorption reference spectra to optical depths measured by SCIAMACHY. Spectral structures of VRS and phytoplankton absorption were clearly found in these optical depths. Both fitting approaches lead to consistent results. DOAS fits correlate with estimates of chlorophyll concentrations: low fit factors for VRS retrievals correspond to large chlorophyll concentrations and vice versa; large fit factors for phytoplankton absorption correspond with high chlorophyll concentrations and vice versa. From these results a simple retrieval technique taking advantage of both measurements is shown. First maps of global chlorophyll concentrations were compared to the corresponding MODIS measurements with very promising results. In addition, results from this study will be used to improve atmospheric trace gas DOAS-retrievals from visible wavelengths by including these oceanographic signatures.

Evidence for long-range transport of carbon monoxide in the Southern Hemisphere from SCIAMACHY observations

NARCIS (Netherlands)

Gloudemans, A.M.S.; Krol, M.C.; Meirink, J.F.; de Laat, A.T.J.; van der Werf, G.R.; Schrijver, H.; van den Broek, M.M.P.; Aben, I.

2006-01-01

The SCIAMACHY satellite instrument shows enhanced carbon monoxide (CO) columns in the Southern Hemisphere during the local Spring. Chemistry-transport model simulations using the new GFEDv2 biomass-burning emission database show a similar temporal and spatial CO distribution, indicating that the

The ENVISAT Atmospheric Chemistry mission (GOMOS, MIPAS and SCIAMACHY) -Processing status and data availability

Science.gov (United States)

Dehn, Angelika; Brizzi, G.; Barrot, G.; Bovensmann, H.; Canela, M.; Fehr, T.; Laur, H.; Lichtenberg, G.; Niro, F.; Perron, G.; Raspollini, P.; Saavedra de Miguel, L.; Scarpino, G.; Vogel, P.

The atmospheric chemistry instruments on board the ENVISAT platform (GOMOS, MIPAS and SCIAMACHY) provide a unique dataset of geophysical parameters (e.g.: trace gases, clouds, and aerosol) that allows a comprehensive characterization of the atmosphere's chemical and climatological processes [1]. These instruments started to provide significant science data shortly after the launch of the ENVISAT satellite (March 2002). At the time of writing this paper, these instruments and the whole payload modules are fully working and are well beyond the expected lifetime of 5 years. In addition the orbit control strategy of the platform will be modified starting from 2010, in order to extend the mission lifetime up to 2013 [2]. This means that if no instrument problems will appear, the ENVISAT atmospheric sensors will provide at the end of their life, three separated, but complementary datasets of the most important atmospheric state parameters, spanning a time interval of about 11 years. This represents an extraordinary source of information for the scientific user community, both for the completeness and quality of the data and for the extent of the dataset. The aim of this paper is to present the actual status of the ESA operational atmospheric chemistry dataset provided by the three ENVISAT atmospheric chemistry instruments and the future evolution. The processing and reprocessing status will be described in details for each instrument. The outcomes of the geophysical validation and the planned validation activities will be discussed. Finally the data availability and the source of information will be specified. [1] H. Nett, J. Frerick, T. Paulsen, and G. Levrini, "The atmospheric instruments and their applications: GOMOS, MIPAS and SCIAMACHY", ESA Bulletin (ISSN 0376-4265), No. 106, p. 77 -87 (2001) [2] J. Frerick, B. Duesmann, and M. Canela, "2010 and beyond -The ENVISAT mission extension", Proc. `Envisat Symposium 2007', Montreux, Switzerland, 23-27 April 2007 (ESA SP

A comparison of lightning and aircraft sources of NO{sub x} in the upper troposphere

Energy Technology Data Exchange (ETDEWEB)

Penner, J E; Walton, J J [Michigan Univ., Ann Arbor, MI (United States). Dept. of Atmospheric, Oceanic and Space Physics; Bergmann, D J; Kinnison, D; Rotman, D [Lawrence Livermore National Lab., CA (United States). Atmospheric Science Div.; Price, C [Tel Aviv Univ. (Israel). Dept. of Geophysics and Planetary Sciences; Prather, M J [California Univ., Irvine, CA (United States). Dept. of Earth System Science; Pickering, K E [Maryland Univ., College Park, MD (United States). Dept. of Meteorology; Baughcum, S L [Boeing Commerial Airplane Group, Seatlle, WA (United States)

1998-12-31

Uncertainties in the assessment of the contribution of aircraft to upper tropospheric NO{sub x} arise from uncertainties in model treatment of transport, uncertainties in source strengths, and uncertainties in chemical rates and reactions determining the partitioning between NO{sub x} and NO{sub y}. Two different chemical transport models are used to examine the range of uncertainty in the contribution of aircraft to upper tropospheric NO{sub x} from model representations of transport. Uncertainties caused by uncertainties in the rate of production of NO{sub x} from lightning and uncertainties from the range of background concentrations of HNO{sub 3} are also examined. Uncertainties in the treatment of vertical transport and uncertainties in the source strength from lightning contribute to a large range in model results for background NO{sub x}. (author) 18 refs.

A comparison of lightning and aircraft sources of NO{sub x} in the upper troposphere

Energy Technology Data Exchange (ETDEWEB)

Penner, J.E.; Walton, J.J. [Michigan Univ., Ann Arbor, MI (United States). Dept. of Atmospheric, Oceanic and Space Physics; Bergmann, D.J.; Kinnison, D.; Rotman, D. [Lawrence Livermore National Lab., CA (United States). Atmospheric Science Div.; Price, C. [Tel Aviv Univ. (Israel). Dept. of Geophysics and Planetary Sciences; Prather, M.J. [California Univ., Irvine, CA (United States). Dept. of Earth System Science; Pickering, K.E. [Maryland Univ., College Park, MD (United States). Dept. of Meteorology; Baughcum, S.L. [Boeing Commerial Airplane Group, Seatlle, WA (United States)

1997-12-31

Uncertainties in the assessment of the contribution of aircraft to upper tropospheric NO{sub x} arise from uncertainties in model treatment of transport, uncertainties in source strengths, and uncertainties in chemical rates and reactions determining the partitioning between NO{sub x} and NO{sub y}. Two different chemical transport models are used to examine the range of uncertainty in the contribution of aircraft to upper tropospheric NO{sub x} from model representations of transport. Uncertainties caused by uncertainties in the rate of production of NO{sub x} from lightning and uncertainties from the range of background concentrations of HNO{sub 3} are also examined. Uncertainties in the treatment of vertical transport and uncertainties in the source strength from lightning contribute to a large range in model results for background NO{sub x}. (author) 18 refs.

Detection of carbon monoxide pollution from cities and wildfires on regional and urban scales: the benefit of CO column retrievals from SCIAMACHY 2.3 µm measurements under cloudy conditions

Directory of Open Access Journals (Sweden)

T. Borsdorff

2018-05-01

Full Text Available In the perspective of the upcoming TROPOMI Sentinel-5 Precursor carbon monoxide data product, we discuss the benefit of using CO total column retrievals from cloud-contaminated SCIAMACHY 2.3 µm shortwave infrared spectra to detect atmospheric CO enhancements on regional and urban scales due to emissions from cities and wildfires. The study uses the operational Sentinel-5 Precursor algorithm SICOR, which infers the vertically integrated CO column together with effective cloud parameters. We investigate its capability to detect localized CO enhancements distinguishing between clear-sky observations and observations with low (<  1.5 km and medium–high clouds (1.5–5 km. As an example, we analyse CO enhancements over the cities Paris, Los Angeles and Tehran as well as the wildfire events in Mexico–Guatemala 2005 and Alaska–Canada 2004. The CO average of the SCIAMACHY full-mission data set of clear-sky observations can detect weak CO enhancements of less than 10 ppb due to air pollution in these cities. For low-cloud conditions, the CO data product performs similarly well. For medium–high clouds, the observations show a reduced CO signal both over Tehran and Los Angeles, while for Paris no significant CO enhancement can be detected. This indicates that information about the vertical distribution of CO can be obtained from the SCIAMACHY measurements. Moreover, for the Mexico–Guatemala fires, the low-cloud CO data captures a strong outflow of CO over the Gulf of Mexico and the Pacific Ocean and so provides complementary information to clear-sky retrievals, which can only be obtained over land. For both burning events, enhanced CO values are even detectable with medium–high-cloud retrievals, confirming a distinct vertical extension of the pollution. The larger number of additional measurements, and hence the better spatial coverage, significantly improve the detection of wildfire pollution using both the clear-sky and cloudy

Description and Evaluation of the Multiscale Online Nonhydrostatic AtmospheRe CHemistry Model (NMMB-MONARCH) Version 1.0: Gas-Phase Chemistry at Global Scale

Science.gov (United States)

Badia, Alba; Jorba, Oriol; Voulgarakis, Apostolos; Dabdub, Donald; Garcia-Pando, Carlos Perez; Hilboll, Andreas; Goncalves, Maria; Janjic, Zavisa

2017-01-01

This paper presents a comprehensive description and benchmark evaluation of the tropospheric gas-phase chemistry component of the Multiscale Online Nonhydrostatic AtmospheRe CHemistry model (NMMBMONARCH), formerly known as NMMB/BSC-CTM, that can be run on both regional and global domains. Here, we provide an extensive evaluation of a global annual cycle simulation using a variety of background surface stations (EMEP, WDCGG and CASTNET), ozonesondes (WOUDC, CMD and SHADOZ), aircraft data (MOZAIC and several campaigns), and satellite observations (SCIAMACHY and MOPITT).We also include an extensive discussion of our results in comparison to other state-of-the-art models. We note that in this study, we omitted aerosol processes and some natural emissions (lightning and volcano emissions). The model shows a realistic oxidative capacity across the globe. The seasonal cycle for CO is fairly well represented at different locations (correlations around 0.3-0.7 in surface concentrations), although concentrations are underestimated in spring and winter in the Northern Hemisphere, and are overestimated throughout the year at 800 and 500 hPa in the Southern Hemisphere. Nitrogen species are well represented in almost all locations, particularly NO2 in Europe (root mean square error - RMSE - below 5 ppb). The modeled vertical distributions of NOx and HNO3 are in excellent agreement with the observed values and the spatial and seasonal trends of tropospheric NO2 columns correspond well to observations from SCIAMACHY, capturing the highly polluted areas and the biomass burning cycle throughout the year. Over Asia, the model underestimates NOx from March to August, probably due to an underestimation of NOx emissions in the region. Overall, the comparison of the modeled CO and NO2 with MOPITT and SCIAMACHY observations emphasizes the need for more accurate emission rates from anthropogenic and biomass burning sources (i.e., specification of temporal variability).

A full-mission data set of H2O and HDO columns from SCIAMACHY 2.3 µm reflectance measurements

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A. Schneider

2018-06-01

Full Text Available A new data set of vertical column densities of the water vapour isotopologues H2O and HDO from the SCanning Imaging Absorption spectroMeter for Atmospheric CHartographY (SCIAMACHY instrument for the whole of the mission period from January 2003 to April 2012 is presented. The data are retrieved from reflectance measurements in the spectral range 2339 to 2383 nm with the Shortwave Infrared CO Retrieval (SICOR algorithm, ignoring atmospheric light scattering in the measurement simulation. The retrievals are validated with ground-based Fourier transform infrared measurements obtained within the Multi-platform remote Sensing of Isotopologues for investigating the Cycle of Atmospheric water (MUSICA project. A good agreement for low-altitude stations is found with an average bias of −3.6×1021 for H2O and −1.0×1018 molec cm−2 for HDO. The a posteriori computed δD shows an average bias of −8 ‰, even though polar stations have a larger negative bias. The latter is due to the large amount of sensor noise in SCIAMACHY in combination with low albedo and high solar zenith angles. To demonstrate the benefit of accounting for light scattering in the retrieval, the quality of the data product fitting effective cloud parameters simultaneously with trace gas columns is evaluated in a dedicated case study for measurements round high-altitude stations. Due to a large altitude difference between the satellite ground pixel and the mountain station, clear-sky scenes yield a large bias, resulting in a δD bias of 125 ‰. When selecting scenes with optically thick clouds within 1000 m above or below the station altitude, the bias in a posteriori δD is reduced from 125 to 44 ‰. The insights from the present study will also benefit the analysis of the data from the new Sentinel-5 Precursor mission.

Decline in tropospheric NO2 and the effects of the 2008-09 economic crisis observed by OMI over Europe

Science.gov (United States)

Castellanos, P.; Boersma, F. F.

2011-12-01

We present a trend analysis of tropospheric NO2 for the time period of 2004-2010. Necessary for monitoring pollution abatement strategies, NO2 trends analyses are often based on surface networks, which suffer from high NO2 biases and spatial representativity issues inherent to the standard monitoring method (thermal reduction of NO2 followed by reaction with ozone and chemiluminescence). Space based NO2 trends are unbiased and self-consistent, but over Europe they have not been as obvious as those observed over North America and East Asia. In this work we exploit the daily NO2 column observations from the Ozone Monitoring Instrument (OMI) in order to isolate long-term (timescales greater than one year) variability in NO2 over Europe without imposing a parametric fit to the data. In general, we find between 2005 and 2008, 1-5% per year declines in NO2 concentration in many polluted regions (e.g. Germany, Netherlands, Belgium, Italy, Spain), but also 1-5% per year increases over the English Channel and the southern North Sea (a major shipping channel), as well as the United Kingdom, northern France and Eastern Europe. In 2009, NO2 almost exclusively decreased over Europe at a rate of 5-10% per year, coinciding with the abrupt decrease in industrial production and construction prompted by the global economic crisis. By 2010, in many areas the NO2 rate of change returned to pre-2009 levels suggesting economic recovery. We employ a simple fitting model to separate the forcing by meteorological variability, which can influence apparent NO2 trends, from that of NOx emissions. We calculate 1-3% per year NOx emissions reduction rates over most of Europe and an additional 15-30% per year decrease in NOx emissions during the economic crisis time period.

Assessing the Suitability and Limitations of Satellite-based Measurements for Estimating CO, CO2, NO2 and O3 Concentrations over the Niger Delta

Science.gov (United States)

Fagbeja, M. A.; Hill, J. L.; Chatterton, T. J.; Longhurst, J. W.; Akinyede, J. O.

2011-12-01

Space-based satellite sensor technology may provide important tools in the study and assessment of national, regional and local air pollution. However, the application of optical satellite sensor observation of atmospheric trace gases, including those considered to be 'air pollutants', within the lower latitudes is limited due to prevailing climatic conditions. The lack of appropriate air pollution ground monitoring stations within the tropical belt reduces the ability to verify and calibrate space-based measurements. This paper considers the suitability of satellite remotely sensed data in estimating concentrations of atmospheric trace gases in view of the prevailing climate over the Niger Delta region. The methodological approach involved identifying suitable satellite data products and using the ArcGIS Geostatistical Analyst kriging interpolation technique to generate surface concentrations from satellite column measurements. The observed results are considered in the context of the climate of the study area. Using data from January 2001 to December 2005, an assessment of the suitability of satellite sensor data to interpolate column concentrations of trace gases over the Niger Delta has been undertaken and indicates varying degrees of reliability. The level of reliability of the interpolated surfaces is predicated on the number and spatial distributions of column measurements. Accounting for the two climatic seasons in the region, the interpolation of total column concentrations of CO and CO2 from SCIAMACHY produced both reliable and unreliable results over inland parts of the region during the dry season, while mainly unreliable results are observed over the coastal parts especially during the rainy season due to inadequate column measurements. The interpolation of tropospheric measurements of NO2 and O3 from GOME and OMI respectively produced reliable results all year. This is thought to be due to the spatial distribution of available column measurements

The semianalytical cloud retrieval algorithm for SCIAMACHY I. The validation

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A. A. Kokhanovsky

2006-01-01

Full Text Available A recently developed cloud retrieval algorithm for the SCanning Imaging Absorption spectroMeter for Atmospheric CHartographY (SCIAMACHY is briefly presented and validated using independent and well tested cloud retrieval techniques based on the look-up-table approach for MODeration resolutIon Spectrometer (MODIS data. The results of the cloud top height retrievals using measurements in the oxygen A-band by an airborne crossed Czerny-Turner spectrograph and the Global Ozone Monitoring Experiment (GOME instrument are compared with those obtained from airborne dual photography and retrievals using data from Along Track Scanning Radiometer (ATSR-2, respectively.

Water vapour and methane coupling in the stratosphere observed using SCIAMACHY solar occultation measurements

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S. Noël

2018-04-01

Full Text Available An improved stratospheric water vapour data set has been retrieved from SCIAMACHY/ENVISAT solar occultation measurements. It is similar to that successfully applied to methane and carbon dioxide. There is now a consistent set of data products for the three constituents covering the altitudes 17–45 km, the latitude range between about 50 and 70° N, and the period August 2002 to April 2012. The new water vapour concentration profiles agree with collocated results from ACE-FTS and MLS/Aura to within  ∼  5 %. A significant positive linear change in water vapour for the time 2003–2011 is observed at lower stratospheric altitudes with a value of about 0.015 ± 0.008 ppmv year−1 around 17 km. Between 30 and 37 km the changes become significantly negative (about −0.01 ± 0.008 ppmv year−1; all errors are 2σ values. The combined analysis of the SCIAMACHY methane and water vapour time series shows the expected anti-correlation between stratospheric methane and water vapour and a clear temporal variation related to the Quasi-Biennial Oscillation (QBO. Above about 20 km most of the additional water vapour is attributed to the oxidation of methane. In addition short-term fluctuations and longer-term variations on a timescale of 5–6 years are observed. The SCIAMACHY data confirm that at lower altitudes the amount of water vapour and methane are transported from the tropics to higher latitudes via the shallow branch of the Brewer–Dobson circulation.

Modeling of tropospheric NO2 column over different climatic zones and land use/land cover types in South Asia

Science.gov (United States)

ul-Haq, Zia; Rana, Asim Daud; Tariq, Salman; Mahmood, Khalid; Ali, Muhammad; Bashir, Iqra

2018-03-01

We have applied regression analyses for the modeling of tropospheric NO2 (tropo-NO2) as the function of anthropogenic nitrogen oxides (NOx) emissions, aerosol optical depth (AOD), and some important meteorological parameters such as temperature (Temp), precipitation (Preci), relative humidity (RH), wind speed (WS), cloud fraction (CLF) and outgoing long-wave radiation (OLR) over different climatic zones and land use/land cover types in South Asia during October 2004-December 2015. Simple linear regression shows that, over South Asia, tropo-NO2 variability is significantly linked to AOD, WS, NOx, Preci and CLF. Also zone-5, consisting of tropical monsoon areas of eastern India and Myanmar, is the only study zone over which all the selected parameters show their influence on tropo-NO2 at statistical significance levels. In stepwise multiple linear modeling, tropo-NO2 column over landmass of South Asia, is significantly predicted by the combination of RH (standardized regression coefficient, β = - 49), AOD (β = 0.42) and NOx (β = 0.25). The leading predictors of tropo-NO2 columns over zones 1-5 are OLR, AOD, Temp, OLR, and RH respectively. Overall, as revealed by the higher correlation coefficients (r), the multiple regressions provide reasonable models for tropo-NO2 over South Asia (r = 0.82), zone-4 (r = 0.90) and zone-5 (r = 0.93). The lowest r (of 0.66) has been found for hot semi-arid region in northwestern Indus-Ganges Basin (zone-2). The highest value of β for urban area AOD (of 0.42) is observed for megacity Lahore, located in warm semi-arid zone-2 with large scale crop-residue burning, indicating strong influence of aerosols on the modeled tropo-NO2 column. A statistical significant correlation (r = 0.22) at the 0.05 level is found between tropo-NO2 and AOD over Lahore. Also NOx emissions appear as the highest contributor (β = 0.59) for modeled tropo-NO2 column over megacity Dhaka.

The global variation of CH4 and CO as seen by SCIAMACHY

NARCIS (Netherlands)

Straume, A.G.; Schrijver, H.; Gloudemans, A.M.S.; Houweling, S.; Aben, I.; Maurellis, A.N.; de Laat, A.T.J.; Kleipool, Q.; Lichtenberg, G.; van Hees, R.; Meirink, J.F.; Krol, M.

2005-01-01

The methane (CH4) and carbon monoxide (CO) total columns retrieved from SCIAMACHY's near-infrared channel 8 have been compared to satellite measurements by the MOPITT instrument and chemistry transport model calculations (TM3). Results from the SRON retrieval algorithm IMLM (v5.1) are presented here

Combining Bayesian methods and aircraft observations to constrain the HO. + NO2 reaction rate

Science.gov (United States)

Tropospheric ozone is the third strongest greenhouse gas, and has the highest uncertainty in radiative forcing of the top five greenhouse gases. Throughout the troposphere, ozone is produced by radical oxidation of nitrogen oxides (NO,x =NO+NO2). In the uppe...

TROPOMI and TROPI: UV/VIS/NIR/SWIR instruments

NARCIS (Netherlands)

Levelt, P.F.; Oord, G.H.J. van den; Dobber, M.; Eskes, H.; Weele, M. van; Veefkind, P.; Oss, R. van; Aben, I.; Jongma, R.T.; Landgraf, J.; Vries, J. de; Visser, H.

2006-01-01

TROPOMI (Tropospheric Ozone-Monitoring Instrument) is a five-channel UV-VIS-NIR-SWIR non-scanning nadir viewing imaging spectrometer that combines a wide swath (114°) with high spatial resolution (10 × 10 km 2). The instrument heritage consists of GOME on ERS-2, SCIAMACHY on Envisat and, especially,

Chemical ozone losses in Arctic and Antarctic polar winter/spring season derived from SCIAMACHY limb measurements 2002–2009

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T. Sonkaew

2013-02-01

Full Text Available Stratospheric ozone profiles are retrieved for the period 2002–2009 from SCIAMACHY measurements of limb-scattered solar radiation in the Hartley and Chappuis absorption bands of ozone. This data set is used to determine the chemical ozone losses in both the Arctic and Antarctic polar vortices by averaging the ozone in the vortex at a given potential temperature. The chemical ozone losses at isentropic levels between 450 K and 600 K are derived from the difference between observed ozone abundances and the ozone modelled taking diabatic cooling into account, but no chemical ozone loss. Chemical ozone losses of up to 30–40% between mid-January and the end of March inside the Arctic polar vortex are reported. Strong inter-annual variability of the Arctic ozone loss is observed, with the cold winters 2004/2005 and 2006/2007 showing chemical ozone losses inside the polar vortex at 475 K, where 1.7 ppmv and 1.4 ppmv of ozone were removed, respectively, over the period from 22 January to beginning of April and 0.9 ppmv and 1.2 ppmv, respectively, during February. For the winters of 2007/2008 and 2002/2003, ozone losses of about 0.8 ppmv and 0.4 ppmv, respectively are estimated at the 475 K isentropic level for the period from 22 January to beginning of April. Essentially no ozone losses were diagnosed for the relatively warm winters of 2003/2004 and 2005/2006. The maximum ozone loss in the SCIAMACHY data set was found in 2007 at the 600 K level and amounted to about 2.1 ppmv for the period between 22 January and the end of April. Enhanced losses close to this altitude were found in all investigated Arctic springs, in contrast to Antarctic spring. The inter-annual variability of ozone losses and PSC occurrence rates observed during Arctic spring is consistent with the known QBO effects on the Arctic polar vortex, with exception of the unusual Arctic winter 2008/2009.

The maximum total ozone mass loss of about 25 million tons was found in the

Satellite NO2 data improve national land use regression models for ambient NO2 in a small densely populated country

NARCIS (Netherlands)

Hoek, G.; Eeftens, M.; Beelen, R.; Fischer, P.; Brunekreef, B.; Boersma, K.F.; Veefkind, P.

2015-01-01

Land use regression (LUR) modelling has increasingly been applied to model fine scale spatial variation of outdoor air pollutants including nitrogen dioxide (NO2). Satellite observations of tropospheric NO2 improved LUR model in very large study areas, including Canada, United States and Australia.

Satellite NO2 data improve national land use regression models for ambient NO2 in a small densely populated country

NARCIS (Netherlands)

Hoek, Gerard; Eeftens, Marloes; Beelen, Rob; Fischer, Paul; Brunekreef, Bert; Boersma, K. Folkert; Veefkind, Pepijn

Land use regression (LUR) modelling has increasingly been applied to model fine scale spatial variation of outdoor air pollutants including nitrogen dioxide (NO2). Satellite observations of tropospheric NO2 improved LUR model in very large study areas, including Canada, United States and Australia.

Carbon monoxide column retrieval for clear-sky and cloudy atmospheres : A full-mission data set from SCIAMACHY 2.3 μm reflectance measurements

NARCIS (Netherlands)

Borsdorff, Tobias; De Brugh, Joost Aan; Hu, Haili; Nédélec, Philippe; Aben, Ilse; Landgraf, Jochen

2017-01-01

We discuss the retrieval of carbon monoxide (CO) vertical column densities from clear-sky and cloud contaminated 2311-2338 nm reflectance spectra measured by the Scanning Imaging Absorption Spectrometer for Atmospheric Chartography (SCIAMACHY) from January 2003 until the end of the mission in April

Next-Generation Aura/OMI NO2 and SO2 Products

Science.gov (United States)

Krotkov, Nickolay; Yang, Kai; Bucsela, Eric; Lamsal, Lok; Celarier, Edward; Swartz, William; Carn, Simon; Bhartia, Pawan; Gleason, James; Pickering, Ken;

Exploring the Impact of ClNO2 on the Tropospheric Oxidation Capacity in South East Asia during KORUS-AQ 2016

Science.gov (United States)

Jeong, D.; Seco, R.; Gu, D.; Lee, Y.; Knote, C. J.; McGee, T. J.; Sullivan, J. T.; Nault, B.; Jimenez, J. L.; Campuzano Jost, P.; Blake, D. R.; Sanchez, D.; Guenther, A. B.; Tanner, D.; Huey, L. G.; Ahn, J. Y.; Kim, S.

2017-12-01

Nitryl chloride (ClNO2) is a night time radical and NOx reservoir that photolyzes in the morning to release chlorine radicals (Cl·) and NO2. This highly reactive Cl· will react with volatile organic compounds (VOCs) to produce organic peroxy radicals (RO2) eventually producing O3 and increasing the HOx (OH+HO2) radical pool. ClNO2 is generated from heterogeneous reactions of chlorine containing aerosols and dinitrogen pentoxide (N2O5), which is also a night time NOx reservoir. The reactive chlorine can come from both natural (e.g., ocean, biomass burning) and anthropogenic (e.g., steel making, coal combustion, pulp industries etc.) sources. Previous model studies show that the photolysis of ClNO2 can increase O3 and HOx by 20 %. However, ClNO2 observations have been very limited especially in East Asia with only a few field measurements conducted. In this study, we present the ClNO2 observation results from the KORUS-AQ 2016 field campaign conducted in May-June in South Korea. ClNO2 was measured with a chemical ionization mass spectrometry (CIMS) on the DC-8 and in two ground sites. Olympic park and Taehwa research forest represents a heavily populated urban area and a forest nearby respectively. Both ground sites are 50 km from the ocean, the largest source of chlorine. A comprehensive set of trace gas, aerosol, and meteorology parameters have also been carried out during the observation period. We explore the influence of ClNO2 on tropospheric oxidation chemistry mainly focusing on 3 main points: 1) What are the factors controlling the production of ClNO2 (night time v.s. morning)? 2) What are the relative importance of the possible sources of reactive chlorine (oceanic v.s. anthropogenic)? 3) What are the implications of ClNO2 on the local radical chemistry based on box model simulations (F0AM v3.1) embedded with heterogeneous and a comprehensive Cl· + VOC chemistry?

Improved mapping of tropospheric air quality gases based on the Copernicus Sentinel 5 Precursor/TROPOMI mission

Science.gov (United States)

Van Roozendael, Michel; De Smedt, Isabelle; Theys, Nicolas; Danckaert, Thomas; Yu, Huan; Lerot, Christophe; van Gent, Jeroen; Vlietinck, Jonas

2017-04-01

Scheduled for launch in summer 2017, the Sentinel 5 Precursor (S5P) mission having onboard the TROPOMI payload will fly on a sun-synchronous polar orbit and provide daily global early-afternoon observations of a number of key atmospheric trace gases at the unprecedented spatial resolution of 7x3.5 km2. By the early 2020's, S5P will be complemented by geostationary observations from the Sentinel 4 UVN instrument to be delivered at hourly resolution over Europe, and by mid-morning global observations from the low-earth orbiting Sentinel 5 mission. Altogether these missions will form a constellation serving the needs of the Copernicus Atmospheric Monitoring Services (CAMS). Owing to their unprecedented spatial resolution and spectral performance, TROPOMI/S5P and the subsequent Sentinel 4 and 5 missions will significantly push forward monitoring capabilities addressing anthropogenic and natural emissions of air quality-related trace gases. They will also extend the long-term datasets from past and existing UV-Vis sensors (GOME, SCIAMACHY, OMI, GOME-2, OMPS). In this presentation, we explore the potential of S5P to improve on several aspects of the monitoring of tropospheric pollutants, with a focus on the short-lived species NO2, SO2 and HCHO. Based on algorithms designed at BIRA as part of TROPOMI/S5P and S4/S5 level-2 development projects, and their application to the current OMI and GOME-2 sensors, we illustrate and discuss the expected ability of the new sensors to detect smaller scale point sources with better accuracy and selectivity. The retrieval challenges associated with higher resolution measurements are also addressed.

A high-resolution and observationally constrained OMI NO2 satellite retrieval

International Nuclear Information System (INIS)

Goldberg, Daniel L.; Lamsal, Lok N.; Loughner, Christopher P.

2017-01-01

Here, this work presents a new high-resolution NO 2 dataset derived from the NASA Ozone Monitoring Instrument (OMI) NO 2 version 3.0 retrieval that can be used to estimate surface-level concentrations. The standard NASA product uses NO 2 vertical profile shape factors from a 1.25° × 1° (~110 km × 110 km) resolution Global Model Initiative (GMI) model simulation to calculate air mass factors, a critical value used to determine observed tropospheric NO 2 vertical columns. To better estimate vertical profile shape factors, we use a high-resolution (1.33 km × 1.33 km) Community Multi-scale Air Quality (CMAQ) model simulation constrained by in situ aircraft observations to recalculate tropospheric air mass factors and tropospheric NO 2 vertical columns during summertime in the eastern US. In this new product, OMI NO 2 tropospheric columns increase by up to 160% in city centers and decrease by 20–50 % in the rural areas outside of urban areas when compared to the operational NASA product. Our new product shows much better agreement with the Pandora NO 2 and Airborne Compact Atmospheric Mapper (ACAM) NO 2 spectrometer measurements acquired during the DISCOVER-AQ Maryland field campaign. Furthermore, the correlation between our satellite product and EPA NO 2 monitors in urban areas has improved dramatically: r 2 = 0.60 in the new product vs. r 2 = 0.39 in the operational product, signifying that this new product is a better indicator of surface concentrations than the operational product. Our work emphasizes the need to use both high-resolution and high-fidelity models in order to recalculate satellite data in areas with large spatial heterogeneities in NO x emissions. Although the current work is focused on the eastern US, the methodology developed in this work can be applied to other world regions to produce high-quality region-specific NO 2 satellite retrievals.

Consistent Evaluation of ACOS-GOSAT, BESD-SCIAMACHY, CarbonTracker, and MACC Through Comparisons to TCCON

Science.gov (United States)

Kulawik, Susan; Wunch, Debra; O’Dell, Christopher; Frankenberg, Christian; Reuter, Maximilian; Chevallier, Frederic; Oda, Tomohiro; Sherlock, Vanessa; Buchwitz, Michael; Osterman, Greg;

Aerosol indirect effects on lightning in the generation of induced NOx and tropospheric ozone over an Indian urban metropolis

Science.gov (United States)

Saha, Upal; Maitra, Animesh; Talukdar, Shamitaksha; Jana, Soumyajyoti

Lightning flashes, associated with vigorous convective activity, is one of the most prominent weather phenomena in the tropical atmosphere. High aerosol loading is indirectly associated with the increase in lightning flash rates via the formation of tropospheric ozone during the pre-monsoon and monsoon over the tropics. Tropospheric ozone, an important greenhouse pollutant gas have impact on Earth’s radiation budget and play a key role in changing the atmospheric circulation patterns. Lightning-induced NOx is a primary pollutant found in photochemical smog and an important precursor for the formation of tropospheric ozone. A critical analysis is done to study the indirect effects of high aerosol loading on the formation of tropospheric ozone via lightning flashes and induced NOx formation over an urban metropolitan location Kolkata (22°32'N, 88°20'E), India during the period 2001-2012. The seasonal variation of lightning flash rates (LFR), taken from TRMM-LIS 2.5o x 2.5o gridded dataset, show that the LFR was observed to be intensified in the pre-monsoon (March-May) and high in monsoon (June-September) months over the region. Aerosol Optical Depth (AOD) at 555nm, taken from MISR 0.5o x 0.5o gridded level-3 dataset, plays an indirect effect on the increase in LFR during the pre-monsoon and monsoon months and has positive correlations between them during these periods. This is also justified from the seasonal variation of the increase in LFR due to the increase in AOD over the region during 2001-2012. The calibrated GOME and OMI/AURA satellite data analysis shows that the tropospheric ozone, formed as a result of lightning-induced NOx and due to the increased AOD at 555 nm, also increases during the pre-monsoon and monsoon months. The seasonal variation of lightning-induced tropospheric NOx, taken from SCIAMACHY observations also justified the fact that the pre-monsoon and monsoon LFR solely responsible for the generation of induced NOx over the region. The

Impact of climate change on tropospheric ozone and its global budgets

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G. Zeng

2008-01-01

Full Text Available We present the chemistry-climate model UM_CAM in which a relatively detailed tropospheric chemical module has been incorporated into the UK Met Office's Unified Model version 4.5. We obtain good agreements between the modelled ozone/nitrogen species and a range of observations including surface ozone measurements, ozone sonde data, and some aircraft campaigns.

Four 2100 calculations assess model responses to projected changes of anthropogenic emissions (SRES A2, climate change (due to doubling CO₂, and idealised climate change-associated changes in biogenic emissions (i.e. 50% increase of isoprene emission and doubling emissions of soil-NO_x. The global tropospheric ozone burden increases significantly for all the 2100 A2 simulations, with the largest response caused by the increase of anthropogenic emissions. Climate change has diverse impacts on O₃ and its budgets through changes in circulation and meteorological variables. Increased water vapour causes a substantial ozone reduction especially in the tropical lower troposphere (>10 ppbv reduction over the tropical ocean. On the other hand, an enhanced stratosphere-troposphere exchange of ozone, which increases by 80% due to doubling CO₂, contributes to ozone increases in the extratropical free troposphere which subsequently propagate to the surface. Projected higher temperatures favour ozone chemical production and PAN decomposition which lead to high surface ozone levels in certain regions. Enhanced convection transports ozone precursors more rapidly out of the boundary layer resulting in an increase of ozone production in the free troposphere. Lightning-produced NO_x increases by about 22% in the doubled CO₂ climate and contributes to ozone production.

The response to the increase of isoprene emissions shows that the change of ozone is largely determined by background NO_x levels: high

Comparison of total water vapour content in the Arctic derived from GNSS, AIRS, MODIS and SCIAMACHY

Science.gov (United States)

Alraddawi, Dunya; Sarkissian, Alain; Keckhut, Philippe; Bock, Olivier; Noël, Stefan; Bekki, Slimane; Irbah, Abdenour; Meftah, Mustapha; Claud, Chantal

2018-05-01

Atmospheric water vapour plays a key role in the Arctic radiation budget, hydrological cycle and hence climate, but its measurement with high accuracy remains an important challenge. Total column water vapour (TCWV) datasets derived from ground-based GNSS measurements are used to assess the quality of different existing satellite TCWV datasets, namely from the Moderate Resolution Imaging Spectroradiometer (MODIS), the Atmospheric Infrared Sounder (AIRS) and the SCanning Imaging Absorption spectroMeter for Atmospheric CHartographY (SCIAMACHY). The comparisons between GNSS and satellite data are carried out for three reference Arctic observation sites (Sodankylä, Ny-Ålesund and Thule) where long homogeneous GNSS time series of more than a decade (2001-2014) are available. We select hourly GNSS data that are coincident with overpasses of the different satellites over the three sites and then average them into monthly means that are compared with monthly mean satellite products for different seasons. The agreement between GNSS and satellite time series is generally within 5 % at all sites for most conditions. The weakest correlations are found during summer. Among all the satellite data, AIRS shows the best agreement with GNSS time series, though AIRS TCWV is often slightly too high in drier atmospheres (i.e. high-latitude stations during autumn and winter). SCIAMACHY TCWV data are generally drier than GNSS measurements at all the stations during the summer. This study suggests that these biases are associated with cloud cover, especially at Ny-Ålesund and Thule. The dry biases of MODIS and SCIAMACHY observations are most pronounced at Sodankylä during the snow season (from October to March). Regarding SCIAMACHY, this bias is possibly linked to the fact that the SCIAMACHY TCWV retrieval does not take accurately into account the variations in surface albedo, notably in the presence of snow with a nearby canopy as in Sodankylä. The MODIS bias at Sodankylä is found

On the dependence of the OH* Meinel emission altitude on vibrational level: SCIAMACHY observations and model simulations

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J. P. Burrows

2012-09-01

Full Text Available Measurements of the OH Meinel emissions in the terrestrial nightglow are one of the standard ground-based techniques to retrieve upper mesospheric temperatures. It is often assumed that the emission peak altitudes are not strongly dependent on the vibrational level, although this assumption is not based on convincing experimental evidence. In this study we use Envisat/SCIAMACHY (Scanning Imaging Absorption spectroMeter for Atmospheric CHartographY observations in the near-IR spectral range to retrieve vertical volume emission rate profiles of the OH(3-1, OH(6-2 and OH(8-3 Meinel bands in order to investigate whether systematic differences in emission peak altitudes can be observed between the different OH Meinel bands. The results indicate that the emission peak altitudes are different for the different vibrational levels, with bands originating from higher vibrational levels having higher emission peak altitudes. It is shown that this finding is consistent with the majority of the previously published results. The SCIAMACHY observations yield differences in emission peak altitudes of up to about 4 km between the OH(3-1 and the OH(8-3 band. The observations are complemented by model simulations of the fractional population of the different vibrational levels and of the vibrational level dependence of the emission peak altitude. The model simulations reproduce the observed vibrational level dependence of the emission peak altitude well – both qualitatively and quantitatively – if quenching by atomic oxygen as well as multi-quantum collisional relaxation by O2 is considered. If a linear relationship between emission peak altitude and vibrational level is assumed, then a peak altitude difference of roughly 0.5 km per vibrational level is inferred from both the SCIAMACHY observations and the model simulations.

An estimation of tropospheric corrections using GPS and synoptic data: Improving Urmia Lake water level time series from Jason-2 and SARAL/AltiKa satellite altimetry

Science.gov (United States)

Arabsahebi, Reza; Voosoghi, Behzad; Tourian, Mohammad J.

2018-05-01

Tropospheric correction is one of the most important corrections in satellite altimetry measurements. Tropospheric wet and dry path delays have strong dependence on temperature, pressure and humidity. Tropospheric layer has particularly high variability over coastal regions due to humidity, wind and temperature gradients. Depending on the extent of water body and wind conditions over an inland water, Wet Tropospheric Correction (WTC) is within the ranges from a few centimeters to tens of centimeters. Therefore, an extra care is needed to estimate tropospheric corrections on the altimetric measurements over inland waters. This study assesses the role of tropospheric correction on the altimetric measurements over the Urmia Lake in Iran. For this purpose, four types of tropospheric corrections have been used: (i) microwave radiometer (MWR) observations, (ii) tropospheric corrections computed from meteorological models, (iii) GPS observations and (iv) synoptic station data. They have been applied to Jason-2 track no. 133 and SARAL/AltiKa track no. 741 and 356 corresponding to 117-153 and the 23-34 cycles, respectively. In addition, the corresponding measurements of PISTACH and PEACHI, include new retracking method and an innovative wet tropospheric correction, have also been used. Our results show that GPS observation leads to the most accurate tropospheric correction. The results obtained from the PISTACH and PEACHI projects confirm those obtained with the standard SGDR, i.e., the role of GPS in improving the tropospheric corrections. It is inferred that the MWR data from Jason-2 mission is appropriate for the tropospheric corrections, however the SARAL/AltiKa one is not proper because Jason-2 possesses an enhanced WTC near the coast. Furthermore, virtual stations are defined for assessment of the results in terms of time series of Water Level Height (WLH). The results show that GPS tropospheric corrections lead to the most accurate WLH estimation for the selected

Observed atmospheric total column ozone distribution from SCIAMACHY over Peninsular Malaysia

International Nuclear Information System (INIS)

Chooi, T K; San, L H; Jafri, M Z M

2014-01-01

The increase in atmospheric ozone has received great attention because it degrades air quality and brings hazard to human health and ecosystems. The aim of this study was to assess the seasonal variations of ozone concentrations in Peninsular Malaysia from January 2003 to December 2009 using Scanning Imaging Absorption Spectrometer for Atmospheric Cartography (SCIAMACHY). Level-2 data of total column ozone WFMD version 1.0 with spatial resolution 1° × 1.25° were acquired through SCIAMACHY. Analysis for trend of five selected sites exhibit strong seasonal variation in atmospheric ozone concentrations, where there is a significant difference between northeast monsoon and southwest monsoon. The highest ozone values occurred over industrial and congested urban zones (280.97 DU) on August at Bayan Lepas. The lowest ozone values were observed during northeast monsoon on December at Subang (233.08 DU). In addition, the local meteorological factors also bring an impact on the atmospheric ozone. During northeast monsoon, with the higher rate of precipitation, higher relative humidity, low temperature, and less sunlight hours let to the lowest ozone concentrations. Inversely, the highest ozone concentrations observed during southwest monsoon, with the low precipitation rate, lower relative humidity, higher temperature, and more sunlight hours. Back trajectories analysis is carried out, in order to trace the path of the air parcels with high ozone concentration event, suggesting cluster of trajectory (from southwest of the study area) caused by the anthropogenic sources associated with biogenic emissions from large tropical forests, which can make important contribution to regional and global pollution

Remote sensed and in situ constraints on processes affecting tropical tropospheric ozone

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B. Sauvage

2007-01-01

Full Text Available We use a global chemical transport model (GEOS-Chem to evaluate the consistency of satellite measurements of lightning flashes and ozone precursors with in situ measurements of tropical tropospheric ozone. The measurements are tropospheric O3, NO2, and HCHO columns from the GOME satellite instrument, lightning flashes from the OTD and LIS satellite instruments, profiles of O3, CO, and relative humidity from the MOZAIC aircraft program, and profiles of O3 from the SHADOZ ozonesonde network. We interpret these multiple data sources with our model to better understand what controls tropical tropospheric ozone. Tropical tropospheric ozone is mainly affected by lightning NOx and convection in the upper troposphere and by surface emissions in the lower troposphere. Scaling the spatial distribution of lightning in the model to the observed flashes improves the simulation of O3 in the upper troposphere by 5–20 ppbv versus in situ observations and by 1–4 Dobson Units versus GOME retrievals of tropospheric O3 columns. A lightning source strength of 6±2 Tg N/yr best represents in situ observations from aircraft and ozonesonde. Tropospheric NO2 and HCHO columns from GOME are applied to provide top-down constraints on emission inventories of NOx (biomass burning and soils and VOCs (biomass burning. The top-down biomass burning inventory is larger than the bottom-up inventory by a factor of 2 for HCHO and alkenes, and by a factor of 2.6 for NOx over northern equatorial Africa. These emissions increase lower tropospheric O3 by 5–20 ppbv, improving the simulation versus aircraft observations, and by 4 Dobson Units versus GOME observations of tropospheric O3 columns. Emission factors in the a posteriori inventory are more consistent with a recent compilation from in situ measurements. The ozone simulation using two different dynamical schemes (GEOS-3 and GEOS-4 is evaluated versus observations; GEOS-4 better represents O3 observations by 5–15 ppbv

Hydrogen Radicals, Nitrogen Radicals, and the Production of O3 in the Upper Troposphere

Science.gov (United States)

Wennberg, P. O.; Hanisco, T. F.; Jaegle, L.; Jacob, D. J.; Hintsa, E. J.; Lanzendorf, E. J.; Anderson, J. G.; Gao, R.-S.; Keim, E. R.; Donnelly, S. G.;

Evaluation of OMI operational standard NO2 column retrievals using in situ and surface-based NO2 observations

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L. N. Lamsal

2014-11-01

Full Text Available We assess the standard operational nitrogen dioxide (NO2 data product (OMNO2, version 2.1 retrieved from the Ozone Monitoring Instrument (OMI onboard NASA's Aura satellite using a combination of aircraft and surface in~situ measurements as well as ground-based column measurements at several locations and a bottom-up NOx emission inventory over the continental US. Despite considerable sampling differences, NO2 vertical column densities from OMI are modestly correlated (r = 0.3–0.8 with in situ measurements of tropospheric NO2 from aircraft, ground-based observations of NO2 columns from MAX-DOAS and Pandora instruments, in situ surface NO2 measurements from photolytic converter instruments, and a bottom-up NOx emission inventory. Overall, OMI retrievals tend to be lower in urban regions and higher in remote areas, but generally agree with other measurements to within ± 20%. No consistent seasonal bias is evident. Contrasting results between different data sets reveal complexities behind NO2 validation. Since validation data sets are scarce and are limited in space and time, validation of the global product is still limited in scope by spatial and temporal coverage and retrieval conditions. Monthly mean vertical NO2 profile shapes from the Global Modeling Initiative (GMI chemistry-transport model (CTM used in the OMI retrievals are highly consistent with in situ aircraft measurements, but these measured profiles exhibit considerable day-to-day variation, affecting the retrieved daily NO2 columns by up to 40%. This assessment of OMI tropospheric NO2 columns, together with the comparison of OMI-retrieved and model-simulated NO2 columns, could offer diagnostic evaluation of the model.

