Global observations of tropospheric BrO columns using GOME-2 satellite data

Directory of Open Access Journals (Sweden)

N. Theys

2011-02-01

Full Text Available Measurements from the GOME-2 satellite instrument have been analyzed for tropospheric BrO using a residual technique that combines measured BrO columns and estimates of the stratospheric BrO content from a climatological approach driven by O₃ and NO₂ observations. Comparisons between the GOME-2 results and BrO vertical columns derived from correlative ground-based and SCIAMACHY nadir observations, present a good level of consistency. We show that the adopted technique enables separation of stratospheric and tropospheric fractions of the measured total BrO columns and allows quantitative study of the BrO plumes in polar regions. While some satellite observed plumes of enhanced BrO can be explained by stratospheric descending air, we show that most BrO hotspots are of tropospheric origin, although they are often associated to regions with low tropopause heights as well. Elaborating on simulations using the p-TOMCAT tropospheric chemical transport model, this result is found to be consistent with the mechanism of bromine release through sea salt aerosols production during blowing snow events. No definitive conclusion can be drawn however on the importance of blowing snow sources in comparison to other bromine release mechanisms. Outside polar regions, evidence is provided for a global tropospheric BrO background with column of 1–3 × 10¹³ molec cm⁻², consistent with previous estimates.

Eleven years of tropospheric NO2 measured by GOME, SCIAMACHY and OMI

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.

2006-12-01

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

Global observations of BrO in the troposphere using GOME-2 satellite data

Science.gov (United States)

Theys, N.; van Roozendael, M.; Hendrick, F.; Xin, Y.; Isabelle, D.; Richter, A.; Mathias, B.; Quentin, E.; Johnston, P. V.; Kreher, K.; Martine, D.

2010-12-01

Measurements from the GOME-2 satellite instrument have been analyzed for tropospheric BrO using a residual technique that combines measured BrO columns and estimates of the stratospheric BrO content from a climatological approach driven by O3 and NO2 observations. Comparisons between the GOME-2 results and correlative data including ground-based BrO vertical columns and total BrO columns derived from SCIAMACHY nadir observations, present a good level of consistency. We show that the adopted technique enables to separate the stratospheric and tropospheric fractions of the measured total BrO columns and allows studying the BrO plumes in polar region in more detail. While several satellite BrO plumes can largely be explained by an influence of stratospheric descending air, we show that numerous tropospheric BrO hotspots are associated to regions with low tropopause heights as well. Elaborating on simulations using the p-TOMCAT tropospheric chemical transport model, this finding is found to be consistent with the mechanism of bromine release through sea salt aerosols production during blowing snow events. Outside the polar region, evidences are provided for a global tropospheric BrO background with columns of 1-3 x 1013 molec/cm2.

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

Science.gov (United States)

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

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

Science.gov (United States)

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

Directory of Open Access Journals (Sweden)

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.

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

Science.gov (United States)

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

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

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.

Testing and improving OMI DOMINO tropospheric NO2 using observations from the DANDELIONS and INTEX-B validation campaigns

NARCIS (Netherlands)

Hains, J.C.; Boersma, K.F.; Kroon, M.; Dirksen, R.J.; Cohen, R.C.; Perring, A.E.; Bucsela, E.J.; Volten, H.; Swart, D.P.J.; Richter, A.; Wittrock, F.; Schönhardt, A.; Wagner, T.; Ibrahim, O.W.; Roozendael, Van M.; Pinardi, G.; Gleason, J.F.; Veefkind, J.P.; Levelt, P.F.

2010-01-01

We present a sensitivity analysis of the tropospheric NO2 retrieval from the Ozone Monitoring Instrument (OMI) using measurements from the Dutch Aerosol and Nitrogen Dioxide Experiments for Validation of OMI and SCIAMACHY (DANDELIONS) and Intercontinental Chemical Transport Experiment-B (INTEX-B)

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

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

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

Directory of Open Access Journals (Sweden)

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

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.

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)

FRESCO+: an improved O2 A-band cloud retrieval algorithm for tropospheric trace gas retrievals

Directory of Open Access Journals (Sweden)

M. van Roozendael

2008-11-01

Full Text Available The FRESCO (Fast Retrieval Scheme for Clouds from the Oxygen A-band algorithm has been used to retrieve cloud information from measurements of the O2 A-band around 760 nm by GOME, SCIAMACHY and GOME-2. The cloud parameters retrieved by FRESCO are the effective cloud fraction and cloud pressure, which are used for cloud correction in the retrieval of trace gases like O3 and NO2. To improve the cloud pressure retrieval for partly cloudy scenes, single Rayleigh scattering has been included in an improved version of the algorithm, called FRESCO+. We compared FRESCO+ and FRESCO effective cloud fractions and cloud pressures using simulated spectra and one month of GOME measured spectra. As expected, FRESCO+ gives more reliable cloud pressures over partly cloudy pixels. Simulations and comparisons with ground-based radar/lidar measurements of clouds show that the FRESCO+ cloud pressure is about the optical midlevel of the cloud. Globally averaged, the FRESCO+ cloud pressure is about 50 hPa higher than the FRESCO cloud pressure, while the FRESCO+ effective cloud fraction is about 0.01 larger. The effect of FRESCO+ cloud parameters on O3 and NO2 vertical column density (VCD retrievals is studied using SCIAMACHY data and ground-based DOAS measurements. We find that the FRESCO+ algorithm has a significant effect on tropospheric NO2 retrievals but a minor effect on total O3 retrievals. The retrieved SCIAMACHY tropospheric NO2 VCDs using FRESCO+ cloud parameters (v1.1 are lower than the tropospheric NO2VCDs which used FRESCO cloud parameters (v1.04, in particular over heavily polluted areas with low clouds. The difference between SCIAMACHY tropospheric NO2 VCDs v1.1 and ground-based MAXDOAS measurements performed in Cabauw, The Netherlands, during the DANDELIONS campaign is about −2.12×1014molec cm−2.

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.

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;

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.

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

International Nuclear Information System (INIS)

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.

Latitudinal distribution of total ozone and NO[sub 2] over the Atlantic Ocean according to measurements in May 1988

Energy Technology Data Exchange (ETDEWEB)

Elokhov, A.S; Gruzdev, A.N. (Inst. Fiziki Atmosfery, Moscow (Russian Federation))

1992-07-01

Measurements of the total ozone and NO[sub 2] content conducted on board a ship in the 40 deg S - 40 deg N latitudinal belt in the Atlantic Ocean in the second half of May 1988 are reported. The main features of the latitudinal distributions of total ozone and NO[sub 2] are similar. Both distributions have minima in the equatorial zone of the Southern Hemisphere, and both the ozone and NO[sub 2] contents increase from tropical to subtropical latitudes. This increase is the strongest in the subtropical jet stream zone. The fine structure of the studied distributions is also revealed, and its relationship to stratosphere-troposphere exchange processes in the tropopause folding region is discussed. The evening total NO[sub 2] content systematically exceeds that of the morning due to diurnal variations. 20 refs.

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.

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...

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.

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?

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.

Impact of climate change on tropospheric ozone and its global budgets

Directory of Open Access Journals (Sweden)

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

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

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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.

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

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

Directory of Open Access Journals (Sweden)

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

Directory of Open Access Journals (Sweden)

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.;

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.

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.

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.

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.

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

The representation of tropical upper tropospheric water in EC Earth V2

Energy Technology Data Exchange (ETDEWEB)

Johnston, M.S. [Chalmers University of Technology, Department of Earth and Space Sciences, Goeteburg (Sweden); Swedish Meteorological and Hydrological Institute (SMHI), Norrkoeping (Sweden); Eriksson, P.; Murtagh, D.P. [Chalmers University of Technology, Department of Earth and Space Sciences, Goeteburg (Sweden); Eliasson, S. [Luleaa University of Technology, Department of Computer Science, Electrical and Space Engineering, Kiruna (Sweden); Jones, C.G. [Swedish Meteorological and Hydrological Institute (SMHI), Norrkoeping (Sweden); Forbes, R.M. [ECMWF, Reading, Berkshire (United Kingdom)

2012-12-15

Tropical upper tropospheric humidity, clouds, and ice water content, as well as outgoing longwave radiation (OLR), are evaluated in the climate model EC Earth with the aid of satellite retrievals. The Atmospheric Infrared Sounder and Microwave Limb Sounder together provide good coverage of relative humidity. EC Earth's relative humidity is in fair agreement with these observations. CloudSat and CALIPSO data are combined to provide cloud fractions estimates throughout the altitude region considered (500-100 hPa). EC Earth is found to overestimate the degree of cloud cover above 200 hPa and underestimate it below. Precipitating and non-precipitating EC Earth ice definitions are combined to form a complete ice water content. EC Earth's ice water content is below the uncertainty range of CloudSat above 250 hPa, but can be twice as high as CloudSat's estimate in the melting layer. CERES data show that the model underestimates the impact of clouds on OLR, on average with about 9 W m{sup -2}. Regionally, EC Earth's outgoing longwave radiation can be {proportional_to}20 W m{sup -2} higher than the observation. A comparison to ERA-Interim provides further perspectives on the model's performance. Limitations of the satellite observations are emphasised and their uncertainties are, throughout, considered in the analysis. Evaluating multiple model variables in parallel is a more ambitious approach than is customary. (orig.)

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.

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

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 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.

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

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

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

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

Principal Component Analysis of Chlorophyll Content in Tobacco, Bean and Petunia Plants Exposed to Different Tropospheric Ozone Concentrations

Science.gov (United States)

Borowiak, Klaudia; Zbierska, Janina; Budka, Anna; Kayzer, Dariusz

2014-06-01

Three plant species were assessed in this study - ozone-sensitive and -resistant tobacco, ozone-sensitive petunia and bean. Plants were exposed to ambient air conditions for several weeks in two sites differing in tropospheric ozone concentrations in the growing season of 2009. Every week chlorophyll contents were analysed. Cumulative ozone effects on the chlorophyll content in relation to other meteorological parameters were evaluated using principal component analysis, while the relation between certain days of measurements of the plants were analysed using multivariate analysis of variance. Results revealed variability between plant species response. However, some similarities were noted. Positive relations of all chlorophyll forms to cumulative ozone concentration (AOT 40) were found for all the plant species that were examined. The chlorophyll b/a ratio revealed an opposite position to ozone concentration only in the ozone-resistant tobacco cultivar. In all the plant species the highest average chlorophyll content was noted after the 7th day of the experiment. Afterwards, the plants usually revealed various responses. Ozone-sensitive tobacco revealed decrease of chlorophyll content, and after few weeks of decline again an increase was observed. Probably, due to the accommodation for the stress factor. While during first three weeks relatively high levels of chlorophyll contents were noted in ozone-resistant tobacco. Petunia revealed a slow decrease of chlorophyll content and the lowest values at the end of the experiment. A comparison between the plant species revealed the highest level of chlorophyll contents in ozone-resistant tobacco.

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

Directory of Open Access Journals (Sweden)

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.

(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.

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.

Study of stratosphere-troposphere exchange via 10Be/7Be isotope ratios

International Nuclear Information System (INIS)

Priller, A.; Berger, M.; Golser, R.; Kutschera, W.; Steier, P.; Vockenhuber, C.; Wild, E.M.

2001-01-01

Full text: The present study is part of the European project STACCATO (influence of stratosphere-troposphere exchange in a changing climate on atmospheric transport and oxidation capacity). Stratosphere-troposphere exchange (STE) is one of the key factors controlling the budgets of ozone, water vapor and other substances in both the troposphere and the lower stratosphere. However, its contribution to their ozone budget relative to photo-chemical ozone formation from natural and anthropogenic precursor emissions is still uncertain. An international effort is made to estimate the strength of STE and its impact on tropospheric chemistry. The two cosmogenic radioisotopes of beryllium, 10 Be and 7 Be have very different half-lives of 1.51 Ma and 53.4 d, respectively. The combination of production rates, half-lives and different residence times in the stratosphere and troposphere, respectively, results in 10 Be/ 7 Be isotope ratios which can be used as fingerprints for STE. This ratio helps to give a much improved estimate of STE. However, only few 10 Be measurements exist, because its detection requires the rather elaborate method of accelerator mass spectrometry (AMS). At the AMS facility VERA we are now measuring the 10 Be content of air filters from the high-alpine stations 'Hoher Sonnblick', Austria, and 'Zugspitze', Germany. The TBe content is measured separately by decay counting. In this presentation, we want to describe the method of measuring 10 Be with AMS, and to discuss the results of first 10 Be/ 7 Be ratios. (author)

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

Seasonal patterns of ascorbate in the needles of Scots Pine (Pinus sylvestris L.) trees: Correlation analyses with atmospheric O3 and NO2 gas mixing ratios and meteorological parameters

International Nuclear Information System (INIS)

Haberer, Kristine; Jaeger, Lutz; Rennenberg, Heinz

2006-01-01

In the present field study the role of ascorbate in scavenging the harmful atmospheric trace gases O 3 and NO 2 was examined. For this purpose ascorbate contents were determined in needles of adult Scots pine trees (Pinus sylvestris L.) during three consecutive years. Ascorbate contents were correlated with ambient tropospheric O 3 and NO 2 concentrations and with meteorological parameters. The results showed a strong correlation of atmospheric O 3 but not of atmospheric NO 2 concentrations with the apoplastic content of ascorbate during the seasonal course. Ascorbate contents in needle extracts did not correlate with ambient trace gas concentrations. In the apoplastic space, but not in needle extracts ascorbate contents correlate highly significantly with global radiation. From these results it is assumed that apoplastic ascorbate in Scots pine needles is adapted to the actual atmospheric O 3 concentration to mediate immediate detoxification of O 3 , while the atmospheric O 3 concentration itself is largely dependent on light intensity. - Contents of apoplastic but not symplastic ascorbate correlate significantly with atmospheric ozone concentrations

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.

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

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.

Effect of exposure to O/sub 3/, SO/sub 2/, and NO/sub 2/ upon the lung histamine content of guinea pigs

Energy Technology Data Exchange (ETDEWEB)

Suzuki, T

1969-01-01

Male guinea pigs were exposed to 1 or 4 to 8 ppM O/sub 3/, 10 or 50 ppM SO/sub 2/, or 10 or 80 ppM NO/sub 2/ for 3 hr. Histamine and water content of lungs were measured. Animals exposed to higher concentrations of O/sub 3/ or NO/sub 2/ had edematous lungs. Lungs of those exposed to lower concentrations of O/sub 3/ or NO/sub 2/ also had slightly higher water contents. Lung histamine content and concentration decreased by O/sub 3/ exposure but not by any other treatment. In vitro exposure of lung to O/sub 3/ showed released histamine occurring in the perfusion outflow. Endogenous, cellular, inert histamine evidently was released by O/sub 3/ stimulant. However, the mechanism for NO/sub 2/-caused edema was not revealed, but could be direct action on lung vessels rather than through histamine mediation.

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.

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

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.

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.

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.

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

Does acetone react with HO2 in the upper-troposphere?

Directory of Open Access Journals (Sweden)

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

Validation of real-time zenith tropospheric delay estimation with TOMION software within WAGNSS networks

OpenAIRE

Graffigna, Victoria

2017-01-01

The TOmographic Model of the IONospheric electron content (TOMION) software implements a simultaneous precise geodetic and ionospheric modeling, which can be used to test new approaches for real-time precise GNSS modeling (positioning, ionospheric and tropospheric delays, clock errors, among others). In this work, the software is used to estimate the Zenith Tropospheric Delay (ZTD) emulating real time and its performance is evaluated through a comparative analysis with a built-in GIPSY estima...

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

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

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

Directory of Open Access Journals (Sweden)

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

Directory of Open Access Journals (Sweden)

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

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

Directory of Open Access Journals (Sweden)

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...

Impact of tropospheric scintillation in the Ku/K bands on the communications between two LEO satellites in a radio occultation geometry

DEFF Research Database (Denmark)

Martini, Enrica; Freni, A.; Facheris, L.

2006-01-01

A theoretical analysis of the impact of clear-air tropospheric scintillation on a radio occultation link between two low Earth orbit satellites in K- and Ku-bands is presented, with particular reference to differential approaches for the measure of the total content of water vapor. The troposphere...

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.

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

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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

Nitrogen dioxide column content measurements made from an aircraft between 5 deg and 82 deg N

Energy Technology Data Exchange (ETDEWEB)

Matthews, W A

1984-01-01

In the first two weeks of May 1981, the research jet of the German Aerospace Research Estlablishment (DFVLR) was charted to fly a meridional section between 5 deg and 82 deg N. A scanning filter photometer, developed at the Max-Planck-Institut fuer Aeronomie to measure column content values of atmospheric ozone and nitrogen dioxide, using ultraviolet and visible absorption techniques, constituted part of the experimental payload for this campaign that was called SIMOC. The vertical NO2 column content above the aircraft, flying at approximately 10 km, was found to decrease rapidly from 6.9 x 10 to the 15th molecules/sq cm to 2.5 x 10 to the 15th molecules/sq cm around 50 deg N and then to increase again north of 75 deg N. A sharp rise in the NO2 content was observed south of the subtropical jet but this could possibly be due to the increased depth of the troposphere above the aircraft in these regions. 8 references.