Troc: a proposed tropospheric sounder for chemistry and climate

Science.gov (United States)

Camy-Peyret, C.

/backscattered sunlight. The diurnal/nocturnal cycle is sampled with a non-sun synchronous circular orbit of 728 km altitude and 65 inclination. Global coverage between 68N and 68S is ensured by a swath of 800 km (11 pixels) and at least one clear pixel in every 100 km × 100 km area is revisited every 3 days. TROC will provide tropospheric profiles for O3, CO and CH4 (3 independent pieces of information in the troposphere) as well as total and tropospheric columns for NO2, H2CO, SO2, BrO and C2H6 together with height resolved information on tropospheric aerosols. Information on other species (H2O, CO2, N2O, CFCs, OCS, ldots) of importance for climate studies will also be obtained. The scientific/technical aspects and status of this project will be presented.

Tropospheric Emissions: Monitoring of Pollution (TEMPO)

Science.gov (United States)

Zoogman, P.; Liu, X.; Suleiman, R. M.; Pennington, W. F.; Flittner, D. E.; Al-Saadi, J. A.; Hilton, B. B.; Nicks, D. K.; Newchurch, M. J.; Carr, J. L.;

Further evaluation of wetland emission estimates from the JULES land surface model using SCIAMACHY and GOSAT atmospheric column methane measurements

Science.gov (United States)

Hayman, Garry; Comyn-Platt, Edward; McNorton, Joey; Chipperfield, Martyn; Gedney, Nicola

2016-04-01

The atmospheric concentration of methane began rising again in 2007 after a period of near-zero growth [1,2], with the largest increases observed over polar northern latitudes and the Southern Hemisphere in 2007 and in the tropics since then. The observed inter-annual variability in atmospheric methane concentrations and the associated changes in growth rates have variously been attributed to changes in different methane sources and sinks [2,3]. Wetlands are generally accepted as being the largest, but least well quantified, single natural source of CH4, with global emission estimates ranging from 142-284 Tg yr-1 [3]. The modelling of wetlands and their associated emissions of CH4 has become the subject of much current interest [4]. We have previously used the HadGEM2 chemistry-climate model to evaluate the wetland emission estimates derived using the UK community land surface model (JULES, the Joint UK Land Earth Simulator) against atmospheric observations of methane, including SCIAMACHY total methane columns [5] up to 2007. We have undertaken a series of new HadGEM2 runs using new JULES emission estimates extended in time to the end of 2012, thereby allowing comparison with both SCIAMACHY and GOSAT atmospheric column methane measurements. We will describe the results of these runs and the implications for methane wetland emissions. References [1] Rigby, M., et al.: Renewed growth of atmospheric methane. Geophys. Res. Lett., 35, L22805, 2008; [2] Nisbet, E.G., et al.: Methane on the Rise-Again, Science 343, 493, 2014; [3] Kirschke, S., et al.,: Three decades of global methane sources and sinks, Nature Geosciences, 6, 813-823, 2013; [4] Melton, J. R., et al.: Present state of global wetland extent and wetland methane modelling: conclusions from a model inter-comparison project (WETCHIMP), Biogeosciences, 10, 753-788, 2013; [5] Hayman, G.D., et al.: Comparison of the HadGEM2 climate-chemistry model against in situ and SCIAMACHY atmospheric methane data, Atmos. Chem

An analysis of the global spatial variability of column-averaged CO2 from SCIAMACHY and its implications for CO2 sources and sinks

Science.gov (United States)

Zhang, Zhen; Jiang, Hong; Liu, Jinxun; Zhang, Xiuying; Huang, Chunlin; Lu, Xuehe; Jin, Jiaxin; Zhou, Guomo

2014-01-01

Satellite observations of carbon dioxide (CO2) are important because of their potential for improving the scientific understanding of global carbon cycle processes and budgets. We present an analysis of the column-averaged dry air mole fractions of CO2 (denoted XCO2) of the Scanning Imaging Absorption Spectrometer for Atmospheric Cartography (SCIAMACHY) retrievals, which were derived from a satellite instrument with relatively long-term records (2003–2009) and with measurements sensitive to the near surface. The spatial-temporal distributions of remotely sensed XCO2 have significant spatial heterogeneity with about 6–8% variations (367–397 ppm) during 2003–2009, challenging the traditional view that the spatial heterogeneity of atmospheric CO2 is not significant enough (2 and surface CO2 were found for major ecosystems, with the exception of tropical forest. In addition, when compared with a simulated terrestrial carbon uptake from the Integrated Biosphere Simulator (IBIS) and the Emissions Database for Global Atmospheric Research (EDGAR) carbon emission inventory, the latitudinal gradient of XCO2 seasonal amplitude was influenced by the combined effect of terrestrial carbon uptake, carbon emission, and atmospheric transport, suggesting no direct implications for terrestrial carbon sinks. From the investigation of the growth rate of XCO2 we found that the increase of CO2 concentration was dominated by temperature in the northern hemisphere (20–90°N) and by precipitation in the southern hemisphere (20–90°S), with the major contribution to global average occurring in the northern hemisphere. These findings indicated that the satellite measurements of atmospheric CO2 improve not only the estimations of atmospheric inversion, but also the understanding of the terrestrial ecosystem carbon dynamics and its feedback to atmospheric CO2.

Multi-year satellite observations of tropospheric NO2 concentrations ...

Indian Academy of Sciences (India)

39

Continuous measurements of atmospheric trace gases are now available that can ... Style Definition: Heading 2. Formatted: Right: ... The major anthropogenic sources of NO2 are industrial and vehicular emissions, soil emissions. (natural) and ...

Concentrations of ethane (C2H6) in the lower stratosphere and upper troposphere and acetylene (C2H2) in the upper troposphere deduced from Atmospheric Trace Molecule Spectroscopy/Spacelab 3 spectra

Science.gov (United States)

Rinsland, C. P.; Russell, J. M., III; Zander, R.; Farmer, C. B.; Norton, R. H.

1987-01-01

This paper reports the results of the spectroscopic analysis of C2H6 and C2H2 absorption spectra obtained by the Atmospheric Trace Molecule Spectroscopy (ATMOS) instrument flown on the Shuttle as part of the Spacelab 3 mission. The spectra were recorded during sunset occultations occurring between 25 deg N and 31 deg N latitudes, yielding volume-mixing ratio profiles of C2H6 in the lower stratosphere and the upper troposphere, and an upper tropospheric profile of C2H2. These results compare well with previous in situ and remote sounding data obtained at similar latitudes and with model calculations. The results demonstrate the feasibility of the ATMOS instrument to sound the lower atmosphere from space.

PM2.5 and tropospheric ozone in China: overview of situation and responses

Science.gov (United States)

Zhang, Hua

This work reviewed the observational status of PM2.5 and tropospheric ozone in China. It told us the observational facts on the ratios of typical types of aerosol components to the total PM2.5/PM10, and daily and seasonal change of near surface ozone concentration at different cities of China; the global concentration distribution of tropospheric ozone observed by satellite in 2010-2013 was also given for comparison; the PM2.5 concentration distribution and their seasonal change in China region were simulated by an aerosol chemistry-global climate modeling system. Different contribution from five kinds of aerosols to the simulated PM2.5 was analyzed. Then, it linked the emissions of aerosol and greenhouse gases and their radiative forcing and thus gave their climatic effect by reducing their emissions on the basis of most recently published IPCC AR5. Finally it suggested policies on reducing emissions of short-lived climate pollutants (SLCPs) (such as PM2.5 and tropospheric ozone) in China from protecting both climate and environment.

Applications of Satellite Observations of Tropospheric Composition

Science.gov (United States)

Monks, Paul S.; Beirle, Steffen

A striking feature of the field of tropospheric composition is the sheer number of chemical species that have been detected and measured with satellite instruments. The measurements have found application both in atmospheric chemistry itself, providing evidence, for example, of unexpected cryochemistry in the Arctic regions, and also in environmental monitoring with, for example, the observed growth in NO2 emissions over eastern Asia. Chapter 8 gives an overview of the utility of satellite observations for measuring tropospheric composition, dealing with each of the many compounds seen in detail. A comprehensive compound by compound table of the many studies performed is a most useful feature.

Estimates of the changes in tropospheric chemistry which result from human activity and their dependence on NO(x) emissions and model resolution

Science.gov (United States)

Kanakidou, Maria; Crutzen, Paul J.; Zimmermann, Peter H.

1994-01-01

As a consequence of the non-linear behavior of the chemistry of the atmosphere and because of the short lifetime of nitrogen oxides (NO(x)), two-dimensional models do not give an adequate description of the production and destruction rates of NO(x) and their effects on the distributions of the concentration of ozone and hydroxyl radical. In this study, we use a three-dimensional model to evaluate the contribution of increasing NO(x) emissions from industrial activity and biomass burning to changes in the chemical composition of the troposphere. By comparing results obtained from longitudinally-uniform and longitudinally-varying emissions of NO(x), we demonstrate that the geographical representation of the NO(x) emissions is crucial in simulating tropospheric chemistry.

Sulfur dioxide retrievals from OMI and GOME-2 in preparation of TROPOMI

Science.gov (United States)

Theys, Nicolas; De Smedt, Isabelle; Danckaert, Thomas; Yu, Huan; van Gent, Jeroen; Van Roozendael, Michel

2016-04-01

The TROPOspheric Monitoring Instrument (TROPOMI) will be launched in 2016 onboard the ESA Sentinel-5 Precursor (S5P) platform and will provide global observations of atmospheric trace gases, with unprecedented spatial resolution. Sulfur dioxide (SO2) measurements from S5P will significantly improve the current capabilities for anthropogenic and volcanic emissions monitoring, and will extend the long-term datasets from past and existing UV sensors (TOMS, GOME, SCIAMACHY, OMI, GOME-2, OMPS). This work presents the SO2 retrieval schemes performed at BIRA-IASB as part of level-2 algorithm prototyping activities for S5P and tested on OMI and GOME-2. With a focus on anthropogenic sources, we show comparisons between OMI and GOME-2 as well as ground-based measurements, and discuss the possible reasons for the differences.

Retrieval of tropospheric NO2 vertical column densities and aerosol optical properties form MAXDOAS measurements in Yangtze River Delta, China

Science.gov (United States)

Hao, Nan; Van. Roozendael, Michel; Ding, Aijun; Zhou, Bin; Hendrick, François; Shen, Yicheng; Wang, Tin; Valks, Pieter

2014-05-01

Air pollution is one of the most important environmental problems in developing Asian countries like China. Due to huge consumption of fossil fuels and rapid increase of traffic emissions in the past decades, many regions in China have been experiencing heavy air pollution. The Yangtze River Delta (YRD) region includes the mega-city Shanghai and the well-industrialized and urbanized areas of Zhejiang Province and Jiangsu Province, with over ten large cities, such as Hangzhou, Suzhou and Nanjing. Covering only 2% land area, this region produces over 20% of China's Gross Domestic Product (GDP) which makes it the most densely populated region and one of the most polluted regions in China. For instance, there more than 60% of a year was haze days with poor visibility in Shanghai over the last few years. In the YRD region, knowledge gaps still exist in the understanding of the source and transport of air pollutants because only few measurement studies have been conducted. MAX-DOAS measurements were performed in Shanghai city center and Wujiang (border of Shanghai and Jiangsu Province) from 2010 to 2012 and in Nanjing (capital of Jiangsu Province) from April 2013. A retrieval algorithm, based on an on-line implementation of the radiative transfer code LIDORT and the optimal estimation technique, has been used to provide information on aerosol extinction vertical profiles. The total aerosol optical depths (AODs) calculated from the retrieved profiles were compared to MODIS, AERONET and local PM measurements. The aerosol information was input to LIDORT to calculate NO2 air mass factors. The retrieved tropospheric NO2 vertical column densities (VCDs) were compared to in-situ and satellite NO2 measurements.

Methane from the Tropospheric Emission Spectrometer (TES)

Science.gov (United States)

Payne, Vivienne; Worden, John; Kulawik, Susan; Frankenberg, Christian; Bowman, Kevin; Wecht, Kevin

2012-01-01

TES V5 CH4 captures latitudinal gradients, regional variability and interannual variation in the free troposphere. V5 joint retrievals offer improved sensitivity to lower troposphere. Time series extends from 2004 to present. V5 reprocessing in progress. Upper tropospheric bias. Mitigated by N2O correction. Appears largely spatially uniform, so can be corrected. How to relate free-tropospheric values to surface emissions.

Tropospheric nitrogen dioxide inversions based on spectral measurements of scattered sunlight

NARCIS (Netherlands)

Vlemmix, T.

2011-01-01

This thesis describes the development of inversion methods for tropospheric nitrogen dioxide (NO2), based on ground based observations of scattered sunlight with themulti-axis differential optical absorption spectroscopy (MAX-DOAS) technique. NO2 is an atmospheric trace gas which, when present near

Detection of carbon monoxide pollution from cities and wildfires on regional and urban scales: the benefit of CO column retrievals from SCIAMACHY 2.3 µm measurements under cloudy conditions

OpenAIRE

Borsdorff, Tobias; Andrasec, Josip; aan de Brugh, Joost; Hu, Haili; Aben, Ilse; Landgraf, Jochen

2018-01-01

In the perspective of the upcoming TROPOMI Sentinel-5 Precursor carbon monoxide data product, we discuss the benefit of using CO total column retrievals from cloud-contaminated SCIAMACHY 2.3 µm shortwave infrared spectra to detect atmospheric CO enhancements on regional and urban scales due to emissions from cities and wildfires. The study uses the operational Sentinel-5 Precursor algorithm SICOR, which infers the vertically integrated CO column together with effective cl...

Analysis of Rosetta/VIRTIS spectra of earth using observations from ENVISAT/AATSR, TERRA/MODIS and ENVISAT/SCIAMACHY, and radiative-transfer simulations

Science.gov (United States)

Hurley, J.; Irwin, P. G. J.; Adriani, A.; Moriconi, M.; Oliva, F.; Capaccioni, F.; Smith, A.; Filacchione, G.; Tosi, F.; Thomas, G.

2014-01-01

Rosetta, the Solar System cornerstone mission of ESA's Horizon 2000 programme, consists of an orbiter and a lander, and is due to arrive at the comet 67P/Churyumov-Gerasimenko in May 2014. Following its 2004 launch, Rosetta carried out a series of planetary fly-bys and gravitational assists. On these close fly-bys of the Earth, measurements were taken by the Visible Infrared Thermal Imaging Spectrometer (VIRTIS). Analysis of these spectra and comparison with spectra acquired by Earth-observing satellites can support the verification of the inflight calibration of Rosetta/VIRTIS. In this paper, measurements taken by VIRTIS in November 2009 are compared with suitable coincident data from Earth-observing instruments (ESA-ENVISAT/AATSR and SCIAMACHY, and EOS-TERRA/MODIS). Radiative transfer simulations using NEMESIS (Irwin et al., 2008) are fit to the fly-by data taken by VIRTIS, using representative atmospheric and surface parameters. VIRTIS measurements correlate 90% with AATSR's, 85-94% with MODIS, and 82-88% with SCIAMACHYs. The VIRTIS spectra are reproducible in the 1-5 μm region, except in the 1.4 μm deep water vapour spectral absorption band in the near-infrared in cases in which the radiance is very low (cloud-free topographies), where VIRTIS consistently registers more radiance than do MODIS and SCIAMACHY. Over these cloud-free regions, VIRTIS registers radiances a factor of 3-10 larger than SCIAMACHY and of 3-8 greater than MODIS. It is speculated that this discrepancy could be due to a spectral light leak originating from reflections from the order-sorting filters above the detector around 1.4 μm.

Characteristics of the NO-NO2-O3 system in different chemical regimes during the MIRAGE-Mex field campaign

Science.gov (United States)

Shon, Z.-H.; Madronich, S.; Song, S.-K.; Flocke, F. M.; Knapp, D. J.; Anderson, R. S.; Shetter, R. E.; Cantrell, C. A.; Hall, S. R.; Tie, X.

2008-12-01

The NO-NO2 system was analyzed in different chemical regimes/air masses based on observations of reactive nitrogen species and peroxy radicals made during the intensive field campaign MIRAGE-Mex (4 to 29 March 2006). The air masses were categorized into 5 groups based on combinations of macroscopic observations, geographical location, meteorological parameters, models, and observations of trace gases: boundary layer (labeled as "BL"), biomass burning ("BB"), free troposphere (continental, "FTCO" and marine, "FTMA"), and Tula industrial complex ("TIC"). In general, NO2/NO ratios in different air masses are near photostationary state. Analysis of this ratio can be useful for testing current understanding of tropospheric chemistry. The ozone production efficiency (OPE) for the 5 air mass categories ranged from 4.5 (TIC) to 8.5 (FTMA), consistent with photochemical aging of air masses exiting the Mexico City Metropolitan Area.

The version 3 OMI NO2 standard product

Directory of Open Access Journals (Sweden)

N. A. Krotkov

2017-09-01

Full Text Available We describe the new version 3.0 NASA Ozone Monitoring Instrument (OMI standard nitrogen dioxide (NO2 products (SPv3. The products and documentation are publicly available from the NASA Goddard Earth Sciences Data and Information Services Center (https://disc.gsfc.nasa.gov/datasets/OMNO2_V003/summary/. The major improvements include (1 a new spectral fitting algorithm for NO2 slant column density (SCD retrieval and (2 higher-resolution (1° latitude and 1.25° longitude a priori NO2 and temperature profiles from the Global Modeling Initiative (GMI chemistry–transport model with yearly varying emissions to calculate air mass factors (AMFs required to convert SCDs into vertical column densities (VCDs. The new SCDs are systematically lower (by ∼ 10–40 % than previous, version 2, estimates. Most of this reduction in SCDs is propagated into stratospheric VCDs. Tropospheric NO2 VCDs are also reduced over polluted areas, especially over western Europe, the eastern US, and eastern China. Initial evaluation over unpolluted areas shows that the new SPv3 products agree better with independent satellite- and ground-based Fourier transform infrared (FTIR measurements. However, further evaluation of tropospheric VCDs is needed over polluted areas, where the increased spatial resolution and more refined AMF estimates may lead to better characterization of pollution hot spots.

Tropospheric ozone annual variation and possible troposphere-stratosphere coupling in the Arctic and Antarctic as derived from ozone soundings at Resolute and Amundsen-Scott stations

Energy Technology Data Exchange (ETDEWEB)

Gruzdev, A.N.; Sitnov, S.A. (Russian Academy of Sciences, Moscow (Russian Federation). Inst. of Atmospheric Physics)

1993-01-01

The tropospheric ozone annual variation in the northern and southern polar regions is analyzed from ozone sounding data obtained at Resolute during a 15-year period and Amundsen-Scott during a 7-year period. The phase of ozone annual variation above Resolute changes (increases) gradually from the stratosphere across the tropopause to the middle troposphere. Unlike this, the phase of the Antarctic ozone annual harmonic has a discontinuity in the layer of the changing tropopause level, so that the annual harmonic in the upper troposphere, lower stratosphere is 4-to-5 months out of phase (earlier) to that above and beneath. Above both the Arctic and Antarctic stations, the ozone mixing ratio and its vertical gradient evolve in a similar manner in the wide layer from the lower stratosphere to the middle troposphere. This likely points out that ozone in this layer is controlled from above. An indication of the stratospheric-tropospheric ozone exchange above Resolute is noted from mid-winter to spring. The analysis of columnar tropospheric ozone changes gives a lower estimate of the cross-tropopause ozone flux up to 5x10[sup 10] mol cm[sup -2] s[sup -1]. Above the South Pole, the cross-tropopause ozone flux is not usually large. There is also some evidence that early in the spring, when the stratospheric ozone 'hole' is developed, the stratospheric-tropospheric exchange conducts the influence of the 'hole' into the upper troposphere, where the integrated ozone destruction is estimated to be 8x10[sup 10] mol cm[sup -2] s[sup -1]. Correlation analysis gives no ozone-tropopause correlation in the Antarctic in winter, while in other seasons as well as during all seasons in the Arctic, there are negative correlation peaks just above the tropopause. (19 refs., 6 figs.).

Retrieval of nitric oxide in the mesosphere and lower thermosphere from SCIAMACHY limb spectra

Directory of Open Access Journals (Sweden)

S. Bender

2013-09-01

Full Text Available We use the ultra-violet (UV spectra in the range 230–300 nm from the SCanning Imaging Absorption spectroMeter for Atmospheric CHartographY (SCIAMACHY to retrieve the nitric oxide (NO number densities from atmospheric emissions in the gamma-bands in the mesosphere and lower thermosphere. Using 3-D ray tracing, a 2-D retrieval grid, and regularisation with respect to altitude and latitude, we retrieve a whole semi-orbit simultaneously for the altitude range from 60 to 160 km. We present details of the retrieval algorithm, first results, and initial comparisons to data from the Michelson Interferometer for Passive Atmospheric Sounding (MIPAS. Our results agree on average well with MIPAS data and are in line with previously published measurements from other instruments. For the time of available measurements in 2008–2011, we achieve a vertical resolution of 5–10 km in the altitude range 70–140 km and a horizontal resolution of about 9° from 60° S–60° N. With this we have independent measurements of the NO densities in the mesosphere and lower thermosphere with approximately global coverage. This data can be further used to validate climate models or as input for them.

Tropospheric emissions: Monitoring of pollution (TEMPO)

Science.gov (United States)

Zoogman, P.; Liu, X.; Suleiman, R. M.; Pennington, W. F.; Flittner, D. E.; Al-Saadi, J. A.; Hilton, B. B.; Nicks, D. K.; Newchurch, M. J.; Carr, J. L.; Janz, S. J.; Andraschko, M. R.; Arola, A.; Baker, B. D.; Canova, B. P.; Chan Miller, C.; Cohen, R. C.; Davis, J. E.; Dussault, M. E.; Edwards, D. P.; Fishman, J.; Ghulam, A.; González Abad, G.; Grutter, M.; Herman, J. R.; Houck, J.; Jacob, D. J.; Joiner, J.; Kerridge, B. J.; Kim, J.; Krotkov, N. A.; Lamsal, L.; Li, C.; Lindfors, A.; Martin, R. V.; McElroy, C. T.; McLinden, C.; Natraj, V.; Neil, D. O.; Nowlan, C. R.; O`Sullivan, E. J.; Palmer, P. I.; Pierce, R. B.; Pippin, M. R.; Saiz-Lopez, A.; Spurr, R. J. D.; Szykman, J. J.; Torres, O.; Veefkind, J. P.; Veihelmann, B.; Wang, H.; Wang, J.; Chance, K.

2017-01-01

TEMPO was selected in 2012 by NASA as the first Earth Venture Instrument, for launch between 2018 and 2021. It will measure atmospheric pollution for greater North America from space using ultraviolet and visible spectroscopy. TEMPO observes from Mexico City, Cuba, and the Bahamas to the Canadian oil sands, and from the Atlantic to the Pacific, hourly and at high spatial resolution ( 2.1 km N/S×4.4 km E/W at 36.5°N, 100°W). TEMPO provides a tropospheric measurement suite that includes the key elements of tropospheric air pollution chemistry, as well as contributing to carbon cycle knowledge. Measurements are made hourly from geostationary (GEO) orbit, to capture the high variability present in the diurnal cycle of emissions and chemistry that are unobservable from current low-Earth orbit (LEO) satellites that measure once per day. The small product spatial footprint resolves pollution sources at sub-urban scale. Together, this temporal and spatial resolution improves emission inventories, monitors population exposure, and enables effective emission-control strategies. TEMPO takes advantage of a commercial GEO host spacecraft to provide a modest cost mission that measures the spectra required to retrieve ozone (O3), nitrogen dioxide (NO2), sulfur dioxide (SO2), formaldehyde (H2CO), glyoxal (C2H2O2), bromine monoxide (BrO), IO (iodine monoxide), water vapor, aerosols, cloud parameters, ultraviolet radiation, and foliage properties. TEMPO thus measures the major elements, directly or by proxy, in the tropospheric O3 chemistry cycle. Multi-spectral observations provide sensitivity to O3 in the lowermost troposphere, substantially reducing uncertainty in air quality predictions. TEMPO quantifies and tracks the evolution of aerosol loading. It provides these near-real-time air quality products that will be made publicly available. TEMPO will launch at a prime time to be the North American component of the global geostationary constellation of pollution monitoring

Intercomparison of 4 Years of Global Formaldehyde Observations from the GOME-2 and OMI Sensors

Science.gov (United States)

De Smedt, Isabelle; Van Roozendael, Michel; Stravrakou, Trissevgeni; Muller, Jean-Francois; Chance, Kelly; Kurosu, Thomas

2012-11-01

Formaldehyde (H2CO) tropospheric columns have been retrieved since 2007 from backscattered UV radiance measurements performed by the GOME-2 instrument on the EUMETSAT METOP-A platform. This data set extends the successful time-series of global H2CO observations established with GOME/ ERS-2 (1996-2003), SCIAMACHY/ ENVISAT (2003-2012), and OMI on the NASA AURA platform (2005-now). In this work, we perform an intercomparison of the H2CO tropospheric columns retrieved from GOME-2 and OMI between 2007 and 2010, respectively at BIRA-IASB and at Harvard SAO. We first compare the global formaldehyde data products that are provided by each retrieval group. We then investigate each step of the retrieval procedure: the slant column fitting, the reference sector correction and the air mass factor calculation. New air mass factors are computed for OMI using external parameters consistent with those used for GOME-2. By doing so, the impacts of the different a priori profiles and aerosol corrections are quantified. The remaining differences are evaluated in view of the expected diurnal variations of the formaldehyde concentrations, based on ground-based measurements performed in the Beijing area.

Using Satellite Remote Sensing and Modelling for Insights into N02 Air Pollution and NO2 Emissions

Science.gov (United States)

Lamsal, L. N.; Martin, R. V.; Krotkov, N. A.; Bucsela, E. J.; Celarier, E. A.; vanDonkelaar, A.; Parrish, D.

2012-01-01

Nitrogen oxides (NO(x)) are key actors in air quality and climate change. Satellite remote sensing of tropospheric NO2 has developed rapidly with enhanced spatial and temporal resolution since initial observations in 1995. We have developed an improved algorithm and retrieved tropospheric NO2 columns from Ozone Monitoring Instrument. Column observations of tropospheric NO2 from the nadir-viewing satellite sensors contain large contributions from the boundary layer due to strong enhancement of NO2 in the boundary layer. We infer ground-level NO2 concentrations from the OMI satellite instrument which demonstrate significant agreement with in-situ surface measurements. We examine how NO2 columns measured by satellite, ground-level NO2 derived from satellite, and NO(x) emissions obtained from bottom-up inventories relate to world's urban population. We perform inverse modeling analysis of NO2 measurements from OMI to estimate "top-down" surface NO(x) emissions, which are used to evaluate and improve "bottom-up" emission inventories. We use NO2 column observations from OMI and the relationship between NO2 columns and NO(x) emissions from a GEOS-Chem model simulation to estimate the annual change in bottom-up NO(x) emissions. The emission updates offer an improved estimate of NO(x) that are critical to our understanding of air quality, acid deposition, and climate change.

Tropospheric Emissions: Monitoring of Pollution (TEMPO)

Science.gov (United States)

Chance, Kelly; Liu, Xiong; Suleiman, Raid M.; Flittner, David E.; Al-Saadi, Jassim; Janz, Scott J.

2014-06-01

TEMPO, selected by NASA as the first Earth Venture Instrument, will measure atmospheric pollution for greater North America from space using ultraviolet and visible spectroscopy. TEMPO measures from Mexico City to the Canadian oil sands, and from the Atlantic to the Pacific, hourly and at high spatial resolution. TEMPO provides a tropospheric measurement suite that includes the key elements of tropospheric air pollution chemistry. Measurements are from geostationary (GEO) orbit, to capture the inherent high variability in the diurnal cycle of emissions and chemistry. The small product spatial footprint resolves pollution sources at sub-urban scale. Together, this temporal and spatial resolution improves emission inventories, monitors population exposure, and enables effective emission-control strategies. TEMPO takes advantage of a GEO host spacecraft to provide a modest-cost mission that measures the spectra required to retrieve O3, NO2, SO2, H2CO, C2H2O2, H2O, aerosols, cloud parameters, and UVB radiation. TEMPO thus measures the major elements, directly or by proxy, in the tropospheric O3 chemistry cycle. Multi-spectral observations provide sensitivity to O3 in the lowermost troposphere, reducing uncertainty in air quality predictions by 50 %. TEMPO quantifies and tracks the evolution of aerosol loading. It provides near-real-time air quality products that will be made widely, publicly available. TEMPO makes the first tropospheric trace gas measurements from GEO, by building on the heritage of five spectrometers flown in low-earth-orbit (LEO). These LEO instruments measure the needed spectra, although at coarse spatial and temporal resolutions, to the precisions required for TEMPO and use retrieval algorithms developed for them by TEMPO Science Team members and currently running in operational environments. This makes TEMPO an innovative use of a well-proven technique, able to produce a revolutionary data set. TEMPO provides much of the atmospheric measurement

Filling-in of Near-infrared Solar Lines by Terrestrial Fluorescence and Other Geophysical Effects: Simulations and Space-based Observations from SCIAMACHY and GOSAT

Science.gov (United States)

Joiner, Joanna (Editor); Yoshida, Yasuko; Vasilkov, A. P.; Middleton, E. M. (Editor); Campbell, P. K. E.; Yoshida, Y.; Huze, A.; Corp, L. A.

2012-01-01

Global mapping of terrestrial vegetation fluorescence from space has recently been accomplished with high spectral resolution (nu/nu greater than 35 000) measurements from the Japanese Greenhouse gases Observing SAellite (GOSAT). These data are of interest because they can potentially provide global information on the functional status of vegetation including light-use efficiency and global primary productivity that can be used for global carbon cycle modeling. Quantifying the impact of fluorescence on the O2-A band is important as this band is used for photon pathlength characterization in cloud- and aerosol-contaminated pixels for trace-gas retrievals including CO2. Here, we examine whether fluorescence information can be derived from space using potentially lower-cost hyperspectral instrumentation, i.e., more than an order of magnitude less spectral resolution (nu/nu approximately 1600) than GOSAT, with a relatively simple algorithm. We discuss laboratory measurements of fluorescence near one of the few wide and deep solar Fraunhofer lines in the long-wave tail of the fluorescence emission region, the calcium (Ca) II line at 866 nm that is observable with a spectral resolution of approximately 0.5 nm. The filling-in of the Ca II line due to additive signals from various atmospheric and terrestrial effects, including fluorescence, is simulated. We then examine filling-in of this line using the SCanning Imaging Absorption spectroMeter for Atmospheric CHartographY (SCIAMACHY) satellite instrument. In order to interpret the satellite measurements, we developed a general approach to correct for various instrumental artifacts that produce false filling-in of solar lines in satellite measurements. The approach is applied to SCIAMACHY at the 866 nm Ca II line and to GOSAT at 758 and 770 nm on the shoulders of the O2-A feature where there are several strong solar Fraunhofer lines that are filled in primarily by vegetation fluorescence. Finally, we compare temporal and

Characteristics of the NO-NO2-O3 system in different chemical regimes during the MIRAGE-Mex field campaign

Directory of Open Access Journals (Sweden)

X. Tie

2008-12-01

Full Text Available The NO-NO2 system was analyzed in different chemical regimes/air masses based on observations of reactive nitrogen species and peroxy radicals made during the intensive field campaign MIRAGE-Mex (4 to 29 March 2006. The air masses were categorized into 5 groups based on combinations of macroscopic observations, geographical location, meteorological parameters, models, and observations of trace gases: boundary layer (labeled as "BL", biomass burning ("BB", free troposphere (continental, "FTCO" and marine, "FTMA", and Tula industrial complex ("TIC". In general, NO2/NO ratios in different air masses are near photostationary state. Analysis of this ratio can be useful for testing current understanding of tropospheric chemistry. The ozone production efficiency (OPE for the 5 air mass categories ranged from 4.5 (TIC to 8.5 (FTMA, consistent with photochemical aging of air masses exiting the Mexico City Metropolitan Area.

Quantifying the causes of differences in tropospheric OH within global models

Science.gov (United States)

Nicely, Julie M.; Salawitch, Ross J.; Canty, Timothy; Anderson, Daniel C.; Arnold, Steve R.; Chipperfield, Martyn P.; Emmons, Louisa K.; Flemming, Johannes; Huijnen, Vincent; Kinnison, Douglas E.; Lamarque, Jean-François; Mao, Jingqiu; Monks, Sarah A.; Steenrod, Stephen D.; Tilmes, Simone; Turquety, Solene

2017-02-01

The hydroxyl radical (OH) is the primary daytime oxidant in the troposphere and provides the main loss mechanism for many pollutants and greenhouse gases, including methane (CH4). Global mean tropospheric OH differs by as much as 80% among various global models, for reasons that are not well understood. We use neural networks (NNs), trained using archived output from eight chemical transport models (CTMs) that participated in the Polar Study using Aircraft, Remote Sensing, Surface Measurements and Models, of Climate, Chemistry, Aerosols and Transport Model Intercomparison Project (POLMIP), to quantify the factors responsible for differences in tropospheric OH and resulting CH4 lifetime (τCH4) between these models. Annual average τCH4, for loss by OH only, ranges from 8.0 to 11.6 years for the eight POLMIP CTMs. The factors driving these differences were quantified by inputting 3-D chemical fields from one CTM into the trained NN of another CTM. Across all CTMs, the largest mean differences in τCH4 (ΔτCH4) result from variations in chemical mechanisms (ΔτCH4 = 0.46 years), the photolysis frequency (J) of O3 → O(1D) (0.31 years), local O3 (0.30 years), and CO (0.23 years). The ΔτCH4 due to CTM differences in NOx (NO + NO2) is relatively low (0.17 years), although large regional variation in OH between the CTMs is attributed to NOx. Differences in isoprene and J(NO2) have negligible overall effect on globally averaged tropospheric OH, although the extent of OH variations due to each factor depends on the model being examined. This study demonstrates that NNs can serve as a useful tool for quantifying why tropospheric OH varies between global models, provided that essential chemical fields are archived.

Source attribution of tropospheric ozone

Science.gov (United States)

Butler, T. M.

2015-12-01

Tropospheric ozone is a harmful pollutant with adverse effects on human health and ecosystems. As well as these effects, tropospheric ozone is also a powerful greenhouse gas, with an anthropogenic radiative forcing one quarter of that of CO2. Along with methane and atmospheric aerosol, tropospheric ozone belongs to the so-called Short Lived Climate forcing Pollutants, or SLCP. Recent work has shown that efforts to reduce concentrations of SLCP in the atmosphere have the potential to slow the rate of near-term climate change, while simultaneously improving public health and reducing crop losses. Unlike many other SLCP, tropospehric ozone is not directly emitted, but is instead influenced by two distinct sources: transport of air from the ozone-rich stratosphere; and photochemical production in the troposphere from the emitted precursors NOx (oxides of nitrogen), CO (Carbon Monoxide), and VOC (volatile organic compounds, including methane). Better understanding of the relationship between ozone production and the emissions of its precursors is essential for the development of targeted emission reduction strategies. Several modeling methods have been employed to relate the production of tropospheric ozone to emissions of its precursors; emissions perturbation, tagging, and adjoint sensitivity methods all deliver complementary information about modelled ozone production. Most studies using tagging methods have focused on attribution of tropospheric ozone production to emissions of NOx, even though perturbation methods have suggested that tropospheric ozone is also sensitive to VOC, particularly methane. In this study we describe the implementation into a global chemistry-climate model of a scheme for tagging emissions of NOx and VOC with an arbitrary number of labels, which are followed through the chemical reactions of tropospheric ozone production in order to perform attribution of tropospehric ozone to its emitted precursors. Attribution is performed to both

Estimating 40 years of nitrogen deposition in global biomes using the SCIAMACHY NO2 column

Science.gov (United States)

Lu, Xuehe; Zhang, Xiuying; Liu, Jinxun; Jin, Jiaxin

2016-01-01

Owing to human activity, global nitrogen (N) cycles have been altered. In the past 100 years, global N deposition has increased. Currently, the monitoring and estimating of N deposition and the evaluation of its effects on global carbon budgets are the focus of many researchers. NO2 columns retrieved by space-borne sensors provide us with a new way of exploring global N cycles and these have the ability to estimate N deposition. However, the time range limitation of NO2 columns makes the estimation of long timescale N deposition difficult. In this study we used ground-based NOx emission data to expand the density of NO2columns, and 40 years of N deposition (1970–2009) was inverted using the multivariate linear model with expanded NO2 columns. The dynamic of N deposition was examined in both global and biome scales. The results show that the average N deposition was 0.34 g N m–2 year–1 in the 2000s, which was an increase of 38.4% compared with the 1970s’. The total N deposition in different biomes is unbalanced. N deposition is only 38.0% of the global total in forest biomes; this is made up of 25.9%, 11.3, and 0.7% in tropical, temperate, and boreal forests, respectively. As N-limited biomes, there was little increase of N deposition in boreal forests. However, N deposition has increased by a total of 59.6% in tropical forests and croplands, which are N-rich biomes. Such characteristics may influence the effects on global carbon budgets.

Tropospheric mixing ratios of NO and NOy obtained during TROPOZ II in the latitude region 67 deg N-56 deg S

Energy Technology Data Exchange (ETDEWEB)

Rohrer, F.; Bruening, D.; Ehhalt, D.H. [Forschungszentrum Juelich GmbH (Germany). Inst. fuer Atmosphaerische Chemie

1997-12-31

Tropospheric mixing ratios of NO and NOy were measured along the flight track of the TROPOZ II aircraft campaign. These measurements cover regions along the east coast of North America, the Pacific and Atlantic coast of South America and the Atlantic coast of North Africa and Europe. The meteorological conditions are close to the climatological mean: westerly winds at high and mid latitudes, variable and weak winds at low latitudes. (author) 2 refs.

Tropospheric mixing ratios of NO and NOy obtained during TROPOZ II in the latitude region 67 deg N-56 deg S

Energy Technology Data Exchange (ETDEWEB)

Rohrer, F; Bruening, D; Ehhalt, D H [Forschungszentrum Juelich GmbH (Germany). Inst. fuer Atmosphaerische Chemie

1998-12-31

Tropospheric mixing ratios of NO and NOy were measured along the flight track of the TROPOZ II aircraft campaign. These measurements cover regions along the east coast of North America, the Pacific and Atlantic coast of South America and the Atlantic coast of North Africa and Europe. The meteorological conditions are close to the climatological mean: westerly winds at high and mid latitudes, variable and weak winds at low latitudes. (author) 2 refs.

Impact of climate variability on tropospheric ozone

International Nuclear Information System (INIS)

Grewe, Volker

2007-01-01

A simulation with the climate-chemistry model (CCM) E39/C is presented, which covers both the troposphere and stratosphere dynamics and chemistry during the period 1960 to 1999. Although the CCM, by its nature, is not exactly representing observed day-by-day meteorology, there is an overall model's tendency to correctly reproduce the variability pattern due to an inclusion of realistic external forcings, like observed sea surface temperatures (e.g. El Nino), major volcanic eruption, solar cycle, concentrations of greenhouse gases, and Quasi-Biennial Oscillation. Additionally, climate-chemistry interactions are included, like the impact of ozone, methane, and other species on radiation and dynamics, and the impact of dynamics on emissions (lightning). However, a number of important feedbacks are not yet included (e.g. feedbacks related to biogenic emissions and emissions due to biomass burning). The results show a good representation of the evolution of the stratospheric ozone layer, including the ozone hole, which plays an important role for the simulation of natural variability of tropospheric ozone. Anthropogenic NO x emissions are included with a step-wise linear trend for each sector, but no interannual variability is included. The application of a number of diagnostics (e.g. marked ozone tracers) allows the separation of the impact of various processes/emissions on tropospheric ozone and shows that the simulated Northern Hemisphere tropospheric ozone budget is not only dominated by nitrogen oxide emissions and other ozone pre-cursors, but also by changes of the stratospheric ozone budget and its flux into the troposphere, which tends to reduce the simulated positive trend in tropospheric ozone due to emissions from industry and traffic during the late 80s and early 90s. For tropical regions the variability in ozone is dominated by variability in lightning (related to ENSO) and stratosphere-troposphere exchange (related to Northern Hemisphere Stratospheric

The ENVISAT Atmospheric Chemistry mission (GOMOS, MIPAS and SCIAMACHY) -Instrument status and mission evolution

Science.gov (United States)

Dehn, Angelika

atmospheric instruments and their applications: GOMOS, MIPAS and SCIAMACHY", ESA Bulletin (ISSN 0376-4265), No. 106, p. 77 -87 (2001) [2] J. Frerick, B. Duesmann, and M. Canela, "2010 and beyond -The ENVISAT mission extension", Proc. `Envisat Symposium 2007', Montreux, Switzerland, 23-27 April 2007 (ESA SP-636, July 2007)

DOAS measurements of NO2 from an ultralight aircraft during the Earth Challenge expedition

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O. Ronveaux

2012-08-01

Full Text Available We report on airborne Differential Optical Absorption Spectroscopy (DOAS measurements of NO2 tropospheric columns above South Asia, the Arabic peninsula, North Africa, and Italy in November and December 2009. The DOAS instrument was installed on an ultralight aircraft involved in the Earth Challenge project, an expedition of seven pilots flying on four ultralight aircraft between Australia and Belgium. The instrument recorded spectra in limb geometry with a large field of view, a set-up which provides a high sensitivity to the boundary layer NO2 while minimizing the uncertainties related to the attitude variations. We compare our measurements with OMI (Ozone Monitoring Instrument and GOME-2 (Global Ozone Monitoring Experiment 2 tropospheric NO2 products when the latter are available. Above Rajasthan and the Po Valley, two areas where the NO2 field is homogeneous, data sets agree very well. Our measurements in these areas are 0.1 ± 0.1 to 3 ± 1 × 1015 molec cm−2 and 2.6 ± 0.8 × 1016 molec cm−2, respectively. Flying downwind of Riyadh, our NO2 measurements show the structure of the megacity's exhaust plume with a higher spatial resolution than OMI. Moreover, our measurements are larger (up to 40% than those seen by satellites. We also derived tropospheric columns when no satellite data were available if it was possible to get information on the visibility from satellite measurements of aerosol optical thickness. This experiment also provides a confirmation for the recent finding of a soil signature above desert.

Predicting tropospheric ozone and hydroxyl radical in a global, three-dimensional, chemistry, transport, and deposition model

Energy Technology Data Exchange (ETDEWEB)

Atherton, C.S.

1995-01-05

Two of the most important chemically reactive tropospheric gases are ozone (O{sub 3}) and the hydroxyl radical (OH). Although ozone in the stratosphere is a necessary protector against the sun`s radiation, tropospheric ozone is actually a pollutant which damages materials and vegetation, acts as a respiratory irritant, and is a greenhouse gas. One of the two main sources of ozone in the troposphere is photochemical production. The photochemistry is initiated when hydrocarbons and carbon monoxide (CO) react with nitrogen oxides (NO{sub x} = NO + NO{sub 2}) in the presence of sunlight. Reaction with the hydroxyl radical, OH, is the main sink for many tropospheric gases. The hydroxyl radical is highly reactive and has a lifetime on the order of seconds. Its formation is initiated by the photolysis of tropospheric ozone. Tropospheric chemistry involves a complex, non-linear set of chemical reactions between atmospheric species that vary substantially in time and space. To model these and other species on a global scale requires the use of a global, three-dimensional chemistry, transport, and deposition (CTD) model. In this work, I developed two such three dimensional CTD models. The first model incorporated the chemistry necessary to model tropospheric ozone production from the reactions of nitrogen oxides with carbon monoxide (CO) and methane (CH{sub 4}). The second also included longer-lived alkane species and the biogenic hydrocarbon isoprene, which is emitted by growing plants and trees. The models` ability to predict a number of key variables (including the concentration of O{sub 3}, OH, and other species) were evaluated. Then, several scenarios were simulated to understand the change in the chemistry of the troposphere since preindustrial times and the role of anthropogenic NO{sub x} on present day conditions.

Tropospheric Emissions: Monitoring of Pollution Overview

Science.gov (United States)

Chance, Kelly; Liu, Xiong; Suleiman, Raid M.; Flittner, David; Al-Saadi, Jay; Janz, Scott

2015-01-01

TEMPO is now well into its implementation phase, having passed both its Key Decision Point C and the Critical Design Review (CDR) for the instrument. The CDR for the ground systems will occur in March 2016 and the CDR for the Mission component at a later date, after the host spacecraft has been selected. TEMPO is on schedule to measure atmospheric pollution for greater North America from space using ultraviolet and visible spectroscopy. TEMPO measures from Mexico City to the Canadian oil sands, and from the Atlantic to the Pacific, hourly and at high spatial resolution. TEMPO provides a tropospheric measurement suite that includes the key elements of tropospheric air pollution chemistry. Measurements are from geostationary (GEO) orbit, to capture the inherent high variability in the diurnal cycle of emissions and chemistry. The small product spatial footprint resolves pollution sources at sub-urban scale. Together, this temporal and spatial resolution improves emission inventories, monitors population exposure, and enables effective emission-control strategies. TEMPO takes advantage of a GEO host spacecraft to provide a modest cost mission that measures the spectra required to retrieve O3, NO2, SO2, H2CO, C2H2O2, H2O, aerosols, cloud parameters, and UVB radiation. TEMPO thus measures the major elements, directly or by proxy, in the tropospheric O3 chemistry cycle. Multi-spectral observations provide sensitivity to O3 in the lowermost troposphere, substantially reducing uncertainty in air quality predictions by 50 percent. TEMPO quantifies and tracks the evolution of aerosol loading. It provides near-real-time air quality products that will be made widely, publicly available. TEMPO provides much of the atmospheric measurement capability recommended for GEO-CAPE in the 2007 National Research Council Decadal Survey, Earth Science and Applications from Space: National Imperatives for the Next Decade and Beyond. Instruments from Europe (Sentinel 4) and Asia (GEMS) will

Tropospheric Ozone from the TOMS TDOT (TOMS-Direct-Ozone-in-Troposphere) Technique During SAFARI-2000

Science.gov (United States)

Stone, J. B.; Thompson, A. M.; Frolov, A. D.; Hudson, R. D.; Bhartia, P. K. (Technical Monitor)

2002-01-01

There are a number of published residual-type methods for deriving tropospheric ozone from TOMS (Total Ozone Mapping Spectrometer). The basic concept of these methods is that within a zone of constant stratospheric ozone, the tropospheric ozone column can be computed by subtracting stratospheric ozone from the TOMS Level 2 total ozone column, We used the modified-residual method for retrieving tropospheric ozone during SAFARI-2000 and found disagreements with in-situ ozone data over Africa in September 2000. Using the newly developed TDOT (TOMS-Direct-Ozone-in-Troposphere) method that uses TOMS radiances and a modified lookup table based on actual profiles during high ozone pollution periods, new maps were prepared and found to compare better to soundings over Lusaka, Zambia (15.5 S, 28 E), Nairobi and several African cities where MOZAIC aircraft operated in September 2000. The TDOT technique and comparisons are described in detail.

Evaluation of balloon and satellite water vapour measurements in the Southern tropical and subtropical UTLS during the HIBISCUS campaign

Science.gov (United States)

Montoux, N.; Hauchecorne, A.; Pommereau, J.-P.; Lefèvre, F.; Durry, G.; Jones, R. L.; Rozanov, A.; Dhomse, S.; Burrows, J. P.; Morel, B.; Bencherif, H.

2009-07-01

Balloon water vapour in situ and remote measurements in the tropical upper troposphere and lower stratosphere (UTLS) obtained during the HIBISCUS campaign around 20° S in Brazil in February-March 2004 using a tunable diode laser (μSDLA), a surface acoustic wave (SAW) and a Vis-NIR solar occultation spectrometer (SAOZ) on a long duration balloon, have been used for evaluating the performances of satellite borne remote water vapour instruments available at the same latitude and measurement period. In the stratosphere, HALOE displays the best precision (2.5%), followed by SAGE II (7%), MIPAS (10%), SAOZ (20-25%) and SCIAMACHY (35%), all of which show approximately constant H2O mixing ratios between 20-25 km. Compared to HALOE of ±10% accuracy between 0.1-100 hPa, SAGE II and SAOZ show insignificant biases, MIPAS is wetter by 10% and SCIAMACHY dryer by 20%. The currently available GOMOS profiles of 25% precision show a positive vertical gradient in error for identified reasons. Compared to these, the water vapour of the Reprobus Chemistry Transport Model, forced at pressures higher than 95 hPa by the ECMWF analyses, is dryer by about 1 ppmv (20%). In the lower stratosphere between 16-20 km, most notable features are the steep degradation of MIPAS precision below 18 km, and the appearance of biases between instruments far larger than their quoted total uncertainty. HALOE and SAGE II (after spectral adjustment for reducing the bias with HALOE at northern mid-latitudes) both show decreases of water vapour with a minimum at the tropopause not seen by other instruments or the model, possibly attributable to an increasing error in the HALOE altitude registration. Between 16-18 km where the water vapour concentration shows little horizontal variability, and where the μSDLA balloon measurements are not perturbed by outgassing, the average mixing ratios reported by the remote sensing instruments are substantially lower than the 4-5 ppmv observed by the μSDLA. Differences

A photostationary state analysis of the NO2-NO system based on airborne observations from the subtropical/tropical North and South Atlantic

Science.gov (United States)

Davis, D. D.; Chen, G.; Chameides, W.; Bradshaw, J.; Sandholm, S.; Rodgers, M.; Schendal, J.; Madronich, S.; Sachse, G.; Gregory, G.

1993-01-01

The Chemical Instrumentation Test and Evaluation 3 (CITE 3) NO-NO2 database has provided a unique opportunity to examine important aspects of tropospheric photochemistry as related to the rapid cycling between NO and NO2. Our results suggest that when quantitative testing of this photochemical system is based on airborne field data, extra precautions may need to be taken in the analysis. This was particularly true in the CITE 3 data analysis where different regional environments produced quite different results when evaluating the photochemical test ratio (NO2)(sub expt)/(NO2)(sub calc), designated here as R(sub E)/R(sub C). The quantity (NO2)(sub Calc) was evaluated using the following photostationary state expression: (NO2)(sub Calc) = k(sub 1)(O3) + k(sub 4)(HO2) + k(sub 5)(CH3O2) + k(sub 6)(RO2))(NO)(sub Expt)/J(sub 2). The four most prominent regional environmental data sets identified in this analysis were those labeled here as free-tropospheric northern hemisphere (FTNH), free-tropospheric tropical northern hemisphere (FTTNH), free-tropospheric southern hemisphere (FTSH), and tropical-marine boundary layer (plume) (TMBL(P)). The respective R(sub E)/R(sub C) mean and median values for these four data subsets were 1.74, 1.69; 3.00, 2.79; 1.01, 0.97; and 0.99, 0.94. Of the four data subsets listed, the two that were statistically the most robust were FTNH and FTSH; for these the respective R(sub E)/R(sub C) mean and standard deviation of the mean values were 1.74 +/- 0.07 and 1.01 +/- 0.04. The FTSH observations were in good agreement with theory, whereas those from the FTNH data set were in significant disagreement. An examination of the critical photochemical parameters O3, UV(zenith), NO, NO2, and non-methane hydrocarbons (NMHCs) for these two databases indicated that the most likely source of the R(sub E)/R(sub C) bias in the FTNH results was the presence of a systematic error in the observational data rather than a shortening in our understanding of

SOLAR VARIABILITY FROM 240 TO 1750 nm IN TERMS OF FACULAE BRIGHTENING AND SUNSPOT DARKENING FROM SCIAMACHY

International Nuclear Information System (INIS)

Pagaran, J.; Weber, M.; Burrows, J.

2009-01-01

The change of spectral decomposition of the total radiative output on various timescales of solar magnetic activity is of large interest to terrestrial and solar-stellar atmosphere studies. Starting in 2002, SCIAMACHY was the first satellite instrument to observe daily solar spectral irradiance (SSI) continuously from 230 nm (UV) to 1750 nm (near-infrared; near-IR). In order to address the question of how much UV, visible (vis), and IR spectral regions change on 27 day and 11 year timescales, we parameterize short-term SSI variations in terms of faculae brightening (Mg II index) and sunspot darkening (photometric sunspot index) proxies. Although spectral variations above 300 nm are below 1% and, therefore, well below the accuracy of absolute radiometric calibration, relative accuracy for short-term changes is shown to be in the per mill range. This enables us to derive short-term spectral irradiance variations from the UV to the near-IR. During Halloween solar storm in 2003 with a record high sunspot area, we observe a reduction of 0.3% in the near-IR to 0.5% in the vis and near-UV. This is consistent with a 0.4% reduction in total solar irradiance (TSI). Over an entire 11 year solar cycle, SSI variability covering simultaneously the UV, vis, and IR spectral regions have not been directly observed so far. Using variations of solar proxies over solar cycle 23, solar cycle spectral variations have been estimated using scaling factors that best matched short-term variations of SCIAMACHY. In the 300-400 nm region, which strongly contributes to TSI solar cycle change, a contribution of 34% is derived from SCIAMACHY observations, which is lower than the reported values from SUSIM satellite data and the empirical SATIRE model. The total UV contribution (below 400 nm) to TSI solar cycle variations is estimated to be 55%.

Performance Evaluation of Blind Tropospheric Delay correction ...

African Journals Online (AJOL)

lekky

and Temperature 2 wet (GPT2w) models) for tropospheric delay correction, ... In practice, a user often employs a certain troposphere model based on the popularity ... comparisons between some of the models have been carried out in the past for .... prediction of meteorological parameter values, which are then used to ...

The Governing Processes and Timescales of Stratosphere-to-Troposphere Transport and its Contribution to Ozone in the Arctic Troposphere

Science.gov (United States)

Liang, Q.; Douglass, A. R.; Duncan, B. N.; Stolarski, R. S.; Witte, J. C.

2009-01-01

We used the seasonality of a combination of atmospheric trace gases and idealized tracers to examine stratosphere-to-troposphere transport and its influence on tropospheric composition in the Arctic. Maximum stratosphere-to-troposphere transport of CFCs and O3 occurs in April as driven by the Brewer-Dobson circulation. Stratosphere-troposphere exchange (STE) occurs predominantly between 40 deg N to 80 deg N with stratospheric influx in the mid-latitudes (30-70 deg N) accounting for 67.81 percent of the air of stratospheric origin in the Northern Hemisphere extratropical troposphere. Transport from the lower stratosphere to the lower troposphere (LT) takes three months on average, one month to cross the tropopause, the second month to travel from the upper troposphere (UT) to the middle troposphere (MT), and the third month to reach the LT. During downward transport, the seasonality of a trace gas can be greatly impacted by wet removal and chemistry. A comparison of idealized tracers with varying lifetimes suggests that when initialized with the same concentrations and seasonal cycles at the tropopause, trace gases that have shorter lifetimes display lower concentrations, smaller amplitudes, and earlier seasonal maxima during transport to the LT. STE contributes to O3 in the Arctic troposphere directly from the transport of O3 and indirectly from the transport of NOy . Direct transport of O3 from the stratosphere accounts for 78 percent of O3 in the Arctic UT with maximum contributions occurring from March to May. The stratospheric contribution decreases significantly in the MT/LT (20.25 percent of total O3) and shows a very weak March.April maximum. Our NOx budget analysis in the Arctic UT shows that during spring and summer, the stratospheric injection of NO y-rich air increases NOx concentrations above the 20 pptv threshold level, thereby shifting the Arctic UT from a regime of net photochemical ozone loss to one of net production with rates as high as +16 ppbv/month.

Photochemical ozone production in tropical squall line convection during NASA Global Tropospheric Experiment/Amazon Boundary Layer Experiment 2A

Science.gov (United States)

Pickering, Kenneth E.; Thompson, Anne M.; Tao, Wei-Kuo; Simpson, Joanne; Scala, John R.

1991-01-01

The role of convection was examined in trace gas transport and ozone production in a tropical dry season squall line sampled on August 3, 1985, during NASA Global Tropospheric Experiment/Amazon Boundary Layer Experiment 2A (NASA GTE/ABLE 2A) in Amazonia, Brazil. Two types of analyses were performed. Transient effects within the cloud are examined with a combination of two-dimensional cloud and one-dimensional photochemical modeling. Tracer analyses using the cloud model wind fields yield a series of cross sections of NO(x), CO, and O3 distribution during the lifetime of the cloud; these fields are used in the photochemical model to compute the net rate of O3 production. At noon, when the cloud was mature, the instantaneous ozone production potential in the cloud is between 50 and 60 percent less than in no-cloud conditions due to reduced photolysis and cloud scavenging of radicals. Analysis of cloud inflows and outflows is used to differentiate between air that is undisturbed and air that has been modified by the storm. These profiles are used in the photochemical model to examine the aftereffects of convective redistribution in the 24-hour period following the storm. Total tropospheric column O3 production changed little due to convection because so little NO(x) was available in the lower troposphere. However, the integrated O3 production potential in the 5- to 13-km layer changed from net destruction to net production as a result of the convection. The conditions of the August 3, 1985, event may be typical of the early part of the dry season in Amazonia, when only minimal amounts of pollution from biomass burning have been transported into the region.

GOME-2 observations of oxygenated VOCs: what can we learn from the ratio glyoxal to formaldehyde on a global scale?

Directory of Open Access Journals (Sweden)

M. Vrekoussis

2010-11-01

Full Text Available Collocated data sets of glyoxal (CHO.CHO and formaldehyde (HCHO were retrieved for the first time from measurements of the Global Ozone Monitoring Experiment-2 (GOME-2 during the first two years of operation in 2007 and 2008. Both oxygenated Volatile Organic Compounds, OVOC, are key intermediate species produced during the oxidation of precursor hydrocarbons. Their short lifetime of a few hours in the lower troposphere links them to emission sources and makes them useful tracers of photochemical activity. The global composite maps of GOME-2 HCHO and CHO.CHO have strong similarities confirming their common atmospheric and/or surface sources. The highest column amounts of these OVOCs are recorded over regions with enhance biogenic emissions (e.g. tropical forests in South America, Africa and Indonesia. Enhanced OVOC values are also present over areas of anthropogenic activity and biomass burning (e.g. over China, N. America, Europe and Australia. The ratio of CHO.CHO to HCHO, R_GF, has been used, for the first time on a global scale, to classify the sources according to biogenic and/or anthropogenic emissions of the precursors; R_GF between 0.040 to 0.060 point to the existence of biogenic emissions with the highest values being observed at the highest Enhanced Vegetation Index, EVI. R_GFs below 0.040 are indicative of anthropogenic emissions and associated with high levels of NO₂. This decreasing tendency of R_GF with increasing NO₂ is also observed when analyzing data for individual large cities, indicating that it is a common feature. The results obtained for R_GF from GOME-2 data are compared with the findings based on regional SCIAMACHY observations showing good agreement. This is explained by the excellent correlation of the global retrieved column amounts of CHO.CHO and HCHO from the GOME-2 and SCIAMACHY instruments for the period 2007

SO2 over Central China: Measurements, Numerical Simulations and the Tropospheric Sulfur Budget

Science.gov (United States)

He, Hao; Li, Can; Loughner, Christopher P.; Li, Zhangqing; Krotkov, Nickolay A.; Yang, Kai; Wang, Lei; Zheng, Youfei; Bao, Xiangdong; Zhao, Guoqiang;

Global financial crisis making a V-shaped fluctuation in NO2 pollution over the Yangtze River Delta

Science.gov (United States)

Du, Yin; Xie, Zhiqing

2017-04-01

The Yangtze River Delta (YRD), China's main cultural and economic center, has become one of the most seriously polluted areas in the world with respect to nitrogen oxides (NOx), owing to its rapid industrialization and urbanization, as well as substantial coal consumption. On the basis of nitrogen dioxide (NO2) density data from ozone monitoring instrument (OMI) and ground-based observations, the effects of industrial fluctuations due to the financial crisis on local NO2 pollution were quantitatively assessed. The results were as follows. (1) A distinct V-shaped fluctuation of major industrial products, thermal generating capacity, electricity consumption, and tropospheric NO2 densities was associated with the global financial crisis from May 2007 to December 2009, with the largest anomalies 1.5 times more than standard deviations at the height of the crisis period from November 2008 to February 2009. (2) Among all industrial sectors, thermal power plants were mainly responsible for fluctuations in local NO2 pollution during the crisis period. Thermal generating capacity had its greatest decrease of 12.10% at the height of the crisis compared with that during November 2007-February 2008, leading to local tropospheric NO2 density decreasing by 16.97%. As the crisis appeased, thermal generating capacity increased by 29.63% from November 2009 to February 2010, and tropospheric NO2 densities correspondingly increased by 30.07%. (3) Among all industrial sectors in the YRD, the thermal power sector has the greatest coal consumption of about 65.96%. A decline in thermal power of about 10% can induce a decrease of about 30% in NOx emissions and NO2 densities, meaning that a relative small fluctuation in industrial production can lead to a large decrease in tropospheric NO2 densities over industrially developed areas like the YRD region. Since electricity is mainly obtained from local coal-burning thermal plants without NOx-processing equipment, installing NOx

Implementation of Tropospheric Emissions: Monitoring of Pollution (TEMPO)

Science.gov (United States)

Chance, K.; Liu, X.; Suleiman, R. M.; Flittner, D. E.; Al-Saadi, J. A.; Janz, S. J.

2014-12-01

The updated status of TEMPO, as it proceeds from formulation phase into implementation phase is presented. TEMPO, the first NASA Earth Venture Instrument, will measure atmospheric pollution for greater North America from space using ultraviolet and visible spectroscopy. TEMPO measures from Mexico City to the Canadian oil sands, and from the Atlantic to the Pacific, hourly and at high spatial resolution. TEMPO provides a tropospheric measurement suite that includes the key elements of tropospheric air pollution chemistry. Measurements are from geostationary (GEO) orbit, to capture the inherent high variability in the diurnal cycle of emissions and chemistry. The small product spatial footprint resolves pollution sources at sub-urban scale. Together, this temporal and spatial resolution improves emission inventories, monitors population exposure, and enables effective emission-control strategies. TEMPO takes advantage of a GEO host spacecraft to provide a modest cost mission that measures the spectra required to retrieve O3, NO2, SO2, H2CO, C2H2O2, H2O, aerosols, cloud parameters, and UVB radiation. TEMPO thus measures the major elements, directly or by proxy, in the tropospheric O3 chemistry cycle. Multi-spectral observations provide sensitivity to O3 in the lowermost troposphere, reducing uncertainty in air quality predictions by 50%. TEMPO quantifies and tracks the evolution of aerosol loading. It provides near-real-time air quality products that will be made widely, publicly available. TEMPO provides much of the atmospheric measurement capability recommended for GEO-CAPE in the 2007 National Research Council Decadal Survey, Earth Science and Applications from Space: National Imperatives for the Next Decade and Beyond. GEO-CAPE is not planned for implementation this decade. However, instruments from Europe (Sentinel 4) and Asia (GEMS) will form parts of a global GEO constellation for pollution monitoring later this decade, with a major focus on intercontinental

Model and algorithm development for the retrieval of atmospheric aerosol properties from nadir mode measurements by the DOAS instrument SCIAMACHY onboard Envisat

OpenAIRE

Sanghavi, Suniti Vinod

2008-01-01

Der Einfluss von Aerosolen auf den Strahlungshaushalt der Atmosphäre ist mit grossen Unsicherheiten verbunden und bedarf intensiver Forschung. In dieser Arbeit wurde ein Inversionsalgorithmus entwickelt, um aus Daten des SCIAMACHY-Spektrometers an Bord von Envisat die optische Dichte von Aerosolen (AOT), deren Angstrom Exponent sowie die vertikale Höhenverteilung unter Verwendung von Spektren im Bereich der O2 A- und B-Banden abzuleiten. Modellieren gemessener Reflektanzen ist für die Bestimm...

Tropospheric Ozone as a Short-lived Chemical Climate Forcer

Science.gov (United States)

Pickering, Kenneth E.

2012-01-01

Tropospheric ozone is the third most important greenhouse gas according to the most recent IPCC assessment. However, tropospheric ozone is highly variable in both space and time. Ozone that is located in the vicinity of the tropopause has the greatest effect on climate forcing. Nitrogen oxides (NOx) are the most important precursors for ozone In most of the troposphere. Therefore, pollution that is lofted upward in thunderstorm updrafts or NOx produced by lightning leads to efficient ozone production in the upper troposphere, where ozone is most important climatically. Global and regional model estimates of the impact of North American pollution and lightning on ozone radiative forcing will be presented. It will be shown that in the Northern Hemisphere summer, the lightning effect on ozone radiative forcing can dominate over that of pollution, and that the radiative forcing signal from North America extends well into Europe and North Africa. An algorithm for predicting lightning flash rates and estimating lightning NOx emissions is being incorporated into the NASA GEOS-5 Chemistry and Climate Model. Changes in flash rates and emissions over an ENSO cycle and in future climates will be assessed, along with the resulting changes in upper tropospheric ozone. Other research on the production of NOx per lightning flash and its distribution in the vertical based on cloud-resolving modeling and satellite observations will be presented. Distributions of NO2 and O3 over the Middle East from the OMI instrument on NASA's Aura satellite will also be shown.

Impact of uncertainties in inorganic chemical rate constants on tropospheric composition and ozone radiative forcing

Directory of Open Access Journals (Sweden)

B. Newsome

2017-12-01

Full Text Available Chemical rate constants determine the composition of the atmosphere and how this composition has changed over time. They are central to our understanding of climate change and air quality degradation. Atmospheric chemistry models, whether online or offline, box, regional or global, use these rate constants. Expert panels evaluate laboratory measurements, making recommendations for the rate constants that should be used. This results in very similar or identical rate constants being used by all models. The inherent uncertainties in these recommendations are, in general, therefore ignored. We explore the impact of these uncertainties on the composition of the troposphere using the GEOS-Chem chemistry transport model. Based on the Jet Propulsion Laboratory (JPL and International Union of Pure and Applied Chemistry (IUPAC evaluations we assess the influence of 50 mainly inorganic rate constants and 10 photolysis rates on tropospheric composition through the use of the GEOS-Chem chemistry transport model. We assess the impact on four standard metrics: annual mean tropospheric ozone burden, surface ozone and tropospheric OH concentrations, and tropospheric methane lifetime. Uncertainty in the rate constants for NO2 + OH →M  HNO3 and O3 + NO  →  NO2 + O2 are the two largest sources of uncertainty in these metrics. The absolute magnitude of the change in the metrics is similar if rate constants are increased or decreased by their σ values. We investigate two methods of assessing these uncertainties, addition in quadrature and a Monte Carlo approach, and conclude they give similar outcomes. Combining the uncertainties across the 60 reactions gives overall uncertainties on the annual mean tropospheric ozone burden, surface ozone and tropospheric OH concentrations, and tropospheric methane lifetime of 10, 11, 16 and 16 %, respectively. These are larger than the spread between models in recent model intercomparisons. Remote

Satellite observations of tropospheric nitrogen dioxide : retrieval, interpretation, and modelling

NARCIS (Netherlands)

Boersma, K.F.

2005-01-01

The research questions set out in Chapter 1 that guided the investigation in this thesis are repeated here. The answers to these questions contain the most important conclusions of the various chapters and are given below. 1. How can we retrieve accurate information on total and tropospheric NO2

Hydrological controls on the tropospheric ozone greenhouse gas effect

Directory of Open Access Journals (Sweden)

Le Kuai

2017-03-01

Full Text Available The influence of the hydrological cycle in the greenhouse gas (GHG effect of tropospheric ozone (O3 is quantified in terms of the O3longwave radiative effect (LWRE, which is defined as the net reduction of top-of-atmosphere flux due to total tropospheric O3absorption. The O3LWRE derived from the infrared spectral measurements by Aura’s Tropospheric Emission Spectrometer (TES show that the spatiotemporal variation of LWRE is relevant to relative humidity, surface temperature, and tropospheric O3column. The zonally averaged subtropical LWRE is ~0.2 W m-2higher than the zonally averaged tropical LWRE, generally due to lower water vapor concentrations and less cloud coverage at the downward branch of the Hadley cell in the subtropics. The largest values of O3LWRE over the Middle East (>1 W/m2 are further due to large thermal contrasts and tropospheric ozone enhancements from atmospheric circulation and pollution. Conversely, the low O3LWRE over the Inter-Tropical Convergence Zone (on average 0.4 W m-2 is due to strong water vapor absorption and cloudiness, both of which reduce the tropospheric O3absorption in the longwave radiation. These results show that changes in the hydrological cycle due to climate change could affect the magnitude and distribution of ozone radiative forcing.

TROPOMI, the Sentinel 5 precursor instrument for air quality and climate observations: status of the current design

Science.gov (United States)

Voors, Robert; de Vries, Johan; Bhatti, Ianjit S.; Lobb, Dan; Wood, Trevor; van der Valk, Nick; Aben, Ilse; Veefkind, Pepijn

2017-11-01

TROPOMI, the Tropospheric Monitoring Instrument, is a passive UV-VIS-NIR-SWIR trace gas spectrograph in the line of SCIAMACHY (2002) and OMI (2004), instruments with the Netherlands in a leading role. Both instruments are very successful and remained operational long after their nominal life time. TROPOMI is the next step, scheduled for launch in 2015. It combines the broad wavelength range from SCIAMACHY from UV to SWIR and the broad viewing angle push-broom concept from OMI, which makes daily global coverage in combination with good spatial resolution possible. Using spectral bands from 270-500nm (UV-VIS) 675-775nm (NIR) and 2305-2385nm (SWIR) at moderate resolution (0.25 to 0.6nm) TROPOMI will measure O3, NO2, SO2, BrO, HCHO and H2O tropospheric columns from the UV-VIS-NIR wavelength range and CO and CH4 tropospheric columns from the SWIR wavelength range. Cloud information will be derived primarily from the O2A band in the NIR. This will help, together with the aerosol information, in constraining the light path of backscattered solar radiation. Methane (CH4), CO2 and Carbon monoxide (CO) are the key gases of the global carbon cycle. Of these, Methane is by far the least understood in terms of its sources and is most difficult to predict its future trend. Global space observations are needed to inform atmospheric models. The SWIR channel of TROPOMI is designed to achieve the spectral, spatial and SNR resolution required for this task. TROPOMI will yield an improved accuracy of the tropospheric products compared to the instruments currently in orbit. TROPOMI will take a major step forward in spatial resolution and sensitivity. The nominal observations are at 7 x 7 km2 at nadir and the signal-to-noises are sufficient for trace gas retrieval even at very low albedos (down to 2%). This spatial resolution allows observation of air quality at sub-city level and the high signal-to-noises means that the instrument can perform useful measurements in the darkest

Limb-Nadir Matching Using Non-Coincident NO2 Observations: Proof of Concept and the OMI-minus-OSIRIS Prototype Product

Science.gov (United States)

Adams, Cristen; Normand, Elise N.; Mclinden, Chris A.; Bourassa, Adam E.; Lloyd, Nicholas D.; Degenstein, Douglas A.; Krotkov, Nickolay A.; Rivas, Maria Belmonte; Boersma, K. Folkert; Eskes, Henk

2016-01-01

A variant of the limb-nadir matching technique for deriving tropospheric NO2 columns is presented in which the stratospheric component of the NO2 slant column density (SCD) measured by the Ozone Monitoring Instrument (OMI) is removed using non-coincident profiles from the Optical Spectrograph and InfraRed Imaging System (OSIRIS). In order to correct their mismatch in local time and the diurnal variation of stratospheric NO2, OSIRIS profiles, which were measured just after sunrise, were mapped to the local time of OMI observations using a photochemical boxmodel. Following the profile time adjustment, OSIRIS NO2 stratospheric vertical column densities (VCDs) were calculated. For profiles that did not reach down to the tropopause, VCDs were adjusted using the photochemical model. Using air mass factors from the OMI Standard Product (SP), a new tropospheric NO2 VCD product - referred to as OMI-minus-OSIRIS (OmO) - was generated through limb-nadir matching. To accomplish this, the OMI total SCDs were scaled using correction factors derived from the next-generation SCDs that improve upon the spectral fitting used for the current operational products. One year, 2008, of OmO was generated for 60 deg S to 60 deg N and a cursory evaluation was performed. The OmO product was found to capture the main features of tropospheric NO2, including a background value of about 0.3 x 10(exp 15) molecules per sq cm over the tropical Pacific and values comparable to the OMI operational products over anthropogenic source areas. While additional study is required, these results suggest that a limb-nadir matching approach is feasible for the removal of stratospheric NO2 measured by a polar orbiter from a nadir-viewing instrument in a geostationary orbit such as Tropospheric Emissions: Monitoring of Pollution (TEMPO) or Sentinel-4.

In-situ BrO measurements in the upper troposphere / lower stratosphere. Validation of the ENVISAT satellite measurements and photochemical model studies

Energy Technology Data Exchange (ETDEWEB)

Hrechanyy, S.

2007-04-15

and SCOUT-O3 in the 15-20 km altitude regime are at the low side of comparable DOAS measurements a CLaMS study of the evolution of Bry from the source gases has been carried out. For this purpose an ensemble of trajectories rising from the lower troposphere to the TTL within 6 to more than 90 days were initialized with observed mixing ratios in the boundary layer of all important organic bromine source gases and the free-up of Bry by chemical and photochemical reactions was simulated. Bromoform, CHBr3, was found to be the main source of inorganic bromine at the tropopause. The derived tropospheric lifetime of bromoform is 33 days. The modelled BrO mixing ratio at the tropopause (less than 2.5 pptv) is consistent with HALOX measurements which do not detect significant amounts of BrO there (<1-2 pptv). Therefore measurements of more than 4 pptv (as retrieved from SCIAMACHY) can only be explained trough processes not included in the model. (orig.)

Seasonal variations and vertical features of aerosol particles in the Antarctic troposphere

Directory of Open Access Journals (Sweden)

Keiichiro Hara

2010-12-01

Full Text Available Tethered balloon-borne aerosol measurements were carried out at Syowa Station, Antarctica during the 46th Japanese Antarctic Research Expedition. CN concentration had a maximum in the summer, whereas the number concentrations of fine particles (D_p>0.3 μm and coarse particles (D_p>2.0 μm increased during the winter-spring. The range of CN concentration was 30-2200 cm^ near the surface (surface-500 m and 7-7250 cm^ in the lower free troposphere (>1500 m. During the austral summer, higher CN concentration was often observed in the lower free troposphere. Frequent appearance of higher CN concentration in the free troposphere relative to the surface measurements strongly suggests that new particle formation in the Antarctic regions occurs in the lower free troposphere. Single particle analysis indicated that most of the aerosol particles during the winter were composed of Mg-enriched sea-salt particles originated from sea-salt fractionation on the sea-ice and their modified particles by NO_3^ and SO_4^. This suggests that sea-salt fractionation on sea-ice and modification of sea-salt particles were affected greatly by aerosol hygroscopicity during the winter. Antarctic haze layer was observed not only in the boundary layer but also in the lower free troposphere.

Profiles of CH4, HDO, H2O, and N2O with improved lower tropospheric vertical resolution from Aura TES radiances

Directory of Open Access Journals (Sweden)

D. Noone

2012-02-01

Full Text Available Thermal infrared (IR radiances measured near 8 microns contain information about the vertical distribution of water vapor (H2O, the water isotopologue HDO, and methane (CH4, key gases in the water and carbon cycles. Previous versions (Version 4 or less of the TES profile retrieval algorithm used a "spectral-window" approach to minimize uncertainty from interfering species at the expense of reduced vertical resolution and sensitivity. In this manuscript we document changes to the vertical resolution and uncertainties of the TES version 5 retrieval algorithm. In this version (Version 5, joint estimates of H2O, HDO, CH4 and nitrous oxide (N2O are made using radiances from almost the entire spectral region between 1100 cm−1 and 1330 cm−1. The TES retrieval constraints are also modified in order to better use this information. The new H2O estimates show improved vertical resolution in the lower troposphere and boundary layer, while the new HDO/H2O estimates can now profile the HDO/H2O ratio between 925 hPa and 450 hPa in the tropics and during summertime at high latitudes. The new retrievals are now sensitive to methane in the free troposphere between 800 and 150 mb with peak sensitivity near 500 hPa; whereas in previous versions the sensitivity peaked at 200 hPa. However, the upper troposphere methane concentrations are biased high relative to the lower troposphere by approximately 4% on average. This bias is likely related to temperature, calibration, and/or methane spectroscopy errors. This bias can be mitigated by normalizing the CH4 estimate by the ratio of the N2O estimate relative to the N2O prior, under the assumption that the same systematic error affects both the N2O and CH4 estimates. We demonstrate that applying this ratio theoretically reduces the CH4 estimate for non-retrieved parameters that jointly affect both the N2O and CH4 estimates. The relative upper troposphere to lower troposphere bias is approximately 2.8% after this bias

Aerosol particle size distribution in the stratosphere retrieved from SCIAMACHY limb measurements

Science.gov (United States)

Malinina, Elizaveta; Rozanov, Alexei; Rozanov, Vladimir; Liebing, Patricia; Bovensmann, Heinrich; Burrows, John P.

2018-04-01

health, stratospheric aerosol plays an important role in atmospheric chemistry and climate change. In particular, information about the amount and distribution of stratospheric aerosols is required to initialize climate models, as well as validate aerosol microphysics models and investigate geoengineering. In addition, good knowledge of stratospheric aerosol loading is needed to increase the retrieval accuracy of key trace gases (e.g. ozone or water vapour) when interpreting remote sensing measurements of the scattered solar light. The most commonly used characteristics to describe stratospheric aerosols are the aerosol extinction coefficient and Ångström coefficient. However, the use of particle size distribution parameters along with the aerosol number density is a more optimal approach. In this paper we present a new retrieval algorithm to obtain the particle size distribution of stratospheric aerosol from space-borne observations of the scattered solar light in the limb-viewing geometry. While the mode radius and width of the aerosol particle size distribution are retrieved, the aerosol particle number density profile remains unchanged. The latter is justified by a lower sensitivity of the limb-scattering measurements to changes in this parameter. To our knowledge this is the first data set providing two parameters of the particle size distribution of stratospheric aerosol from space-borne measurements of scattered solar light. Typically, the mode radius and w can be retrieved with an uncertainty of less than 20 %. The algorithm was successfully applied to the tropical region (20° N-20° S) for 10 years (2002-2012) of SCIAMACHY observations in limb-viewing geometry, establishing a unique data set. Analysis of this new climatology for the particle size distribution parameters showed clear increases in the mode radius after the tropical volcanic eruptions, whereas no distinct behaviour of the absolute distribution width could be identified. A tape recorder

Does acetone react with HO2 in the upper-troposphere?

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J. Lelieveld

2012-02-01

Full Text Available Recent theoretical calculations showed that reaction with HO2 could be an important sink for acetone (CH3C(OCH3 and source of acetic acid (CH3C(OOH in cold parts of the atmosphere (e.g. the tropopause region. This work details studies of HO2 + CH3C(OCH3 (CH32C(OHOO (R1 in laboratory-based and theoretical chemistry experiments; the atmospheric significance of Reaction (R1 was assessed in a global 3-D chemical model. Pulsed laser-kinetic experiments were conducted, for the first time, at the low-temperatures representative of the tropopause. Reaction with NO converted HO2 to OH for detection by laser induced fluorescence. Reduced yields of OH at T 2 by CH3C(OCH3 with a forward rate coefficient greater than 2 × 10−12 cm3 molecule−1 s−1. No evidence for Reaction (R1 was observed at T > 230 K, probably due to rapid thermal dissociation back to HO2 + CH3C(OCH3. Numerical simulations of the data indicate that these experiments were sensitive to only (R1a HO2-CH3C(OCH3 complex formation, the first step in (R1. Rearrangement (R1b of the complex to form peroxy radicals, and hence the atmospheric significance of (R1 has yet to be rigorously verified by experiment. Results from new quantum chemical calculations indicate that K1 is characterised by large uncertainties of at least an order of magnitude at T 3C(OCH3 near the tropopause, it cannot explain observations of CH3C(OOH throughout the troposphere.

Tropospheric aerosol backscatter background mode at CO2 wavelengths

Science.gov (United States)

Rothermel, Jeffry; Bowdle, David A.; Menzies, Robert T.; Post, Madison J.; Vaughan, J. Michael

1989-01-01

A comparison is made between three climatologies of backscatter measurements in the troposphere and lower stratosphere at CO2 wavelengths. These were obtained from several locations using ground-based and airborne lidar systems. All three measurement sets show similar features, specifically, a high frequency of occurrence of low backscatter over a limited range of values in the middle and upper atmosphere (the 'background mode'). This background mode is important for the design and performance simulation of the prospective satellite sensors that rely on atmospheric aerosols as scattering targets.