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

(Network for the Detection of Atmospheric Composition Change, http://www.ndacc.org) of the Jungfraujoch International Scientific Station (Swiss Alps, 46.5° N, 8.0° E, 3580m asl). Information content analysis of the retrieved H2O products allows us to produce a long-term trend from 1996 to 2011 for different tropospheric levels. We will compare the annual cycle of tropospheric HDO/H2O ratio profiles with those already produced at other sites (Schneider et al., 2010). We will also focus on the diurnal variability of water vapour to determine a time limit in the inter-comparison of different water vapour measurement techniques. Acknowledgments The University of Liège involvement has primarily been supported by the PRODEX program funded by the Belgian Federal Science Policy Office, Brussels and by the Swiss GAW-CH program. The FRS-FNRS and the Fédération Wallonie-Bruxelles are further acknowledged for observational activities support. We thank the International Foundation High Altitude Research Stations Jungfraujoch and Gornergrat (HFSJG, Bern) for supporting the facilities needed to perform the observations. MUSICA is funded by the European Research Council under the European Community's Seventh Framework Programme (FP7/2007-2013) / ERC Grant agreement n° 256961.

Impact of selected troposphere models on Precise Point Positioning convergence

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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

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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.

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

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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

Consistency of different tropospheric models and mapping functions for precise GNSS processing

Science.gov (United States)

Graffigna, Victoria; Hernández-Pajares, Manuel; García-Rigo, Alberto; Gende, Mauricio

2017-04-01

The TOmographic Model of the IONospheric electron content (TOMION) software implements a simultaneous precise geodetic and ionospheric modeling, which can be used to test new approaches for real-time precise GNSS modeling (positioning, ionospheric and tropospheric delays, clock errors, among others). In this work, the software is used to estimate the Zenith Tropospheric Delay (ZTD) emulating real time and its performance is evaluated through a comparative analysis with a built-in GIPSY estimation and IGS final troposphere product, exemplified in a two-day experiment performed in East Australia. Furthermore, the troposphere mapping function was upgraded from Niell to Vienna approach. On a first scenario, only forward processing was activated and the coordinates of the Wide Area GNSS network were loosely constrained, without fixing the carrier phase ambiguities, for both reference and rover receivers. On a second one, precise point positioning (PPP) was implemented, iterating for a fixed coordinates set for the second day. Comparisons between TOMION, IGS and GIPSY estimates have been performed and for the first one, IGS clocks and orbits were considered. The agreement with GIPSY results seems to be 10 times better than with the IGS final ZTD product, despite having considered IGS products for the computations. Hence, the subsequent analysis was carried out with respect to the GIPSY computations. The estimates show a typical bias of 2cm for the first strategy and of 7mm for PPP, in the worst cases. Moreover, Vienna mapping function showed in general a fairly better agreement than Niell one for both strategies. The RMS values' were found to be around 1cm for all studied situations, with a slightly fitter performance for the Niell one. Further improvement could be achieved for such estimations with coefficients for the Vienna mapping function calculated from raytracing as well as integrating meteorological comparative parameters.

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.

Diurnal variation of tropospheric temperature at a tropical station

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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.

Highly Sensitive ZnO(Ga, In for Sub-ppm Level NO2 Detection: Effect of Indium Content

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Natalia Vorobyeva

2017-06-01

Full Text Available Nanocrystalline ZnO, ZnO(Ga, and ZnO(Ga, In samples with different indium contents were prepared by wet-chemical method and characterized in detail by ICP-MS and XRD methods. Gas sensing properties toward NO2 were studied at 150–450 °C by DC conductance measurements. The optimal temperature for gas sensing experiments was determined. The dependence of the ZnO(Ga, In sensor signal to NO2 at 250 °C correlates with the change of conductivity of the samples. The introduction of indium into the system leads to an increase in the values of the sensor signal in the temperature range T < 250 °C. The investigation of the local sample conductivity by scanning spreading resistance microscopy demonstrates that, at high indium content, the sensor properties are determined by the In–Ga–Zn–O layer that forms on the ZnO surface.

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.

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

Science.gov (United States)

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.

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

Impact of sulfur content regulations of shipping fuel on coastal air quality

Science.gov (United States)

Seyler, André; Wittrock, Folkard; Kattner, Lisa; Mathieu-Üffing, Barbara; Weigelt, Andreas; Peters, Enno; Richter, Andreas; Schmolke, Stefan; Burrows, John P.

2016-04-01

Shipping traffic is a sector that faces an enormous growth rate and contributes substantially to the emissions from the transportation sector, but lacks regulations and controls. Shipping is not enclosed in the Kyoto Protocol. However, the International Maritime Organization (IMO) introduced sufhur limits for marine heavy fuels, nitrogen oxide limits for newly-built ship engines and established Emission Control Areas (ECA) in the North and Baltic Sea as well as around North America with the International Convention for the Prevention of Pollution from Ships (MARPOL 73/78 Annex VI). Recently, on the 1st of January 2015, the allowed sulfur content of marine fuels inside Sulfur Emission Control Areas has been significantly decreased from 1.0% to 0.1%. However, measurements of reactive trace gases and the chemical composition of the marine troposphere along shipping routes are sparse and up to now there is no regular monitoring system available. The project MeSmarT (measurements of shipping emissions in the marine troposphere) is a cooperation between the University of Bremen, the German Federal Maritime and Hydrographic Agency (Bundesamt für Seeschifffahrt und Hydrographie, BSH) and the Helmholtz-Zentrum Geesthacht. This study aims to analyse the influence of shipping emissions on the coastal air quality by evaluating ground-based remote sensing measurements using the MAX-DOAS (Multi AXis Differential Optical Absorption Spectroscopy) technique. Measurements of the atmospheric trace gases nitrogen dioxide (NO2) and sulfur dioxide (SO2) have been carried out in the marine troposphere at the MeSmarT measurement sites in Wedel and on Neuwerk and on-board several ship cruises on the North and Baltic Sea. The capability of two-channel MAX-DOAS systems to do simultaneous measurements in the UV and visible spectral range has been used in the so called "onion-peeling" approach to derive spatial distributions of ship emissions and to analyse the movement of the exhausted

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

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

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).

Summary of photochemical and radiative data used in the LLNL one-dimensional transport-kinetics model of the troposphere and stratosphere: 1982

International Nuclear Information System (INIS)

Connell, P.S.; Wuebbles, D.J.

1983-01-01

This report summarizes the contents and sources of the photochemical and radiative segment of the LLNL one-dimensional transport-kinetics model of the troposphere and stratosphere. Data include the solar flux incident at the top of the atmosphere, absorption spectra for O 2 , O 3 and NO 2 , and effective absorption coefficients for about 40 photolytic processes as functions of wavelength and, in a few cases, temperature and pressure. The current data set represents understanding of atmospheric photochemical processes as of late 1982 and relies largely on NASA Evaluation Number 5 of Chemical Kinetics and Photochemical Data for Use in Stratospheric Modeling, JPL Publication 82-57 (DeMore et al., 1982). Implementation in the model, including the treatment of multiple scattering and cloud cover, is discussed in Wuebbles (1981)

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

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.

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

Science.gov (United States)

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.

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

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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

Conteúdo lipídico e composição de ácidos graxos de microalgas expostas aos gases CO2, SO2 e NO Lipid content and fatty acids composition variation of microalgae exposed to CO2, SO2 and NO

Directory of Open Access Journals (Sweden)

Elisangela Martha Radmann

2008-01-01

Full Text Available The objective of the present work was to verify the lipid content and the fatty acid composition of the microalgae Spirulina sp., Scenedesmus obliquus, Synechococcus nidulans and Chlorella vulgaris cultivated in a medium containing CO2, SO2 and NO. The microalga Scenedesmus obliquus presented the highest lipid content (6.18%. For the other microalgae the lipid content ranged from 4.56 to 5.97%. The major monounsaturated fatty acids content was 66.01% for S. obliquus. The PUFA were obtained in major amount by the microalgae Spirulina sp. (29.37% and S. nidulans (29.54%. The palmitoleic acid was in larger amount, with 41.02% concentration (Spirulina sp..

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

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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

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. �

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.

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

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

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

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

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

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

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 ...

Time-dependent inversion estimates of global biomass-burning CO emissions using Measurement of Pollution in the Troposphere (MOPITT) measurements

NARCIS (Netherlands)

Arellano, A.F.; Kasibhatla, P.S.; Giglio, L.; van der Werf, G.R.; Randerson, J.T; Collatz, G.J.

2006-01-01

We present an inverse-modeling analysis of CO emissions using column CO retrievals from the Measurement of Pollution in the Troposphere (MOPITT) instrument and a global chemical transport model (GEOS-CHEM). We first focus on the information content of MOPITT CO column retrievals in terms of

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

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.

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,...

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

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

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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

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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

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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

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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

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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

Chemical and aerosol characterisation of the troposphere over West Africa during the monsoon period as part of AMMA

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C. E. Reeves

2010-08-01

Full Text Available During June, July and August 2006 five aircraft took part in a campaign over West Africa to observe the aerosol content and chemical composition of the troposphere and lower stratosphere as part of the African Monsoon Multidisciplinary Analysis (AMMA project. These are the first such measurements in this region during the monsoon period. In addition to providing an overview of the tropospheric composition, this paper provides a description of the measurement strategy (flights performed, instrumental payloads, wing-tip to wing-tip comparisons and points to some of the important findings discussed in more detail in other papers in this special issue.