Investigating vertical distribution patterns of lower tropospheric PM2.5 using unmanned aerial vehicle measurements

Science.gov (United States)

Li, Xiao-Bing; Wang, Dong-Sheng; Lu, Qing-Chang; Peng, Zhong-Ren; Wang, Zhan-Yong

2018-01-01

A lightweight unmanned aerial vehicle (UAV) was outfitted with miniaturized sensors to investigate the vertical distribution patterns and sources of fine aerosol particles (PM2.5) within the 1 000 m lower troposphere. A total of 16 UAV flights were conducted in the Yangtze River Delta (YRD) region, China, from the summer to winter in 2014. The associated ground-level measurements from two environmental monitoring stations were also used for background analysis. The results show that ground-level PM2.5 concentrations demonstrated a decreasing trend from Feb. to Jul. and an increasing trend from Aug. to Jan. (the following year). Higher PM2.5 concentrations during the day were mainly observed in the morning (Local Time, LT 05-09) in the spring and summer. However, higher PM2.5 concentrations occurred mainly in the late afternoon and evening (LT 16-20) in the autumn and winter, excluding severe haze pollution days when higher PM2.5 concentrations were also observed during the morning periods. Lower tropospheric PM2.5 concentrations exhibited similar diurnal vertical distribution patterns from the summer to winter. The PM2.5 concentrations decreased with height in the morning, with significantly large vertical gradients from the summer to winter. By contrast, the aerosol particles were well mixed with PM2.5 concentrations of lower than 35 μg ṡm-3 in the early afternoon (LT 12-16) due to sufficient expansions of the planetary boundary layer. The mean vertical PM2.5 concentrations within the 1 000 m lower troposphere in the morning were much larger in the winter (∼87.5 μg ṡm-3) than in the summer and autumn (∼20 μg ṡm-3). However, subtle differences of ∼11 μg ṡm-3 in the mean vertical PM2.5 concentrations were observed in the early afternoon from the summer to winter. The vertical distribution patterns of black carbon and its relationships with PM2.5 indicated that the lower tropospheric aerosol particles might be mainly derived from fossil

MAX-DOAS measurements of NO2 column densities in Vienna

Science.gov (United States)

Schreier, Stefan; Weihs, Philipp; Peters, Enno; Richter, Andreas; Ostendorf, Mareike; Schönhardt, Anja; Burrows, John P.; Schmalwieser, Alois

2017-04-01

In the VINDOBONA (VIenna horizontal aNd vertical Distribution OBservations Of Nitrogen dioxide and Aerosols) project, two Multi AXis Differential Optical Absorption Spectroscopy (MAX-DOAS) systems will be set up at two different locations and altitudes in Vienna, Austria. After comparison measurements in Bremen, Germany, and Cabauw, The Netherlands, the first of the two MAX-DOAS instruments was set up at the University of Veterinary Medicine in the northeastern part of Vienna in December 2016. The instrument performs spectral measurements of visible scattered sunlight at defined horizontal and vertical viewing directions. From these measurements, column densities of NO2 and aerosols are derived by applying the DOAS analysis. First preliminary results are presented. The second MAX-DOAS instrument will be set up in April/May 2017 at the University of Natural Resources and Life Sciences in the northwestern part of Vienna. Once these two instruments are measuring simultaneously, small campaigns including car DOAS zenith-sky and tower DOAS off-axis measurements are planned. The main emphasis of this project will be on the installation and operation of two MAX-DOAS instruments, the improvement of tropospheric NO2 and aerosol retrieval, and the characterization of the horizontal, vertical, and temporal variations of tropospheric NO2 and aerosols in Vienna, Austria.

UV Fourier transform measurements of tropospheric O3, NO2, SO2, benzene, and toluene

International Nuclear Information System (INIS)

Vandaele, A.C.; Tsouli, A.; Carleer, M.; Colin, R.

2002-01-01

Using the differential optical absorption spectroscopy (DOAS) technique and a Fourier transform spectrometer, NO 2 , SO 2 , O 3 , benzene, and toluene were measured during three measurement campaigns held in Brussels in 1995, 1996, and 1997. The O 3 concentrations could be explained as the results of the local photochemistry and the dynamical properties of the mixing layer. NO 2 concentrations were anti-correlated to the O 3 concentrations, is expected. SO 2 also showed a pronounced dependence on car traffic. Average benzene and toluene concentrations were, respectively 1.7 ppb and between 4.4 and 6.6 pbb, but high values of toluene up to 98.8 ppb were observed. SO 2 concentrations and to a lesser extent, those of NO 2 and O 3 , were dependent on the wind direction. Ozone in Brussels has been found to be influenced by the meteorological conditions prevailing in central Europe. Comparisons with other measurements have shown that O 3 and SO 2 data are in general in good agreement, but our NO 2 concentrations seem to be generally higher. (author)

On the origin of tropospheric ozone and NOx over the tropical South Pacific

OpenAIRE

Schultz, Martin G.; Jacob, Daniel James; Wang, Yuhang; Logan, Jennifer A.; Atlas, Elliot L.; Blake, Donald R.; Blake, Nicola J.; Bradshaw, John D.; Browell, Edward V.; Fenn, Marta A.; Flocke, Frank; Gregory, Gerald L.; Heikes, Brian G.; Sachse, Glen W.; Sandholm, Scott T.

1999-01-01

The budgets of ozone and nitrogen oxides (NOx = NO + NO2) in the tropical South Pacific troposphere are analyzed by photochemical point modeling of aircraft observations at 0–12 km altitude from the Pacific Exploratory Mission-Tropics A campaign flown in September-October 1996. The model reproduces the observed NO2/NO concentration ratio to within 30% and has similar success in simulating observed concentrations of peroxides ( H2O2, CH3OOH), lending confidence in its use to investigate ozone ...

Accounting for surface reflectance anisotropy in satellite retrievals of tropospheric NO₂

NARCIS (Netherlands)

Zhou, Yipin; Brunner, D.; Spurr, R.J.D.; Boersma, K.F.; Sneep, M.; Popp, C.; Buchmann, B.

2010-01-01

Surface reflectance is a key parameter in satellite trace gas retrievals in the UV/visible range and in particular for the retrieval of nitrogen dioxide (NO2) vertical tropospheric columns (VTCs). Current operational retrievals rely on coarse-resolution reflectance data and do not account for the

Cryosat-2 and Sentinel-3 tropospheric corrections: their evaluation over rivers and lakes

Science.gov (United States)

Fernandes, Joana; Lázaro, Clara; Vieira, Telmo; Restano, Marco; Ambrózio, Américo; Benveniste, Jérôme

2017-04-01

In the scope of the Sentinel-3 Hydrologic Altimetry PrototypE (SHAPE) project, errors that presently affect the tropospheric corrections i.e. dry and wet tropospheric corrections (DTC and WTC, respectively) given in satellite altimetry products are evaluated over inland water regions. These errors arise because both corrections, function of altitude, are usually computed with respect to an incorrect altitude reference. Several regions of interest (ROI) where CryoSat-2 (CS-2) is operating in SAR/SAR-In modes were selected for this evaluation. In this study, results for Danube River, Amazon Basin, Vanern and Titicaca lakes, and Caspian Sea, using Level 1B CS-2 data, are shown. DTC and WTC have been compared to those derived from ECMWF Operational model and computed at different altitude references: i) ECMWF orography; ii) ACE2 (Altimeter Corrected Elevations 2) and GWD-LR (Global Width Database for Large Rivers) global digital elevation models; iii) mean lake level, derived from Envisat mission data, or river profile derived in the scope of SHAPE project by AlongTrack (ATK) using Jason-2 data. Whenever GNSS data are available in the ROI, a GNSS-derived WTC was also generated and used for comparison. Overall, results show that the tropospheric corrections present in CS-2 L1B products are provided at the level of ECMWF orography, which can depart from the mean lake level or river profile by hundreds of metres. Therefore, the use of the model orography originates errors in the corrections. To mitigate these errors, both DTC and WTC should be provided at the mean river profile/lake level. For example, for the Caspian Sea with a mean level of -27 m, the tropospheric corrections provided in CS-2 products were computed at mean sea level (zero level), leading therefore to a systematic error in the corrections. In case a mean lake level is not available, it can be easily determined from satellite altimetry. In the absence of a mean river profile, both mentioned DEM

Tropospheric Halogen Chemistry

Science.gov (United States)

von Glasow, R.; Crutzen, P. J.

2003-12-01

so far highest atmospheric mixing ratios of BrO were measured (Hebestreit et al., 1999). Volcanoes are sources of halogens as well, mainly in the form of HCl. Biomass burning releases halogens as do industrial processes.So far we have only mentioned chlorine, bromine, and iodine. This is justified because chemistry of fluorine is of no consequence, as very unreactive HF is efficiently formed in the atmosphere, e.g., via the reaction F+H2O→HF+OH. However, several fluorine-containing gases of anthropogenic origin are potentially powerful greenhouse gases, because they absorb strongly in the infrared atmospheric window region near 10 μm. Fully fluorinated gases - such as SF6, CF4, and C2F6 - have atmospheric lifetimes of the order of thousands of years and thus possess very high global warming potential (GWP). Although their abundance in the atmosphere has not yet grown large enough to be of concern for Earth's climate, their production must ultimately be curtailed in the future. The most abundant fully fluorinated gas, CF4, had an atmospheric volume mixing ratio of ˜75 pmol mol-1 in 1995 (Warneck, 1999). Because of their higher concentrations in the atmosphere, about 270 pmol mol-1 and 530 pmol mol-1, respectively, the CFC gases, CFCl3 and CF2Cl2, already exert a significant radiative greenhouse forcing (Ramanathan, 1975) on Earth's climate. For further discussion about atmospheric fluorine, the reader is referred to a thorough review article by Harnisch (1999).Several overview articles have been published on tropospheric halogen chemistry since the early 1980s, starting with Cicerone (1981). Wayne et al. (1995) list in great detail reaction paths, laboratory data, and atmospheric implications of halogen oxides. A good overview on laboratory measurements was also given by de Haan et al. (1999). Reaction cycles involved in tropospheric halogen chemistry and measurements are also thoroughly discussed by Platt (2000) and Platt and Hönninger (2003). Important

New Methods for Retrieval of Chlorophyll Red Fluorescence from Hyperspectral Satellite Instruments: Simulations and Application to GOME-2 and SCIAMACHY

Science.gov (United States)

Joiner, Joanna; Yoshida, Yasuko; Guanter, Luis; Middleton, Elizabeth M.

2016-01-01

Global satellite measurements of solar-induced fluorescence (SIF) from chlorophyll over land and ocean have proven useful for a number of different applications related to physiology, phenology, and productivity of plants and phytoplankton. Terrestrial chlorophyll fluorescence is emitted throughout the red and far-red spectrum, producing two broad peaks near 683 and 736nm. From ocean surfaces, phytoplankton fluorescence emissions are entirely from the red region (683nm peak). Studies using satellite-derived SIF over land have focused almost exclusively on measurements in the far red (wavelengths greater than 712nm), since those are the most easily obtained with existing instrumentation. Here, we examine new ways to use existing hyperspectral satellite data sets to retrieve red SIF (wavelengths less than 712nm) over both land and ocean. Red SIF is thought to provide complementary information to that from the far red for terrestrial vegetation. The satellite instruments that we use were designed to make atmospheric trace-gas measurements and are therefore not optimal for observing SIF; they have coarse spatial resolution and only moderate spectral resolution (0.5nm). Nevertheless, these instruments, the Global Ozone Monitoring Instrument 2 (GOME-2) and the SCanning Imaging Absorption spectroMeter for Atmospheric CHartographY (SCIAMACHY), offer a unique opportunity to compare red and far-red terrestrial SIF at regional spatial scales. Terrestrial SIF has been estimated with ground-, aircraft-, or satellite-based instruments by measuring the filling-in of atmospheric andor solar absorption spectral features by SIF. Our approach makes use of the oxygen (O2) gamma band that is not affected by SIF. The SIF-free O2 gamma band helps to estimate absorption within the spectrally variable O2 B band, which is filled in by red SIF. SIF also fills in the spectrally stable solar Fraunhofer lines (SFLs) at wavelengths both inside and just outside the O2 B band, which further helps

Worldwide biogenic soil NOx emissions inferred from OMI NO2 observations

NARCIS (Netherlands)

Vinken, G.C.M.; Boersma, K.F.; Maasakkers, J.D.; Adon, M.; Martin, R.V.

2014-01-01

Biogenic NOx emissions from soils are a large natural source with substantial uncertainties in global bottom-up estimates (ranging from 4 to 15 Tg N yr-1). We reduce this range in emission estimates, and present a top-down soil NOx emission inventory for 2005 based on retrieved tropospheric NO2

Worldwide biogenic soil NOx emissions inferred from OMI NO2 observations.

NARCIS (Netherlands)

Vinken, G.C.M.; Boersma, K.F.; Maasakkers, J.D.; Adon, M.; Martin, R.V.

2014-01-01

Biogenic NOx emissions from soils are a large natural source with substantial uncertainties in global bottom-up estimates (ranging from 4 to 15 Tg N yr-1). We reduce this range in emission estimates, and present a top-down soil NOx emission inventory for 2005 based on retrieved tropospheric NO2

VLBI-derived troposphere parameters during CONT08

Science.gov (United States)

Heinkelmann, R.; Böhm, J.; Bolotin, S.; Engelhardt, G.; Haas, R.; Lanotte, R.; MacMillan, D. S.; Negusini, M.; Skurikhina, E.; Titov, O.; Schuh, H.

2011-07-01

Time-series of zenith wet and total troposphere delays as well as north and east gradients are compared, and zenith total delays ( ZTD) are combined on the level of parameter estimates. Input data sets are provided by ten Analysis Centers (ACs) of the International VLBI Service for Geodesy and Astrometry (IVS) for the CONT08 campaign (12-26 August 2008). The inconsistent usage of meteorological data and models, such as mapping functions, causes systematics among the ACs, and differing parameterizations and constraints add noise to the troposphere parameter estimates. The empirical standard deviation of ZTD among the ACs with regard to an unweighted mean is 4.6 mm. The ratio of the analysis noise to the observation noise assessed by the operator/software impact (OSI) model is about 2.5. These and other effects have to be accounted for to improve the intra-technique combination of VLBI-derived troposphere parameters. While the largest systematics caused by inconsistent usage of meteorological data can be avoided and the application of different mapping functions can be considered by applying empirical corrections, the noise has to be modeled in the stochastic model of intra-technique combination. The application of different stochastic models shows no significant effects on the combined parameters but results in different mean formal errors: the mean formal errors of the combined ZTD are 2.3 mm (unweighted), 4.4 mm (diagonal), 8.6 mm [variance component (VC) estimation], and 8.6 mm (operator/software impact, OSI). On the one hand, the OSI model, i.e. the inclusion of off-diagonal elements in the cofactor-matrix, considers the reapplication of observations yielding a factor of about two for mean formal errors as compared to the diagonal approach. On the other hand, the combination based on VC estimation shows large differences among the VCs and exhibits a comparable scaling of formal errors. Thus, for the combination of troposphere parameters a combination of the two

Global estimates of CO sources with high resolution by adjoint inversion of multiple satellite datasets (MOPITT, AIRS, SCIAMACHY, TES

Directory of Open Access Journals (Sweden)

M. Kopacz

2010-02-01

Full Text Available We combine CO column measurements from the MOPITT, AIRS, SCIAMACHY, and TES satellite instruments in a full-year (May 2004–April 2005 global inversion of CO sources at 4°×5° spatial resolution and monthly temporal resolution. The inversion uses the GEOS-Chem chemical transport model (CTM and its adjoint applied to MOPITT, AIRS, and SCIAMACHY. Observations from TES, surface sites (NOAA/GMD, and aircraft (MOZAIC are used for evaluation of the a posteriori solution. Using GEOS-Chem as a common intercomparison platform shows global consistency between the different satellite datasets and with the in situ data. Differences can be largely explained by different averaging kernels and a priori information. The global CO emission from combustion as constrained in the inversion is 1350 Tg a⁻¹. This is much higher than current bottom-up emission inventories. A large fraction of the correction results from a seasonal underestimate of CO sources at northern mid-latitudes in winter and suggests a larger-than-expected CO source from vehicle cold starts and residential heating. Implementing this seasonal variation of emissions solves the long-standing problem of models underestimating CO in the northern extratropics in winter-spring. A posteriori emissions also indicate a general underestimation of biomass burning in the GFED2 inventory. However, the tropical biomass burning constraints are not quantitatively consistent across the different datasets.

Iodine's impact on tropospheric oxidants: a global model study in GEOS-Chem

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T. Sherwen

2016-02-01

Full Text Available We present a global simulation of tropospheric iodine chemistry within the GEOS-Chem chemical transport model. This includes organic and inorganic iodine sources, standard gas-phase iodine chemistry, and simplified higher iodine oxide (I2OX, X = 2, 3, 4 chemistry, photolysis, deposition, and parametrized heterogeneous reactions. In comparisons with recent iodine oxide (IO observations, the simulation shows an average bias of  ∼ +90 % with available surface observations in the marine boundary layer (outside of polar regions, and of  ∼ +73 % within the free troposphere (350 hPa  <  p  <  900 hPa over the eastern Pacific. Iodine emissions (3.8 Tg yr−1 are overwhelmingly dominated by the inorganic ocean source, with 76 % of this emission from hypoiodous acid (HOI. HOI is also found to be the dominant iodine species in terms of global tropospheric IY burden (contributing up to 70 %. The iodine chemistry leads to a significant global tropospheric O3 burden decrease (9.0 % compared to standard GEOS-Chem (v9-2. The iodine-driven OX loss rate1 (748 Tg OX yr−1 is due to photolysis of HOI (78 %, photolysis of OIO (21 %, and reaction between IO and BrO (1 %. Increases in global mean OH concentrations (1.8 % by increased conversion of hydroperoxy radicals exceeds the decrease in OH primary production from the reduced O3 concentration. We perform sensitivity studies on a range of parameters and conclude that the simulation is sensitive to choices in parametrization of heterogeneous uptake, ocean surface iodide, and I2OX (X = 2, 3, 4 photolysis. The new iodine chemistry combines with previously implemented bromine chemistry to yield a total bromine- and iodine-driven tropospheric O3 burden decrease of 14.4 % compared to a simulation without iodine and bromine chemistry in the model, and a small increase in OH (1.8 %. This is a significant impact and so halogen chemistry needs to be

Measurements of O3, NO2 and BrO during the INDOEX campaign using ground based DOAS and GOME satellite data

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A. Ladstätter-Weißenmayer

2007-01-01

Full Text Available The INDian Ocean EXperiment (INDOEX was an international, multi-platform field campaign to measure long-range transport of air masses from South and South-East-(SE Asia towards the Indian Ocean. During the dry monsoon season between January and March 1999, local measurements were carried out from ground based platforms and were compared with satellite based data. The objective of this study was to characterise stratospheric and tropospheric trace gas amounts in the equatorial region, and to investigate the impact of air pollution at this remote site. For the characterisation of the chemical composition of the outflow from the S-SE-Asian region, we performed ground based dual-axis-DOAS (Differential Optical Absorption Spectroscopy measurements at the KCO (Kaashidhoo Climate Observatory in the Maldives (5.0° N, 73.5° E. The measurements were conducted using two different observation modes (off-axis and zenith-sky. This technique allows the separation of the tropospheric and stratospheric columns for different trace gases like O3 and NO2. These dual-axis DOAS data were compared with O3-sonde measurements performed at KCO and satellite based GOME (Global Ozone Measuring Experiment data during the intensive measuring phase of the INDOEX campaign in February and March 1999. From GOME observations, tropospheric and stratospheric columns for O3 and NO2 were retrieved. In addition, the analysis of the O3-sonde measurements allowed the determination of the tropospheric O3 amount. The comparison shows that the results of all three measurement systems agree within their error limits. During the INDOEX campaign, mainly background conditions were observed, but in a single case an increase of tropospheric NO2 during a short pollution event was observed from the ground and the impact on the vertical columns was calculated. GOME measurements showed evidence for small tropospheric contributions to the BrO budget, probably located in the free troposphere and

Climate variability and trends in biogenic emissions imprinted on satellite observations of formaldehyde from SCIAMACHY and OMI sounders

Science.gov (United States)

Stavrakou, Trissevgeni; Müller, Jean-François; Bauwens, Maite; De Smedt, Isabelle; Van Roozendael, Michel

2017-04-01

Biogenic hydrocarbon emissions (BVOC) respond to temperature, photosynthetically active radiation, leaf area index, as well as to factors like leaf age, soil moisture, and ambient CO2 concentrations. Isoprene is the principal contributor to BVOC emissions and accounts for about half of the estimated total emissions on the global scale, whereas monoterpenes are also significant over boreal ecosystems. Due to their large emissions, their major role in the tropospheric ozone formation and contribution to secondary organic aerosols, BVOCs are highly relevant to both air quality and climate. Their oxidation in the atmosphere leads to the formation of formaldehyde (HCHO) at high yields. Satellite observations of HCHO abundances can therefore inform us on the spatial and temporal variability of the underlying sources and on their emission trends. The main objective of this study is to investigate the interannual variability and trends of observed HCHO columns during the growing season, when BVOC emissions are dominant, and interpret them in terms of BVOC emission flux variability. To this aim, we use the MEGAN-MOHYCAN model driven by the ECMWF ERA-interim meteorology to calculate bottom-up BVOC fluxes on the global scale (Müller et al. 2008, Stavrakou et al. 2014) over 2003-2015, and satellite HCHO observations from SCIAMACHY (2003-2011) and OMI (2005-2015) instruments (De Smedt et al. 2008, 2015). We focus on mid- and high-latitude regions of the Northern Hemisphere in summertime, as well as tropical regions taking care to exclude biomass burning events which also lead to HCHO column enhancements. We find generally a very strong temporal correlation (>0.7) between the simulated BVOC emissions and the observed HCHO columns over temperate and boreal ecosystems. Positive BVOC emission trends associated to warming climate are found in almost all regions and are well corroborated by the observations. Furthermore, using OMI HCHO observations over 2005-2015 as constraints in

Observing Tropospheric Ozone From Space

Science.gov (United States)

Fishman, Jack

2000-01-01

The importance of tropospheric ozone embraces a spectrum of relevant scientific issues ranging from local environmental concerns, such as damage to the biosphere and human health, to those that impact global change questions, Such is climate warming. From an observational perspective, the challenge is to determine the tropospheric ozone global distribution. Because its lifetime is short compared with other important greenhouse gases that have been monitored over the past several decades, the distribution of tropospheric ozone cannot be inferred from a relatively small set of monitoring stations. Therefore, the best way to obtain a true global picture is from the use of space-based instrumentation where important spatial gradients over vast ocean expanses and other uninhabited areas can be properly characterized. In this paper, the development of the capability to measure tropospheric ozone from space over the past 15 years is summarized. Research in the late 1980s successfully led to the determination of the climatology of tropospheric ozone as a function of season; more recently, the methodology has improved to the extent where regional air pollution episodes can be characterized. The most recent modifications now provide quasi-global (50 N) to 50 S) maps on a daily basis. Such a data set would allow for the study of long-range (intercontinental) transport of air pollution and the quantification of how regional emissions feed into the global tropospheric ozone budget. Future measurement capabilities within this decade promise to offer the ability to provide Concurrent maps of the precursors to the in situ formation of tropospheric ozone from which the scientific community will gain unprecedented insight into the processes that control global tropospheric chemistry

Estimation of Chinese surface NO2 concentrations combining satellite data and Land Use Regression

Science.gov (United States)

Anand, J.; Monks, P.

2016-12-01

Monitoring surface-level air quality is often limited by in-situ instrument placement and issues arising from harmonisation over long timescales. Satellite instruments can offer a synoptic view of regional pollution sources, but in many cases only a total or tropospheric column can be measured. In this work a new technique of estimating surface NO2 combining both satellite and in-situ data is presented, in which a Land Use Regression (LUR) model is used to create high resolution pollution maps based on known predictor variables such as population density, road networks, and land cover. By employing a mixed effects approach, it is possible to take advantage of the spatiotemporal variability in the satellite-derived column densities to account for daily and regional variations in surface NO2 caused by factors such as temperature, elevation, and wind advection. In this work, surface NO2 maps are modelled over the North China Plain and Pearl River Delta during high-pollution episodes by combining in-situ measurements and tropospheric columns from the Ozone Monitoring Instrument (OMI). The modelled concentrations show good agreement with in-situ data and surface NO2 concentrations derived from the MACC-II global reanalysis.

Acetylene C2H 2 retrievals from MIPAS data and regions of enhanced upper tropospheric concentrations in August 2003

Directory of Open Access Journals (Sweden)

V. P. Kanawade

2011-10-01

Full Text Available Acetylene (C2H2 volume mixing ratios (VMRs have been successfully retrieved from the Michelson Interferometer for Passive Atmospheric Sounding (MIPAS Level 1B radiances during August 2003, providing the first global map of such data and ratios to CO in the literature. The data presented here contain most information between 300 hPa and 100 hPa with systematic errors less than 10% at the upper levels. Random errors per point are less than 15% at lower levels and are closer to 30% at 100 hPa. Global distributions of the C2H2 and C2H2/CO ratio confirm significant features associated with both the Asian monsoon anticyclone and biomass burning for this important hydrocarbon in a characteristic summer month (August 2003, showing tight correlations regionally, particularly at lower to medium values, but globally emphasising the differences between sources and lifetimes of CO and C2H2. The correlations are seen to be particularly disturbed in the regions of highest C2H2 concentrations, indicating variability in the surface emissions or fast processing. A strong isolation of C2H2 within the Asian monsoon anticyclone is observed, evidencing convective transport into the upper troposphere, horizontal advection within the anticyclone at 200 hPa, distinct gradients at the westward edge of the vortex and formation of a secondary dynamical feature from the eastward extension of the anticyclone outflow over the Asian Pacific. Ratios of C2H2/CO are consistent with the evidence from the cross-sections that the C2H2 is uplifted rapidly in convection. Observations are presented of enhanced C2H2 associated with the injection from biomass burning into the upper troposphere and the outflow from Africa at 200 hPa into both the Atlantic and Indian Oceans. In the biomass burning regions, C2H2 and CO are well correlated, but the uplift is less marked and peaks at lower altitudes compared to the strong effects observed in the Asian monsoon anticyclone. Ratios of C2H2/CO

Reactive Nitrogen, Ozone and Ozone Production in the Arctic Troposphere and the Impact of Stratosphere-Troposphere Exchange

Science.gov (United States)

Liang, Q.; Rodriquez, J. M.; Douglass, A. R.; Crawford, J. H.; Apel, E.; Bian, H.; Blake, D. R.; Brune, W.; Chin, M.; Colarco, P. R.;

AIRS/Aqua Level 3 Monthly CO2 in the free troposphere (AIRS-only) V005

Data.gov (United States)

National Aeronautics and Space Administration — This is the AIRS mid-tropospheric Carbon Dioxide (CO2) Level 3 Monthly Gridded Retrieval, from the AIRS instrument on board of Aqua satellite. It is a monthly...

Secondary ozone peaks in the troposphere over the Himalayas

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N. Ojha

2017-06-01

Full Text Available Layers with strongly enhanced ozone concentrations in the middle–upper troposphere, referred to as secondary ozone peaks (SOPs, have been observed in different regions of the world. Here we use the global ECHAM5/MESSy atmospheric chemistry model (EMAC to (i investigate the processes causing SOPs, (ii explore both their frequency of occurrence and seasonality, and (iii assess their effects on the tropospheric ozone budget over the Himalayas. The vertical profiles of potential vorticity (PV and a stratospheric ozone tracer (O3s in EMAC simulations, in conjunction with the structure of SOPs, suggest that SOPs over the Himalayas are formed by stratosphere-to-troposphere transport (STT of ozone. The spatial distribution of O3s further shows that such effects are in general most pronounced in the northern part of India. Model simulated ozone distributions and backward air trajectories show that ozone rich air masses, associated with STT, originate as far as northern Africa and the North Atlantic Ocean, the Middle East, as well as in nearby regions in Afghanistan and Pakistan, and are rapidly (within 2–3 days transported to the Himalayas. Analysis of a 15-year (2000–2014 EMAC simulation shows that the frequency of SOPs is highest during the pre-monsoon season (e.g. 11 % of the time in May, while no intense SOP events are found during the July–October period. The SOPs are estimated to enhance the tropospheric column ozone (TCO over the central Himalayas by up to 21 %.

AIRS/Aqua Level 3 Monthly CO2 in the free troposphere (AIRS+AMSU) V005

Data.gov (United States)

National Aeronautics and Space Administration — This is the AIRS mid-tropospheric Carbon Dioxide (CO2) Level 3 Monthly Gridded Retrieval, from the AIRS and AMSU instruments on board of Aqua satellite. It is a...

Mobile MAX-DOAS observation of NO2 and comparison with OMI satellite data in the western coastal areas of the Korean peninsula.

Science.gov (United States)

Chong, Jihyo; Kim, Young J; Gu, Myojeong; Wagner, Thomas; Song, Chul H

2016-01-01

Ground-based MAX-DOAS measurements have been used to retrieve column densities of atmospheric absorbers such as NO2, SO2, HCHO, and O3. In this study, mobile MAX-DOAS measurements were conducted to map the 2-D distributions of atmospheric NO2 in the western coastal areas of the Korean peninsula. A Mini-MAX-DOAS instrument was mounted on the rooftop of a mobile lab vehicle with a telescope mounted parallel to the driving direction, pointing forward. The measurements were conducted from 21 to 24 December 2010 along the western coastal areas from Gomso harbor (35.59N, 126.61E) to Gunsan harbor (35.98N, 126.67E). During mobile MAX-DOAS observations, high elevation angles were used to avoid shades from nearby obstacles. For the determination of the tropospheric vertical column density (VCD), the air mass factor (AMF) was retrieved by the so-called geometric approximation. The NO2 VCDs from 20 and 45 degree elevation angles were retrieved from mobile MAX-DOAS measurements. The tropospheric NO2 VCDs derived from mobile MAX-DOAS measurements were compared directly to those retrieved by the OMI satellite observations. Mobile MAX-DOAS VCD was in good agreement with OMI tropospheric VCD on most days. However, OMI tropospheric VCD was much higher than that of mobile MAX-DOAS on 23 December 2010. One probable reason for this difference is that OMI retrieval might overestimate NO2 VCD under haze conditions, when a pollution plume was transported over the measurement site. The mobile MAX-DOAS observations reveal much finer spatial patterns of NO2 distributions, which can provide useful information for the validation of satellite observation of atmospheric trace gases. Copyright © 2015 Elsevier Ltd. All rights reserved.

Sensitivity analysis of a new SWIR-channel measuring tropospheric CH 4 and CO from space

Science.gov (United States)

Jongma, Rienk T.; Gloudemans, Annemieke M. S.; Hoogeveen, Ruud W. M.; Aben, Ilse; de Vries, Johan; Escudero-Sanz, Isabel; van den Oord, Gijsbertus; Levelt, Pieternel F.

2006-08-01

In preparation for future atmospheric space missions a consortium of Dutch organizations is performing design studies on a nadir viewing grating-based imaging spectrometer using OMI and SCIAMACHY heritage. The spectrometer measures selected species (O 3, NO II, HCHO, H IIO, SO II, aerosols (optical depth, type and absorption index), CO and CH4) with sensitivity down to the Earth's surface, thus addressing science issues on air quality and climate. It includes 3 UV-VIS channels continuously covering the 270-490 nm range, a NIR-channel covering the 710-775 nm range, and a SWIR-channel covering the 2305-2385 nm range. This instrument concept is, named TROPOMI, part of the TRAQ-mission proposal to ESA in response to the Call for Earth Explorer Ideas 2005, and, named TROPI, part of the CAMEO-proposal prepared for the US NRC decadal study-call on Earth science and applications from space. The SWIR-channel is optional in the TROPOMI/TRAQ instrument and included as baseline in the TROPI/CAMEO instrument. This paper focuses on derivation of the instrument requirements of the SWIR-channel by presenting the results of retrieval studies. Synthetic detector spectra are generated by the combination of a forward model and an instrument simulator that includes the properties of state-of-the-art detector technology. The synthetic spectra are input to the CO and CH 4 IMLM retrieval algorithm originally developed for SCIAMACHY. The required accuracy of the Level-2 SWIR data products defines the main instrument parameters like spectral resolution and sampling, telescope aperture, detector temperature, and optical bench temperature. The impact of selected calibration and retrieval errors on the Level-2 products has been characterized. The current status of the SWIR-channel optical design with its demanding requirements on ground-pixel size, spectral resolution, and signal-to-noise ratio will be presented.

Tropospheric radiative forcing of CH4

International Nuclear Information System (INIS)

Grossman, A.S.; Grant, K.E.

1994-04-01

We have evaluated the tropospheric radiative forcing of CH 4 in the 0-3000 cm -1 wavenumber range and compared this with prior published calculations. The atmospheric test cases involved perturbed methane scenarios in both a McClatchey mid latitude, summer, clear sky approximation, model atmosphere, as well as a globally and seasonally averaged model atmosphere containing a representative cloud distribution. The scenarios involved pure CH 4 radiative forcing and CH 4 plus a mixture of H 2 O, CO 2 , O 3 , and N 2 O. The IR radiative forcing was calculated using a correlated k-distribution transmission model. The major purposes of this paper are to first, use the correlated k-distribution model to calculate the tropospheric radiative forcing for CH 4 , as the only radiatively active gas, and in a mixture with H 2 O, CO 2 , O 3 , and N 2 O, for a McClatchey mid-latitude summer, clear-sky model atmosphere, and to compare the results to those obtained in the studies mentioned above. Second, we will calculate the tropospheric methane forcing in a globally and annually averaged atmosphere with and without a representative cloud distribution in order to validate the conjecture given in IPCC (1990) that the inclusion of clouds in the forcing calculations results in forcing values which are approximately 20 percent less than those obtained using clear sky approximations

Model Calculations of Changes in Tropospheric Ozone Over Europe and the Role of Surface Sources and Aircraft Emissions

Energy Technology Data Exchange (ETDEWEB)

Hov, Oe [Bergen Univ. (Norway)

1996-01-01

This conference paper deals with a study of the impact of various sources of NO{sub x} on the ozone production in the free troposphere. A comprehensive two-dimensional zonally averaged chemistry/transport model and a three-dimensional meso-scale chemical transport (MCT) model are used in the study. Using the two-dimensional model, three surches of NO{sub x} in the upper troposphere were examined covering NO{sub x} produced by lightening, NO{sub x} (and NO{sub y}) brought to the upper troposphere from the planetary boundary layer by rapid vertical transport processes, and NO{sub x} emitted from aircraft. 4 refs.

The influence of biogenic emissions from Africa on tropical tropospheric ozone during 2006: a global modeling study

Directory of Open Access Journals (Sweden)

J. E. Williams

2009-08-01

Full Text Available We have performed simulations using a 3-D global chemistry-transport model to investigate the influence that biogenic emissions from the African continent exert on the composition of the troposphere in the tropical region. For this purpose we have applied two recently developed biogenic emission inventories provided for use in large-scale global models (Granier et al., 2005; Lathière et al., 2006 whose seasonality and temporal distribution for biogenic emissions of isoprene, other volatile organic compounds and NO is markedly different. The use of the 12 year average values for biogenic emissions provided by Lathière et al. (2006 results in an increase in the amount of nitrogen sequestrated into longer lived reservoir compounds which contributes to the reduction in the tropospheric ozone burden in the tropics. The associated re-partitioning of nitrogen between PAN, HNO₃ and organic nitrates also results in a ~5% increase in the loss of nitrogen by wet deposition. At a global scale there is a reduction in the oxidizing capacity of the model atmosphere which increases the atmospheric lifetimes of CH₄ and CO by ~1.5% and ~4%, respectively. Comparisons against a range of different measurements indicate that applying the 12 year average of Lathière et al. (2006 improves the performance of TM4_AMMA for 2006 in the tropics. By the use of sensitivity studies we show that the release of NO from soils in Africa accounts for between ~2–45% of tropospheric ozone in the African troposphere, ~10% in the upper troposphere and between ~5–20% of the tropical tropospheric ozone column over the tropical Atlantic Ocean. The subsequent reduction in OH over the source regions allows enhanced transport of CO out of the region. For biogenic volatile organic C1 to C3 species released from Africa, the effects on tropical tropospheric ozone are rather limited, although this source contributes to the global burden of VOC by between ~2–4% and

Tropospheric ozone and aerosols in climate agreements: scientific and political challenges

International Nuclear Information System (INIS)

Rypdal, Kristin; Berntsen, Terje; Fuglestvedt, Jan S.; Aunan, Kristin; Torvanger, Asbjorn; Stordal, Frode; Pacyna, Jozef M.; Nygaard, Lynn P.

2005-01-01

In addition to the six greenhouse gases included in the Kyoto Protocol, the tropospheric ozone precursors CO, NMVOC and NO x and the aerosols/aerosol precursors black carbon, organic carbon and SO 2 also play significant roles in climate change. The aim of this paper is to review some of the main scientific and political challenges associated with incorporating tropospheric ozone and aerosol precursors into climate agreements, and to discuss how these challenges have a bearing on the design of future climate agreements. We argue that the optimal policy design for a particular substance depends on a combination of scientific and political concerns. We look particularly at regional climate effects, negative forcing, metrics (measuring climate effects against other gases on a common scale), political attractiveness, and verification and compliance. We systematically review the existing knowledge on these issues, explore their impact on policy design, and conclude that, with current scientific knowledge, CO and NMVOC could conceivably be included in a global climate agreement, either in a basket with the long-lived greenhouse gases or in a separate basket, while NO x and aerosols might be regulated more appropriately through regional agreements with links to a global agreement. However, the complexity and fairness implications of including tropospheric ozone precursors and aerosols might negatively affect the political feasibility of a future agreement

Airborne measurement of peroxy radicals in the lower troposphere

Science.gov (United States)

Andrés Hernández, Maria Dolores; Horstjann, Markus; Kartal, Deniz; Krebsbach, Marc; Linke, Christian; Lichtenstern, Michael; Andrey, Javier; Burrows, John P.

2013-04-01

The importance of peroxy radicals in the tropospheric chemistry is well recognized in the scientific literature. Hydroxy- and organic peroxy radicals (HO2 and RO2, R being an organic chain) are key intermediates in the OH radical initiated oxidation of CO and SO2, of volatile organic compounds (VOC), in the ozonolysis of alkenes and photo-oxidation of carbonyl species. Peroxy radicals are responsible for the ozone production in the troposphere, the formation of peroxides and other oxidants. Although radical chemistry in the troposphere has been subject of intensive research in the past three decades, it is still very few known about the vertical distribution of peroxy radicals. Airborne observations are scarce in spite of their particular importance to improve the understanding of the tropospheric chemistry and the oxidising capacity of the atmosphere at different altitudes. In situ trace gas measurements were carried out in summer 2010 on board of the INTA (Instituto Nacional de Técnicas Aeroespaciales) C212 aircraft over Spain in the frame of the EUFAR project VERDRILLT (VERtical Distribution of Radicals In the Lower Layers of the Troposphere), and in cooperation with the DLR (Deutsches Zentrum für Luft- und Raumfahrt), the University of Wuppertal, the CEAM (Centro de Estudios Ambientales del Mediterráneo) and the UPV-EHU University in Bilbao. VERDRILLT aimed at getting a deeper understanding of the vertical distribution of peroxy radicals in the lower layers of the troposphere. Measurements were taken over urban areas and extensions of different vegetation under meteorological conditions favouring active photochemistry and convection from the ground into close atmospheric layers. Results and main findings will be presented and discussed.

Rapid increases in tropospheric ozone production and export from China

NARCIS (Netherlands)

Verstraeten, W.W.; Neu, J.L.; Williams, J.E.; Bowman, K.W.; Worden, J.R.; Boersma, K.F.

2015-01-01

Rapid population growth and industrialization have driven substantial increases in Asian ozone precursor emissions over the past decade1, with highly uncertain impacts on regional and global tropospheric ozone levels. According to ozonesonde measurements2, 3, tropospheric ozone concentrations at two

Impact of selected troposphere models on Precise Point Positioning convergence

Science.gov (United States)

Kalita, Jakub; Rzepecka, Zofia

2016-04-01

The Precise Point Positioning (PPP) absolute method is currently intensively investigated in order to reach fast convergence time. Among various sources that influence the convergence of the PPP, the tropospheric delay is one of the most important. Numerous models of tropospheric delay are developed and applied to PPP processing. However, with rare exceptions, the quality of those models does not allow fixing the zenith path delay tropospheric parameter, leaving difference between nominal and final value to the estimation process. Here we present comparison of several PPP result sets, each of which based on different troposphere model. The respective nominal values are adopted from models: VMF1, GPT2w, MOPS and ZERO-WET. The PPP solution admitted as reference is based on the final troposphere product from the International GNSS Service (IGS). The VMF1 mapping function was used for all processing variants in order to provide capability to compare impact of applied nominal values. The worst case initiates zenith wet delay with zero value (ZERO-WET). Impact from all possible models for tropospheric nominal values should fit inside both IGS and ZERO-WET border variants. The analysis is based on data from seven IGS stations located in mid-latitude European region from year 2014. For the purpose of this study several days with the most active troposphere were selected for each of the station. All the PPP solutions were determined using gLAB open-source software, with the Kalman filter implemented independently by the authors of this work. The processing was performed on 1 hour slices of observation data. In addition to the analysis of the output processing files, the presented study contains detailed analysis of the tropospheric conditions for the selected data. The overall results show that for the height component the VMF1 model outperforms GPT2w and MOPS by 35-40% and ZERO-WET variant by 150%. In most of the cases all solutions converge to the same values during first

Tropospheric Ozone Pollution from Space: New Views from the TOMS (Total Ozone Mapping Spectrometer) Instrument

Science.gov (United States)

Thompson, Anne M.; Hudson, Robert D.; Frolov, Alexander D.; Witte, Jacquelyn C.; Kucsera, Tom L.; Einaudi, Franco (Technical Monitor)

2000-01-01

New products from the TOMS (Total Ozone Mapping Spectrometer) >satellite instrument can resolve pollution events in tropical and mid-latitudes, Over the past several years, we have developed tropospheric ozone data sets by two methods. The modified-residual technique [Hudson and Thompson, 1998; Thompson and Hudson, 1999] uses v. 7 TOMS total ozone and is applicable to tropical regimes in which the wave-one pattern in total ozone is observed. The TOMSdirect method [Hudson et at., 2000] represents a new algorithm that uses TOMS radiances to extract tropospheric ozone in regions of constant stratospheric ozone and tropospheric ozone displaying high mixing ratios and variability characteristic of pollution, Absorbing aerosols (dust and smoke; Herman et at., 1997 Hsu et al., 1999), a standard TOMS product, provide transport and/or source marker information to interpret tropospheric ozone. For the Nimbus 7/TOMS observing period (1979-1992), modified-residual TTO (tropical tropospheric ozone) appears as two maps/month at I-degree latitude 2-degree longitude resolution at a homepage and digital data are available (20S to 20N) by ftp at http://metosrv2. umd.edu/tropo/ 14y_data.d. Preliminary modified-residual TTO data from the operational Earth-Probe/TOMS (1996- present) are posted in near-real-time at the same website. Analyses with the new tropospheric ozone and aerosol data are illustrated by the following (I)Signals in tropical tropospheric ozone column and smoke amount during ENSO (El Nino-Southern Oscillation) events, e.g. 1982-1983 and the intense ENSO induced biomass fires of 1997-1998 over the Indonesian region [Thompson et a[, 2000a, Thompson and Hudson, 1999]. (2) Trends in tropospheric ozone and smoke aerosols in various tropical regions (Atlantic, Pacific, Africa, Brazil). No significant trends were found for ozone from1980-1990 [Thompson and Hudson, 19991 although smoke aerosols increased during the period [Hsu et al.,1999]. (3) Temporal and spatial offsets

Radiative forcing for changes in tropospheric O3

International Nuclear Information System (INIS)

Grossman, A.S.; Wuebbles, D.J.; Grant, K.E.