The ozone data exhibits an "S" shaped vertical profile which appears to result from significant losses in the lower troposphere due to rapid deposition to forested areas and photochemical destruction in the moist monsoon air, and convective uplift of ozone-poor air to the upper troposphere. This profile is disturbed, particularly in the south of the region, by the intrusions in the lower and middle troposphere of air from the southern hemisphere impacted by biomass burning. Comparisons with longer term data sets suggest the impact of these intrusions on West Africa in 2006 was greater than in other recent wet seasons. There is evidence for net photochemical production of ozone in these biomass burning plumes as well as in urban plumes, in particular that from Lagos, convective outflow in the upper troposphere and in boundary layer air affected by nitrogen oxide emissions from recently wetted soils. This latter effect, along with enhanced deposition to the forested areas, contributes to a latitudinal gradient of ozone in the lower troposphere. Biogenic volatile organic compounds are also important in defining the composition both for the boundary layer and upper tropospheric convective outflow.

Mineral dust was found to be the most abundant and ubiquitous aerosol type in the

New Particle Formation in the Mid-Latitude Upper Troposphere

Science.gov (United States)

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

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

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.

The benefit of limb cloud imaging for infrared limb sounding of tropospheric trace gases

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G. Heinemann

2009-06-01

Full Text Available Advances in detector technology enable a new generation of infrared limb sounders to measure 2-D images of the atmosphere. A proposed limb cloud imager (LCI mode will detect clouds with a spatial resolution unprecedented for limb sounding. For the inference of temperature and trace gas distributions, detector pixels of the LCI have to be combined into super-pixels which provide the required signal-to-noise and information content for the retrievals. This study examines the extent to which tropospheric coverage can be improved in comparison to limb sounding using a fixed field of view with the size of the super-pixels, as in conventional limb sounders. The study is based on cloud topographies derived from (a IR brightness temperatures (BT of geostationary weather satellites in conjunction with ECMWF temperature profiles and (b ice and liquid water content data of the Consortium for Small-scale Modeling-Europe (COSMO-EU of the German Weather Service. Limb cloud images are simulated by matching the cloud topography with the limb sounding line of sight (LOS. The analysis of the BT data shows that the reduction of the spatial sampling along the track has hardly any effect on the gain in information. The comparison between BT and COSMO-EU data identifies the strength of both data sets, which are the representation of the horizontal cloud extent for the BT data and the reproduction of the cloud amount for the COSMO-EU data. The results of the analysis of both data sets show the great advantage of the cloud imager. However, because both cloud data sets do not present the complete fine structure of the real cloud fields in the atmosphere it is assumed that the results tend to underestimate the increase in information. In conclusion, real measurements by such an instrument may result in an even higher benefit for tropospheric limb retrievals.

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

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

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.

Atmospheric transport of persistent semi-volatile organic chemicals to the Arctic and cold condensation in the mid-troposphere – Part 1: 2-D modeling in mean atmosphere

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J. Ma

2010-08-01

Full Text Available In the first part of this study for revisiting the cold condensation effect on global distribution of semi-volatile organic chemicals (SVOCs, the atmospheric transport of SVOCs to the Arctic in the mid-troposphere in a mean meridional atmospheric circulation over the Northern Hemisphere was simulated by a two-dimensional (2-D atmospheric transport model. Results show that under the mean meridional atmospheric circulation the long-range atmospheric transport of SVOCs from warm latitudes to the Arctic occurs primarily in the mid-troposphere. Although major sources are in low and mid-latitude soils, the modeled air concentration of SVOCs in the mid-troposphere is of the same order as or higher than that near the surface, demonstrating that the mid-troposphere is an important pathway and reservoir of SVOCs. The cold condensation of the chemicals is also likely to take place in the mid-troposphere over a source region of SVOCs in warm low latitudes through interacting with clouds. We demonstrate that the temperature dependent vapour pressure and atmospheric degradation rate of SVOCs exhibit similarities between lower atmosphere over the Arctic and the mid-troposphere over a tropical region. Frequent occurrence of atmospheric ascending motion and convection over warm latitudes carry the chemicals to a higher altitude where some of these chemicals may partition onto solid or aqueous phase through interaction with atmospheric aerosols, cloud water droplets and ice particles, and become more persistent at lower temperatures. Stronger winds in the mid-troposphere then convey solid and aqueous phase chemicals to the Arctic where they sink by large-scale descending motion and wet deposition. Using calculated water droplet-air partitioning coefficient of several persistent organic semi-volatile chemicals under a mean air temperature profile from the equator to the North Pole we propose that clouds are likely important sorbing media for SVOCs and pathway of

On the relationship between tropospheric conditions and widespread hot days in Iran

Science.gov (United States)

Asakereh, Hossein; Shadman, Hassan

2018-01-01

The present study investigated how the tropospheric conditions relate to the occurrence of widespread hot days (WHD) in Iran using the data of maximum daily temperature and other tropospheric variables. To better understand the tropospheric conditions during WHD, different patterns of tropospheric circulation were examined systematically. Four tropospheric types were identified based on sea level pressure (SLP). SLP, 500 hPa height, anomaly patterns, and warm advection maps were constructed for typical days of each group. The tropospheric conditions associated with hot days occurred simultaneously with a low-pressure system at sea level, a ridge at middle troposphere over Iran, and a pronounced trough over the Mediterranean Sea at 500 hPa. These conditions caused air mass from subtropical regions toward Iran. That is, northward, northeastward, and even eastward winds injected heat with warm origins toward the country. Hot days compounded by drought conditions have affected many parts of the country in different ways such as decrease in the agricultural products in numerous areas and significant discharge reduction in many rivers. The society is also very likely to face considerable challenges to cope with hot days. The findings of the study can be utilized in climate modeling and climate prediction of hot days in the country. Accordingly, water and electricity consumption can be planned with further precision and water consumption can be managed in crises.

Measurements of total and tropospheric ozone from IASI: comparison with correlative satellite, ground-based and ozonesonde observations

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A. Boynard

2009-08-01

Full Text Available In this paper, we present measurements of total and tropospheric ozone, retrieved from infrared radiance spectra recorded by the Infrared Atmospheric Sounding Interferometer (IASI, which was launched on board the MetOp-A European satellite in October 2006. We compare IASI total ozone columns to Global Ozone Monitoring Experiment-2 (GOME-2 observations and ground-based measurements from the Dobson and Brewer network for one full year of observations (2008. The IASI total ozone columns are shown to be in good agreement with both GOME-2 and ground-based data, with correlation coefficients of about 0.9 and 0.85, respectively. On average, IASI ozone retrievals exhibit a positive bias of about 9 DU (3.3% compared to both GOME-2 and ground-based measurements. In addition to total ozone columns, the good spectral resolution of IASI enables the retrieval of tropospheric ozone concentrations. Comparisons of IASI tropospheric columns to 490 collocated ozone soundings available from several stations around the globe have been performed for the period of June 2007–August 2008. IASI tropospheric ozone columns compare well with sonde observations, with correlation coefficients of 0.95 and 0.77 for the [surface–6 km] and [surface–12 km] partial columns, respectively. IASI retrievals tend to overestimate the tropospheric ozone columns in comparison with ozonesonde measurements. Positive average biases of 0.15 DU (1.2% and 3 DU (11% are found for the [surface–6 km] and for the [surface–12 km] partial columns respectively.

Southern Hemisphere Additional Ozonesondes (SHADOZ) Ozone Climatology (2005-2009): Tropospheric and Tropical Tropopause Layer (TTL) Profiles with Comparisons to Omi-based Ozone Products

Science.gov (United States)

Thompson, Anne M.; Miller, Sonya K.; Tilmes, Simone; Kollonige, Debra W.; Witte, Jacquelyn C.; Oltmans, Samuel J.; Johnson, Brian J.; Fujiwara, Masatomo; Schmidlin, F. J.; Coetzee, G. J. R.;

Stratosphere-troposphere exchange in a summertime extratropical low: analysis

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J. Brioude

2006-01-01

Full Text Available Ozone and carbon monoxide measurements sampled during two commercial flights in airstreams of a summertime midlatitude cyclone are analysed with a Lagrangian-based study (backward trajectories and a Reverse Domain Filling technique to gain a comprehensive understanding of transport effects on trace gas distributions. The study demonstrates that summertime cyclones can be associated with deep stratosphere-troposphere transport. A tropopause fold is sampled twice in its life cycle, once in the lower troposphere (O3≃100 ppbv; CO≃90 ppbv in the dry airstream of the cyclone, and again in the upper troposphere (O3≃200 ppbv; CO≃90 ppbv on the northern side of the large scale potential vorticity feature associated with baroclinic development. In agreement with the maritime development of the cyclone, the chemical composition of the anticyclonic portion of the warm conveyor belt outflow (O3≃40 ppbv; CO≃85 ppbv corresponds to the lowest mixing ratios of both ozone and carbon monoxide in the upper tropospheric airborne observations. The uncertain degree of confidence of the Lagrangian-based technique applied to a 100 km segment of upper level airborne observations with high ozone (200 ppbv and relatively low CO (80 ppbv observed northwest of the cyclone prevents identification of the ozone enrichment process of air parcels embedded in the cyclonic part of the upper level outflow of the warm conveyor belt. Different hypotheses of stratosphere-troposphere exchange are discussed.

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

Science.gov (United States)

Schneider, M.; Barthlott, S.; Hase, F.; González, Y.; Yoshimura, K.; García, O. E.; Sepúlveda, E.; Gomez-Pelaez, A.; Gisi, M.; Kohlhepp, R.; Dohe, S.; Blumenstock, T.; Wiegele, A.; Christner, E.; Strong, K.; Weaver, D.; Palm, M.; Deutscher, N. M.; Warneke, T.; Notholt, J.; Lejeune, B.; Demoulin, P.; Jones, N.; Griffith, D. W. T.; Smale, D.; Robinson, J.

2012-12-01

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.

Re-evaluating the NO 2 hotspot over the South African Highveld

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Alexandra S.M. Lourens

2012-10-01

Full Text Available Globally, numerous pollution hotspots have been identified using satellite-based instruments. One of these hotspots is the prominent NO2hotspot over the South African Highveld. The tropospheric NO2column density of this area is comparable to that observed for central and northern Europe, eastern North America and south-east Asia. The most well-known pollution source in this area is a large array of coal-fired power stations. Upon closer inspection, long-term means of satellite observations also show a smaller area, approximately 100 km west of the Highveld hotspot, with a seemingly less substantial NO2column density. This area correlates with the geographical location of the Johannesburg–Pretoria conurbation or megacity, one of the 40 largest metropolitan areas in the world. Ground-based measurements indicate that NO2concentrations in the megacity have diurnal peaks in the early morning and late afternoon, which coincide with peak traffic hours and domestic combustion. During these times, NO2concentrations in the megacity are higher than those in the Highveld hotspot. These diurnal NO2 peaks in the megacity have generally been overlooked by satellite observations because the satellites have fixed local overpass times that do not coincide with these peak periods. Consequently, the importance of NO2 over the megacity has been underestimated. We examined the diurnal cycles of NO2 ground-based measurements for the two areas – the megacity and the Highveld hotspot – and compared them with the satellite-based NO2 observations. Results show that the Highveld hotspot is accompanied by a second hotspot over the megacity, which is of significance for the more than 10 million people living in this megacity.

Global 3-D modeling of atmospheric ozone in the free troposphere and the stratosphere with emphasis on midlatitude regions. Final report

Energy Technology Data Exchange (ETDEWEB)

Brasseur, G.; Tie, X.; Walters, S.

1999-03-01

The authors have used several global chemical/transport models (1) to study the contribution of various physical, chemical, and dynamical processes to the budget of mid-latitude ozone in the stratosphere and troposphere; (2) to analyze the potential mechanisms which are responsible for the observed ozone perturbations at mid-latitudes of the lower stratosphere and in the upper troposphere; (3) to calculate potential changes in atmospheric ozone response to anthropogenic changes (e.g., emission of industrially manufactured CFCs, CO, and NO{sub x}) and to natural perturbations (e.g., volcanic eruptions and biomass burning); and (4) to estimate the impact of these changes on the radiative forcing to the climate system and on the level of UV-B radiation at the surface.

The Impact of Upper Tropospheric Humidity from Microwave Limb Sounder on the Midlatitude Greenhouse Effect

Science.gov (United States)

Hu, Hua; Liu, W. Timothy

1998-01-01

This paper presents an analysis of upper tropospheric humidity, as measured by the Microwave Limb Sounder, and the impact of the humidity on the greenhouse effect in the midlatitudes. Enhanced upper tropospheric humidity and an enhanced greenhouse effect occur over the storm tracks in the North Pacific and North Atlantic. In these areas, strong baroclinic activity and the large number of deep convective clouds transport more water vapor to the upper troposphere, and hence increase greenhouse trapping. The greenhouse effect increases with upper tropospheric humidity in areas with a moist upper troposphere (such as areas over storm tracks), but it is not sensitive to changes in upper tropospheric humidity in regions with a dry upper troposphere, clearly demonstrating that there are different mechanisms controlling the geographical distribution of the greenhouse effect in the midlatitudes.

Multi-station synthesis of early twentieth century surface atmospheric electricity measurements for upper tropospheric properties

Directory of Open Access Journals (Sweden)

R. G. Harrison

2007-07-01

Full Text Available The vertical columnar current density in the global atmospheric electrical circuit depends on the local columnar resistance. A simple model for the columnar resistance is suggested, which separates the local boundary layer component from the upper troposphere cosmic ray component, and calculates the boundary layer component from a surface measurement of air conductivity. This theory is shown to provide reasonable agreement with observations. One application of the simple columnar model theory is to provide a basis for the synthesis of surface atmospheric electrical measurements made simultaneously at several European sites. Assuming the ionospheric potential to be common above all the sites, the theoretical air-earth current density present in the absence of a boundary layer columnar resistance can be found by extrapolation. This is denoted the free troposphere limit air-earth current density, J₀. Using early surface data from 1909 when no ionospheric potential data are available for corroboration, J₀ is found to be ~6 pA m⁻², although this is subject to uncertainties in the data and limitations in the theory. Later (1966–1971 European balloon and surface data give J₀=2.4 pA m⁻².

Effect of MgSO4 on the contents of Ca2+ in brain cell and NO in brain tissue of rats with radiation-induced acute brain injury

International Nuclear Information System (INIS)

Yuan Wenjia; Cui Fengmei; Liu Ping; He Chao; Tu Yu; Wang Lili

2009-01-01

The work is to explore the protection of magnesium sulfate(MgSO 4 ) on radiation-induced acute brain injury. Thirty six mature Sprague-Dawley(SD) rats were randomly divided into 3 groups of control, experimental control and experimental therapy group. The whole brains of SD rats of experimental control and experimental therapy group were irradiated with a dose of 20 Gy using 6 MeV electron beam. MgSO 4 was injected into the abdomen of experimental therapy rats group 1 day before, immediately and continue for 5 days after irradiation respectively. The brain tissues were taken on 3, 10, 17 and 24 d after irradiation. Ca 2+ content in brain cell was measured by laser scanning confocal microscopy, and the NO content in brain tissue was detected by the method of nitric acid reductase. Compared with the blank control group, the contents of Ca 2+ in brain cell and NO in brain tissue of the experimental control group increase (P 4 used in early stage can inhibit the contents of Ca 2+ in brain cell and NO in brain tissue after radiation-induced acute brain injury. It means that MgSO 4 has a protective effect on radiation-induced acute brain injury. (authors)

How does Interactive Chemistry Influence the Representation of Stratosphere-Troposphere Coupling in a Climate Model?

Science.gov (United States)

Haase, S.; Matthes, K. B.

2017-12-01

Changes in stratospheric ozone can trigger tropospheric circulation changes. In the Southern hemisphere (SH), the observed shift of the Southern Annular Mode was attributed to the observed trend in lower stratospheric ozone. In the Northern Hemisphere (NH), a recent study showed that extremely low stratospheric ozone conditions during spring produce robust anomalies in the troposphere (zonal wind, temperature and precipitation). This could only be reproduced in a coupled chemistry climate model indicating that chemical-dynamical feedbacks are also important on the NH. To further investigate the importance of interactive chemistry for surface climate, we conducted a set of experiments using NCAR's Community Earth System Model (CESM1) with the Whole Atmosphere Community Climate Model (WACCM) as the atmosphere component. WACCM contains a fully interactive stratospheric chemistry module in its standard configuration. It also allows for an alternative configuration, referred to as SC-WACCM, in which the chemistry (O3, NO, O, O2, CO2 and chemical and shortwave heating rates) is specified as a 2D field in the radiation code. A comparison of the interactive vs. the specified chemistry version enables us to evaluate the relative importance of interactive chemistry by systematically inhibiting the feedbacks between chemistry and dynamics. To diminish the effect of temporal interpolation when prescribing ozone, we use daily resolved zonal mean ozone fields for the specified chemistry run. Here, we investigate the differences in stratosphere-troposphere coupling between the interactive and specified chemistry simulations for the mainly chemically driven SH as well as for the mainly dynamically driven NH. We will especially consider years that are characterized by extremely low stratospheric ozone on the one hand and by large dynamical disturbances, i.e. Sudden Stratospheric Warmings, on the other hand.