1994-06-01

We have evaluated the radiative forcing for assumed changes in tropospheric O 3 in the 500-1650 cm -1 wavenumber range. The radiative forcing calculations were performed as a function of latitude as well as for a globally and seasonally averaged model atmosphere, both in a clear sky approximation and in a model containing a representative cloud distribution. The scenarios involved radiative forcing calculations for O 3 at normal atmospheric abundance and at a tropospheric abundance depleted by 25 ppbv, at each altitude, for all northern hemisphere latitudes. Normal abundances of H 2 O, CO 2 , CH 4 , and N 2 O were included in the calculations. The IR radiative forcing was calculated using a correlated k-distribution radiative transfer model. The tropospheric radiative forcing values are compared to the IPCC formulae for ozone tropospheric forcing as well as other published values to determine the validity of the correlated k-distribution approach to the radiative forcing calculations. The results for the global average atmosphere show agreement with previous results to the order of 10 percent. We conclude that the O 3 forcing is linear in the background abundance and that the radiative forcing for ozone for the globally averaged atmosphere and the latitude averaged radiative forcing in the clear sky approximation are in agreement to within 10 percent. For the case of an atmosphere in which the tropospheric ozone has been depleted by 25 ppbv at all altitudes in the northern hemisphere, the mid latitude zone contributes ∼50 percent of the forcing, tropic zone contributes ∼37 percent of the forcing and the polar zone contributes ∼13 percent of the total forcing

Global budget of tropospheric ozone: Evaluating recent model advances with satellite (OMI), aircraft (IAGOS), and ozonesonde observations

Science.gov (United States)

Hu, Lu; Jacob, Daniel J.; Liu, Xiong; Zhang, Yi; Zhang, Lin; Kim, Patrick S.; Sulprizio, Melissa P.; Yantosca, Robert M.

2017-10-01

The global budget of tropospheric ozone is governed by a complicated ensemble of coupled chemical and dynamical processes. Simulation of tropospheric ozone has been a major focus of the GEOS-Chem chemical transport model (CTM) over the past 20 years, and many developments over the years have affected the model representation of the ozone budget. Here we conduct a comprehensive evaluation of the standard version of GEOS-Chem (v10-01) with ozone observations from ozonesondes, the OMI satellite instrument, and MOZAIC-IAGOS commercial aircraft for 2012-2013. Global validation of the OMI 700-400 hPa data with ozonesondes shows that OMI maintained persistent high quality and no significant drift over the 2006-2013 period. GEOS-Chem shows no significant seasonal or latitudinal bias relative to OMI and strong correlations in all seasons on the 2° × 2.5° horizontal scale (r = 0.88-0.95), improving on previous model versions. The most pronounced model bias revealed by ozonesondes and MOZAIC-IAGOS is at high northern latitudes in winter-spring where the model is 10-20 ppbv too low. This appears to be due to insufficient stratosphere-troposphere exchange (STE). Model updates to lightning NOx, Asian anthropogenic emissions, bromine chemistry, isoprene chemistry, and meteorological fields over the past decade have overall led to gradual increase in the simulated global tropospheric ozone burden and more active ozone production and loss. From simulations with different versions of GEOS meteorological fields we find that tropospheric ozone in GEOS-Chem v10-01 has a global production rate of 4960-5530 Tg a-1, lifetime of 20.9-24.2 days, burden of 345-357 Tg, and STE of 325-492 Tg a-1. Change in the intensity of tropical deep convection between these different meteorological fields is a major factor driving differences in the ozone budget.

Tropospheric Degradation of Perfluorinated Aromatics: A Case of Hexafluorobenzene

Directory of Open Access Journals (Sweden)

Goran Kovačević

2015-12-01

Full Text Available The major tropospheric removal process for hexafluorobenzene is its oxidation by hydroxyl (OH radicals. However, there is no information on the reaction mechanism of this important process. All geometries and energies significant for the tropospheric degradation of hexafluorobenzene were characterized using the MP2/6-311+G(d,p and/or G3 methods. It was found out that the addition of OH radical to hexafluorobenzene proceeds via a prereaction complex. In the prereaction complex the OH radical is almost perpendicular to the aromatic ring and oxygen is pointing to its center. The reaction rate constants for addition of OH radical to hexafluorobenzene were determined for the temperature range 230–330 K, using RRKM theory and corrected G3 energies. For the whole range of environmentally relevant temperatures (230–330 K there is a very good qualitative agreement between the calculated and experimental rate constants. Finally, our results almost perfectly reproduce the unusually weak temperature dependence for OH radical addition to hexafluorobenzene.

Concentration variations of the tropospheric carbon dioxide over the Antarctic region

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Shohei Murayama

1997-03-01

Full Text Available Aircraft measurements of the atmospheric CO_2 concentration have been made over Syowa Station, Antarctica since 1983. The minimum concentration of the average seasonal CO_2 cycle appears in March throughout the troposphere, while the maximum concentration occurs in mid-August in the upper troposphere and in late September in the middle and lower troposphere. The peak-to-peak amplitude of the seasonal cycle decreases with height. The CO_2 concentration increases with height during most of the year; however, this height dependency is larger from summer to early winter than in the remaining seasons. The average concentration difference between the upper troposphere and the ground surface is about 0.3ppmv. From comparisons with the results of the ground-based and aircraft measurements at southern middle and high latitudes and trajectory analysis, it is hypothesized that the seasonal cycle of height-dependent atmospheric transport processes could influence the seasonal cycle and the vertical distribution of the CO_2 concentration over Syowa Station.

Hydrogen Radicals, Nitrogen Radicals, and the Production of Ozone in the Middle and Upper Troposphere

Science.gov (United States)

Bui, T. P.

1997-01-01

The concentrations of hydrogen radicals, OH and HO2, in the middle and upper troposphere were measured simultaneously with those of NO, O3,CO, H20, CH4, non-methane hydrocarbons, and with the ultraviolet and visible radiation field.

Balloon-borne stratospheric BrO measurements: comparison with Envisat/SCIAMACHY BrO limb profiles

Directory of Open Access Journals (Sweden)

M. Dorf

2006-01-01

Full Text Available For the first time, results of four stratospheric BrO profiling instruments, are presented and compared with reference to the SLIMCAT 3-dimensional chemical transport model (3-D CTM. Model calculations are used to infer a BrO profile validation set, measured by 3 different balloon sensors, for the new Envisat/SCIAMACHY (ENVIronment SATellite/SCanning Imaging Absorption spectroMeter for Atmospheric CHartographY satellite instrument. The balloon observations include (a balloon-borne in situ resonance fluorescence detection of BrO (Triple, (b balloon-borne solar occultation DOAS measurements (Differential Optical Absorption Spectroscopy of BrO in the UV, and (c BrO profiling from the solar occultation SAOZ (Systeme d'Analyse par Observation Zenithale balloon instrument. Since stratospheric BrO is subject to considerable diurnal variation and none of the measurements are performed close enough in time and space for a direct comparison, all balloon observations are considered with reference to outputs from the 3-D CTM. The referencing is performed by forward and backward air mass trajectory calculations to match the balloon with the satellite observations. The diurnal variation of BrO is considered by 1-D photochemical model calculation along the trajectories. The 1-D photochemical model is initialised with output data of the 3-D model with additional constraints on the vertical transport, the total amount and photochemistry of stratospheric bromine as given by the various balloon observations. Total [Bry]=(20.1±2.5 pptv obtained from DOAS BrO observations at mid-latitudes in 2003, serves as an upper limit of the comparison. Most of the balloon observations agree with the photochemical model predictions within their given error estimates. First retrieval exercises of BrO limb profiling from the SCIAMACHY satellite instrument on average agree to around 20% with the photochemically-corrected balloon observations of the remote sensing instruments (SAOZ

Multi-model ensemble simulations of troposheric NO2 compared with GOME retrievals for the year 2000

NARCIS (Netherlands)

Noije, van T.P.C.; Eskes, H.J.; Dentener, F.J.; Stevenson, D.S.; Ellingsen, K.; Schultz, M.G.; Wild, O.; Amann, M.; Atherton, C.S.; Bergmann, D.; Bey, I.; Boersma, K.F.; Butler, T.; Cofala, J.; Drevet, J.; Fiore, A.M.; Gauss, M.; Hauglustaine, D.A.; Horowitz, L.W.; Isaksen, I.S.A.; Krol, M.C.; Lamarque, J.F.; Lawrence, M.G.; Martin, R.V.; Montanaro, V.; Muller, J.F.; Pitari, G.; Prather, M.J.; Pyle, J.A.; Richter, A.; Rodriguez, J.M.; Savage, N.H.; Strahan, S.E.; Sudo, K.; Szopa, S.; Roozendael, van M.

2006-01-01

We present a systematic comparison of tropospheric NO2 from 17 global atmospheric chemistry models with three state-of-the-art retrievals from the Global Ozone Monitoring Experiment (GOME) for the year 2000. The models used constant anthropogenic emissions from IIASA/EDGAR3.2 and monthly emissions

Photochemistry and transport of tropospheric ozone and its precursors in urban and remote environments

Science.gov (United States)

Anderson, Daniel Craig

Tropospheric ozone (O3) adversely affects human health, reduces crop yields, and contributes to climate forcing. To limit these effects, the processes controlling O3 abundance as well as that of its precursor molecules must be fully characterized. Here, I examine three facets of O 3 production, both in heavily polluted and remote environments. First, using in situ observations from the DISCOVER-AQ field campaign in the Baltimore/Washington region, I evaluate the emissions of the O 3 precursors CO and NOx (NOx = NO + NO2) in the National Emissions Inventory (NEI). I find that CO/NOx emissions ratios derived from observations are 21% higher than those predicted by the NEI. Comparisons to output from the CMAQ model suggest that CO in the NEI is accurate within 15 +/- 11%, while NOx emissions are overestimated by 51-70%, likely due to errors in mobile sources. These results imply that ambient ozone concentrations will respond more efficiently to NOx controls than current models suggest. I then investigate the source of high O3 and low H2O structures in the Tropical Western Pacific (TWP). A combination of in situ observations, satellite data, and models show that the high O3 results from photochemical production in biomass burning plumes from fires in tropical Southeast Asia and Central Africa; the low relative humidity results from large-scale descent in the tropics. Because these structures have frequently been attributed to mid-latitude pollution, biomass burning in the tropics likely contributes more to the radiative forcing of climate than previously believed. Finally, I evaluate the processes controlling formaldehyde (HCHO) in the TWP. Convective transport of near surface HCHO leads to a 33% increase in upper tropospheric HCHO mixing ratios; convection also likely increases upper tropospheric CH 3OOH to ~230 pptv, enough to maintain background HCHO at ~75 pptv. The long-range transport of polluted air, with NO four times the convectively controlled background

Tropospheric Ozone Assessment Report: Present-day distribution and trends of tropospheric ozone relevant to climate and global atmospheric chemistry model evaluation

Directory of Open Access Journals (Sweden)

A. Gaudel

2018-05-01

Full Text Available 'The Tropospheric Ozone Assessment Report' (TOAR is an activity of the International Global Atmospheric Chemistry Project. This paper is a component of the report, focusing on the present-day distribution and trends of tropospheric ozone relevant to climate and global atmospheric chemistry model evaluation. Utilizing the TOAR surface ozone database, several figures present the global distribution and trends of daytime average ozone at 2702 non-urban monitoring sites, highlighting the regions and seasons of the world with the greatest ozone levels. Similarly, ozonesonde and commercial aircraft observations reveal ozone’s distribution throughout the depth of the free troposphere. Long-term surface observations are limited in their global spatial coverage, but data from remote locations indicate that ozone in the 21st century is greater than during the 1970s and 1980s. While some remote sites and many sites in the heavily polluted regions of East Asia show ozone increases since 2000, many others show decreases and there is no clear global pattern for surface ozone changes since 2000. Two new satellite products provide detailed views of ozone in the lower troposphere across East Asia and Europe, revealing the full spatial extent of the spring and summer ozone enhancements across eastern China that cannot be assessed from limited surface observations. Sufficient data are now available (ozonesondes, satellite, aircraft across the tropics from South America eastwards to the western Pacific Ocean, to indicate a likely tropospheric column ozone increase since the 1990s. The 2014–2016 mean tropospheric ozone burden (TOB between 60°N–60°S from five satellite products is 300 Tg ± 4%. While this agreement is excellent, the products differ in their quantification of TOB trends and further work is required to reconcile the differences. Satellites can now estimate ozone’s global long-wave radiative effect, but evaluation is difficult due to limited

Diurnal variation of tropospheric temperature at a tropical station

Directory of Open Access Journals (Sweden)

K. Revathy

2001-08-01

Full Text Available The vertical velocity in the troposphere-lower stratosphere region measured using MST radar has been utilized to evaluate the temperature profile in the region. The diurnal variation of the tropospheric temperature on one day in August 1998 at the tropical station Gadanki (13.5° N, 79.2° E has been studied using the MST radar technique. The diurnal variation of the temperature revealed a prominent diurnal variation with the peak in the afternoon hours increasingly delayed in altitude. The tropopause temperature and altitude exhibited a clear diurnal cycle.Key words. Atmospheric composition and structure (pressure, density and temperature; troposphere - composition and chemistry; instruments and technique

Global CO emission estimates inferred from assimilation of MOPITT and IASI CO data, together with observations of O3, NO2, HNO3, and HCHO.

Science.gov (United States)

Zhang, X.; Jones, D. B. A.; Keller, M.; Jiang, Z.; Bourassa, A. E.; Degenstein, D. A.; Clerbaux, C.; Pierre-Francois, C.

2017-12-01

Atmospheric carbon monoxide (CO) emissions estimated from inverse modeling analyses exhibit large uncertainties, due, in part, to discrepancies in the tropospheric chemistry in atmospheric models. We attempt to reduce the uncertainties in CO emission estimates by constraining the modeled abundance of ozone (O3), nitrogen dioxide (NO2), nitric acid (HNO3), and formaldehyde (HCHO), which are constituents that play a key role in tropospheric chemistry. Using the GEOS-Chem four-dimensional variational (4D-Var) data assimilation system, we estimate CO emissions by assimilating observations of CO from the Measurement of Pollution In the Troposphere (MOPITT) and the Infrared Atmospheric Sounding Interferometer (IASI), together with observations of O3 from the Optical Spectrograph and InfraRed Imager System (OSIRIS) and IASI, NO2 and HCHO from the Ozone Monitoring Instrument (OMI), and HNO3 from the Microwave Limb Sounder (MLS). Our experiments evaluate the inferred CO emission estimates from major anthropogenic, biomass burning and biogenic sources. Moreover, we also infer surface emissions of nitrogen oxides (NOx = NO + NO2) and isoprene. Our results reveal that this multiple species chemical data assimilation produces a chemical consistent state that effectively adjusts the CO-O3-OH coupling in the model. The O3-induced changes in OH are particularly large in the tropics. Overall, our analysis results in a better constrained tropospheric chemical state.

MAX-DOAS tropospheric nitrogen dioxide column measurements compared with the Lotos-Euros air quality model

NARCIS (Netherlands)

Vlemmix, T.; Eskes, H.J.; Piters, A.J.M.; Schaap, M.; Sauter, F.J.; Kelder, H.; Levelt, P.F.

2015-01-01

A 14-month data set of MAX-DOAS (Multi-Axis Differential Optical Absorption Spectroscopy) tropospheric NO2 column observations in De Bilt, the Netherlands, has been compared with the regional air quality model Lotos-Euros. The model was run on a 7×7 km2 grid, the same resolution as the emission

Distribution of tropical tropospheric water vapor

Science.gov (United States)

Sun, De-Zheng; Lindzen, Richard S.

1993-01-01

Utilizing a conceptual model for tropical convection and observational data for water vapor, the maintenance of the vertical distribution of the tropical tropospheric water vapor is discussed. While deep convection induces large-scale subsidence that constrains the turbulent downgradient mixing to within the convective boundary layer and effectively dries the troposphere through downward advection, it also pumps hydrometeors into the upper troposphere, whose subsequent evaporation appears to be the major source of moisture for the large-scale subsiding motion. The development of upper-level clouds and precipitation from these clouds may also act to dry the outflow, thus explaining the low relative humidity near the tropopause. A one-dimensional model is developed to simulate the mean vertical structure of water vapor in the tropical troposphere. It is also shown that the horizontal variation of water vapor in the tropical troposphere above the trade-wind boundary layer can be explained by the variation of a moisture source that is proportional to the amount of upper-level clouds. Implications for the nature of water vapor feedback in global warming are discussed.

Evaluating a New Homogeneous Total Ozone Climate Data Record from GOME/ERS-2, SCIAMACHY/Envisat, and GOME-2/MetOp-A

Science.gov (United States)

Koukouli, M.E.; Lerot, C.; Granville, J.; Goutail, F.; Lambert, J.-C.; Pommereau, J.-P.; Balis, D.; Zyrichidou, I.; Van Roozendael, M.; Coldewey-Egbers, M.;

Stratospheric Ozone Distribution and Tropospheric General Circulation: Interconnections in the UTLS Region

Science.gov (United States)

Barodka, S.; Krasovsky, A.; Shalamyansky, A.

2014-12-01

The height of the tropopause, which divided the stratosphere and the troposphere, is a result of two rival categories of processes: the tropospheric vertical convection and the radiative heating of the stratosphere resulting from the ozone cycle. Hence, it is natural that tropospheric and stratospheric phenomena can have effect each other in manifold processes of stratosphere-troposphere interactions. In the present study we focus our attention to the "top-down" side of the interaction: the impact of stratospheric ozone distribution on the features of tropospheric circulation and the associated weather patterns and regional climate conditions. We proceed from analyzes of the observational data performed at the A.I. Voeikov Main Geophysical Observatory, which suggest a distinct correlation between stratospheric ozone distribution, synoptic formations and air-masses boundaries in the upper troposphere and the temperature field of the lower stratosphere [1]. Furthermore, we analyze local features of atmospheric general circulation and stratospheric ozone distribution from the atmospheric reanalyses and general circulation model data, focusing our attention to instantaneous positions of subtropical and polar stationary atmospheric fronts, which define regional characteristics of the general circulation cells in the troposphere and separate global tropospheric air-masses, correspond to distinct meteorological regimes in the TOC field [2, 3]. We assume that by altering the tropopause height, stratospheric ozone-related processes can have an impact on the location of the stationary atmospheric fronts, thereby exerting influence on circulation processes in troposphere and lower stratosphere. For midlatitudes, the tropopause height controls the position of the polar stationary front, which has a direct impact on the trajectory of motion of active vortices on synoptic tropospheric levels, thereby controlling weather patterns in that region and the regional climate. This

Tropospheric radiowave propagation beyond the horizon

CERN Document Server

Du Castel, François

1966-01-01

Tropospheric Radiowave Propagation Beyond the Horizon deals with developments concerning the tropospheric propagation of ultra-short radio waves beyond the horizon, with emphasis on the relationship between the theoretical and the experimental. Topics covered include the general conditions of propagation in the troposphere; general characteristics of propagation beyond the horizon; and attenuation in propagation. This volume is comprised of six chapters and begins with a brief historical look at the various stages that have brought the technique of transhorizon links to its state of developmen

The zonal structure of tropical O3 and CO as observed by the Tropospheric Emission Spectrometer in November 2004 – Part 2: Impact of surface emissions on O3 and its precursors

Directory of Open Access Journals (Sweden)

G. Osterman

2009-06-01

Full Text Available The impact of surface emissions on the zonal structure of tropical tropospheric ozone and carbon monoxide is investigated for November 2004 using satellite observations, in-situ measurements, and chemical transport models in conjunction with inverse-estimated surface emissions.Vertical ozone profiles from the Tropospheric Emission Spectrometer (TES and ozone sonde measurements from the Southern Hemisphere Additional Ozonesondes (SHADOZ network show elevated concentrations of ozone over Indonesia and Australia (60–70 ppb in the lower troposphere against the backdrop of the well-known zonal "wave-one" pattern with ozone concentrations of (70–80 ppb centered over the Atlantic . Observational evidence from TES CO vertical profiles and Ozone Monitoring Instrument (OMI NO2 columns point to regional surface emissions as an important contributor to the elevated ozone over Indonesia. This contribution is investigated with the GEOS-Chem chemistry and transport model using surface emission estimates derived from an optimal inverse model, which was constrained by TES and Measurements Of Pollution In The Troposphere (MOPITT CO profiles (Jones et al., 2009. These a posteriori estimates, which were over a factor of 2 greater than climatological emissions, reduced differences between GEOS-Chem and TES ozone observations by 30–40% over Indonesia. The response of the free tropospheric chemical state to the changes in these emissions is investigated for ozone, CO, NOx, and PAN. Model simulations indicate that ozone over Indonesian/Australian is sensitive to regional changes in surface emissions of NOx but relatively insensitive to lightning NOx. Over sub-equatorial Africa and South America, free tropospheric NOx was reduced in response to increased surface emissions potentially muting ozone production.

Influence of aerosols and surface reflectance on satellite NO2 retrieval: seasonal and spatial characteristics and implications for NOx emission constraints

NARCIS (Netherlands)

Lin, J.T.; Liu, M.Y.; Xin, J.Y.; Boersma, K.F.; Spurr, R.; Zhang, Q.; Martin, R.

2015-01-01

Satellite retrievals of vertical column densities (VCDs) of tropospheric nitrogen dioxide (NO2) normally do not explicitly account for aerosol optical effects and surface reflectance anisotropy that vary with space and time. Here, we conduct an improved retrieval of NO2 VCDs over China, called the

A Prototype of Tropospheric Delay Correction in L1-SAIF Augmentation

Science.gov (United States)

Takeichi, Noboru; Sakai, Takeyasu; Fukushima, Sounosuke; Ito, Ken

L1-SAIF signal is one of the navigation signals of Quasi-Zenith Satellite System, which provides an augmentation function for mobile users in Japan. This paper presents the detail of the tropospheric delay correction in L1-SAIF augmentation. The tropospheric delay correction information is generated at the ground station using the data collected at GEONET (GPS Earth Observation NETwork) stations. The correction message contains the information of the zenith tropospheric delay (ZTD) values at 105 Tropospheric Grid Points (TGP) in the experiment area. From this message a mobile user can acquire the ZTD value at some neighboring TGPs, and estimate the local ZTD value accurately by using a suitable ZTD model function. Only 3 L1-SAIF messages are necessary to provide all of the tropospheric correction information. Several investigations using the actual data observed at many GEONET stations overall Japan have proved that it is possible to achieve the correction accuracy of 13.2mm (rms).

Quantitative analysis of SCIAMACHY carbon monoxide total column measurements

NARCIS (Netherlands)

Laat, de A.T.J.; Gloudemans, A.M.S.; Schrijver, H.; Broek, van den M.M.P.; Meirink, J.F.; Aben, I.; Krol, M.C.

2006-01-01

Global tropospheric ozone distributions, budgets, and radiative forcings from an ensemble of 26 state-of-the-art atmospheric chemistry models have been intercompared and synthesized as part of a wider study into both the air quality and climate roles of ozone. Results from three 2030 emissions

A tropospheric ozone maximum over the equatorial Southern Indian Ocean

Directory of Open Access Journals (Sweden)

L. Zhang

2012-05-01

Full Text Available We examine the distribution of tropical tropospheric ozone (O₃ from the Microwave Limb Sounder (MLS and the Tropospheric Emission Spectrometer (TES by using a global three-dimensional model of tropospheric chemistry (GEOS-Chem. MLS and TES observations of tropospheric O₃ during 2005 to 2009 reveal a distinct, persistent O₃ maximum, both in mixing ratio and tropospheric column, in May over the Equatorial Southern Indian Ocean (ESIO. The maximum is most pronounced in 2006 and 2008 and less evident in the other three years. This feature is also consistent with the total column O₃ observations from the Ozone Mapping Instrument (OMI and the Atmospheric Infrared Sounder (AIRS. Model results reproduce the observed May O₃ maximum and the associated interannual variability. The origin of the maximum reflects a complex interplay of chemical and dynamic factors. The O₃ maximum is dominated by the O₃ production driven by lightning nitrogen oxides (NO_x emissions, which accounts for 62% of the tropospheric column O₃ in May 2006. We find the contribution from biomass burning, soil, anthropogenic and biogenic sources to the O₃ maximum are rather small. The O₃ productions in the lightning outflow from Central Africa and South America both peak in May and are directly responsible for the O₃ maximum over the western ESIO. The lightning outflow from Equatorial Asia dominates over the eastern ESIO. The interannual variability of the O₃ maximum is driven largely by the anomalous anti-cyclones over the southern Indian Ocean in May 2006 and 2008. The lightning outflow from Central Africa and South America is effectively entrained by the anti-cyclones followed by northward transport to the ESIO.

Tropospheric trace gas measurement by tunable diode laser spectroscopy. Final report. Messung troposphaerischer Spurengase mittels Dioden-Laser-Spektroskopie. Abschlussbericht

Energy Technology Data Exchange (ETDEWEB)

Burrows, J P; Crutzen, P J; Harris, G W; Klemp, D; Johnson, T J; Perner, D; Wienhold, F G; Zenker, T

1991-01-01

This final report is concerned with tropospheric trace gas measurements by Tunable Diode Laser Spectroscopy (TDLAS). A TDLAS instrument was built which simultaneously measures four selected trace gases and is sufficiently sensitive for use in 'clean' air conditions. The instrument is the first of its kind to be used for measurements aboard ship platforms in clean marine air. In order to guarantee that the instrument function continuously for several weeks at a time under the difficult conditions encountered at sea, a variety of innovative technical developments were necessary. The TDLAS instrument was used to investigate boundary layer tropospheric chemistry in one engineering test and four field campaigns. Three of the field campaigns took place on board the German research vessels. The measurements on board the research vessels enabled different types of tropospheric air to be investigated: (i) clean maritime air; (ii) maritime regions influenced by continental sources of trace gases and pollutants, in particular the coastal region around the west coast of Africa was thoroughly investigated under downwind conditions. A large set of data of simultaneous measurements of key tropospheric trace gases (NO{sub 2}, CO, HCHO, H{sub 2}O{sub 2} and O{sub 3}) were obtained which help paint a more complete picture of tropospheric oxidation cycles. The first measurements of H{sub 2}O{sub 2} in the remote marine boundary layer are reported. In selected regions successful TDLAS measurements of HCl and COS were obtained, results in themselves of importance. Intercomparisons of TDLAS and other measurement techniques were successfully undertaken. (orig./BBR).

A model study of the effects of intermittent loss on odd nitrogen concentrations in the lower troposphere

Science.gov (United States)

Stewart, R. W.; Hameed, S.; Matloff, G.

1983-01-01

A time-dependent box model of the lower troposphere which includes a description of photochemical and physical processes has been developed. This model has been applied to the calculation of nitric acid and NO(x)(NO + NO2) concentrations over a diurnal cycle which includes precipitation. Nitric acid concentrations and the HNO3/NO(x) ratio are found to be highly variable under the assumptions regarding the frequency, duration, and intensity of precipitation employed in this model. The chemistry of odd nitrogen compounds during the night is potentially important in establishing the level of nitric acid in the lower troposphere. These calculations also indicate that relatively large errors may occur when the continuity equation describing nitric acid variations is averaged over a diurnal cycle which includes precipitation. Interpretation of simultaneous measurements of HNO3 and NO(x) will require some knowledge of the history of the observed air mass and may require an improved understanding of nighttime odd nitrogen chemistry.

The governing processes and timescales of stratosphere-to-troposphere transport and its contribution to ozone in the Arctic troposphere

Science.gov (United States)

Liang, Q.; Douglass, A. R.; Duncan, B. N.; Stolarski, R. S.; Witte, J. C.

2009-05-01

We used the seasonality of a combination of atmospheric trace gases and idealized tracers to examine stratosphere-to-troposphere transport and its influence on tropospheric composition in the Arctic. Maximum stratosphere-to-troposphere transport of CFCs and O3 occurs in April as driven by the Brewer-Dobson circulation. Stratosphere-troposphere exchange (STE) occurs predominantly between 40° N to 80° N with stratospheric influx in the mid-latitudes (30-70° N) accounting for 67-81% of the air of stratospheric origin in the Northern Hemisphere extratropical troposphere. Transport from the lower stratosphere to the lower troposphere (LT) takes three months on average, one month to cross the tropopause, the second month to travel from the upper troposphere (UT) to the middle troposphere (MT), and the third month to reach the LT. During downward transport, the seasonality of a trace gas can be greatly impacted by wet removal and chemistry. A comparison of idealized tracers with varying lifetimes suggests that when initialized with the same concentrations and seasonal cycles at the tropopause, trace gases that have shorter lifetimes display lower concentrations, smaller amplitudes, and earlier seasonal maxima during transport to the LT. STE contributes to O3 in the Arctic troposphere directly from the transport of O3 and indirectly from the transport of NOy. Direct transport of O3 from the stratosphere accounts for 78% of O3 in the Arctic UT with maximum contributions occurring from March to May. The stratospheric contribution decreases significantly in the MT/LT (20-25% of total O3) and shows a very weak March-April maximum. Our NOx budget analysis in the Arctic UT shows that during spring and summer, the stratospheric injection of NOy-rich air increases NOx concentrations above the 20 pptv threshold level, thereby shifting the Arctic UT from a regime of net photochemical ozone loss to one of net production with rates as high as +16 ppbv/month.

Recent Biomass Burning in the Tropics and Related Changes in Tropospheric Ozone

Science.gov (United States)

Ziemke; Chandra, J. R. S.; Duncan, B. N.; Schoeberl, M. R.; Torres, O.; Damon, M. R.; Bhartia, P. K.

2009-01-01

Biomass burning is an important source of chemical precursors of tropospheric ozone. In the tropics, biomass burning produces ozone enhancements over broad regions of Indonesia, Africa, and South America including Brazil. Fires are intentionally set in these regions during the dry season each year to clear cropland and to clear land for human/industrial expansion. In Indonesia enhanced burning occurs during dry El Nino conditions such as in 1997 and 2006. These burning activities cause enhancement in atmospheric particulates and trace gases which are harmful to human health. Measurements from the Aura Ozone Monitoring Instrument (OMI) and Microwave Limb Sounder (MLS) from October 2004-November 2008 are used to evaluate the effects of biomass burning on tropical tropospheric ozone. These measurements show sizeable decreases approx.15-20% in ozone in Brazil during 2008 compared to 2007 which we attribute to the reduction in biomass burning. Three broad biomass burning regions in the tropics (South America including Brazil, western Africa, and Indonesia) were analyzed in the context of OMI/MLS measurements and the Global Modeling Initiative (GMI) chemical transport model developed at Goddard Space Flight Center. The results indicate that the impact of biomass burning on ozone is significant within and near the burning regions with increases of approx.10-25% in tropospheric column ozone relative to average background concentrations. The model suggests that about half of the increases in ozone from these burning events come from altitudes below 3 km. Globally the model indicates increases of approx.4-5% in ozone, approx.7-9% in NO, (NO+NO2), and approx.30-40% in CO.

Tropospheric nitrogen dioxide column retrieval based on ground-based zenith-sky DOAS observations

Science.gov (United States)

Tack, F. M.; Hendrick, F.; Pinardi, G.; Fayt, C.; Van Roozendael, M.

2013-12-01

A retrieval approach has been developed to derive tropospheric NO2 vertical column amounts from ground-based zenith-sky measurements of scattered sunlight. Zenith radiance spectra are observed in the visible range by the BIRA-IASB Multi-Axis Differential Optical Absorption Spectroscopy (MAX-DOAS) instrument and analyzed by the DOAS technique, based on a least-squares spectral fitting. In recent years, this technique has shown to be a well-suited remote sensing tool for monitoring atmospheric trace gases. The retrieval algorithm is developed and validated based on a two month dataset acquired from June to July 2009 in the framework of the Cabauw (51.97° N, 4.93° E) Intercomparison campaign for Nitrogen Dioxide measuring Instruments (CINDI). Once fully operational, the retrieval approach can be applied to observations from stations of the Network for the Detection of Atmospheric Composition Change (NDACC). The obtained tropospheric vertical column amounts are compared with the multi-axis retrieval from the BIRA-IASB MAX-DOAS instrument and the retrieval from a zenith-viewing only SAOZ instrument (Système d'Analyse par Observations Zénithales), owned by Laboratoire Atmosphères, Milieux, Observations Spatiales (LATMOS). First results show a good agreement for the whole time series with the multi-axis retrieval (R = 0.82; y = 0.88x + 0.30) as well as with the SAOZ retrieval (R = 0.85; y = 0.76x + 0.28 ). Main error sources arise from the uncertainties in the determination of tropospheric and stratospheric air mass factors, the stratospheric NO2 abundances and the residual amount in the reference spectrum. However zenith-sky measurements have been commonly used over the last decades for stratospheric monitoring, this study also illustrates the suitability for retrieval of tropospheric column amounts. As there are long time series of zenith-sky acquisitions available, the developed approach offers new perspectives with regard to the use of observations from the NDACC

Tropospheric chemistry research in the U.S.: 1991-1994

Science.gov (United States)

Penner, Joyce E.; Atherton, Cynthia S.; Dignon, Jane

1995-07-01

The troposphere is chemically complex. Many of the important species in the troposphere are short-lived, with lifetimes less than or of order of a month. Hence, the composition of the troposphere is regionally diverse, leading to regionally diverse chemical processes which control that composition. With the advent of three-dimensional models and regionally-specific estimates of emissions, however, it has become clear that human activity has perturbed the composition of even short-lived species over vast regions of the globe. The list of short-lived species of concern includes the reactive nitrogen oxides, reactive sulfur, ozone, nonmethane hydrocarbons and carbon monoxide. Observations have established that increases in the long-lived species such as carbon dioxide, methane, nitrous oxide, and the chlorofluorocarbons are taking place with important resulting impacts on stratospheric chemistry. Further, there is some indication that carbonyl sulfide (a major precursor to stratospheric aerosols) may have an important anthropogenic source. Growth of pollutants such as these are of concern because they act as greenhouse gases or aerosol precursors (CO2, CH4, O3, N2O, chlorofluorocarbons, carbonyl sufide, reactive sulfur), as agents for depletion of stratospheric ozone (N2O, chlorofluorocarbons), are harmful to vegetation (O3, acids) or act as nutrients (nitrate, sulfate, trace metals). The chemical interactions are important to understand, because the build up of pollutants depends not only on the rates of their release into the troposphere but on their rate of removal in the troposphere. Removal rates depend on processes which determine the rate of oxidation of the component (which for most species proceeds mainly by reaction with the hydroxyl radical) or through precipitation scavenging or dissolution in the ocean (which requires that the pollutant or its oxidation product(s) be soluble in water).

Five years of NO2 Mobile-DOAS measurements in Europe: an overview

Science.gov (United States)

Merlaud, Alexis; Fayt, Caroline; Pinardi, Gaia; Tack, Frederik; Hendrick, François; Le Roux, Anabel-Lise; Constantin, Daniel-Eduard; Voiculescu, Mirela; Shaiganfar, Reza; Wagner, Thomas; Van Roozendael, Michel

2014-05-01

Since the CINDI campaign held in the Netherlands in July 2009, BIRA-IASB has been operating a car-based mobile-DOAS system, primarily dedicated to tropospheric NO2 measurements. The instrument is based on two similar compact spectrometers and records scattered light spectra simultaneously in the zenith direction and 30° above the horizon, following the MAX-DOAS approach. After CINDI, Mobile-DOAS measurements were performed on a routine basis between March 2010 and August 2011, mostly across Belgium, but also in Luxembourg, France, and Germany. From 2011, another BIRA-IASB mobile-DOAS instrument, using a single zenith channel, was operated in Romania through a collaboration with the University of Galati. In June 2013, these two mobile-DOAS instruments took part in the MADCAT campaign in Mainz, Germany, together with the MPIC mobile-DOAS system, based on a mini MAX-DOAS. We describe the BIRA-IASB instruments, our strategy to retrieve the NO2 tropospheric column, and the large database that was constituted. The latter is particularly interesting for its size: it covers some 500 hours of measurements and 20 000 km, including rural, periurban and urban areas with different air quality conditions. A 2011 cloud-free subset of the measurements is compared with OMI data. We also present preliminary results of an intercomparison between the three mobile-DOAS instruments operated during MADCAT. The high spatial frequency of the measurements (around 100 m) makes them valuable to study the NO2 horizontal gradients in polluted areas. This has implications in the context of air quality satellite validation studies, in which the variability of NO2 inside a satellite pixel must be taken into account.

The global warming potential of methane reassessed with combined stratosphere and troposphere chemistry

Science.gov (United States)

Holmes, C. D.; Archibald, A. T.; Eastham, S. D.; Søvde, O. A.

2017-12-01

Methane is a direct and indirect greenhouse gas. The direct greenhouse effect comes from the radiation absorbed and emitted by methane itself. The indirect greenhouse effect comes from radiatively active gases that are produced during methane oxidation: principally O3, H2O, and CO2. Methane also suppresses tropospheric OH, which indirectly affects numerous greenhouses gases and aerosols. Traditionally, the methane global warming potential (GWP) has included the indirect effects on tropospheric O3 and OH and stratospheric H2O, with these effects estimated independently from unrelated tropospheric and stratospheric chemistry models and observations. Using this approach the CH4 is about 28 over 100 yr (without carbon cycle feedbacks, IPCC, 2013). Here we present a comprehensive analysis of the CH4 GWP in several 3-D global atmospheric models capable of simulating both tropospheric and stratospheric chemistry (GEOS-Chem, Oslo CTM3, UKCA). This enables us to include, for the first time, the indirect effects of CH4 on stratospheric O3 and stratosphere-troposphere coupling. We diagnose the GWP from paired simulations with and without a 5% perturbation to tropospheric CH4 concentrations. Including stratospheric chemistry nearly doubles the O3 contribution to CH4 GWP because of O3 production in the lower stratosphere and because CH4 inhibits Cl-catalyzed O3 loss in the upper stratosphere. In addition, stratosphere-troposphere coupling strengthens the chemical feedback on its own lifetime. In the stratosphere, this feedback operates by a CH4 perturbation thickening the stratospheric O3 layer, which impedes UV-driven OH production in the troposphere and prolongs the CH4 lifetime. We also quantify the impact of CH4-derived H2O on the stratospheric HOx cycles but these effects are small. Combining all of the above, these models suggest that the 100-yr GWP of CH4 is over 33.5, a 20% increase over the latest IPCC assessment.

Development of ground-based lidars for measuring H2O and O3 profiles in the troposphere

Science.gov (United States)

Sakai, T.; Abo, M.; Pham, L. H. P.; Uchino, O.; Nagai, T.; Izumi, T.; Morino, I.; Ohyama, H.; Nagasawa, C.

2015-12-01

Water vapor is the strongest natural greenhouse gas and a highly variable atmospheric constituent. It plays an important role of the energy transfer and the meteorological phenomena such as evaporation, vapor transport, cloud formation, and rainfall in the troposphere. Ozone is an important air pollutant that at high concentrations impacts on human health and ecosystem including crops and also a greenhouse gas that plays an important role in climate change. Aerosol is an important climate parameter and also one of the largest error sources (causes) in retrieval from solar reflected short wavelength infrared radiances observed with greenhouse gases observing satellites such as the GOSAT and OCO-2. Therefore, we have been developing ground-based differential absorption lidars (DIALs) for measuring the tropospheric water vapor, ozone and aerosols.The water vapor DIAL employs two distributed Bragg reflector (DBR) lasers operating at 829.054 nm for the online wavelength and 829.124 nm for the offline wavelength with tapered semiconductor optical amplifier (TSOA) in a master oscillator power amplifier (MOPA) configuration, and utilizes pseudorandom coded pulse modulation technique.It has started to measure the vertical distribution of lower tropospheric water vapor in order to improve accuracy and lead time of numerical weather prediction of local heavy rainfalls. Well-organized and regularly spaced convective cells of which vertical thickness were 200 m and the periods were 10 minutes were observed in the top of planetary boundary layer at 2.5 km altitude over Tokyo (35.66°N, 139.37°E) on 22 June 2015.The ozone DIAL employs a Nd:YAG laser and a 2 m long Raman cell filled with CO2 gas which generates four Stokes lines (276.2, 287.2, 299.1, and 312.0 nm) of stimulated Raman scattering, and two receiving telescopes with diameters of 49 and 10 cm.It has started to measure the vertical distributions of the tropospheric ozone as well as aerosols and thin cirrus cloud in

Three years of global carbon monoxide from SCIAMACHY: comparison with MOPITT and first results related to the detection of enhanced CO over cities

Directory of Open Access Journals (Sweden)

M. Buchwitz

2007-01-01

Full Text Available Carbon monoxide (CO is an important atmospheric constituent affecting air quality and climate. SCIAMACHY on ENVISAT is currently the only satellite instrument that can measure the vertical column of CO with nearly equal sensitivity at all altitudes down to the Earth's surface because of its near-infrared nadir observations of reflected solar radiation. Here we present three years' (2003–2005 of SCIAMACHY CO columns consistently retrieved with the latest version of our retrieval algorithm (WFMDv0.6. We describe the retrieval method and discuss the multi-year global CO data set focusing on a comparison with the operational CO column data product of MOPITT. We found reasonable to good agreement (~20% with MOPITT, with the best agreement for 2004. We present detailed results for various regions (Europe, Middle East, India, China and discuss to what extent enhanced levels of CO can be detected over populated areas including individual cities. The expected CO signal from cities is close to or even below the detection limit of individual measurements. We show that cities can be identified when averaging long time series.

Tropospheric ozone observations - How well can we assess tropospheric ozone changes?

Science.gov (United States)

Tarasick, D. W.; Galbally, I. E.; Ancellet, G.; Leblanc, T.; Wallington, T. J.; Ziemke, J. R.; Steinbacher, M.; Stähelin, J.; Vigouroux, C.; Hannigan, J. W.; García, O. E.; Foret, G.; Zanis, P.; Liu, X.; Weatherhead, E. C.; Petropavlovskikh, I. V.; Worden, H. M.; Osman, M.; Liu, J.; Lin, M.; Cooper, O. R.; Schultz, M. G.; Granados-Muñoz, M. J.; Thompson, A. M.; Cuesta, J.; Dufour, G.; Thouret, V.; Hassler, B.; Trickl, T.