Interpretation of TOMS Observations of Tropical Tropospheric Ozone with a Global Model and In Situ Observations

Science.gov (United States)

Martin, Randall V.; Jacob, Daniel J.; Logan, Jennifer A.; Bey, Isabelle; Yantosca, Robert M.; Staudt, Amanda C.; Fiore, Arlene M.; Duncan, Bryan N.; Liu, Hongyu; Ginoux, Paul

2004-01-01

We interpret the distribution of tropical tropospheric ozone columns (TTOCs) from the Total Ozone Mapping Spectrometer (TOMS) by using a global three-dimensional model of tropospheric chemistry (GEOS-CHEM) and additional information from in situ observations. The GEOS-CHEM TTOCs capture 44% of the variance of monthly mean TOMS TTOCs from the convective cloud differential method (CCD) with no global bias. Major discrepancies are found over northern Africa and south Asia where the TOMS TTOCs do not capture the seasonal enhancements from biomass burning found in the model and in aircraft observations. A characteristic feature of these northern topical enhancements, in contrast to southern tropical enhancements, is that they are driven by the lower troposphere where the sensitivity of TOMS is poor due to Rayleigh scattering. We develop an efficiency correction to the TOMS retrieval algorithm that accounts for the variability of ozone in the lower troposphere. This efficiency correction increases TTOC's over biomass burning regions by 3-5 Dobson units (DU) and decreases them by 2-5 DU over oceanic regions, improving the agreement between CCD TTOCs and in situ observations. Applying the correction to CCD TTOCs reduces by approximately DU the magnitude of the "tropical Atlantic paradox" [Thompson et al, 2000], i.e. the presence of a TTOC enhancement over the southern tropical Atlantic during the northern African biomass burning season in December-February. We reproduce the remainder of the paradox in the model and explain it by the combination of upper tropospheric ozone production from lightning NOx, peristent subsidence over the southern tropical Atlantic as part of the Walker circulation, and cross-equatorial transport of upper tropospheric ozone from northern midlatitudes in the African "westerly duct." These processes in the model can also account for the observed 13-17 DU persistent wave-1 pattern in TTOCs with a maximum above the tropical Atlantic and a minimum

A grid-based tropospheric product for China using a GNSS network

Science.gov (United States)

Zhang, Hongxing; Yuan, Yunbin; Li, Wei; Zhang, Baocheng; Ou, Jikun

2017-11-01

Tropospheric delay accounts for one source of error in global navigation satellite systems (GNSS). To better characterize the tropospheric delays in the temporal and spatial domain and facilitate the safety-critical use of GNSS across China, a method is proposed to generate a grid-based tropospheric product (GTP) using the GNSS network with an empirical tropospheric model, known as IGGtrop. The prototype system generates the GTPs in post-processing and real-time modes and is based on the undifferenced and uncombined precise point positioning (UU-PPP) technique. GTPs are constructed for a grid form (2.0{°}× 2.5{°} latitude-longitude) over China with a time resolution of 5 min. The real-time GTP messages are encoded in a self-defined RTCM3 format and broadcast to users using NTRIP (networked transport of RTCM via internet protocol), which enables efficient and safe transmission to real-time users. Our approach for GTP generation consists of three sequential steps. In the first step, GNSS-derived zenith tropospheric delays (ZTDs) for a network of GNSS stations are estimated using UU-PPP. In the second step, vertical adjustments for the GNSS-derived ZTDs are applied to address the height differences between the GNSS stations and grid points. The ZTD height corrections are provided by the IGGtrop model. Finally, an inverse distance weighting method is used to interpolate the GNSS-derived ZTDs from the surrounding GNSS stations to the location of the grid point. A total of 210 global positioning system (GPS) stations from the crustal movement observation network of China are used to generate the GTPs in both post-processing and real-time modes. The accuracies of the GTPs are assessed against with ERA-Interim-derived ZTDs and the GPS-derived ZTDs at 12 test GPS stations, respectively. The results show that the post-processing and real-time GTPs can provide the ZTDs with accuracies of 1.4 and 1.8 cm, respectively. We also apply the GTPs in real-time kinematic GPS PPP

Effects of anthropogenic emissions on tropospheric ozone and its radiative forcing

Energy Technology Data Exchange (ETDEWEB)

Berntsen, T.; Isaksen, I.S.A.; Fuglestvedt, J.S.; Myhre, G.; Larsen, T. Alsvik; Stordal, F.; Freckleton, R.S.; Shine, K.P.

1997-12-31

As described in this report, changes in tropospheric ozone since pre-industrial times due to changes in emissions have been calculated by the University of Oslo global three-dimensional photochemical model. The radiative forcing caused by the increase in ozone has been calculated by means of two independent radiative transfer models: the University of Reading model (Reading), and the University of Oslo/Norwegian Institute for Air Research model (OsloRad). Significant increases in upper tropospheric ozone concentrations are found at northern mid-latitudes at about 10 km altitude. In the tropical regions the largest increase is found at about 15 km altitude. The increase is found to be caused mainly by enhanced in situ production due to transport of precursors from the boundary layer, with a smaller contribution from increased transport of ozone produced in the boundary layer. The lifetime of ozone in the troposphere decreased by about 35% as a result of enhanced concentrations of HO{sub 2}. The calculated increase in surface ozone in Europe is in good agreement with observations. The calculations of radiative forcing include the effect of clouds and allow for thermal adjustment in the stratosphere. The global and annual averaged radiative forcing at the tropopause from both models are in the lower part of the Intergovernmental Panel on Climate Change estimated range. The calculated radiative forcing is similar in magnitude to the negative radiative forcing by sulfate aerosols, but displaced southward in source regions at northern mid-latitudes. The increase in tropospheric ozone is calculated to have cooled the lower stratosphere by up to 0.9 K, with possibly half of this cooling occurring in the past 2 to 3 decades. 76 refs., 16 figs., 9 tabs.

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

Directory of Open Access Journals (Sweden)

Y. Liu

2018-02-01

Full Text Available 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

Effect of tropospheric models on derived precipitable water vapor over Southeast Asia

Science.gov (United States)

Rahimi, Zhoobin; Mohd Shafri, Helmi Zulhaidi; Othman, Faridah; Norman, Masayu

2017-05-01

An interesting subject in the field of GPS technology is estimating variation of precipitable water vapor (PWV). This estimation can be used as a data source to assess and monitor rapid changes in meteorological conditions. So far, numerous GPS stations are distributed across the world and the number of GPS networks is increasing. Despite these developments, a challenging aspect of estimating PWV through GPS networks is the need of tropospheric parameters such as temperature, pressure, and relative humidity (Liu et al., 2015). To estimate the tropospheric parameters, global pressure temperature (GPT) model developed by Boehm et al. (2007) is widely used in geodetic analysis for GPS observations. To improve the accuracy, Lagler et al. (2013) introduced GPT2 model by adding annual and semi-annual variation effects to GPT model. Furthermore, Boehm et al. (2015) proposed the GPT2 wet (GPT2w) model which uses water vapor pressure to improve the calculations. The global accuracy of GPT2 and GPT2w models has been evaluated by previous researches (Fund et al., 2011; Munekane and Boehm, 2010); however, investigations to assess the accuracy of global tropospheric models in tropical regions such as Southeast Asia is not sufficient. This study tests and examines the accuracy of GPT2w as one of the most recent versions of tropospheric models (Boehm et al., 2015). We developed a new regional model called Malaysian Pressure Temperature (MPT) model, and compared this model with GPT2w model. The compared results at one international GNSS service (IGS) station located in the south of Peninsula Malaysia shows that MPT model has a better performance than GPT2w model to produce PWV during monsoon season. According to the results, MPT has improved the accuracy of estimated pressure and temperature by 30% and 10%, respectively, in comparison with GPT2w model. These results indicate that MPT model can be a good alternative tool in the absence of meteorological sensors at GPS stations in

The detection of post-monsoon tropospheric ozone variability over south Asia using IASI data

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B. Barret

2011-09-01

Full Text Available The ozone (O₃ variability over south Asia during the 2008 post-monsoon season has been assessed using measurements from the MetOP-A/IASI instrument and O₃ profiles retrieved with the SOftware for a Fast Retrieval of IASI Data (SOFRID. The information content study and error analyses carried out in this paper show that IASI Level 1 data can be used to retrieve tropospheric O₃ columns (TOC, surface-225 hPa and UTLS columns (225–70 hPa with errors smaller than 20%. Validation with global radiosonde O₃ profiles obtained during a period of 6 months show the excellent agreement between IASI and radiosonde for the UTLS with correlation coefficient R > 0.91 and good agreement in the troposphere with correlation coefficient R > 0.74. For both the UTLS and the troposphere Relative Standard Deviations (RSD are lower than 23%. Comparison with in-situ measurements from the MOZAIC program around Hyderabad demonstrates that IASI is able to capture the TOC inter and intra-seasonal variability in central India. Nevertheless, the agreement is mitigated by the fact that the smoothing of the true O₃ profiles by the retrieval results in a reduction of the TOC variability detected by IASI relative to the variability observed by in situ instruments. The post-monsoon temporal variability of the vertical profile of O₃ around Hyderabad has been investigated with MOZAIC observations. These observations from airborne instruments show that tropospheric O₃ is steadily elevated during most of the studied period with the exception of two sharp drops following the crossing of tropical storms over India. Lagrangian simulations with the FLEXPART model indicate that elevated O₃ concentrations in the middle troposphere near Hyderabad are associated with the transport of UTLS air-masses that have followed the Subtropical Westerly Jet (SWJ and subsided over northern India together

Tropospheric O3 compromises net primary production in young stands of trembling aspen, paper birch and sugar maple in response to elevated atmospheric CO2

Science.gov (United States)

John S. King; Mark E. Kubiske; Kurt S. Pregitzer; George R. Hendrey; Evan P. McDonald; Christian P. Giardina; Vanessa S. Quinn; David F. Karnosky

2005-01-01

Concentrations of atmospheric CO2 and tropospheric ozone (O3) are rising concurrently in the atmosphere, with potentially antagonistic effects on forest net primary production (NPP) and implications for terrestrial carbon sequestration. Using free-air CO2 enrichment (FACE) technology, we exposed north...

Analysing the Zenith Tropospheric Delay Estimates in On-line Precise Point Positioning (PPP) Services and PPP Software Packages.

Science.gov (United States)

Mendez Astudillo, Jorge; Lau, Lawrence; Tang, Yu-Ting; Moore, Terry

2018-02-14

As Global Navigation Satellite System (GNSS) signals travel through the troposphere, a tropospheric delay occurs due to a change in the refractive index of the medium. The Precise Point Positioning (PPP) technique can achieve centimeter/millimeter positioning accuracy with only one GNSS receiver. The Zenith Tropospheric Delay (ZTD) is estimated alongside with the position unknowns in PPP. Estimated ZTD can be very useful for meteorological applications, an example is the estimation of water vapor content in the atmosphere from the estimated ZTD. PPP is implemented with different algorithms and models in online services and software packages. In this study, a performance assessment with analysis of ZTD estimates from three PPP online services and three software packages is presented. The main contribution of this paper is to show the accuracy of ZTD estimation achievable in PPP. The analysis also provides the GNSS users and researchers the insight of the processing algorithm dependence and impact on PPP ZTD estimation. Observation data of eight whole days from a total of nine International GNSS Service (IGS) tracking stations spread in the northern hemisphere, the equatorial region and the southern hemisphere is used in this analysis. The PPP ZTD estimates are compared with the ZTD obtained from the IGS tropospheric product of the same days. The estimates of two of the three online PPP services show good agreement (<1 cm) with the IGS ZTD values at the northern and southern hemisphere stations. The results also show that the online PPP services perform better than the selected PPP software packages at all stations.

Analysing the Zenith Tropospheric Delay Estimates in On-line Precise Point Positioning (PPP Services and PPP Software Packages

Directory of Open Access Journals (Sweden)

Jorge Mendez Astudillo

2018-02-01

Full Text Available As Global Navigation Satellite System (GNSS signals travel through the troposphere, a tropospheric delay occurs due to a change in the refractive index of the medium. The Precise Point Positioning (PPP technique can achieve centimeter/millimeter positioning accuracy with only one GNSS receiver. The Zenith Tropospheric Delay (ZTD is estimated alongside with the position unknowns in PPP. Estimated ZTD can be very useful for meteorological applications, an example is the estimation of water vapor content in the atmosphere from the estimated ZTD. PPP is implemented with different algorithms and models in online services and software packages. In this study, a performance assessment with analysis of ZTD estimates from three PPP online services and three software packages is presented. The main contribution of this paper is to show the accuracy of ZTD estimation achievable in PPP. The analysis also provides the GNSS users and researchers the insight of the processing algorithm dependence and impact on PPP ZTD estimation. Observation data of eight whole days from a total of nine International GNSS Service (IGS tracking stations spread in the northern hemisphere, the equatorial region and the southern hemisphere is used in this analysis. The PPP ZTD estimates are compared with the ZTD obtained from the IGS tropospheric product of the same days. The estimates of two of the three online PPP services show good agreement (<1 cm with the IGS ZTD values at the northern and southern hemisphere stations. The results also show that the online PPP services perform better than the selected PPP software packages at all stations.

OMI/Aura Nitrogen Dioxide (NO2) Total and Tropospheric Column 1-orbit L2 Swath 13x24 km V003

Data.gov (United States)

National Aeronautics and Space Administration — The second release of collection 3 OMI/Aura Level-2 NO2 data product OMNO2 is now available (http://disc.gsfc.nasa.gov/Aura/OMI/omno2_v003.shtml ) to public and...

Relationship between surface, free tropospheric and total column ozone in 2 contrasting areas in South-Africa

CSIR Research Space (South Africa)

Combrink, J

1995-04-01

Full Text Available Measurements of surface ozone in two contrasting areas of South Africa are compared with free tropospheric and Total Ozone Mapping Spectrometer (TOMS) total column ozone data. Cape Point is representative of a background monitoring station which...

Estimating Western U.S. Oil & Gas Emissions with OMI NO2 Data

Science.gov (United States)

Clifton, O. E.; Holloway, T.; Oberman, J.

2012-12-01

In the last ten years, there has been a steep increase in the number natural gas and oil extraction facilities in the United States due to hydraulic fracturing ("fracking"). Each facility requires a large range of equipment, such as drilling rigs, compressor engines, heaters, and pneumatic devices. These activities can lead to elevated nitrogen dioxide (NO2) emissions in rural areas, often in regions without routine NO2 surface monitoring. Furthermore, permitting rules vary from state to state, and many new extraction facilities are unpermitted and exact emissions unknown. On April 18, 2012, the EPA announced air pollution standards for volatile organic compounds (VOCs) emissions from the oil and gas industry. Until 2015, when these standards must be in effect, NOx (NO2 + NO) will continue to react with VOCs to form unhealthy levels of tropospheric ozone in regions with heavy use of hydraulic fracturing. In order to identify areas of elevated NO2 emissions and constrain associated on-road and off-road sources in areas with prominent shale basins and known drilling, we employ remote sensing estimates of column NO2 from the Ozone Monitoring Instrument (OMI) aboard NASA's Aura satellite. OMI NO2 is sensitive to the planetary boundary layer and to surface air pollution and thus has high temporal and spatial variation. These Level-2 satellite data are processed with the Wisconsin Horizontal Interpolation Program for Satellites (WHIPS), developed at the University of Wisconsin-Madison. We interpolate the data to allow further ease in mapping change in NO2 associated with drilling, and the quantification of pollution trends attributable to hydraulic-fracturing in the Western U.S. from 2004 to the present.

Decreasing the NO3 and increasing the vitamin C contents in spinach by a nitrogen deprivation method.

Science.gov (United States)

Mozafar, A

1996-02-01

Excessive use of nitrogen fertilizers is known to increase the NO3 and reduce the vitamin C contents in fruits and vegetables. We investigated the concentration of these compounds in spinach leaves when plants were transferred to nitrogen-free media prior to their harvest. It was noted that a pre-harvest transfer of spinach to N-free media reduces the NO3 and increases the vitamin C content of the leaves by a substantial amount in a 2-3 day period. It is suggested that this technique may be suited to produce spinach or other leafy vegetables with low NO3 and high vitamin C contents under commercial hydroponic conditions.

The effects of Southeast Asia fire activities on tropospheric ozone, trace gases and aerosols at a remote site over the Tibetan Plateau of Southwest China

International Nuclear Information System (INIS)

Chan, C.Y.; Wong, K.H.; Li, Y.S.; Chan, L.Y.

2006-01-01

Tropospheric ozone (O 3 ), carbon monoxide (CO), total reactive nitrogen (NO y ) and aerosols (PM 2.5 and PM 10 ) were measured on the southeastern Tibetan Plateau at Tengchong (25.01 deg N, 98.3 deg E, 1960 m a.s.l.) in Southwest China, where observational data is scarce, during a field campaign of the TAPTO-China (Transport of Air Pollutants and Tropospheric O 3 over China) in the spring of 2004. Fire maps derived from satellite data and backward air trajectories were used to trace the source regions and transport pathways of pollution. Ozone, CO, NO y , PM 10 and PM 2.5 had average concentrations of 26 ± 8 ppb, 179 ± 91 ppb, 2.7 ± 1.2 ppb and 34 ± 23 and 28 ± 19 μg/m 3 , respectively. The measured O 3 level is low when compared with those reported for similar longitudinal sites in Southeast (SE) Asia and northeastern Tibetan Plateau in Northwest China suggesting that there exist complex O 3 variations in the Tibetan Plateau and its neighbouring SE Asian region. High levels of pollution with hourly averages of O 3 , CO, NO y , PM 10 and PM 2.5 concentrations up to 59, 678 and 7.7 ppb and 158 and 137 μg/m 3 , respectively, were observed. The increase of pollutants in the lower troposphere was caused by regional built-up and transport of pollution from active fire regions of the SE Asia subcontinent and from northern South Asia. Our results showed that pollution transport from SE Asia and South Asia had relatively stronger impacts than that from Central and South China on the abundance of O 3 , trace gases and aerosols in the background atmosphere of the Tibetan Plateau of Southwest China

Acetone in theGlobal Troposphere: Its Possible Role as a Global Source of PAN

Science.gov (United States)

Singh, H. B.; Kanakidou, M.