2017-12-01

Since the early 20th century, measurements of ozone in the free troposphere have evolved and changed. Data records have different uncertainties and biases, and differ with respect to coverage, information content, and representativeness. Almost all validation studies employ ECC ozonesondes. These have been compared to UV-absorption measurements in a number of intercomparison studies, and show a modest ( 1-5%) high bias in the troposphere, with an uncertainty of 5%, but no evidence of a change over time. Umkehr, lidar, FTIR, and commercial aircraft all show modest low biases relative to the ECCs, and so -- if the ECC biases are transferable -- all agree within 1σ with the modern UV standard. Relative to the UV standard, Brewer-Mast sondes show a 20% increase in sensitivity from 1970-1995, while Japanese KC sondes show an increase of 5-10%. Combined with the shift of the global ozonesonde network to ECCs, this can induce a false positive trend, in analyses based on sonde data. Passive sounding methods -- Umkehr, FTIR and satellites -- have much lower vertical resolution than active methods, and this can limit the attribution of trends. Satellite biases are larger than those of other measurement systems, ranging between -10% and +20%, and standard deviations are large: about 10-30%, versus 5-10% for sondes, aircraft, lidar and ground-based FTIR. There is currently little information on measurement drift for satellite measurements of tropospheric ozone. This is an evident area of concern if satellite retrievals are used for trend studies. The importance of ECC sondes as a transfer standard for satellite validation means that efforts to homogenize existing records, by correcting for known changes and by adopting strict standard operating procedures, should continue, and additional research effort should be put into understanding and reducing sonde uncertainties. Representativeness is also a potential source of large errors, which are difficult to quantify. The global

Global model of zenith tropospheric delay proposed based on EOF analysis

Science.gov (United States)

Sun, Langlang; Chen, Peng; Wei, Erhu; Li, Qinzheng

2017-07-01

Tropospheric delay is one of the main error budgets in Global Navigation Satellite System (GNSS) measurements. Many empirical correction models have been developed to compensate this delay, and models which do not require meteorological parameters have received the most attention. This study established a global troposphere zenith total delay (ZTD) model, called Global Empirical Orthogonal Function Troposphere (GEOFT), based on the empirical orthogonal function (EOF, also known as geographically weighted PCAs) analysis method and the Global Geodetic Observing System (GGOS) Atmosphere data from 2012 to 2015. The results showed that ZTD variation could be well represented by the characteristics of the EOF base function Ek and associated coefficients Pk. Here, E1 mainly signifies the equatorial anomaly; E2 represents north-south asymmetry, and E3 and E4 reflects regional variation. Moreover, P1 mainly reflects annual and semiannual variation components; P2 and P3 mainly contains annual variation components, and P4 displays semiannual variation components. We validated the proposed GEOFT model using tropospheric delay data of GGOS ZTD grid data and the tropospheric product of the International GNSS Service (IGS) over the year 2016. The results showed that GEOFT model has high accuracy with bias and RMS of -0.3 and 3.9 cm, respectively, with respect to the GGOS ZTD data, and of -0.8 and 4.1 cm, respectively, with respect to the global IGS tropospheric product. The accuracy of GEOFT demonstrating that the use of the EOF analysis method to characterize ZTD variation is reasonable.

Large-scale upper tropospheric pollution observed by MIPAS HCN and C2H6 global distributions

Science.gov (United States)

Glatthor, N.; von Clarmann, T.; Stiller, G. P.; Funke, B.; Koukouli, M. E.; Fischer, H.; Grabowski, U.; Höpfner, M.; Kellmann, S.; Linden, A.

2009-12-01

We present global upper tropospheric HCN and C2H6 amounts derived from MIPAS/ENVISAT limb emission spectra. HCN and C2H6 are retrieved in the spectral regions 715.5-782.7 cm-1 and 811.5-835.7 cm-1, respectively. The datasets consist of 54 days between September 2003 and March 2004. This period covers the peak and decline of the southern hemispheric biomass burning period and some months thereafter. HCN is a nearly unambiguous tracer of biomass burning with an assumed tropospheric lifetime of several months. Indeed, the most significant feature in the MIPAS HCN dataset is an upper tropospheric plume of enhanced values caused by southern hemispheric biomass burning, which in September and October 2003 extended from tropical South America over Africa, Australia to the Southern Pacific. The spatial extent of this plume agrees well with the MOPITT CO distribution of September 2003. Further there is good agreement with the shapes and mixing ratios of the southern hemispheric HCN and C2H6 fields measured by the ACE experiment between September and November 2005. The MIPAS HCN plume extended from the lowermost observation height of 8 km up to about 16 km altitude, with maximum values of 500-600 pptv in October 2003. It was still clearly visible in December 2003, but had strongly decreased by March 2004, confirming the assumed tropospheric lifetime. The main sources of C2H6 are production and transmission of fossil fuels, followed by biofuel use and biomass burning. The C2H6 distribution also clearly reflected the southern hemispheric biomass burning plume and its seasonal variation, with maximum amounts of 600-700 pptv. Generally there was good spatial overlap between the southern hemispheric distributions of both pollution tracers, except for the region between Peru and the mid-Pacific. Here C2H6was considerably enhanced, whereas the HCN amounts were low. Backward trajectory calculations suggested that industrial pollution was responsible for the elevated C2H6

Large-scale upper tropospheric pollution observed by MIPAS HCN and C2H6 global distributions

Directory of Open Access Journals (Sweden)

A. Linden

2009-12-01

Full Text Available We present global upper tropospheric HCN and C2H6 amounts derived from MIPAS/ENVISAT limb emission spectra. HCN and C2H6 are retrieved in the spectral regions 715.5–782.7 cm−1 and 811.5–835.7 cm−1, respectively. The datasets consist of 54 days between September 2003 and March 2004. This period covers the peak and decline of the southern hemispheric biomass burning period and some months thereafter. HCN is a nearly unambiguous tracer of biomass burning with an assumed tropospheric lifetime of several months. Indeed, the most significant feature in the MIPAS HCN dataset is an upper tropospheric plume of enhanced values caused by southern hemispheric biomass burning, which in September and October 2003 extended from tropical South America over Africa, Australia to the Southern Pacific. The spatial extent of this plume agrees well with the MOPITT CO distribution of September 2003. Further there is good agreement with the shapes and mixing ratios of the southern hemispheric HCN and C2H6 fields measured by the ACE experiment between September and November 2005. The MIPAS HCN plume extended from the lowermost observation height of 8 km up to about 16 km altitude, with maximum values of 500–600 pptv in October 2003. It was still clearly visible in December 2003, but had strongly decreased by March 2004, confirming the assumed tropospheric lifetime. The main sources of C2H6 are production and transmission of fossil fuels, followed by biofuel use and biomass burning. The C2H6 distribution also clearly reflected the southern hemispheric biomass burning plume and its seasonal variation, with maximum amounts of 600–700 pptv. Generally there was good spatial overlap between the southern hemispheric distributions of both pollution tracers, except for the region between Peru and the mid-Pacific. Here C2H6was considerably enhanced, whereas the HCN amounts were low. Backward trajectory calculations suggested that industrial pollution was responsible

Decadal changes in global surface NO

NARCIS (Netherlands)

Miyazaki, Kazuyuki; Eskes, Henk; Sudo, Kengo; Boersma, Folkert; Bowman, Kevin; Kanaya, Yugo

2017-01-01

Global surface emissions of nitrogen oxides (NO_x ) over a 10-year period (2005-2014) are estimated from an assimilation of multiple satellite data sets: tropospheric NO₂ columns from Ozone Monitoring Instrument (OMI), Global Ozone Monitoring Experiment-2 (GOME- 2), and

Mercury oxidation from bromine chemistry in the free troposphere over the southeastern US

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S. Coburn

2016-03-01

Full Text Available The elevated deposition of atmospheric mercury over the southeastern United States is currently not well understood. Here we measure partial columns and vertical profiles of bromine monoxide (BrO radicals, a key component of mercury oxidation chemistry, to better understand the processes and altitudes at which mercury is being oxidized in the atmosphere. We use data from a ground-based MAX-DOAS instrument located at a coastal site ∼  1 km from the Gulf of Mexico in Gulf Breeze, FL, where we had previously detected tropospheric BrO (Coburn et al., 2011. Our profile retrieval assimilates information about stratospheric BrO from the WACCM chemical transport model (CTM, and uses only measurements at moderately low solar zenith angles (SZAs to estimate the BrO slant column density contained in the reference spectrum (SCDRef. The approach has 2.6 degrees of freedom, and avoids spectroscopic complications that arise at high SZA; knowledge about SCDRef further helps to maximize sensitivity in the free troposphere (FT. A cloud-free case study day with low aerosol load (9 April 2010 provided optimal conditions for distinguishing marine boundary layer (MBL: 0–1 km and free-tropospheric (FT: 1–15 km BrO from the ground. The average daytime tropospheric BrO vertical column density (VCD of ∼  2.3  ×  1013 molec cm−2 (SZA  <  70° is consistent with our earlier reports on other days. The vertical profile locates essentially all tropospheric BrO above 4 km, and shows no evidence for BrO inside the MBL (detection limit  <  0.5 pptv. BrO increases to  ∼  3.5 pptv at 10–15 km altitude, consistent with recent aircraft observations. Our case study day is consistent with recent aircraft studies, in that the oxidation of gaseous elemental mercury (GEM by bromine radicals to form gaseous oxidized mercury (GOM is the dominant pathway for GEM oxidation throughout the troposphere above Gulf

How Can TOLNet Help to Better Understand Tropospheric Ozone? A Satellite Perspective

Science.gov (United States)

Johnson, Matthew S.

2018-01-01

Potential sources of a priori ozone (O3) profiles for use in Tropospheric Emissions: Monitoring of Pollution (TEMPO) satellite tropospheric O3 retrievals are evaluated with observations from multiple Tropospheric Ozone Lidar Network (TOLNet) systems in North America. An O3 profile climatology (tropopause-based O3 climatology (TB-Clim), currently proposed for use in the TEMPO O3 retrieval algorithm) derived from ozonesonde observations and O3 profiles from three separate models (operational Goddard Earth Observing System (GEOS-5) Forward Processing (FP) product, reanalysis product from Modern-Era Retrospective analysis for Research and Applications version 2 (MERRA2), and the GEOS-Chem chemical transport model (CTM)) were: 1) evaluated with TOLNet measurements on various temporal scales (seasonally, daily, hourly) and 2) implemented as a priori information in theoretical TEMPO tropospheric O3 retrievals in order to determine how each a priori impacts the accuracy of retrieved tropospheric (0-10 km) and lowermost tropospheric (LMT, 0-2 km) O3 columns. We found that all sources of a priori O3 profiles evaluated in this study generally reproduced the vertical structure of summer-averaged observations. However, larger differences between the a priori profiles and lidar observations were observed when evaluating inter-daily and diurnal variability of tropospheric O3. The TB-Clim O3 profile climatology was unable to replicate observed inter-daily and diurnal variability of O3 while model products, in particular GEOS-Chem simulations, displayed more skill in reproducing these features. Due to the ability of models, primarily the CTM used in this study, on average to capture the inter-daily and diurnal variability of tropospheric and LMT O3 columns, using a priori profiles from CTM simulations resulted in TEMPO retrievals with the best statistical comparison with lidar observations. Furthermore, important from an air quality perspective, when high LMT O3 values were

Homepage for the Global Tropospheric Experiment

Science.gov (United States)

Ward, Eugene

1995-01-01

The objective of my NASA summer research project was to create a homepage to describe and present results from the NASA Global Tropospheric Experiment (GTE). The GTE is a major component of NASA's Tropospheric Chemistry Program and is managed in the Atmospheric Studies Branch, Atmospheric Sciences Division at the NASA Langley Research Center.

Nitrogen oxides in the troposphere – What have we learned from satellite measurements?

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Richter A.

2009-02-01

Full Text Available Nitrogen oxides are key species in the troposphere where they are linked to ozone formation and acid rain. The sources of nitrogen oxides are anthropogenic to large extend, mainly through combustion of fossil fuels. Satellite observations of NO2 provide global measurements of nitrogen oxides since summer 1995, and these data have been applied for many studies on the emission sources and strengths, the chemistry and the transport of NOx. In this paper, an overview will be given on satellite measurements of NO2 , some examples of typical applications and an outlook on future prospects.

Derivation of Tropospheric Ozone Climatology and Trends from TOMS Data

Science.gov (United States)

Newchurch, Michael J.; McPeters, Rich; Logan, Jennifer; Kim, Jae-Hwan

2002-01-01

This research addresses the following three objectives: (1) Derive tropospheric ozone columns from the TOMS instruments by computing the difference between total-ozone columns over cloudy areas and over clear areas in the tropics; (2) Compute secular trends in Nimbus-7 derived tropospheric Ozone column amounts and associated potential trends in the decadal-scale tropical cloud climatology; (3) Explain the occurrence of anomalously high ozone retrievals over high ice clouds.

Diurnal variations in H2O2, O3, PAN, HNO3 and aldehyde concentrations and NO/NO2 ratios at Rishiri Island, Japan: Potential influence from iodine chemistry

International Nuclear Information System (INIS)

Kanaya, Yugo; Tanimoto, Hiroshi; Matsumoto, Jun; Furutani, Hiroshi; Hashimoto, Shigeru; Komazaki, Yuichi; Tanaka, Shigeru; Yokouchi, Yoko; Kato, Shungo; Kajii, Yoshizumi; Akimoto, Hajime

2007-01-01

The presence of iodine chemistry, hypothesized due to the overprediction of HO 2 levels by a photochemical box model at Rishiri Island in June 2000, was quantitatively tested against the observed NO/NO 2 ratios and the net production rates of ozone. The observed NO/NO 2 ratios were reproduced reasonably well by considering the conversion of NO to NO 2 by IO, whose amount was calculated so as to reproduce the observed HO 2 levels. However, the net production rates of ozone were calculated to be negative when such high mixing ratios of IO were considered, which was inconsistent with the observed buildup of ozone during daytime. These results suggest that iodine chemistry may not be the sole mechanism for the reduced mixing ratios of HO 2 , or that 'hot spots' for iodine chemistry were present. Diurnal variations in the mixing ratios of HCHO, CH 3 CHO, peroxy acetyl nitrate (PAN) and HNO 3 observed during the study are presented along with the simulated ones. The box model simulations suggest that the effect of iodine chemistry on these concentrations is small and that important sources of CH 3 CHO and sinks of PAN are probably missing from our current understanding of the tropospheric chemistry mechanism

Application of ray-traced tropospheric slant delays to geodetic VLBI analysis

Science.gov (United States)

Hofmeister, Armin; Böhm, Johannes

2017-08-01

The correction of tropospheric influences via so-called path delays is critical for the analysis of observations from space geodetic techniques like the very long baseline interferometry (VLBI). In standard VLBI analysis, the a priori slant path delays are determined using the concept of zenith delays, mapping functions and gradients. The a priori use of ray-traced delays, i.e., tropospheric slant path delays determined with the technique of ray-tracing through the meteorological data of numerical weather models (NWM), serves as an alternative way of correcting the influences of the troposphere on the VLBI observations within the analysis. In the presented research, the application of ray-traced delays to the VLBI analysis of sessions in a time span of 16.5 years is investigated. Ray-traced delays have been determined with program RADIATE (see Hofmeister in Ph.D. thesis, Department of Geodesy and Geophysics, Faculty of Mathematics and Geoinformation, Technische Universität Wien. http://resolver.obvsg.at/urn:nbn:at:at-ubtuw:1-3444, 2016) utilizing meteorological data provided by NWM of the European Centre for Medium-Range Weather Forecasts (ECMWF). In comparison with a standard VLBI analysis, which includes the tropospheric gradient estimation, the application of the ray-traced delays to an analysis, which uses the same parameterization except for the a priori slant path delay handling and the used wet mapping factors for the zenith wet delay (ZWD) estimation, improves the baseline length repeatability (BLR) at 55.9% of the baselines at sub-mm level. If no tropospheric gradients are estimated within the compared analyses, 90.6% of all baselines benefit from the application of the ray-traced delays, which leads to an average improvement of the BLR of 1 mm. The effects of the ray-traced delays on the terrestrial reference frame are also investigated. A separate assessment of the RADIATE ray-traced delays is carried out by comparison to the ray-traced delays from the

The influence of boreal biomass burning emissions on the distribution of tropospheric ozone over North America and the North Atlantic during 2010

Directory of Open Access Journals (Sweden)

M. Parrington

2012-02-01

Full Text Available We have analysed the sensitivity of the tropospheric ozone distribution over North America and the North Atlantic to boreal biomass burning emissions during the summer of 2010 using the GEOS-Chem 3-D global tropospheric chemical transport model and observations from in situ and satellite instruments. We show that the model ozone distribution is consistent with observations from the Pico Mountain Observatory in the Azores, ozonesondes across Canada, and the Tropospheric Emission Spectrometer (TES and Infrared Atmospheric Sounding Instrument (IASI satellite instruments. Mean biases between the model and observed ozone mixing ratio in the free troposphere were less than 10 ppbv. We used the adjoint of GEOS-Chem to show the model ozone distribution in the free troposphere over Maritime Canada is largely sensitive to NO_x emissions from biomass burning sources in Central Canada, lightning sources in the central US, and anthropogenic sources in the eastern US and south-eastern Canada. We also used the adjoint of GEOS-Chem to evaluate the Fire Locating And Monitoring of Burning Emissions (FLAMBE inventory through assimilation of CO observations from the Measurements Of Pollution In The Troposphere (MOPITT satellite instrument. The CO inversion showed that, on average, the FLAMBE emissions needed to be reduced to 89% of their original values, with scaling factors ranging from 12% to 102%, to fit the MOPITT observations in the boreal regions. Applying the CO scaling factors to all species emitted from boreal biomass burning sources led to a decrease of the model tropospheric distributions of CO, PAN, and NO_x by as much as −20 ppbv, −50 pptv, and −20 pptv respectively. The modification of the biomass burning emission estimates reduced the model ozone distribution by approximately −3 ppbv (−8% and on average improved the agreement of the model ozone distribution compared to the observations throughout the free troposphere

Effects of the 2004 El Nino on tropospheric ozone and water vapor

NARCIS (Netherlands)

Chandra, S.; Ziemke, J.R.; Schoeberl, M.R.; Froidevaux, L.; Read, W.G.; Levelt, P.F.; Bhartia, P.K.

2007-01-01

The global effects of the 2004 El Nino on tropospheric ozone and H/sub 2/O based on Aura OMI and MLS measurements are analyzed. Although it was a weak El Nino from a historical perspective, it produced significant changes in these parameters in tropical latitudes. Tropospheric ozone increased by

Kinetics programs for simulation of tropospheric photochemistry on the global scale

International Nuclear Information System (INIS)

Elliott, S.; Kao, C.Y.J.; Turco, R.P.; Zhao, X.P.

1993-08-01

The study of tropospheric kinetics underlies global change because key greenhouse gases are photochemically active. Modeling of tropospheric chemistry on a global scale is essential because some indirect greenhouse gases are short-lived and interact in a non-linear fashion. It is also extremely challenging, however; the global change grid is extensive in both the physical and temporal domains, and critical lower atmospheric species include the organics and their oxidized derivatives, which are numerous. Several types of optimization may be incorporated into kinetics modules to enhance their ability to simulate the complete lower atmospheric gas phase chemical system. (1) The photochemical integrator can be accelerated by avoiding matrix and iterative solutions and by establishing families. Accuracy and mass conservation are sacrificed in the absence of iteration, but atom balancing is restorable post hoc. (2) Chemistry can be arranged upon the massive grid to exploit parallel processing, and solutions to its continuity equations can be automated to permit experimentation with species and reaction lists or family definitions. Costs in programming effort will be incurred in these cases. (3) Complex hydrocarbon decay sequences can be streamlined either through structural lumping methods descended from smog investigations, which require considerable calibration, or by defining surrogates for classes of compounds, with a loss in constituent detail. From among the available options, the most advantageous permutations will vary with the specific nature of any eventual global scale study, and there is likely to be demand for many approaches. Tracer transport codes serve as a foundation upon which tropospheric chemistry packages will be tested. Encroachment of the NO x sphere of influence upon tropical rain forests and the upper free troposphere are two examples of specific problems to which full three-dimensional chemical simulations might be applied

Retrieval of global upper tropospheric and stratospheric formaldehyde (H2CO distributions from high-resolution MIPAS-Envisat spectra

Directory of Open Access Journals (Sweden)

G. P. Stiller

2008-02-01

Full Text Available The Fourier transform spectrometer MIPAS (Michelson Interferometer for Passive Atmospheric Sounding on Envisat measures infrared emission of the Earth's atmosphere in a limb viewing mode. High spectral resolution measurements of MIPAS are sensitive to formaldehyde from the upper troposphere to the stratopause. Single profile retrievals of formaldehyde are dominated by a 60% noise error; however zonal mean values for 30 days of data during 8 September 2003 and 1 December 2003 reduces this error by a factor of 20 or more. The number of degrees of freedom for single profile retrieval ranges from 2 to 4.5 depending on latitude and number of cloud-free tangent altitudes. In the upper tropical troposphere zonal mean values of about 70 parts per trillion by volume (pptv were found, which have been attributed to biomass burning emissions. In the stratosphere, formaldehyde values are determined by photochemical reactions. In the upper tropical stratosphere, formaldehyde zonal mean maximum values can reach 130 pptv. Diurnal variations in this region can be up to 50 pptv. Comparisons with other satellite instruments show generally good agreement in the region of upper troposphere and lower stratosphere as well as in the upper stratosphere.

Characterization of tropospheric ozone based on lidar measurement in Hangzhou, East China during the G20 Leaders' Summit

Science.gov (United States)

Su, Wenjing; Liu, Cheng; Fan, Guangqiang; Hu, Qihou; Huang, Xin; Dong, Yunsheng; Zhang, Tianshu; Liu, Jianguo

2017-04-01

Owing to the G20 (Group of Twenty Finance Ministers and Central Bank Governors) Leaders' Summit (Sep.5th-6th, 2016), a series of strict air quality control measures were implemented in Hangzhou and its surrounding regions from Aug.26th to Sep.6th. A differential absorption lidar was employed to monitor tropospheric ozone in urban Hangzhou during a campaign from Aug. 24th to Sep. 10th, and the satellite-based NO2 VCDs and HCHO VCDs in the troposphere were also retrieved using the Ozone Monitoring Instrument (OMI). During our campaign, six O3 pollution events, which were determined according to the National Ambient Air Quality Standard of China (GB-3095-2012), and two stages with rapid reduction of O3 concentration on Aug. 26th and Sep.4-6th were observed. The temporal variation tendency of O3 concentrations was well reproduced by the Weather Research and Forecasting model coupled with chemistry (WRF-Chem). Typical cases with the abrupt rise and decline of O3 concentrations were analyzed using Hybrid Single-Particle Lagrangian Integrated Trajectory (HYSPLIT) back trajectory, satellite NO2 and HCHO product and the prediction by WRF-Chem model. The transport from northern cities have an important impact on pollutants observed in Hangzhou, and the chemical sensitivity of O3 production, which were approximately evaluated using the ratio of HCHO VCDs to NO2 VCDs in the troposphere, was turned from a mixed VOC-NOx-limited regime into a NOX-limited regime in Hangzhou due to the strict emission control measures.

The impact from emitted NO{sub x} and VOC in an aircraft plume. Model results for the free troposphere

Energy Technology Data Exchange (ETDEWEB)

Pleijel, K.

1998-04-01

The chemical fate of gaseous species in a specific aircraft plume is investigated using an expanding box model. The model treats the gas phase chemical reactions in detail, while other parameters are subject to a high degree of simplification. Model simulations were carried out in a plume up to an age of three days. The role of emitted VOC, NO{sub x} and CO as well as of background concentrations of VOC, NO{sub x} and ozone on aircraft plume chemistry was investigated. Background concentrations were varied in a span of measured values in the free troposphere. High background concentrations of VOC were found to double the average plume production of ozone and organic nitrates. In a high NO{sub x} environment the plume production of ozone and organic nitrates decreased by around 50%. The production of nitric acid was found to be less sensitive to background concentrations of VOC, and increased by up to 50% in a high NO{sub x} environment. Mainly, emitted NO{sub x} caused the plume production of ozone, nitric acid and organic nitrates. The ozone production during the first hours is determined by the relative amount of NO{sub 2} in the NO{sub x} emissions. The impact from emitted VOC was in relative values up to 20% of the ozone production and 65% of the production of organic nitrates. The strongest relative influence from VOC was found in an environment characterized by low VOC and high NO{sub x} background concentrations, where the absolute peak production was lower than in the other scenarios. The effect from emitting VOC and NO{sub x} at the same time added around 5% for ozone, 15% for nitric acid and 10% for organic nitrates to the plume production caused by NO{sub x} and VOC when emitted separately 47 refs, 15 figs, 4 tabs

On the use of Satellite Remote Sensing and GIS to detect NO2 in the Troposphere

DEFF Research Database (Denmark)

Nielsen, Søren Zebitz

2012-01-01

This thesis studies the spatio-temporal patterns and trends in NO2 air pollution over Denmark using the satellite remote sensing product OMNO2e retrieved from the OMI instrument on the NASA AURA satellite. These data are related to in situ measurements of NO2 made at four rural and four urban...... measured in Denmark. Trends in the data are assessed and declining trends are seen over several European cities, whereas no significant trends are found in the Danish area. The mean distribution of NO2 from the satellite data is also used to evaluate the NOx emission inventory....

Aura OMI observations of changes in SO2 and NO2 emissions at local, regional and global scales

Science.gov (United States)

Krotkov, N. A.; McLinden, C. A.; Li, C.; Lamsal, L. N.; Celarier, E. A.; Marchenko, S. V.; Swartz, W.; Bucsela, E. J.; Joiner, J.; Duncan, B. N.; Boersma, K. F.; Veefkind, P.; Levelt, P.; Fioletov, V.; Dickerson, R. R.; He, H.; Lu, Z.; Streets, D. G.

2015-12-01

Space-based pollution monitoring from current and planned satellite UV-Vis spectrometers play an increasingly important role in studies of tropospheric chemistry and also air quality applications to help mitigate anthropogenic and natural impacts on sensitive ecosystems, and human health. We present long-term changes in tropospheric SO2 and NO2 over some of the most polluted industrialized regions of the world observed by the Ozone Monitoring Instrument (OMI) onboard NASA's Aura satellite. Using OMI data, we identified about 400 SO2 "hot spots" and estimated emissions from them. In many regions emissions and their ambient pollution levels have decreased significantly, such as over eastern US, Europe and China. OMI observed about 50% reduction in SO2 and NO2 pollution over the North China plain in 2012-2014 that can be attributed to both government efforts to restrain emissions from the power and industrial sectors and the economic slowdown. While much smaller, India's SO2 and NO2 emissions from coal power plants and smelters are growing at a fast pace, increasing by about 200% and 50% from 2005 to 2014. Over Europe and the US OMI-observed trends agree well with those from available in situ measurements of surface concentrations, deposition and emissions data. However, for some regions (e.g., Mexico, Middle East) the emission inventories may be incomplete and OMI can provide emission estimates for missing sources, such as SO2 sources observed over the Persian Gulf. It is essential to continue long-term overlapping satellite data records of air quality with increased spatial and temporal resolution to resolve point pollution sources using oversampling technique. We discuss how Aura OMI pollution measurements and emission estimates will be continued with the US JPSS and European Sentinel series for the next 20 years and further enhanced by the addition of three geostationary UV-VIS instruments.

Reductions of NO2 detected from space during the 2008 Beijing Olympic Games

Science.gov (United States)

Mijling, B.; van der A, R. J.; Boersma, K. F.; Van Roozendael, M.; De Smedt, I.; Kelder, H. M.

2009-07-01

During the 2008 Olympic and Paralympic Games in Beijing (from 8 August to 17 September), local authorities enforced strong measures to reduce air pollution during the events. To evaluate the direct effect of these measures, we use the tropospheric NO2 column observations from the satellite instruments GOME-2 and OMI. We interpret these data against simulations from the regional chemistry transport model CHIMERE, based on a 2006 emission inventory, and find a reduction of NO2 concentrations of approximately 60% above Beijing during the Olympic period. The air quality measures were especially effective in the Beijing area, but also noticeable in surrounding cities of Tianjin (30% reduction) and Shijiazhuang (20% reduction).

Development of a portable instrument to measure ozone production rates in the troposphere

Science.gov (United States)

Sklaveniti, Sofia; Locoge, Nadine; Stevens, Philip; Kumar, Vinod; Sinha, Vinayak; Dusanter, Sébastien

2015-04-01

Ground-level ozone is a key species related to air pollution, causing respiratory problems, damaging crops and forests, and affecting the climate. Our current understanding of the tropospheric ozone-forming chemistry indicates that net ozone production occurs via reactions of peroxy radicals (HO2 + RO2) with NO producing NO2, whose photolysis leads to O3 formation. Production rates of tropospheric ozone, P(O3), depend on concentrations of oxides of nitrogen (NOx = NO + NO2) and Volatile Organic Compounds (V OCs), but also on production rates of ROx radicals (OH + HO2 + RO2). The formation of ozone follows a complex nonlinear chemistry that makes strategies for reducing ozone difficult to implement. In this context, atmospheric chemistry models are used to develop emission regulations, but there are still uncertainties associated with the chemical mechanisms used in these models. Testing the ozone formation chemistry in atmospheric models is needed, in order to ensure the development of effective strategies for ozone reduction. We will present the development of an instrument for direct measurements of ozone production rates (OPR) in ambient air. The OPR instrument is made of three components: (i) two quartz flow tubes to sample ambient air, one exposed to solar radiation and one covered by a UV filter, (ii) a NO2-to-O3 conversion unit, and (iii) an ozone analyzer. The total amount of ozone exiting each flow tube is conserved in the form of Ox = NO2 + O3. Ozone production rates P(O3) are derived from the difference in Ox concentration between the two flow tubes, divided by the exposure time of air inside the flow tubes. We will present studies that were carried out in the laboratory to characterize each part of the instrument and we will discuss the performances of the OPR instrument based on experiments carried out using synthetic air mixtures of known composition (NOx and V OCs). Chemical modeling will also be presented to assess the reliability of ozone

Seasonal Variability of Saturn's Tropospheric Temperatures, Winds and Para-H2 from Cassini Far-IR Spectroscopy

Science.gov (United States)

Fletcher, Leigh N.; Irwin, P. G. J; Achterberg, R. K.; Orton, G. S.; Flasar, F. M.

2015-01-01

Far-IR 16-1000 micrometer spectra of Saturn's hydrogen-helium continuum measured by Cassini's Composite Infrared Spectrometer (CIRS) are inverted to construct a near-continuous record of upper tropospheric (70-700 mbar) temperatures and para-H2 fraction as a function of latitude, pressure and time for a third of a saturnian year (2004-2014, from northern winter to northern spring). The thermal field reveals evidence of reversing summertime asymmetries superimposed onto the belt/zone structure. The temperature structure is almost symmetric about the equator by 2014, with seasonal lag times that increase with depth and are qualitatively consistent with radiative climate models. Localised heating of the tropospheric hazes (100-250 mbar) create a distinct perturbation to the temperature profile that shifts in magnitude and location, declining in the autumn hemisphere and growing in the spring. Changes in the para-H2 (f(sub p)) distribution are subtle, with a 0.02-0.03 rise over the spring hemisphere (200-500 mbar) perturbed by (i) low-f(sub p) air advected by both the springtime storm of 2010 and equatorial upwelling; and (ii) subsidence of high-f(sub p) air at northern high latitudes, responsible for a developing north-south asymmetry in f(sub p). Conversely, the shifting asymmetry in the para-H2 disequilibrium primarily reflects the changing temperature structure (and hence the equilibrium distribution of f(sub p)), rather than actual changes in f(sub p) induced by chemical conversion or transport. CIRS results interpolated to the same point in the seasonal cycle as re-analysed Voyager-1 observations (early northern spring) show qualitative consistency from year to year (i.e., the same tropospheric asymmetries in temperature and f(sub p)), with the exception of the tropical tropopause near the equatorial zones and belts, where downward propagation of a cool temperature anomaly associated with Saturn's stratospheric oscillation could potentially perturb tropopause

Free-tropospheric BrO investigations based on GOME

Science.gov (United States)

Post, P.; van Roozendael, M.; Backman, L.; Damski, J.; Thölix, L.; Fayt, C.; Taalas, P.

2003-04-01

Bromine compounds contribute significantly to the stratospheric ozone depletion. However measurements of most bromine compounds are sparse or non-existent, and experimental studies essentially rely on BrO observations. The differences between balloon and ground based measurements of stratospheric BrO columns and satellite total column measurements are too large to be explained by measurement uncertainties. Therefore, it has been assumed that there is a concentration of BrO in the free troposphere of about 1-3 ppt. In a previous work, we have calculated the tropospheric BrO abundance as the difference between total BrO and stratospheric BrO columns. The total vertical column densities of BrO are extracted from GOME measurements using IASB-BIRA algorithms. The stratospheric amount has been calculated using chemical transport models (CTM). Results from SLIMCAT and FinROSE simulations are used for this purpose. SLIMCAT is a widely used 3D CTM that has been tested against balloon measurements. FinROSE is a 3D CTM developed at FMI. We have tried several different tropospheric BrO profiles. Our results show that a profile with high BrO concentrations in the boundary layer usually gives unrealistically high tropospheric column values over areas of low albedo (like oceans). This suggests that the tropospheric BrO would be predominantly distributed in the free troposphere. In this work, attempts are made to identify the signature of a free tropospheric BrO content when comparing cloudy and non-cloudy scenes. The possible impact of orography on measured BrO columns is also investigated.

Performance analysis of NOAA tropospheric signal delay model

International Nuclear Information System (INIS)

Ibrahim, Hassan E; El-Rabbany, Ahmed

2011-01-01

Tropospheric delay is one of the dominant global positioning system (GPS) errors, which degrades the positioning accuracy. Recent development in tropospheric modeling relies on implementation of more accurate numerical weather prediction (NWP) models. In North America one of the NWP-based tropospheric correction models is the NOAA Tropospheric Signal Delay Model (NOAATrop), which was developed by the US National Oceanic and Atmospheric Administration (NOAA). Because of its potential to improve the GPS positioning accuracy, the NOAATrop model became the focus of many researchers. In this paper, we analyzed the performance of the NOAATrop model and examined its effect on ionosphere-free-based precise point positioning (PPP) solution. We generated 3 year long tropospheric zenith total delay (ZTD) data series for the NOAATrop model, Hopfield model, and the International GNSS Services (IGS) final tropospheric correction product, respectively. These data sets were generated at ten IGS reference stations spanning Canada and the United States. We analyzed the NOAATrop ZTD data series and compared them with those of the Hopfield model. The IGS final tropospheric product was used as a reference. The analysis shows that the performance of the NOAATrop model is a function of both season (time of the year) and geographical location. However, its performance was superior to the Hopfield model in all cases. We further investigated the effect of implementing the NOAATrop model on the ionosphere-free-based PPP solution convergence and accuracy. It is shown that the use of the NOAATrop model improved the PPP solution convergence by 1%, 10% and 15% for the latitude, longitude and height components, respectively

Uncertainties in models of tropospheric ozone based on Monte Carlo analysis: Tropospheric ozone burdens, atmospheric lifetimes and surface distributions

Science.gov (United States)

Derwent, Richard G.; Parrish, David D.; Galbally, Ian E.; Stevenson, David S.; Doherty, Ruth M.; Naik, Vaishali; Young, Paul J.

2018-05-01

the observed seasonal cycles were found to fall within the confidence limits of the ACCMIP members, this was because the model seasonal cycles spanned extremely wide ranges and there was no single ACCMIP member that performed best for each station. Further work is required to examine the parameterisation of convective mixing in the models to see if this erodes the isolation of the marine boundary layer from the free troposphere and thus hides the models' real ability to reproduce ozone seasonal cycles over marine stations.

Impact of biogenic terpene emissions from Brassica napus on tropospheric ozone over Saxony (Germany): numerical investigation.

Science.gov (United States)

Renner, Eberhard; Münzenberg, Annette

2003-01-01

The role of biogenic emissions in tropospheric ozone production is currently under discussion and major aspects are not well understood yet. This study aims towards the estimation of the influence of biogenic emissions on tropospheric ozone concentrations over Saxony in general and of biogenic emissions from brassica napus in special. MODELLING TOOLS: The studies are performed by utilizing a coupled numerical modelling system consisting of the meteorological model METRAS and the chemistry transport model MUSCAT. For the chemical part, the Euro-RADM algorithm is used. EMISSIONS: Anthropogenic and biogenic emissions are taken into account. The anthropogenic emissions are introduced by an emission inventory. Biogenic emissions, VOC and NO, are calculated within the chemical transport model MUSCAT at each time step and in each grid cell depending on land use type and on the temperature. The emissions of hydrocarbons from forest areas as well as biogenic NO especially from agricultural grounds are considered. Also terpene emissions from brassica napus fields are estimated. SIMULATION SETUP AND METEOROLOGICAL CONDITIONS: The simulations were performed over an area with an extension of 160 x 140 km2 which covers the main parts of Saxony and neighboring areas of Brandenburg, Sachsen-Anhalt and Thuringia. Summer smog with high ozone concentrations can be expected during high pressure conditions on hot summer days. Typical meteorological conditions for such cases were introduced in an conceptual way. It is estimated that biogenic emissions change tropospheric ozone concentrations in a noticeable way (up to 15% to 20%) and, therefore, should not be neglected in studies about tropospheric ozone. Emissions from brassica napus do have a moderate potential to enhance tropospheric ozone concentrations, but emissions are still under consideration and, therefore, results vary to a high degree. Summing up, the effect of brassica napus terpene emissions on ozone concentrations is

Reanalysis comparisons of upper tropospheric-lower stratospheric jets and multiple tropopauses

Science.gov (United States)

Manney, Gloria L.; Hegglin, Michaela I.; Lawrence, Zachary D.; Wargan, Krzysztof; Millán, Luis F.; Schwartz, Michael J.; Santee, Michelle L.; Lambert, Alyn; Pawson, Steven; Knosp, Brian W.; Fuller, Ryan A.; Daffer, William H.

2017-09-01

The representation of upper tropospheric-lower stratospheric (UTLS) jet and tropopause characteristics is compared in five modern high-resolution reanalyses for 1980 through 2014. Climatologies of upper tropospheric jet, subvortex jet (the lowermost part of the stratospheric vortex), and multiple tropopause frequency distributions in MERRA (Modern-Era Retrospective analysis for Research and Applications), ERA-I (ERA-Interim; the European Centre for Medium-Range Weather Forecasts, ECMWF, interim reanalysis), JRA-55 (the Japanese 55-year Reanalysis), and CFSR (the Climate Forecast System Reanalysis) are compared with those in MERRA-2. Differences between alternate products from individual reanalysis systems are assessed; in particular, a comparison of CFSR data on model and pressure levels highlights the importance of vertical grid spacing. Most of the differences in distributions of UTLS jets and multiple tropopauses are consistent with the differences in assimilation model grids and resolution - for example, ERA-I (with coarsest native horizontal resolution) typically shows a significant low bias in upper tropospheric jets with respect to MERRA-2, and JRA-55 (the Japanese 55-year Reanalysis) a more modest one, while CFSR (with finest native horizontal resolution) shows a high bias with respect to MERRA-2 in both upper tropospheric jets and multiple tropopauses. Vertical temperature structure and grid spacing are especially important for multiple tropopause characterizations. Substantial differences between MERRA and MERRA-2 are seen in mid- to high-latitude Southern Hemisphere (SH) winter upper tropospheric jets and multiple tropopauses as well as in the upper tropospheric jets associated with tropical circulations during the solstice seasons; some of the largest differences from the other reanalyses are seen in the same times and places. Very good qualitative agreement among the reanalyses is seen between the large-scale climatological features in UTLS jet and

Tropospheric ozone climatology over Beijing: analysis of aircraft data from the MOZAIC program

Directory of Open Access Journals (Sweden)

A. J. Ding

2008-01-01

Full Text Available Ozone (O₃ profiles recorded over Beijing from 1995 to 2005 by the Measurement of Ozone and Water Vapor by Airbus In-Service Aircraft (MOZAIC program were analyzed to provide a first climatology of tropospheric O₃ over Beijing and the North China Plains (NCPs, one of the most populated and polluted regions in China. A pooled method was adopted in the data analysis to reduce the influence of irregular sampling frequency. The tropospheric O₃ over Beijing shows a seasonal and vertical distribution typical of mid-latitude locations in the Northern Hemisphere, but has higher daytime concentrations in the lower troposphere, when compared to New York City, Tokyo, and Paris at similar latitude. The tropospheric O₃ over Beijing exhibits a common summer maximum and a winter minimum, with a broad summer maximum in the middle troposphere and a narrower early summer (June peak in the lower troposphere. Examination of meteorological and satellite data suggests that the lower tropospheric O₃ maximum in June is a result of strong photochemical production, transport of regional pollution, and possibly also more intense burnings of biomass in Central-Eastern China. Trajectory analysis indicates that in summer the regional pollution from the NCPs, maybe mixed with urban plumes from Beijing, played important roles on the high O₃ concentrations in the boundary layer, but had limited impact on the O₃ concentrations in the middle troposphere. A comparison of the data recorded before and after 2000 reveals that O₃ in the lower troposphere over Beijing had a strong positive trend (approximately 2% per year from 1995 to 2005 in contrast to a flat or a decreasing trend over Tokyo, New York City, and Paris, indicating worsening photochemical pollution in Beijing and the NCPs.

Tropospheric chemistry over the lower Great Plains of the United States. 2. Trace gas profiles and distributions

Science.gov (United States)

Luke, Winston T.; Dickerson, Russell R.; Ryan, William F.; Pickering, Kenneth E.; Nunnermacker, Linda J.

1992-12-01

Convective clouds and thunderstorms redistribute air pollutants vertically, and by altering the chemistry and radiative balance of the upper troposphere, these local actions can have global consequences. To study these effects, measurements of trace gases ozone, O3, carbon monoxide, CO, and odd nitrogen were made aboard the NCAR Sabreliner on 18 flights over the southern Great Plains during June 1985. To demonstrate chemical changes induced by vertical motions in the atmosphere and to facilitate comparison with computer model calculations, these data were categorized according to synoptic flow patterns. Part 1 of this two-part paper details the alternating pulses of polar and maritime air masses that dominate the vertical mixing in this region. In this paper, trace gas measurements are presented as altitude profiles (0-12 km) with statistical distributions of mixing ratios for each species in each flow pattern. The polar flow regime is characterized by northwesterly winds, subsiding air, and convective stability. Concentrations of CO and total odd nitrogen (NOy) are relatively high in the shallow planetary boundary layer (PBL) but decrease rapidly with altitude. Ozone, on the other hand, is uniformly distributed, suggesting limited photochemical production; in fact, nitric oxide, NO, mixing ratios fell below 10 ppt (parts per 1012 by volume) in the midtroposphere. The maritime regime is characterized by southerly surface winds, convective instability, and a deep PBL; uniformly high concentrations of trace gases were found up to 4 km on one flight. Severe storms occur in maritime flow, especially when capped by a dry layer, and they transport large amounts of CO, O3, and NOy into the upper troposphere. Median NO levels at high altitude exceeded 300 ppt. Lightning produces spikes of NO (but not CO) with mixing ratios sometimes exceeding 1000 ppt. This flow pattern tends to leave the midtroposphere relatively clean with concentrations of trace gases similar to those

Spectropolarimetric Measurements of Scattered Sunlight in the Huggins Bands: Retrieval of Tropospheric Ozone Profiles

Science.gov (United States)

Fu, D.; Sander, S. P.; Stutz, J.; Pongetti, T. J.; Yung, Y. L.; Wong, M.; Natraj, V.; Li, K.; Shia, R.

2009-12-01

Ozone concentrations in the troposphere have increased over the past century as a result of anthropogenic emissions of NOx and volatile organic compounds. In addition to being harmful to human health and plant life, ozone is an important greenhouse gas, especially in the middle and upper troposphere. Therefore, accurate monitoring of tropospheric ozone vertical distributions is crucial for a better understanding of air quality and climate change. Simulations of vector radiative transfer in the near ultraviolet region have shown that tropospheric ozone profiles can be retrieved using polarization measurements. However, to date there has been no experimental test of this method. A new compact, portable spectropolarimeter has been built for atmospheric remote sensing. The first comprehensive description of the configuration and performance of this instrument for ground-based operation is provided and sample atmospheric scattered sunlight spectra are shown. Using optimal estimation retrieval theory we study the information content of polarization spectra in the Huggins band and uncertainties in the retrieval associated with the measurement parameters, such as aerosol scattering.

The effect of clouds on photolysis rates and ozone formation in the unpolluted troposphere

Science.gov (United States)

Thompson, A. M.

1984-01-01

The photochemistry of the lower atmosphere is sensitive to short- and long-term meteorological effects; accurate modeling therefore requires photolysis rates for trace gases which reflect this variability. As an example, the influence of clouds on the production of tropospheric ozone has been investigated, using a modification of Luther's two-stream radiation scheme to calculate cloud-perturbed photolysis rates in a one-dimensional photochemical transport model. In the unpolluted troposphere, where stratospheric inputs of odd nitrogen appear to represent the photochemical source of O3, strong cloud reflectance increases the concentration of NO in the upper troposphere, leading to greatly enhanced rates of ozone formation. Although the rate of these processes is too slow to verify by observation, the calculation is useful in distinguishing some features of the chemistry of regions of differing mean cloudiness.

Tropospheric mercury vertical profiles between 500 and 10 000 m in central Europe

Directory of Open Access Journals (Sweden)

A. Weigelt

2016-03-01

Full Text Available The knowledge of the vertical distribution of atmospheric mercury (Hg plays an important role in determining the transport and cycling of mercury. However, measurements of the vertical distribution are rare, because airborne measurements are expensive and labour intensive. Consequently, only a few vertical Hg profile measurements have been reported since the 1970s. Besides the Civil Aircraft for the Regular Investigation of the atmosphere Based on an Instrument Container (CARIBIC observations, the latest vertical profile over Europe was measured in 1996. Within the Global Mercury Observation System (GMOS project, four vertical profiles were taken on board research aircraft (CASA-212 in August 2013 in background air over different locations in Slovenia and Germany. Each vertical profile consists of at least seven 5 min horizontal flight sections from 500 m above ground to 3000 m a.s.l. Gaseous elemental mercury (GEM and total gaseous mercury (TGM were measured with Tekran 2537X and Tekran 2537B analysers. In addition to the mercury measurements, SO2, CO, O3, NO, and NO2, basic meteorological parameters (pressure, temperature, relative humidity have been measured. Additional ground-based mercury measurements at the GMOS master site in Waldhof, Germany and measurements onboard the CARIBIC passenger aircraft were used to extend the profile to the ground and upper troposphere respectively. No vertical gradient was found inside the well-mixed boundary layer (variation of less than 0.1 ng m−3 at different sites, with GEM varying from location to location between 1.4 and 1.6 ng m−3 (standard temperature and pressure, STP: T  =  273.15 K, p  =  1013.25 hPa. At all locations GEM dropped to 1.3 ng m−3 (STP when entering the free troposphere and remained constant at higher altitudes. The combination of the vertical profile, measured on 21 August 2013 over Leipzig, Germany, with the CARIBIC measurements during ascent and descent to

Tropospheric effects of energy conversion

International Nuclear Information System (INIS)

Derwent, R.G.

1992-01-01

The tropospheric concentrations of a number of trace gases are increasing due to man's activities. For some trace gases, their atmospheric life cycles are not fully understood and it is difficult to be certain about the role of man's activities. Emissions from the energy industries and energy conversion processes represent an important subset of source terms in these life cycles, along with agriculture, deforestation, cement manufacture, biomass burning, process industries and natural biospheric processes. Global Warming Potentials (GWPs) allow the tropospheric effects of a range of climate forcing trace gases to be assessed on a comparable basis. If a short term view of the commitment to global warming is adopted then the contribution from other trace gases may approach and exceed that of carbon dioxide, itself. Over longer time horizons, the long atmospheric lifetime of carbon dioxide shows through as a major influence and the contributions from the other trace gases appear to be much smaller, representing an additional 13-18% contribution on top of that from CO 2 itself

Temperature dependent O3 absorption cross sections for GOME, SCIAMACHY and GOME-2: II. New laboratory measurements

Science.gov (United States)

Serdyuchenko, Anna; Gorshelev, Victor; Chehade, Wissam; Weber, Mark; Burrows, John P.

We report on the work devoted to the up-to-date measurements of the ozone absorption cross-sections. The main goal of the project is to produce a consolidated and consistent set of high resolution cross-sections for satellite spectrometers series that allows a derivation of the harmonized long term data set. The generation of long-term datasets of atmospheric trace gases is a major need and prerequisite for climate and air quality related studies. At present there are three atmospheric chemistry instruments (GOME1, SCIAMACHY and GOME2) in operation and two more spectrometers (GOME2) to be launched five years apart in the next decade resulting in a time series covering two or more decades of ozone observations. Information from different sensors has to be com-bined for a consistent long-term data record, since the lifetime of individual satellite missions is limited. The harmonization of cross-sections is carried out by combination of new experimental work with re-evaluation of the existing cross-sections data. New laboratory measurements of ozone cross-section are underway that will improve a) absolute scaling of cross-sections, b) temper-ature dependence of cross-sections (using very low temperatures starting at 190 K and higher sampling of temperatures up to room temperature) and c) improved wavelength calibration. We take advantage of a Fourier transform spectrometer (visible, near IR) and Echelle spectropho-tometer (UV, visible) to extend the dynamic range of the system (covering several orders of magnitude in cross-sections from UV up to the near IR). We plan to cover the spectral range 220 -1000 nm at a spectral resolution of 0.02 nm in UV/VIS with absolute intensity accuracy of at least 2%, and wavelength accuracy better than 0.001 nm in the temperature range 193-293 K in 10 K steps. A lot of attention is paid to the accuracy of determining the temperature of the ozone flow and new methods for absolute calibration of relative spectra. This work is in

Observing lowermost tropospheric ozone pollution with a new multispectral synergic approach of IASI infrared and GOME-2 ultraviolet satellite measurements

Science.gov (United States)

Cuesta, Juan; Foret, Gilles; Dufour, Gaëlle; Eremenko, Maxim; Coman, Adriana; Gaubert, Benjamin; Beekmann, Matthias; Liu, Xiong; Cai, Zhaonan; Von Clarmann, Thomas; Spurr, Robert; Flaud, Jean-Marie

2014-05-01

Tropospheric ozone is currently one of the air pollutants posing greatest threats to human health and ecosystems. Monitoring ozone pollution at the regional, continental and global scale is a crucial societal issue. Only spaceborne remote sensing is capable of observing tropospheric ozone at such scales. The spatio-temporal coverage of new satellite-based instruments, such as IASI or GOME-2, offer a great potential for monitoring air quality by synergism with regional chemistry-transport models, for both inter-validation and full data assimilation. However, current spaceborne observations using single-band either UV or IR measurements show limited sensitivity to ozone in the atmospheric boundary layer, which is the major concern for air quality. Very recently, we have developed an innovative multispectral approach, so-called IASI+GOME-2, which combines IASI and GOME-2 observations, respectively in the IR and UV. This unique multispectral approach has allowed the observation of ozone plumes in the lowermost troposphere (LMT, below 3 km of altitude) over Europe, for the first time from space. Our first analyses are focused on typical ozone pollution events during the summer of 2009 over Europe. During these events, LMT ozone plumes at different regions are produced photo-chemically in the boundary layer, transported upwards to the free troposphere and also downwards from the stratosphere. We have analysed them using IASI+GOME-2 observations, in comparison with single-band methods (IASI, GOME-2 and OMI). Only IASI+GOME-2 depicts ozone plumes located below 3 km of altitude (both over land and ocean). Indeed, the multispectral sensitivity in the LMT is greater by 40% and it peaks at 2 to 2.5 km of altitude over land, thus at least 0.8 to 1 km below that for all single-band methods. Over Europe during the summer of 2009, IASI+GOME-2 shows 1% mean bias and 21% precision for direct comparisons with ozonesondes and also good agreement with CHIMERE model simulations

Free tropospheric measurements of CS2 over a 45 deg N to 45 deg S latitude range

Science.gov (United States)

Tucker, B. J.; Maroulis, P. J.; Bandy, A. R.

1985-01-01

The mean value obtained from 52 free tropospheric measurements of CS2 over the 45 deg N-45 deg S latitude range was 5.7 pptv, with standard deviation and standard error of 1.9 and 0.3 pptv, respectively. Large fluctuations in the CS2 concentration are observed which reflect the apparent short atmospheric residence time and inhomogeneities in the surface sources of CS2. The amounts of CS2 in the Northern and Southern Hemispheres are statistically equal.

Sulfur dioxide (SO2 from MIPAS in the upper troposphere and lower stratosphere 2002–2012

Directory of Open Access Journals (Sweden)

M. Höpfner

2015-06-01

Full Text Available Vertically resolved distributions of sulfur dioxide (SO2 with global coverage in the height region from the upper troposphere to ~20 km altitude have been derived from observations by the Michelson Interferometer for Passive Atmospheric Sounding (MIPAS on Envisat for the period July 2002 to April 2012. Retrieved volume mixing ratio profiles representing single measurements are characterized by typical errors in the range of 70–100 pptv and by a vertical resolution ranging from 3 to 5 km. Comparison with observations by the Atmospheric Chemistry Experiment Fourier transform spectrometer (ACE-FTS revealed a slightly varying bias with altitude of −20 to 50 pptv for the MIPAS data set in case of volcanically enhanced concentrations. For background concentrations the comparison showed a systematic difference between the two major MIPAS observation periods. After debiasing, the difference could be reduced to biases within −10 to 20 pptv in the altitude range of 10–20 km with respect to ACE-FTS. Further comparisons of the debiased MIPAS data set with in situ measurements from various aircraft campaigns showed no obvious inconsistencies within a range of around ±50 pptv. The SO2 emissions of more than 30 volcanic eruptions could be identified in the upper troposphere and lower stratosphere (UTLS. Emitted SO2 masses and lifetimes within different altitude ranges in the UTLS have been derived for a large part of these eruptions. Masses are in most cases within estimations derived from other instruments. From three of the major eruptions within the MIPAS measurement period – Kasatochi in August 2008, Sarychev in June 2009 and Nabro in June 2011 – derived lifetimes of SO2 for the altitude ranges 10–14, 14–18 and 18–22 km are 13.3 ± 2.1, 23.6 ± 1.2 and 32.3 ± 5.5 days respectively. By omitting periods with obvious volcanic influence we have derived background mixing ratio distributions of SO2. At 10 km altitude these indicate an annual

A large impact of tropical biomass burning on CO and CO{sub 2} in the upper troposphere

Energy Technology Data Exchange (ETDEWEB)

Hidekazu Matsueda; Shoichi Taguchi; Hisayuki Y; Inoue & Masao Ishii [Meteorological Research Institute, Tsukuba-shi (Japan). Geochemical Research Department

2002-07-01

A large interannual variation of biomass burning emissions from Southeast Asia is associated with the ENSO events. During 1997/98 and 1994 El Nino years, uncontrolled wildfires of tropical rainforests and peat lands in Indonesia were enlarged due to a long drought. Enhanced CO injection into the upper troposphere from the intense Indonesian fires was clearly observed in the 8-year measurements from a regular flask sampling over the western Pacific using a JAL airliner between Australia and Japan. This airliner observation also revealed that upper tropospheric CO{sub 2} cycle largely changed during the 1997 El Nio year due partly to the biomass burning emissions. Widespread pollution from the biomass burnings in Southeast Asia was simulated using a CO tracer driven by a 3D global chemical transport model. This simulation indicates that tropical deep convections connected to rapid advection by the subtropical jet play a significant role in dispersing biomass-burning emissions from Southeast Asia on a global scale.

Tropospheric ozone changes, radiative forcing and attribution to emissions in the Atmospheric Chemistry and Climate Model Intercomparison Project (ACCMIP

Directory of Open Access Journals (Sweden)

D. S. Stevenson

2013-03-01

Full Text Available Ozone (O3 from 17 atmospheric chemistry models taking part in the Atmospheric Chemistry and Climate Model Intercomparison Project (ACCMIP has been used to calculate tropospheric ozone radiative forcings (RFs. All models applied a common set of anthropogenic emissions, which are better constrained for the present-day than the past. Future anthropogenic emissions follow the four Representative Concentration Pathway (RCP scenarios, which define a relatively narrow range of possible air pollution emissions. We calculate a value for the pre-industrial (1750 to present-day (2010 tropospheric ozone RF of 410 mW m−2. The model range of pre-industrial to present-day changes in O3 produces a spread (±1 standard deviation in RFs of ±17%. Three different radiation schemes were used – we find differences in RFs between schemes (for the same ozone fields of ±10%. Applying two different tropopause definitions gives differences in RFs of ±3%. Given additional (unquantified uncertainties associated with emissions, climate-chemistry interactions and land-use change, we estimate an overall uncertainty of ±30% for the tropospheric ozone RF. Experiments carried out by a subset of six models attribute tropospheric ozone RF to increased emissions of methane (44±12%, nitrogen oxides (31 ± 9%, carbon monoxide (15 ± 3% and non-methane volatile organic compounds (9 ± 2%; earlier studies attributed more of the tropospheric ozone RF to methane and less to nitrogen oxides. Normalising RFs to changes in tropospheric column ozone, we find a global mean normalised RF of 42 mW m−2 DU−1, a value similar to previous work. Using normalised RFs and future tropospheric column ozone projections we calculate future tropospheric ozone RFs (mW m−2; relative to 1750 for the four future scenarios (RCP2.6, RCP4.5, RCP6.0 and RCP8.5 of 350, 420, 370 and 460 (in 2030, and 200, 300, 280 and 600 (in 2100. Models show some coherent responses of ozone to climate change

OMI and Ground-Based In-Situ Tropospheric Nitrogen Dioxide Observations over Several Important European Cities during 2005–2014

Directory of Open Access Journals (Sweden)

Spiru Paraschiv

2017-11-01

Full Text Available In this work we present the evolution of tropospheric nitrogen dioxide (NO2 content over several important European cities during 2005–2014 using space observations and ground-based in-situ measurements. The NO2 content was derived using the daily observations provided by the Ozone Monitoring Instrument (OMI, while the NO2 volume mixing ratio measurements were obtained from the European Environment Agency (EEA air quality monitoring stations database. The European cities selected are: Athens (37.98° N, 23.72° E, Berlin (52.51° N, 13.41° E, Bucharest (44.43° N, 26.10° E, Madrid (40.38° N, 3.71° W, Lisbon (38.71° N, 9.13° W, Paris (48.85° N, 2.35° E, Rome (41.9° N, 12.50° E, and Rotterdam (51.91° N, 4.46° E. We show that OMI NO2 tropospheric column data can be used to assess the evolution of NO2 over important European cities. According to the statistical analysis, using the seasonal variation, we found good correlations (R > 0.50 between OMI and ground-based in-situ observations for all of the cities presented in this work. Highest correlation coefficients (R > 0.80 between ground-based monitoring stations and OMI observations were calculated for the cities of Berlin, Madrid, and Rome. Both types of observations, in-situ and remote sensing, show an NO2 negative trend for all of locations presented in this study.

TROPOSPHERIC AEROSOL PROGRAM, PROGRAM PLAN, MARCH 2001

Energy Technology Data Exchange (ETDEWEB)

SCHWARTZ,S.E.; LUNN,P.

2001-03-01

The goal of Tropospheric Aerosol Program (TAP) will be to develop the fundamental scientific understanding required to construct tools for simulating the life cycle of tropospheric aerosols--the processes controlling their mass loading, composition, and microphysical properties, all as a function of time, location, and altitude. The TAP approach to achieving this goal will be by conducting closely linked field, modeling, laboratory, and theoretical studies focused on the processes controlling formation, growth, transport, and deposition of tropospheric aerosols. This understanding will be represented in models suitable for describing these processes on a variety of geographical scales; evaluation of these models will be a key component of TAP field activities. In carrying out these tasks TAP will work closely with other programs in DOE and in other Federal and state agencies, and with the private sector. A forum to directly work with our counterparts in industry to ensure that the results of this research are translated into products that are useful to that community will be provided by NARSTO (formerly the North American Research Strategy on Tropospheric Ozone), a public/private partnership, whose membership spans government, the utilities, industry, and university researchers in Mexico, the US, and Canada.

Mapping of the Tropospheric NO2 Spatial Distribution at City-scale Based on Airborne APEX Hyperspectral Imaging

Science.gov (United States)

Tack, F. M.; Merlaud, A.; Danckaert, T.; Yu, H.; Fayt, C.; Iordache, D.; Meuleman, K.; Fierens, F.; Deutsch, F.; Van Roozendael, M.

2016-12-01

NO2 is a key pollutant with highly variable concentrations in space and time. Quantitative information about its spatial variability at high resolution is currently scarce, but very valuable for (air quality) studies at the urban scale. APEX is a pushbroom hyperspectral imager with high spatial (60 by 80 m2) and spectral (2.8-3.3 nm) resolution. APEX flights were conducted over (1) the city and port of Antwerp, Belgium on April 14, 2015 and July 19, 2016, (2) Brussels, Belgium on June 30, 2015 (BUMBA project), and (3) Berlin, Germany on April 21, 2016 (AROMAT and AROMAPEX projects). APEX was operated from a DLR DO-228 plane at 6.1 km altitude. Over Berlin, two additional imagers, AirMAP (IUP Bremen) and SWING (BIRA-IASB), were simultaneously operated from a FUB Cessna at 3 km for intercomparison purposes. NO2 vertical column densities (VCDs) are retrieved based on (1) the DOAS analysis of the observed spectra in the visible region (470 nm - 510 nm), and (2) air mass factor calculations with the RTM VLIDORT 2.6. Results show that APEX is suitable (1) to detect the fast varying spectral signatures of a trace gas like NO2 and (2) to identify small scale gradients in the NO2 field and to resolve individual emission sources. Main NOx sources in the Antwerp area are related to (petro)chemical industry, while traffic emissions are dominant in Brussels. Over Berlin, 2 large industrial NO2 plumes are detected by all three imaging systems, crossing the city from west to east. The NO2 VCD levels range between 0.2 and 3.5 x 1016 molec cm-2. The typical detection limit for the APEX instrument is around 1.7 to 2.2 x 1015 molec cm-2. Correlation coefficients of 0.85 and slopes close to unity are obtained when compared to coincident car mobile-DOAS measurements. The NO2 retrieval algorithm, campaign results, and ongoing research concerning the comparison of the VCDs with in-situ surface concentrations and a high resolution (25 m) air quality model, i.e. RIO-IFDM, will be discussed.

Performance Evaluation of Blind Tropospheric Delay correction ...

African Journals Online (AJOL)

This report represents an appraisal of the performance of the GPT2w and UNB3M models with accurate International GNSS Service (IGS)- tropospheric estimations for fifteen IGS stations over a period of 1 year on the Africa continent. Both models perform significantly better at low latitudes than higher latitudes. There was ...

Tropospheric Bromine Chemistry: Implications for Present and Pre-industrial Ozone and Mercury

Science.gov (United States)

Parella, J. P.; Jacob, D. J.; Liang, Q.; Zhang, Y.; Mickley, L. J.; Miller, B.; Evans, M. J.; Yang, X.; Pyle, J. A.; Theys, N.;

Instrumentation for tropospheric aerosol characterization

Energy Technology Data Exchange (ETDEWEB)

Shi, Z.; Young, S.E.; Becker, C.H.; Coggiola, M.J. [SRI International, Menlo Park, CA (United States); Wollnik, H. [Giessen Univ. (Germany)

1997-12-31

A new instrument has been developed that determines the abundance, size distribution, and chemical composition of tropospheric and lower stratospheric aerosols with diameters down to 0.2 {mu}m. In addition to aerosol characterization, the instrument also monitors the chemical composition of the ambient gas. More than 25.000 aerosol particle mass spectra were recorded during the NASA-sponsored Subsonic Aircraft: Contrail and Cloud Effects Special Study (SUCCESS) field program using NASA`s DC-8 research aircraft. (author) 7 refs.

Instrumentation for tropospheric aerosol characterization

Energy Technology Data Exchange (ETDEWEB)

Shi, Z; Young, S E; Becker, C H; Coggiola, M J [SRI International, Menlo Park, CA (United States); Wollnik, H [Giessen Univ. (Germany)

1998-12-31

A new instrument has been developed that determines the abundance, size distribution, and chemical composition of tropospheric and lower stratospheric aerosols with diameters down to 0.2 {mu}m. In addition to aerosol characterization, the instrument also monitors the chemical composition of the ambient gas. More than 25.000 aerosol particle mass spectra were recorded during the NASA-sponsored Subsonic Aircraft: Contrail and Cloud Effects Special Study (SUCCESS) field program using NASA`s DC-8 research aircraft. (author) 7 refs.

Chemical processes related to net ozone tendencies in the free troposphere

Science.gov (United States)

Bozem, Heiko; Butler, Tim M.; Lawrence, Mark G.; Harder, Hartwig; Martinez, Monica; Kubistin, Dagmar; Lelieveld, Jos; Fischer, Horst

2017-09-01

Ozone (O3) is an important atmospheric oxidant, a greenhouse gas, and a hazard to human health and agriculture. Here we describe airborne in situ measurements and model simulations of O3 and its precursors during tropical and extratropical field campaigns over South America and Europe, respectively. Using the measurements, net ozone formation/destruction tendencies are calculated and compared to 3-D chemistry-transport model simulations. In general, observation-based net ozone tendencies are positive in the continental boundary layer and the upper troposphere at altitudes above ˜ 6 km in both environments. On the other hand, in the marine boundary layer and the middle troposphere, from the top of the boundary layer to about 6-8 km altitude, net O3 destruction prevails. The ozone tendencies are controlled by ambient concentrations of nitrogen oxides (NOx). In regions with net ozone destruction the available NOx is below the threshold value at which production and destruction of O3 balance. While threshold NO values increase with altitude, in the upper troposphere NOx concentrations are generally higher due to the integral effect of convective precursor transport from the boundary layer, downward transport from the stratosphere and NOx produced by lightning. Two case studies indicate that in fresh convective outflow of electrified thunderstorms net ozone production is enhanced by a factor 5-6 compared to the undisturbed upper tropospheric background. The chemistry-transport model MATCH-MPIC generally reproduces the pattern of observation-based net ozone tendencies but mostly underestimates the magnitude of the net tendency (for both net ozone production and destruction).

Analysis of the summertime buildup of tropospheric ozone abundances over the Middle East and North Africa as observed by the Tropospheric Emission Spectrometer instrument

Science.gov (United States)

Liu, Jane J.; Jones, Dylan B. A.; Worden, John R.; Noone, David; Parrington, Mark; Kar, Jay

2009-03-01

We use the GEOS-Chem chemical transport model to interpret observations of tropospheric ozone from the Tropospheric Emission Spectrometer (TES) satellite instrument in summer 2005. Observations from TES reveal elevated ozone in the middle troposphere (500-400 hPa) across North Africa and the Middle East. Observed ozone abundances in the middle troposphere are at a maximum in summer and a minimum in winter, consistent with the previously predicted summertime "Middle East ozone maximum." This summertime enhancement in ozone is associated with the Arabian and Sahara anticyclones, centered over the Zagros and Atlas Mountains, respectively. These anticyclones isolate the middle troposphere over northeast Africa and the Middle East, with westerlies to the north and easterlies to the south, facilitating the buildup of ozone. Over the Middle East, we find that in situ production and transport from Asia provides comparable contributions of 30-35% to the ozone buildup. Over North Africa, in situ production is dominant (at about 20%), with transport from Asia, North America, and equatorial Africa each contributing about 10-15% to the total ozone. We find that although the eastern Mediterranean is characterized by strong descent in the middle and upper troposphere in summer, transport from the boundary layer accounts for about 25% of the local Middle Eastern contribution to the ozone enhancement in the middle troposphere. This upward transport of boundary layer air is associated with orographic lifting along the Zagros Mountains in Iran and the Asir and Hijaz Mountain ranges in Saudi Arabia, and is consistent with TES observations of deuterated water.

Applying Kalman filtering to investigate tropospheric effects in VLBI

Science.gov (United States)

Soja, Benedikt; Nilsson, Tobias; Karbon, Maria; Heinkelmann, Robert; Liu, Li; Lu, Cuixian; Andres Mora-Diaz, Julian; Raposo-Pulido, Virginia; Xu, Minghui; Schuh, Harald

2014-05-01

Very Long Baseline Interferometry (VLBI) currently provides results, e.g., estimates of the tropospheric delays, with a delay of more than two weeks. In the future, with the coming VLBI2010 Global Observing System (VGOS) and increased usage of electronic data transfer, it is planned that the time between observations and results is decreased. This may, for instance, allow the integration of VLBI-derived tropospheric delays into numerical weather prediction models. Therefore, future VLBI analysis software packages need to be able to process the observational data autonomously in near real-time. For this purpose, we have extended the Vienna VLBI Software (VieVS) by a Kalman filter module. This presentation describes the filter and discusses its application for tropospheric studies. Instead of estimating zenith wet delays as piece-wise linear functions in a least-squares adjustment, the Kalman filter allows for more sophisticated stochastic modeling. We start with a random walk process to model the time-dependent behavior of the zenith wet delays. Other possible approaches include the stochastic model described by turbulence theory, e.g. the model by Treuhaft and Lanyi (1987). Different variance-covariance matrices of the prediction error, depending on the time of the year and the geographic latitude, have been tested. In winter and closer to the poles, lower variances and covariances are appropriate. The horizontal variations in tropospheric delays have been investigated by comparing three different strategies: assumption of a horizontally stratified troposphere, using north and south gradients modeled, e.g., as Gauss-Markov processes, and applying a turbulence model assuming correlations between observations in different azimuths. By conducting Monte-Carlo simulations of current standard VLBI networks and of future VGOS networks, the different tropospheric modeling strategies are investigated. For this purpose, we use the simulator module of VieVS which takes into

Retrieval of tropospheric carbon monoxide for the MOPITT experiment

Science.gov (United States)

Pan, Liwen; Gille, John C.; Edwards, David P.; Bailey, Paul L.; Rodgers, Clive D.

1998-12-01

A retrieval method for deriving the tropospheric carbon monoxide (CO) profile and column amount under clear sky conditions has been developed for the Measurements of Pollution In The Troposphere (MOPITT) instrument, scheduled for launch in 1998 onboard the EOS-AM1 satellite. This paper presents a description of the method along with analyses of retrieval information content. These analyses characterize the forward measurement sensitivity, the contribution of a priori information, and the retrieval vertical resolution. Ensembles of tropospheric CO profiles were compiled both from aircraft in situ measurements and from chemical model results and were used in retrieval experiments to characterize the method and to study the sensitivity to different parameters. Linear error analyses were carried out in parallel with the ensemble experiments. Results of these experiments and analyses indicate that MOPITT CO column measurements will have better than 10% precision, and CO profile measurement will have approximately three pieces of independent information that will resolve 3-5 tropospheric layers to approximately 10% precision. These analyses are important for understanding MOPITT data, both for application of data in tropospheric chemistry studies and for comparison with in situ measurements.

The Potential of Tropospheric Gradients for Regional Precipitation Prediction

Science.gov (United States)

Boisits, Janina; Möller, Gregor; Wittmann, Christoph; Weber, Robert

2017-04-01

Changes of temperature and humidity in the neutral atmosphere cause variations in tropospheric path delays and tropospheric gradients. By estimating zenith wet delays (ZWD) and gradients using a GNSS reference station network the obtained time series provide information about spatial and temporal variations of water vapour in the atmosphere. Thus, GNSS-based tropospheric parameters can contribute to the forecast of regional precipitation events. In a recently finalized master thesis at TU Wien the potential of tropospheric gradients for weather prediction was investigated. Therefore, ZWD and gradient time series at selected GNSS reference stations were compared to precipitation data over a period of six months (April to September 2014). The selected GNSS stations form two test areas within Austria. All required meteorological data was provided by the Central Institution for Meteorology and Geodynamics (ZAMG). Two characteristics in ZWD and gradient time series can be anticipated in case of an approaching weather front. First, an induced asymmetry in tropospheric delays results in both, an increased magnitude of the gradient and in gradients pointing towards the weather front. Second, an increase in ZWD reflects the increased water vapour concentration right before a precipitation event. To investigate these characteristics exemplary test events were processed. On the one hand, the sequence of the anticipated increase in ZWD at each GNSS station obtained by cross correlation of the time series indicates the direction of the approaching weather front. On the other hand, the corresponding peak in gradient time series allows the deduction of the direction of movement as well. To verify the results precipitation data from ZAMG was used. It can be deduced, that tropospheric gradients show high potential for predicting precipitation events. While ZWD time series rather indicate the orientation of the air mass boundary, gradients rather indicate the direction of movement

Impact of land convection on troposphere-stratosphere exchange in the tropics

Directory of Open Access Journals (Sweden)

P. Ricaud

2007-11-01

Full Text Available The mechanism of troposphere-stratosphere exchange in the tropics was investigated from space-borne observations of the horizontal distributions of tropospheric-origin long-lived species, nitrous oxide (N₂O, methane (CH₄ and carbon monoxide (CO, from 150 to 70 hPa in March-April-May by the ODIN/Sub-Millimeter Radiometer (SMR, the Upper Atmosphere Research Satellite (UARS/Halogen Occultation Experiment (HALOE and the TERRA/Measurements Of Pollution In The Troposphere (MOPITT instruments in 2002–2004, completed by recent observations of the AURA/Microwave Limb Sounder (MLS instrument during the same season in 2005. The vertical resolution of the satellite measurements ranges from 2 to 4 km. The analysis has been performed on isentropic surfaces: 400 K (lower stratosphere for all the species and 360 K (upper troposphere only for CO. At 400 K (and 360 K for CO, all gases show significant longitudinal variations with peak-to-trough values of ~5–11 ppbv for N₂O, 0.07–0.13 ppmv for CH₄, and ~10 ppbv for CO (~40 ppbv at 360 K. The maximum amounts are primarily located over Africa and, depending on the species, secondary more or less pronounced maxima are reported above northern South America and South-East Asia. The lower stratosphere over the Western Pacific deep convective region where the outgoing longwave radiation is the lowest, the tropopause the highest and the coldest, appears as a region of minimum concentration of tropospheric trace species. The possible impact on trace gas concentration at the tropopause of the inhomogeneous distribution and intensity of the sources, mostly continental, of the horizontal and vertical transports in the troposphere, and of cross-tropopause transport was explored with the MOCAGE Chemistry Transport Model. In the simulations, significant longitudinal variations were found on the medium-lived CO (2-month lifetime with peak-to-trough value of ~20 ppbv at 360 K and

Atmospheric hydroxyl radical production from electronically excited NO2 and H2O.

Science.gov (United States)

Li, Shuping; Matthews, Jamie; Sinha, Amitabha

2008-03-21

Hydroxyl radicals are often called the "detergent" of the atmosphere because they control the atmosphere's capacity to cleanse itself of pollutants. Here, we show that the reaction of electronically excited nitrogen dioxide with water can be an important source of tropospheric hydroxyl radicals. Using measured rate data, along with available solar flux and atmospheric mixing ratios, we demonstrate that the tropospheric hydroxyl contribution from this source can be a substantial fraction (50%) of that from the traditional O(1D) + H2O reaction in the boundary-layer region for high solar zenith angles. Inclusion of this chemistry is expected to affect modeling of urban air quality, where the interactions of sunlight with emitted NOx species, volatile organic compounds, and hydroxyl radicals are central in determining the rate of ozone formation.

Diurnal variations in H{sub 2}O{sub 2}, O{sub 3}, PAN, HNO{sub 3} and aldehyde concentrations and NO/NO{sub 2} ratios at Rishiri Island, Japan: Potential influence from iodine chemistry

Energy Technology Data Exchange (ETDEWEB)

Kanaya, Yugo [Frontier Research Center for Global Change, Japan Agency for Marine-Earth Science and Technology, 3173-25 Showa-machi, Kanazawa-ku, Yokohama, Kanagawa 236-0001 (Japan)]. E-mail: yugo@jamstec.go.jp; Tanimoto, Hiroshi [National Institute for Environmental Studies, Tsukuba (Japan); Matsumoto, Jun [Integrated Research Institute, Tokyo Institute of Technology, Yokohama (Japan); Furutani, Hiroshi [Department of Chemistry and Biochemistry, University of California, San Diego (United States); Hashimoto, Shigeru [National Institute for Environmental Studies, Tsukuba (Japan); Komazaki, Yuichi [Frontier Research Center for Global Change, Japan Agency for Marine-Earth Science and Technology, 3173-25 Showa-machi, Kanazawa-ku, Yokohama, Kanagawa 236-0001 (Japan); Tanaka, Shigeru [Department of Applied Chemistry, Keio University, Yokohama (Japan); Yokouchi, Yoko [National Institute for Environmental Studies, Tsukuba (Japan); Kato, Shungo [Department of Applied Chemistry, Graduate School of Engineering, Tokyo Metropolitan University, Hachioji (Japan); Kajii, Yoshizumi [Department of Applied Chemistry, Graduate School of Engineering, Tokyo Metropolitan University, Hachioji (Japan); Akimoto, Hajime [Frontier Research Center for Global Change, Japan Agency for Marine-Earth Science and Technology, 3173-25 Showa-machi, Kanazawa-ku, Yokohama, Kanagawa 236-0001 (Japan)

2007-04-15

The presence of iodine chemistry, hypothesized due to the overprediction of HO{sub 2} levels by a photochemical box model at Rishiri Island in June 2000, was quantitatively tested against the observed NO/NO{sub 2} ratios and the net production rates of ozone. The observed NO/NO{sub 2} ratios were reproduced reasonably well by considering the conversion of NO to NO{sub 2} by IO, whose amount was calculated so as to reproduce the observed HO{sub 2} levels. However, the net production rates of ozone were calculated to be negative when such high mixing ratios of IO were considered, which was inconsistent with the observed buildup of ozone during daytime. These results suggest that iodine chemistry may not be the sole mechanism for the reduced mixing ratios of HO{sub 2}, or that 'hot spots' for iodine chemistry were present. Diurnal variations in the mixing ratios of HCHO, CH{sub 3}CHO, peroxy acetyl nitrate (PAN) and HNO{sub 3} observed during the study are presented along with the simulated ones. The box model simulations suggest that the effect of iodine chemistry on these concentrations is small and that important sources of CH{sub 3}CHO and sinks of PAN are probably missing from our current understanding of the tropospheric chemistry mechanism.

Sensitivity of the photodissociation of NO2, NO3, HNO3 and H2O2 to the solar radiation diffused by the ground and by atmospheric particles

International Nuclear Information System (INIS)

Mugnai, A.; Petroncelli, P.; Fiocco, G.

1979-01-01

The diffusion of solar radiation by atmospheric molecules and aerosols and by ground albedo affects the photodissociation rates of atmospheric species relevant to the ozone chemistry. In this paper, a previous investigation on the photodissociation of O 3 is extended to NO 2 , NO 3 , HNO 3 , H 2 O 2 . Because of the different character of the absorption spectra of these species, the behaviour of photodissociation profiles with height and their sensitivity to such factors as ground albedo, aerosol loads, solar zenith angle are somewhat different. The results show that the presence of the aerosols usually enhances the photodissociation in the upper troposphere and in the stratosphere, because of scattering, but tends to reduce it at low heights because of the increased extinction. Enhancements in the photodissociation coefficients are as high as 20 to 40% for low values of the albedo and large aerosol loads such as those obtained after a volcanic eruption. On the other hand, at large values of the albedo, the effect of aerosols is mainly in attenuating the radiation going into and coming from the ground and their presence can lead to reduced photolysis even in the stratosphere. (author)

Photochemistry of the African troposphere: Influence of biomass-burning emissions

Science.gov (United States)

Marufu, L.; Dentener, F.; Lelieveld, J.; Andreae, M. O.; Helas, G.

2000-06-01

The relative importance of biomass-burning (pyrogenic) emissions from savannas, deforestation, agricultural waste burning, and biofuel consumption to tropospheric ozone abundance over Africa has been estimated for the year 1993, on the basis of global model calculations. We also calculated the importance of this emission source to tropospheric ozone in other regions of the world and compared it to different sources on the African regional and global scales. The estimated annual average total tropospheric ozone abundance over Africa for the reference year is 26 Tg. Pyrogenic, industrial, biogenic, and lightning emissions account for 16, 19, 12, and 27%, respectively, while stratospheric ozone input accounts for 26%. In the planetary boundary layer over Africa, the contribution by biomass burning is ˜24%. A large fraction of the African biomass-burning-related ozone is transported away from the continent. On a global scale, biomass burning contributes ˜9% to tropospheric ozone. Our model calculations suggest that Africa is the single most important region for biomass-burning-related tropospheric ozone, accounting for ˜35% of the global annual pyrogenic ozone enhancement of 29 Tg in 1993.

Ground-based remote sensing of tropospheric water vapour isotopologues within the project MUSICA

Directory of Open Access Journals (Sweden)

M. Schneider

2012-12-01

Full Text Available Within the project MUSICA (MUlti-platform remote Sensing of Isotopologues for investigating the Cycle of Atmospheric water, long-term tropospheric water vapour isotopologue data records are provided for ten globally distributed ground-based mid-infrared remote sensing stations of the NDACC (Network for the Detection of Atmospheric Composition Change. We present a new method allowing for an extensive and straightforward characterisation of the complex nature of such isotopologue remote sensing datasets. We demonstrate that the MUSICA humidity profiles are representative for most of the troposphere with a vertical resolution ranging from about 2 km (in the lower troposphere to 8 km (in the upper troposphere and with an estimated precision of better than 10%. We find that the sensitivity with respect to the isotopologue composition is limited to the lower and middle troposphere, whereby we estimate a precision of about 30‰ for the ratio between the two isotopologues HD¹⁶O and H₂¹⁶O. The measurement noise, the applied atmospheric temperature profiles, the uncertainty in the spectral baseline, and the cross-dependence on humidity are the leading error sources. We introduce an a posteriori correction method of the cross-dependence on humidity, and we recommend applying it to isotopologue ratio remote sensing datasets in general. In addition, we present mid-infrared CO₂ retrievals and use them for demonstrating the MUSICA network-wide data consistency. In order to indicate the potential of long-term isotopologue remote sensing data if provided with a well-documented quality, we present a climatology and compare it to simulations of an isotope incorporated AGCM (Atmospheric General Circulation Model. We identify differences in the multi-year mean and seasonal cycles that significantly exceed the estimated errors, thereby indicating deficits in the modeled atmospheric water cycle.

(abstract) Tropospheric Calibration for the Mars Observer Gravity Wave Experiment

Science.gov (United States)

Walter, Steven J.; Armstrong, John

1994-01-01

In spring 1993, microwave radiometer-based tropospheric calibration was provided for the Mars Observer gravitational wave search. The Doppler shifted X-band radio signals propagating between Earth and the Mars Observer satellite were precisely measured to determine path length variations that might signal passage of gravitational waves. Experimental sensitivity was restricted by competing sources of variability in signal transit time. Principally, fluctuations in the solar wind and ionospheric plasma density combined with fluctions in tropospheric refractivity determined the detection limit. Troposphere-induced path delay fluctions are dominated by refractive changes caused by water vapor inhomogeneities blowing through the signal path. Since passive microwave remote sensing techniques are able to determine atmospheric propagation delays, radiometer-based tropospheric calibration was provided at the Deep Space Network Uranus tracking site (DSS-15). Two microwave water vapor radiometers (WVRs), a microwave temperature profiler (MTP), and a ground based meterological station were deployed to determine line-of-sight vapor content and vertical temperature profile concurrently with Mars Observer tracking measurements. This calibration system provided the capability to correct Mars Observer Doppler data for troposphere-induced path variations. We present preliminary analysis of the Doppler and WVR data sets illustrating the utility of WVRs to calibrate Doppler data. This takes an important step toward realizing the ambitious system required to support future Ka-band Cassini satellite gravity wave tropospheric calibration system.

Origins of Tropospheric Ozone Interannual Variation (IAV) over Reunion: A Model Investigation

Science.gov (United States)

Liu, Junhua; Rodriguez, Jose M.; Thompson, Anne M.; Logan, Jennifer A.; Douglass, Anne R.; Olsen, Mark A.; Steenrod, Stephen D.; Posny, Francoise

2016-01-01

Observations from long-term ozonesonde measurements show robust variations and trends in the evolution of ozone in the middle and upper troposphere over Reunion Island (21.1 degrees South Latitude, 55.5 degrees East Longitude) in June-August. Here we examine possible causes of the observed ozone variation at Reunion Island using hindcast simulations by the stratosphere-troposphere Global Modeling Initiative chemical transport model for 1992-2014, driven by assimilated Modern-Era Retrospective Analysis for Research and Applications (MERRA) meteorological fields. Reunion Island is at the edge of the subtropical jet, a region of strong stratospheric-tropospheric exchange. Our analysis implies that the large interannual variation (IAV) of upper tropospheric ozone over Reunion is driven by the large IAV of the stratospheric influence. The IAV of the large-scale, quasi-horizontal wind patterns also contributes to the IAV of ozone in the upper troposphere. Comparison to a simulation with constant emissions indicates that increasing emissions do not lead to the maximum trend in the middle and upper troposphere over Reunion during austral winter implied by the sonde data. The effects of increasing emission over southern Africa are limited tothe lower troposphere near the surface in August-September.

The Tropospheric Ozone Assessment Report (TOAR): A community-wide effort to quantify tropospheric ozone in a rapidly changing world

Science.gov (United States)

Cooper, O. R.; Schultz, M.; Paoletti, E.; Galbally, I. E.; Naja, M. K.; Tarasick, D. W.; Evans, M. J.; Thompson, A. M.

2017-12-01

Tropospheric ozone is a greenhouse gas and pollutant detrimental to human health and crop and ecosystem productivity. Since 1990 a large portion of the anthropogenic emissions that react in the atmosphere to produce ozone has shifted from North America and Europe to Asia. This rapid shift, coupled with limited ozone monitoring in developing nations, left scientists unable to answer the most basic questions: Which regions of the world have the greatest human and plant exposure to ozone pollution? Is ozone continuing to decline in nations with strong emissions controls? To what extent is ozone increasing in the developing world? How can the atmospheric sciences community facilitate access to the ozone metrics necessary for quantifying ozone's impact on human health and crop/ecosystem productivity? To answer these questions the International Global Atmospheric Chemistry Project (IGAC) initiated the Tropospheric Ozone Assessment Report (TOAR). With over 220 member scientists and air quality specialists from 36 nations, TOAR's mission is to provide the research community with an up-to-date scientific assessment of tropospheric ozone's global distribution and trends from the surface to the tropopause. TOAR has also built the world's largest database of surface ozone observations and generated ozone exposure and dose metrics at thousands of measurement sites around the world, freely accessible for research on the global-scale impact of ozone on climate, human health and crop/ecosystem productivity. Plots of these metrics show the regions of the world with the greatest ozone exposure for humans and crops/ecosystems, at least in areas where observations are available. The results also highlight regions where air quality is improving and where it has degraded. TOAR has also conducted the first intercomparison of tropospheric column ozone from ozonesondes and multiple satellite instruments, which provide similar estimates of the present-day tropospheric ozone burden.

THEORETICAL STUDY OF THE REMOVAL OF THE TROPOSPHERIC FORMALDEHYDE BY REACTION WITH OH* AND NH3* RADICALS

OpenAIRE

Cjuno H., Jesús A.; Arroyo C., Juan; Cubas C., Roger

2014-01-01

In the context of atmospheric chemistry, two reactions radical-molecule of hydrogen abstraction have been studied. These are the OH' and NO3: radical (oxidizers agents in the troposphere) with formaldehyde in gas-phase. The calculations were carried out using the PM3 and . Ab initio methods of the UHF type. The results have allowed us to estimate the corresponding times of tropospheric permanency and the implications of these reactions in the removal of forrnaldehyde and similars from the low...

The influence of aerosols and land-use type on NO2 satellite retrieval over China

Science.gov (United States)

Liu, Mengyao; Lin, Jintai; Boersma, Folkert; Eskes, Henk; Chimot, Julien

2017-04-01

Both aerosols and surface reflectance have a strong influence on the retrieval of NO2 tropospheric vertical column densities (VCDs), especially over China with its heavy aerosol loading and rapid changes in land-use type. However, satellite retrievals of NO2 VCDs usually do not explicitly account for aerosol optical effects and surface reflectance anisotropy (BRDF) that varies in space and time. We develop an improved algorithm to derive tropospheric AMFs and VCDs over China from the OMI instrument - POMINO and DOMINO. This method can also be applied to TropOMI NO2 retrievals in the future. With small pixels of TropOMI and higher probability of encountering clear-sky scenes, the influence of BRDF and aerosol interference becomes more important than for OMI. Daily aerosol information is taken from the GEOS-Chem chemistry transport model and the aerosol optical depth (AOD) is adjusted via MODIS AOD climatology. We take the MODIS MCD43C2 C5 product to account for BRDF effects. The relative altitude of NO2 and aerosols is critical factor influencing the NO2 retrieval. In order to evaluate the aerosol extinction profiles (AEP) of GEOS-Chem improve our algorithm, we compare the GEOS-Chem simulation with CALIOP and develop a CALIOP AEP climatology to regulate the model's AEP. This provides a new way to include aerosol information into the tracer gas retrieval for OMI and TropOMI. Preliminary results indicate that the model performs reasonably well in reproducing the AEP shape. However, it seems to overestimate aerosols under 2km and underestimate above. We find that relative humidity (RH) is an important factor influencing the AEP shape when comparing the model with observations. If we adjust the GEOS-Chem RH to CALIOP's RH, the correlations of their AEPs also improve. Besides, take advantage of our retrieval method, we executed sensitivity tests to analyze their influences on NO2 trend and spatiotemporal variations in retrieval. It' the first time to investigate

Sulfate Aerosols from Non-Explosive Volcanoes: Chemical-Radiative Effects in the Troposphere and Lower Stratosphere

Directory of Open Access Journals (Sweden)

Giovanni Pitari

2016-06-01

Full Text Available SO2 and H2S are the two most important gas-phase sulfur species emitted by volcanoes, with a global amount from non-explosive emissions of the order 10 Tg-S/yr. These gases are readily oxidized forming SO42− aerosols, which effectively scatter the incoming solar radiation and cool the surface. They also perturb atmospheric chemistry by enhancing the NOx to HNO3 heterogeneous conversion via hydrolysis on the aerosol surface of N2O5 and Br-Cl nitrates. This reduces formation of tropospheric O3 and the OH to HO2 ratio, thus limiting the oxidation of CH4 and increasing its lifetime. In addition to this tropospheric chemistry perturbation, there is also an impact on the NOx heterogeneous chemistry in the lower stratosphere, due to vertical transport of volcanic SO2 up to the tropical tropopause layer. Furthermore, the stratospheric O3 formation and loss, as well as the NOx budget, may be slightly affected by the additional amount of upward diffused solar radiation and consequent increase of photolysis rates. Two multi-decadal time-slice runs of a climate-chemistry-aerosol model have been designed for studying these chemical-radiative effects. A tropopause mean global net radiative flux change (RF of −0.23 W·m−2 is calculated (including direct and indirect aerosol effects with a 14% increase of the global mean sulfate aerosol optical depth. A 5–15 ppt NOx decrease is found in the mid-troposphere subtropics and mid-latitudes and also from pole to pole in the lower stratosphere. The tropospheric NOx perturbation triggers a column O3 decrease of 0.5–1.5 DU and a 1.1% increase of the CH4 lifetime. The surface cooling induced by solar radiation scattering by the volcanic aerosols induces a tropospheric stabilization with reduced updraft velocities that produce ice supersaturation conditions in the upper troposphere. A global mean 0.9% decrease of the cirrus ice optical depth is calculated with an indirect RF of −0.08 W·m−2.

Tropospheric Emission Spectrometer (TES) Data

Data.gov (United States)

National Aeronautics and Space Administration — TES focuses on the troposphere, the layer of atmosphere that stretches from the ground to the altitude at which airplanes fly. With very high spectral resolution,...

Modeling the impact of chlorine emissions from coal combustion and prescribed waste incineration on tropospheric ozone formation in China

Science.gov (United States)

Liu, Yiming; Fan, Qi; Chen, Xiaoyang; Zhao, Jun; Ling, Zhenhao; Hong, Yingying; Li, Weibiao; Chen, Xunlai; Wang, Mingjie; Wei, Xiaolin

2018-02-01

Chlorine radicals can enhance atmospheric oxidation, which potentially increases tropospheric ozone concentration. However, few studies have been done to quantify the impact of chlorine emissions on ozone formation in China due to the lack of a chlorine emission inventory used in air quality models with sufficient resolution. In this study, the Anthropogenic Chlorine Emissions Inventory for China (ACEIC) was developed for the first time, including emissions of hydrogen chloride (HCl) and molecular chlorine (Cl2) from coal combustion and prescribed waste incineration (waste incineration plant). The HCl and Cl2 emissions from coal combustion in China in 2012 were estimated to be 232.9 and 9.4 Gg, respectively, while HCl emission from prescribed waste incineration was estimated to be 2.9 Gg. Spatially the highest emissions of HCl and Cl2 were found in the North China Plain, the Yangtze River Delta, and the Sichuan Basin. Air quality model simulations with the Community Multiscale Air Quality (CMAQ) modeling system were performed for November 2011, and the modeling results derived with and without chlorine emissions were compared. The magnitude of the simulated HCl, Cl2 and ClNO2 agreed reasonably with the observation when anthropogenic chlorine emissions were included in the model. The inclusion of the ACEIC increased the concentration of fine particulate Cl-, leading to enhanced heterogeneous reactions between Cl- and N2O5, which resulted in the higher production of ClNO2. Photolysis of ClNO2 and Cl2 in the morning and the reaction of HCl with OH in the afternoon produced chlorine radicals which accelerated tropospheric oxidation. When anthropogenic chlorine emissions were included in the model, the monthly mean concentrations of fine particulate Cl-, daily maximum 1 h ClNO2, and Cl radicals were estimated to increase by up to about 2.0 µg m-3, 773 pptv, and 1.5 × 103 molecule cm-3 in China, respectively. Meanwhile, the monthly mean daily maximum 8 h O3

Effects of regional-scale and convective transports on tropospheric ozone chemistry revealed by aircraft observations during the wet season of the AMMA campaign

Directory of Open Access Journals (Sweden)

G. Ancellet

2009-01-01

Full Text Available The African Monsoon Multidisciplinary Analyses (AMMA fourth airborne campaign was conducted in July–August 2006 to study the chemical composition of the middle and upper troposphere in West Africa with the major objective to better understand the processing of chemical emissions by the West African Monsoon (WAM and its associated regional-scale and vertical transports. In particular, the french airborne experiment was organized around two goals. The first was to characterize the impact of Mesoscale Convective Systems (MCSs on the ozone budget in the upper troposphere and the evolution of the chemical composition of these convective plumes as they move westward toward the Atlantic Ocean. The second objective was to discriminate the impact of remote sources of pollution over West Africa, including transport from the middle east, Europe, Asia and from southern hemispheric fires. Observations of O₃, CO, NO_x, H₂O and hydroperoxide above West Africa along repeated meridional transects were coupled with transport analysis based on the FLEXPART lagrangian model. The cross analysis of trace gas concentrations and transport pathways revealed 5 types of air masses: convective uplift of industrial and urban emissions, convective uplift of biogenic emissions, slow advection from Cotonou polluted plumes near the coast, meridional transport of upper tropospheric air from the subtropical barrier region, and meridional transport of Southern Hemisphere (SH biomass burning emissions. O₃/CO correlation plots and the correlation plots of H₂O₂ with a OH proxy revealed not only a control of the trace gas variability by transport processes but also significant photochemical reactivity in the mid- and upper troposphere. The study of four MCSs outflow showed contrasted chemical composition and air mass origins depending on the MCSs lifetime and latitudinal position. Favorables conditions for ozone

Oxygenated Organic Chemicals in the Pacific Troposphere: Distribution, Sources and Chemistry

Science.gov (United States)

Singh, Hanwant B.; Salas, L.; Chatfield, R.; Czech, E.; Fried, A.; Evans, M.; Jacob, D. J.; Blake, D.; Heikes, B.; Talbot, R.

2003-01-01

Airborne measurements of a large number of oxygenated organic chemicals (Oxorgs) were carried out in the Pacific troposphere (0.1-12 km) in the Spring of 2001 (Feb. 24-April 10). Specifically these measuremen ts included acetone, methylethyl ketone (MEK), methanol, ethanol, ace taldehyde, propionaldehyde, PANS, and organic nitrates. Complementary measurements of formaldehyde, organic peroxides, and tracers were al so available. Ox-orgs were abundant in the clean troposphere and were greatly enhanced in the outflow regions from Asia. Their mixing ratios were typically highest in the lower troposphere and declined toward s the upper troposphere and the lowermost stratosphere. Their total a bundance (Ox-orgs) significantly exceeded that of NMHC (C2-C8 NMHC). A comparison of these data with observations collected some seven yea rs earlier (Feb.-March, 1994), did not reveal any significant changes . Throughout the troposphere mixing ratios of Ox-orgs were strongly c orrelated with each other as well as with tracers of fossil and bioma sshiof'uel combustion. Analysis of the relative enhancement of selected Oxorgs with respect to CH3Cl and CO in twelve sampled plumes, origi nating from fires, is used to assess their primary and secondary sour ces from biomass combustion. The composition of these plumes also ind icates a large shift of reactive nitrogen into the PAN reservoir ther eby limiting ozone formation. The Harvard 3-D photochemical model, th at uses state of the art chemistry and source information, is used to compare simulated and observed mixing ratios of selected species. A 1 -D model is used to explore the chemistry of aldehydes. These results will be presented.

Characteristics of intercontinental transport of tropospheric ozone from Africa to Asia

Science.gov (United States)

Han, Han; Liu, Jane; Yuan, Huiling; Zhuang, Bingliang; Zhu, Ye; Wu, Yue; Yan, Yuhan; Ding, Aijun

2018-03-01

In this study, we characterize the transport of ozone from Africa to Asia through the analysis of the simulations of a global chemical transport model, GEOS-Chem, from 1987 to 2006. The receptor region Asia is defined within 5-60° N and 60-145° E, while the source region Africa is within 35° S-15° N and 20° W-55° E and within 15-35° N and 20° W-30° E. The ozone generated in the African troposphere from both natural and anthropogenic sources is tracked through tagged ozone simulation. Combining this with analysis of trajectory simulations using the Hybrid Single-Particle Lagrangian Integrated Trajectory (HYSPLIT) model, we find that the upper branch of the Hadley cell connects with the subtropical westerlies in the Northern Hemisphere (NH) to form a primary transport pathway from Africa to Asia in the middle and upper troposphere throughout the year. The Somali jet that runs from eastern Africa near the equator to the Indian subcontinent in the lower troposphere is the second pathway that appears only in NH summer. The influence of African ozone mainly appears over Asia south of 40° N. The influence shows strong seasonality, varying with latitude, longitude, and altitude. In the Asian upper troposphere, imported African ozone is largest from March to May around 30° N (12-16 ppbv) and lowest during July-October around 10° N ( ˜ 2 ppbv). In the Asian middle and lower troposphere, imported African ozone peaks in NH winter between 20 and 25° N. Over 5-40° N, the mean fractional contribution of imported African ozone to the overall ozone concentrations in Asia is largest during NH winter in the middle troposphere ( ˜ 18 %) and lowest in NH summer throughout the tropospheric column ( ˜ 6 %). This seasonality mainly results from the collective effects of the ozone precursor emissions in Africa and meteorology and chemistry in Africa, in Asia and along the transport pathways. The seasonal swing of the Hadley circulation and subtropical westerlies along the

Climate change projections and stratosphere-troposphere interaction

Energy Technology Data Exchange (ETDEWEB)

Scaife, Adam A.; Fereday, David R.; Butchart, Neal; Hardiman, Steven C. [Met Office Hadley Centre, Exeter (United Kingdom); Spangehl, Thomas; Cubasch, Ulrich; Langematz, Ulrike [Freie Universitaet Berlin, Berlin (Germany); Akiyoshi, Hideharu [National Institute for Environmental Studies, Tsukuba (Japan); Bekki, Slimane [LATMOS-IPSL, UVSQ, UPMC, CNRS/INSU, Paris (France); Braesicke, Peter [University of Cambridge, Cambridge (United Kingdom); Chipperfield, Martyn P. [University of Leeds, School of Earth and Environment, Leeds (United Kingdom); Gettelman, Andrew [National Center for Atmospheric Research, Boulder, CO (United States); Michou, Martine [GAME/CNRM (Meteo France, CNRS), Toulouse (France); Rozanov, Eugene [PMOD/WRC and ETHZ, Davos (Switzerland); Shepherd, Theodore G. [University of Toronto, Toronto, ON (Canada)

2012-05-15

Climate change is expected to increase winter rainfall and flooding in many extratropical regions as evaporation and precipitation rates increase, storms become more intense and storm tracks move polewards. Here, we show how changes in stratospheric circulation could play a significant role in future climate change in the extratropics through an additional shift in the tropospheric circulation. This shift in the circulation alters climate change in regional winter rainfall by an amount large enough to significantly alter regional climate change projections. The changes are consistent with changes in stratospheric winds inducing a change in the baroclinic eddy growth rate across the depth of the troposphere. A change in mean wind structure and an equatorward shift of the tropospheric storm tracks relative to models with poor stratospheric resolution allows coupling with surface climate. Using the Atlantic storm track as an example, we show how this can double the predicted increase in extreme winter rainfall over Western and Central Europe compared to other current climate projections. (orig.)

Aerosol indirect effect on tropospheric ozone via lightning

Science.gov (United States)

Yuan, T.; Remer, L. A.; Bian, H.; Ziemke, J. R.; Albrecht, R. I.; Pickering, K. E.; Oreopoulos, L.; Goodman, S. J.; Yu, H.; Allen, D. J.

2012-12-01

Tropospheric ozone (O3) is a pollutant and major greenhouse gas and its radiative forcing is still uncertain. The unresolved difference between modeled and observed natural background O3 concentrations is a key source of the uncertainty. Here we demonstrate remarkable sensitivity of lightning activity to aerosol loading with lightning activity increasing more than 30 times per unit of aerosol optical depth over our study area. We provide observational evidence that indicates the observed increase in lightning activity is caused by the influx of aerosols from a volcano. Satellite data analyses suggest O3 is increased as a result of aerosol-induced increase in lightning and lightning produced NOx. Model simulations with prescribed lightning change corroborate the satellite data analysis. This aerosol-O3 connection is achieved via aerosol increasing lightning and thus lightning produced nitrogen oxides. This aerosol-lightning-ozone link provides a potential physical mechanism that may account for a part of the model-observation difference in background O3 concentration. More importantly, O3 production increase from this link is concentrated in the upper troposphere, where O3 is most efficient as a greenhouse gas. Both of these implications suggest a stronger O3 historical radiative forcing. This introduces a new pathway, through which increasing in aerosols from pre-industrial time to present day enhances tropospheric O3 production. Aerosol forcing thus has a warming component via its effect on O3 production. Sensitivity simulations suggest that 4-8% increase of tropospheric ozone, mainly in the tropics, is expected if aerosol-lighting-ozone link is parameterized, depending on the background emission scenario. We note, however, substantial uncertainties remain on the exact magnitude of aerosol effect on tropospheric O3 via lightning. The challenges for obtaining a quantitative global estimate of this effect are also discussed. Our results have significant implications

Impacts of stratospheric sulfate geoengineering on tropospheric ozone

Directory of Open Access Journals (Sweden)

L. Xia

2017-10-01

Full Text Available A range of solar radiation management (SRM techniques has been proposed to counter anthropogenic climate change. Here, we examine the potential effects of stratospheric sulfate aerosols and solar insolation reduction on tropospheric ozone and ozone at Earth's surface. Ozone is a key air pollutant, which can produce respiratory diseases and crop damage. Using a version of the Community Earth System Model from the National Center for Atmospheric Research that includes comprehensive tropospheric and stratospheric chemistry, we model both stratospheric sulfur injection and solar irradiance reduction schemes, with the aim of achieving equal levels of surface cooling relative to the Representative Concentration Pathway 6.0 scenario. This allows us to compare the impacts of sulfate aerosols and solar dimming on atmospheric ozone concentrations. Despite nearly identical global mean surface temperatures for the two SRM approaches, solar insolation reduction increases global average surface ozone concentrations, while sulfate injection decreases it. A fundamental difference between the two geoengineering schemes is the importance of heterogeneous reactions in the photochemical ozone balance with larger stratospheric sulfate abundance, resulting in increased ozone depletion in mid- and high latitudes. This reduces the net transport of stratospheric ozone into the troposphere and thus is a key driver of the overall decrease in surface ozone. At the same time, the change in stratospheric ozone alters the tropospheric photochemical environment due to enhanced ultraviolet radiation. A shared factor among both SRM scenarios is decreased chemical ozone loss due to reduced tropospheric humidity. Under insolation reduction, this is the dominant factor giving rise to the global surface ozone increase. Regionally, both surface ozone increases and decreases are found for both scenarios; that is, SRM would affect regions of the world differently in terms of air

Impacts of stratospheric sulfate geoengineering on tropospheric ozone

Science.gov (United States)

Xia, Lili; Nowack, Peer J.; Tilmes, Simone; Robock, Alan

2017-10-01

A range of solar radiation management (SRM) techniques has been proposed to counter anthropogenic climate change. Here, we examine the potential effects of stratospheric sulfate aerosols and solar insolation reduction on tropospheric ozone and ozone at Earth's surface. Ozone is a key air pollutant, which can produce respiratory diseases and crop damage. Using a version of the Community Earth System Model from the National Center for Atmospheric Research that includes comprehensive tropospheric and stratospheric chemistry, we model both stratospheric sulfur injection and solar irradiance reduction schemes, with the aim of achieving equal levels of surface cooling relative to the Representative Concentration Pathway 6.0 scenario. This allows us to compare the impacts of sulfate aerosols and solar dimming on atmospheric ozone concentrations. Despite nearly identical global mean surface temperatures for the two SRM approaches, solar insolation reduction increases global average surface ozone concentrations, while sulfate injection decreases it. A fundamental difference between the two geoengineering schemes is the importance of heterogeneous reactions in the photochemical ozone balance with larger stratospheric sulfate abundance, resulting in increased ozone depletion in mid- and high latitudes. This reduces the net transport of stratospheric ozone into the troposphere and thus is a key driver of the overall decrease in surface ozone. At the same time, the change in stratospheric ozone alters the tropospheric photochemical environment due to enhanced ultraviolet radiation. A shared factor among both SRM scenarios is decreased chemical ozone loss due to reduced tropospheric humidity. Under insolation reduction, this is the dominant factor giving rise to the global surface ozone increase. Regionally, both surface ozone increases and decreases are found for both scenarios; that is, SRM would affect regions of the world differently in terms of air pollution. In conclusion

Geometry-specified troposphere decorrelation for subcentimeter real-time kinematic solutions over long baselines

Science.gov (United States)

Li, Bofeng; Feng, Yanming; Shen, Yunzhong; Wang, Charles

2010-11-01

Real-time kinematic (RTK) GPS techniques have been extensively developed for applications including surveying, structural monitoring, and machine automation. Limitations of the existing RTK techniques that hinder their applications for geodynamics purposes are twofold: (1) the achievable RTK accuracy is on the level of a few centimeters and the uncertainty of vertical component is 1.5-2 times worse than those of horizontal components and (2) the RTK position uncertainty grows in proportional to the base-to-rover distances. The key limiting factor behind the problems is the significant effect of residual tropospheric errors on the positioning solutions, especially on the highly correlated height component. This paper develops the geometry-specified troposphere decorrelation strategy to achieve the subcentimeter kinematic positioning accuracy in all three components. The key is to set up a relative zenith tropospheric delay (RZTD) parameter to absorb the residual tropospheric effects and to solve the established model as an ill-posed problem using the regularization method. In order to compute a reasonable regularization parameter to obtain an optimal regularized solution, the covariance matrix of positional parameters estimated without the RZTD parameter, which is characterized by observation geometry, is used to replace the quadratic matrix of their "true" values. As a result, the regularization parameter is adaptively computed with variation of observation geometry. The experiment results show that new method can efficiently alleviate the model's ill condition and stabilize the solution from a single data epoch. Compared to the results from the conventional least squares method, the new method can improve the long-range RTK solution precision from several centimeters to the subcentimeter in all components. More significantly, the precision of the height component is even higher. Several geosciences applications that require subcentimeter real-time solutions can

MIPAS measurements of upper tropospheric C2H6 and O3 during the southern hemispheric biomass burning season in 2003

Directory of Open Access Journals (Sweden)

T. Steck

2007-11-01

Full Text Available Under cloud free conditions, the Michelson Interferometer for Passive Atmospheric Sounding (MIPAS provides measurements of spectrally resolved limb radiances down to the upper troposphere. These are used to infer global distributions of mixing ratios of atmospheric constituents in the upper troposphere and the stratosphere. From 21 October to 12 November 2003, MIPAS observed enhanced amounts of upper tropospheric C2H6 (up to about 400 pptv and ozone (up to about 80 ppbv. The absolute values of C2H6, however, may be systematically low by about 30% due to uncertainties of the spectroscopic data used. By means of trajectory calculations, the enhancements observed in the southern hemisphere are, at least partly, attributed to a biomass burning plume, which covers wide parts of the Southern hemisphere, from South America, the Atlantic Ocean, Africa, the Indian Ocean to Australia. The chemical composition of the part of the plume-like pollution belt associated with South American fires, where rainforest burning is predominant appears different from the part of the plume associated with southern African savanna burning. In particular, African savanna fires lead to a larger ozone enhancement than equatorial American fires. In this analysis, MIPAS observations of high ozone were disregarded where low CFC-11 (below 245 pptv was observed, because this hints at a stratospheric component in the measured signal. Different type of vegetation burning (flaming versus smouldering combustion has been identified as a candidate explanation for the different plume compositions.

Soil respiration, root biomass, and root turnover following long-term exposure of northern forests to elevated atmospheric CO2 and tropospheric O3

Science.gov (United States)

Kurt S. Pregitzer; Andrew J. Burton; John S. King; Donald R. Zak

2008-01-01

The Rhinelander free-air CO2 enrichment (FACE) experiment is designed to understand ecosystem response to elevated atmospheric carbon dioxide (+CO2) and elevated tropospheric ozone (+O3). The objectives of this study were: to understand how soil respiration responded to the experimental treatments; to...

Tropospheric ozone trend over Beijing from 2002–2010: ozonesonde measurements and modeling analysis

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Y. Wang

2012-09-01

Full Text Available Using a combination of ozonesonde data and numerical simulations of the Chemical Lagrangian Model of the Stratosphere (CLaMS, the trend of tropospheric ozone (O₃ during 2002–2010 over Beijing was investigated. Tropospheric ozone over Beijing shows a winter minimum and a broad summer maximum with a clear positive trend in the maximum summer ozone concentration over the last decade. The observed significant trend of tropospheric column ozone is mainly caused by photochemical production (3.1% yr⁻¹ for a mean level of 52 DU. This trend is close to the significant trend of partial column ozone in the lower troposphere (0–3 km resulting from the enhanced photochemical production during summer (3.0% yr⁻¹ for a mean level of 23 DU. Analysis of the CLaMS simulation shows that transport rather than chemistry drives most of the seasonality of tropospheric ozone. However, dynamical processes alone cannot explain the trend of tropospheric ozone in the observational data. Clearly enhanced ozone values and a negative vertical ozone gradient in the lower troposphere in the observational data emphasize the importance of photochemistry within the troposphere during spring and summer, and suggest that the photochemistry within the troposphere significantly contributes to the tropospheric ozone trend over Beijing during the last decade.

Stratospheric ozone intrusion events and their impacts on tropospheric ozone in the Southern Hemisphere

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J. W. Greenslade

2017-09-01

Full Text Available Stratosphere-to-troposphere transport (STT provides an important natural source of ozone to the upper troposphere, but the characteristics of STT events in the Southern Hemisphere extratropics and their contribution to the regional tropospheric ozone budget remain poorly constrained. Here, we develop a quantitative method to identify STT events from ozonesonde profiles. Using this method we estimate the seasonality of STT events and quantify the ozone transported across the tropopause over Davis (69° S, 2006–2013, Macquarie Island (54° S, 2004–2013, and Melbourne (38° S, 2004–2013. STT seasonality is determined by two distinct methods: a Fourier bandpass filter of the vertical ozone profile and an analysis of the Brunt–Väisälä frequency. Using a bandpass filter on 7–9 years of ozone profiles from each site provides clear detection of STT events, with maximum occurrences during summer and minimum during winter for all three sites. The majority of tropospheric ozone enhancements owing to STT events occur within 2.5 and 3 km of the tropopause at Davis and Macquarie Island respectively. Events are more spread out at Melbourne, occurring frequently up to 6 km from the tropopause. The mean fraction of total tropospheric ozone attributed to STT during STT events is  ∼ 1. 0–3. 5 % at each site; however, during individual events, over 10 % of tropospheric ozone may be directly transported from the stratosphere. The cause of STTs is determined to be largely due to synoptic low-pressure frontal systems, determined using coincident ERA-Interim reanalysis meteorological data. Ozone enhancements can also be caused by biomass burning plumes transported from Africa and South America, which are apparent during austral winter and spring and are determined using satellite measurements of CO. To provide regional context for the ozonesonde observations, we use the GEOS-Chem chemical transport model, which is too coarsely

New Particle Formation in the Mid-Latitude Upper Troposphere

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Axisa, Duncan

Primary aerosol production due to new particle formation (NPF) in the upper troposphere and the impact that this might have on cloud condensation nuclei (CCN) concentration can be of sufficient magnitude to contribute to the uncertainty in radiative forcing. This uncertainty affects our ability to estimate how sensitive the climate is to greenhouse gas emissions. Therefore, new particle formation must be accurately defined, parametrized and accounted for in models. This research involved the deployment of instruments, data analysis and interpretation of particle formation events during the Mid-latitude Airborne Cirrus Properties Experiment (MACPEX) campaign. The approach combined field measurements and observations with extensive data analysis and modeling to study the process of new particle formation and growth to CCN active sizes. Simultaneous measurements of O3, CO, ultrafine aerosol particles and surface area from a high-altitude research aircraft were used to study tropospheric-stratospheric mixing as well as the frequency and location of NPF. It was found that the upper troposphere was an active region in the production of new particles by gas-to-particle conversion, that nucleation was triggered by convective clouds and mixing processes, and that NPF occurred in regions with high relative humidity and low surface area. In certain cases, mesoscale and synoptic features enhanced mixing and facilitated the formation of new particles in the northern mid-latitudes. A modeling study of particle growth and CCN formation was done based on measured aerosol size distributions and modeled growth. The results indicate that when SO2 is of sufficient concentration NPF is a significant source of potential CCN in the upper troposphere. In conditions where convective cloud outflow eject high concentrations of SO2, a large number of new particles can form especially in the instance when the preexisting surface area is low. The fast growth of nucleated clusters produces a

Fungal community composition and function after long-term exposure of northern forests to elevated atmospheric CO2 and tropospheric O3

Science.gov (United States)

Ivan P. Edwards; Donald R. Zak

2011-01-01

The long-term effects of rising atmospheric carbon dioxide (CO2) and tropospheric O3 concentrations on fungal communities in soil are not well understood. Here, we examine fungal community composition and the activities of cellobiohydrolase and N-acetylglucosaminidase (NAG) after 10 years of exposure to 1...

Real-Time Tropospheric Product Establishment and Accuracy Assessment in China

Science.gov (United States)

Chen, M.; Guo, J.; Wu, J.; Song, W.; Zhang, D.

2018-04-01

Tropospheric delay has always been an important issue in Global Navigation Satellite System (GNSS) processing. Empirical tropospheric delay models are difficult to simulate complex and volatile atmospheric environments, resulting in poor accuracy of the empirical model and difficulty in meeting precise positioning demand. In recent years, some scholars proposed to establish real-time tropospheric product by using real-time or near-real-time GNSS observations in a small region, and achieved some good results. This paper uses real-time observing data of 210 Chinese national GNSS reference stations to estimate the tropospheric delay, and establishes ZWD grid model in the country wide. In order to analyze the influence of tropospheric grid product on wide-area real-time PPP, this paper compares the method of taking ZWD grid product as a constraint with the model correction method. The results show that the ZWD grid product estimated based on the national reference stations can improve PPP accuracy and convergence speed. The accuracy in the north (N), east (E) and up (U) direction increase by 31.8 %,15.6 % and 38.3 %, respectively. As with the convergence speed, the accuracy of U direction experiences the most improvement.

Tropospheric products of the second GOP European GNSS reprocessing (1996-2014)

Science.gov (United States)

Dousa, Jan; Vaclavovic, Pavel; Elias, Michal

2017-09-01

In this paper, we present results of the second reprocessing of all data from 1996 to 2014 from all stations in International Association of Geodesy (IAG) Reference Frame Sub-Commission for Europe (EUREF) Permanent Network (EPN) as performed at the Geodetic Observatory Pecný (GOP). While the original goal of this research was to ultimately contribute to the realization of a new European Terrestrial Reference System (ETRS), we also aim to provide a new set of GNSS (Global Navigation Satellite System) tropospheric parameter time series with possible applications to climate research. To achieve these goals, we improved a strategy to guarantee the continuity of these tropospheric parameters and we prepared several variants of troposphere modelling. We then assessed all solutions in terms of the repeatability of coordinates as an internal evaluation of applied models and strategies and in terms of zenith tropospheric delays (ZTDs) and horizontal gradients with those of the ERA-Interim numerical weather model (NWM) reanalysis. When compared to the GOP Repro1 (first EUREF reprocessing) solution, the results of the GOP Repro2 (second EUREF reprocessing) yielded improvements of approximately 50 and 25 % in the repeatability of the horizontal and vertical components, respectively, and of approximately 9 % in tropospheric parameters. Vertical repeatability was reduced from 4.14 to 3.73 mm when using the VMF1 mapping function, a priori ZHD (zenith hydrostatic delay), and non-tidal atmospheric loading corrections from actual weather data. Raising the elevation cut-off angle from 3 to 7° and then to 10° increased RMS from coordinates' repeatability, which was then confirmed by independently comparing GNSS tropospheric parameters with the NWM reanalysis. The assessment of tropospheric horizontal gradients with respect to the ERA-Interim revealed a strong sensitivity of estimated gradients to the quality of GNSS antenna tracking performance. This impact was demonstrated at the

Long-term series of tropospheric water vapour amounts and HDO/H2O ratio profiles above Jungfraujoch.

Science.gov (United States)

Lejeune, B.; Mahieu, E.; Schneider, M.; Hase, F.; Servais, C.; Demoulin, P.

2012-04-01

Water vapour is a crucial climate variable involved in many processes which widely determine the energy budget of our planet. In particular, water vapour is the dominant greenhouse gas in the Earth's atmosphere and its radiative forcing is maximum in the middle and upper troposphere. Because of the extremely high variability of water vapour concentration in time and space, it is challenging for the available relevant measurement techniques to provide a consistent data set useful for trend analyses and climate studies. Schneider et al. (2006a) showed that ground-based Fourier Transform Infrared (FTIR) spectroscopy, performed from mountain observatories, allows for the detection of H2O variabilities up to the tropopause. Furthermore, the FTIR measurements allow the retrieval of HDO amounts and therefore the monitoring of HDO/H2O ratio profiles whose variations act as markers for the source and history of the atmospheric water vapour. In the framework of the MUSICA European project (Multi-platform remote Sensing of Isotopologues for investigating the Cycle of Atmospheric water, http://www.imk-asf.kit.edu/english/musica.php), a new approach has been developed and optimized by M. Schneider and F. Hase, using the PROFFIT algorithm, to consistently retrieve tropospheric water vapour profiles from high-resolution ground-based infrared solar spectra and so taking benefit from available long-term data sets of ground-based observations. The retrieval of the water isotopologues is performed on a logarithmic scale from 14 micro-windows located in the 2600-3100 cm-1 region. Other important features of this new retrieval strategy are: a speed dependant Voigt line shape model, a joint temperature profile retrieval and an interspecies constraint for the HDO/H2O profiles. In this contribution, we will combine the quality of the MUSICA strategy and of our observations, which are recorded on a regular basis with FTIR spectrometers, under clear-sky conditions, at the NDACC site

Seasonal variations and vertical features of aerosol particles in the Antarctic troposphere

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K. Hara

2011-06-01

Full Text Available Tethered balloon-borne aerosol measurements were conducted at Syowa Station, Antarctica during the 46th Japanese Antarctic expedition (2005–2006. The CN concentration reached a maximum in the summer, although the number concentrations of fine particles (D_p>0.3 μm and coarse particles (D_p>2.0 μm increased during the winter–spring. The CN concentration was 30–2200 cm⁻³ near the surface (surface – 500 m and 7–7250 cm⁻³ in the lower free troposphere (>1500 m. During the austral summer, higher CN concentration was often observed in the lower free troposphere, where the number concentrations in fine and coarse modes were remarkably lower. The frequent appearance of higher CN concentrations in the free troposphere relative to continuous aerosol measurements at the ground strongly suggests that new particle formation is more likely to occur in the lower free troposphere in Antarctic regions. Seasonal variations of size distribution of fine-coarse particles show that the contribution of the coarse mode was greater in the winter–spring than in summer because of the dominance of sea-salt particles in the winter–spring. The number concentrations of fine and coarse particles were high in air masses from the ocean and mid-latitudes. Particularly, aerosol enhancement was observed not only in the boundary layer, but also in the lower free troposphere during and immediately after Antarctic haze events occurring in May, July and September.

The meteorological environment of the tropospheric ozone maximum over the tropical South Atlantic

Energy Technology Data Exchange (ETDEWEB)

Krishnamurti, T N; Fuelberg, H E; Bensman, E L; Sinha, M C; Oosterhof, D; Kumar, V B [Florida State University, Tallahassee, FL (United States). Department of Meteorology

1993-01-01

This paper examines atmospheric flow patterns over the Southern Atlantic Ocean, where a maximum of tropospheric ozone is observed just west of Southern Africa. The climatology of the South Atlantic basin is shown to favour flow off from South America and Africa converging into the area of high tropospheric ozone. This ozone is initially attributable to byproducts of biomass burning over both these continents. A case study, carried out over 6 days during October 1989, was used to determine the effect of a purely advective scheme (no photochemistry) on the distribution of ozone over the basin. The results showed a pattern in which ozone accumulated off the west coast of South Africa within 72 hours after beginning with an homogenous, zonally-symmetric distribution of ozone. 11 refs.

Physics of the tropospheric radiopropagation

International Nuclear Information System (INIS)

Ajayi, G.O.

1989-02-01

The physics of the tropospheric radiopropagation is presented considering the atmospheric radio refractive index and taking into account the influence of precipitation and the attenuation due to the atmospheric gases. 35 refs, 20 figs, 3 tabs

Spatial Variability of Wet Troposphere Delays Over Inland Water Bodies

Science.gov (United States)

Mehran, Ali; Clark, Elizabeth A.; Lettenmaier, Dennis P.

2017-11-01

Satellite radar altimetry has enabled the study of water levels in large lakes and reservoirs at a global scale. The upcoming Surface Water and Ocean Topography (SWOT) satellite mission (scheduled launch 2020) will simultaneously measure water surface extent and elevation at an unprecedented accuracy and resolution. However, SWOT retrieval accuracy will be affected by a number of factors, including wet tropospheric delay—the delay in the signal's passage through the atmosphere due to atmospheric water content. In past applications, the wet tropospheric delay over large inland water bodies has been corrected using atmospheric moisture profiles based on atmospheric reanalysis data at relatively coarse (tens to hundreds of kilometers) spatial resolution. These products cannot resolve subgrid variations in wet tropospheric delays at the spatial resolutions (of 1 km and finer) that SWOT is intended to resolve. We calculate zenith wet tropospheric delays (ZWDs) and their spatial variability from Weather Research and Forecasting (WRF) numerical weather prediction model simulations at 2.33 km spatial resolution over the southwestern U.S., with attention in particular to Sam Rayburn, Ray Hubbard, and Elephant Butte Reservoirs which have width and length dimensions that are of order or larger than the WRF spatial resolution. We find that spatiotemporal variability of ZWD over the inland reservoirs depends on climatic conditions at the reservoir location, as well as distance from ocean, elevation, and surface area of the reservoir, but that the magnitude of subgrid variability (relative to analysis and reanalysis products) is generally less than 10 mm.

Observations of peroxyacetyl nitrate (PAN) in the upper troposphere by the Atmospheric Chemistry Experiment-Fourier Transform Spectrometer (ACE-FTS)

Science.gov (United States)

Tereszchuk, K. A.; Moore, D. P.; Harrison, J. J.; Boone, C. D.; Park, M.; Remedios, J. J.; Randel, W. J.; Bernath, P. F.

2013-06-01

Peroxyacetyl nitrate (CH3CO·O2NO2, abbreviated as PAN) is a trace molecular species present in the troposphere and lower stratosphere due primarily to pollution from fuel combustion and the pyrogenic outflows from biomass burning. In the lower troposphere, PAN has a relatively short lifetime and is principally destroyed within a few hours through thermolysis, but it can act as a reservoir and carrier of NOx in the colder temperatures of the upper troposphere, where UV photolysis becomes the dominant loss mechanism. Pyroconvective updrafts from large biomass burning events can inject PAN into the upper troposphere and lower stratosphere (UTLS), providing a means for the long-range transport of NOx. Given the extended lifetimes at these higher altitudes, PAN is readily detectable via satellite remote sensing. A new PAN data product is now available for the Atmospheric Chemistry Experiment Fourier Transform Spectrometer (ACE-FTS) version 3.0 data set. We report observations of PAN in boreal biomass burning plumes recorded during the BORTAS (quantifying the impact of BOReal forest fires on Tropospheric oxidants over the Atlantic using Aircraft and Satellites) campaign (12 July to 3 August 2011). The retrieval method employed by incorporating laboratory-recorded absorption cross sections into version 3.0 of the ACE-FTS forward model and retrieval software is described in full detail. The estimated detection limit for ACE-FTS PAN is 5 pptv, and the total systematic error contribution to the ACE-FTS PAN retrieval is ~ 16%. The retrieved volume mixing ratio (VMR) profiles are compared to coincident measurements made by the Michelson Interferometer for Passive Atmospheric Sounding (MIPAS) instrument on the European Space Agency (ESA) Environmental Satellite (ENVISAT). The MIPAS measurements demonstrated good agreement with the ACE-FTS VMR profiles for PAN, where the measured VMR values are well within the associated measurement errors for both instruments and comparative

NOAA Climate Data Record for Mean Layer Temperature (Upper Troposphere & Lower Stratosphere) from UCAR, Version 2

Data.gov (United States)

National Oceanic and Atmospheric Administration, Department of Commerce — The Temperatures of Troposphere / Stratosphere (TTS) (AMSU channel 7 and MSU channel 3) CDR is generated by using National Oceanic and Atmospheric Administration...

The Origins of Air Parcels Uplifted in a Two Dimensional Gravity Wave in the Tropical Upper Troposphere During the NASA Stratosphere Troposphere Exchange Project (STEP)

Science.gov (United States)

Selkirk, Henry B.; Pfister, Leonhard; Chan, K. Roland; Kritz, Mark; Kelly, Ken

1989-01-01

During January and February 1987, as part of the Stratosphere-Troposphere Exchange Project, the NASA ER-2 made 11 flights from Darwin, Australia to investigate dehydration mechanisms in the vicinity of the tropical tropopause. After the monsoon onset in the second week of January, steady easterly flow of 15-25 ms (exp -1) was established in the upper troposphere and lower stratosphere over northern Australia and adjacent seas. Penetrating into this regime were elements of the monsoon convection such as overshooting convective turrets and extensive anvils including cyclone cloud shields. In cases of the latter, the resulting flow obstructions tended to produce mesoscale gravity waves. In several instances the ER- 2 meteorological and trace constituent measurements provide a detailed description of the structure of these gravity waves. Among these was STEP Flight 6, 22-23 January. It is of particular interest to STEP because of the close proximity of ice-laden and dehydrated air on the same isentropic surfaces. Convective events inject large amounts of ice into the upper troposphere and lower stratosphere which may not be completely removed by local precipitation processes. In the present instance, a gravity wave for removed from the source region appears to induce relativity rapid upward motion in the ice-laden air and subsequent dessication. Potential mechanisms for such a localized removal process are under investigation.