1994-01-01

Oxygenated hydrocarbons are thought to be important components of the atmosphere but, with the exception of formaldehyde, very little about their distribution and fate is known. Aircraft measurements of acetone (CH3COCH3), PAN (CH3CO3NO2) and other organic species (e. g. acetaldehyde, methanol and ethanol) have been performed over the Pacific, the southern Atlantic, and the subarctic atmospheres. Sampled areas extended from 0 to 12 km altitude over latitudes of 70 deg N to 40 deg S. All measurements are based on real time in-situ analysis of cryogenically preconcentrated air samples. Substantial concentrations of these oxygenated species (10-2000 ppt) have been observed at all altitudes and geographical locations in the troposphere. Important sources include, emissions from biomass burning, plant and vegetation, secondary oxidation of primary non-methane hydrocarbons, and man-made emissions. Direct measurements within smoke plumes have been used to estimate the biomass burning source. Photochemistry studies are used to suggest that acetone could provide a major source of peroxyacetyl radicals in the atmosphere and play an important role in sequestering reactive nitrogen. Model calculations show that acetone photolysis contributes significantly to PAN formation in the middle and upper troposphere.

Northern Winter Climate Change: Assessment of Uncertainty in CMIP5 Projections Related to Stratosphere-Troposphere Coupling

Science.gov (United States)

Manzini, E.; Karpechko, A.Yu.; Anstey, J.; Shindell, Drew Todd; Baldwin, M.P.; Black, R.X.; Cagnazzo, C.; Calvo, N.; Charlton-Perez, A.; Christiansen, B.;

Combined impacts of nitrous acid and nitryl chloride on lower-tropospheric ozone: new module development in WRF-Chem and application to China

Science.gov (United States)

Zhang, Li; Li, Qinyi; Wang, Tao; Ahmadov, Ravan; Zhang, Qiang; Li, Meng; Lv, Mengyao

2017-08-01

Nitrous acid (HONO) and nitryl chloride (ClNO2) - through their photolysis - can have profound effects on the nitrogen cycle and oxidation capacity of the lower troposphere. Previous numerical studies have separately considered and investigated the sources/processes of these compounds and their roles in the fate of reactive nitrogen and the production of ozone (O3), but their combined impact on the chemistry of the lower part of the troposphere has not been addressed yet. In this study, we updated the WRF-Chem model with the currently known sources and chemistry of HONO and chlorine in a new chemical mechanism (CBMZ_ReNOM), and applied it to a study of the combined effects of HONO and ClNO2 on summertime O3 in the boundary layer over China. We simulated the spatial distributions of HONO, ClNO2, and related compounds at the surface and within the lower troposphere. The results showed that the modeled HONO levels reached up to 800-1800 ppt at the surface (0-30 m) over the North China Plain (NCP), the Yangtze River Delta (YRD), and the Pearl River Delta (PRD) regions and that HONO was concentrated within a 0-200 m layer. In comparison, the simulated surface ClNO2 mixing ratio was around 800-1500 ppt over the NCP, YRD, and central China regions and was predominantly present in a 0-600 m layer. HONO enhanced daytime ROx (OH + HO2 + RO2) and O3 at the surface (0-30 m) by 2.8-4.6 ppt (28-37 %) and 2.9-6.2 ppb (6-13 %), respectively, over the three most developed regions, whereas ClNO2 increased surface O3 in the NCP and YRD regions by 2.4-3.3 ppb (or 5-6 %) and it also had a significant impact (3-6 %) on above-surface O3 within 200-500 m. The combined effects increased surface O3 by 11.5, 13.5, and 13.3 % in the NCP, YRD, and PRD regions, respectively. Over the boundary layer (0-1000 m), the HONO and ClNO2 enhanced O3 by up to 5.1 and 3.2 %, respectively, and their combined effect increased O3 by 7.1-8.9 % in the three regions. The new module noticeably improved O3

The influence of African air pollution on regional and global tropospheric ozone

Directory of Open Access Journals (Sweden)

A. M. Aghedo

2007-01-01

Full Text Available We investigate the influence of African biomass burning, biogenic, lightning and anthropogenic emissions on the tropospheric ozone over Africa and globally using a coupled global chemistry climate model. Our model studies indicate that surface ozone concentration may rise by up to 50 ppbv in the burning region during the biomass burning seasons. Biogenic emissions yield between 5–30 ppbv increase in the near surface ozone concentration over tropical Africa. The impact of lightning on surface ozone is negligible, while anthropogenic emissions yield a maximum of 7 ppbv increase in the annual-mean surface ozone concentration over Nigeria, South Africa and Egypt. Our results show that biogenic emissions are the most important African emission source affecting total tropospheric ozone. The influence of each of the African emissions on the global tropospheric ozone burden (TOB of 384 Tg yields about 9.5 Tg, 19.6 Tg, 9.0 Tg and 4.7 Tg for biomass burning, biogenic, lightning and anthropogenic emissions emitted in Africa respectively. The impact of each of these emission categories on African TOB of 33 Tg is 2.5 Tg, 4.1 Tg, 1.75 Tg and 0.89 Tg respectively, which together represents about 28% of the total TOB calculated over Africa. Our model calculations also suggest that more than 70% of the tropospheric ozone produced by each of the African emissions is found outside the continent, thus exerting a noticeable influence on a large part of the tropical troposphere. Apart from the Atlantic and Indian Ocean, Latin America experiences the largest impact of African emissions, followed by Oceania, the Middle East, Southeast and south-central Asia, northern North America (i.e. the United States and Canada, Europe and north-central Asia, for all the emission categories.

Ozone in the Tropical Troposphere

NARCIS (Netherlands)

Peters, Wouter

2002-01-01

The aim of the research presented here is to acquire knowledge of the past, present, and future composition, stability, sensitivity, and variability of the troposphere. We focus mostly on the tropical regions because it has received little attention so far, measurements here are scarce, and large

Thermodynamic constraint on the depth of the global tropospheric circulation.

Science.gov (United States)

Thompson, David W J; Bony, Sandrine; Li, Ying

2017-08-01

The troposphere is the region of the atmosphere characterized by low static stability, vigorous diabatic mixing, and widespread condensational heating in clouds. Previous research has argued that in the tropics, the upper bound on tropospheric mixing and clouds is constrained by the rapid decrease with height of the saturation water vapor pressure and hence radiative cooling by water vapor in clear-sky regions. Here the authors contend that the same basic physics play a key role in constraining the vertical structure of tropospheric mixing, tropopause temperature, and cloud-top temperature throughout the globe. It is argued that radiative cooling by water vapor plays an important role in governing the depth and amplitude of large-scale dynamics at extratropical latitudes.

Future changes in large-scale transport and stratosphere-troposphere exchange

Science.gov (United States)

Abalos, M.; Randel, W. J.; Kinnison, D. E.; Garcia, R. R.

2017-12-01

Future changes in large-scale transport are investigated in long-term (1955-2099) simulations of the Community Earth System Model - Whole Atmosphere Community Climate Model (CESM-WACCM) under an RCP6.0 climate change scenario. We examine artificial passive tracers in order to isolate transport changes from future changes in emissions and chemical processes. The model suggests enhanced stratosphere-troposphere exchange in both directions (STE), with decreasing tropospheric and increasing stratospheric tracer concentrations in the troposphere. Changes in the different transport processes are evaluated using the Transformed Eulerian Mean continuity equation, including parameterized convective transport. Dynamical changes associated with the rise of the tropopause height are shown to play a crucial role on future transport trends.

Changes in SO2 and NO2 Pollution over the Past Decade Observed by Aura OMI

Science.gov (United States)

Krotkov, N. A.; Li, C.; Lamsal, L. N.; Celarier, E. A.; Marchenko, S. V.; Swartz, W.; Bucsela, E. J.; Fioletov, V.; McLinden, C. A.; Joiner, J.; Bhartia, P. K.; Duncan, B. N.; Dickerson, R. R.

2014-12-01

The Ozone Monitoring Instrument (OMI), a NASA partnership with the Netherlands and Finland, flies on the EOS Aura satellite and uses reflected sunlight to measure two critical atmospheric trace gases, nitrogen dioxide (NO2) and sulfur dioxide (SO2), characterizing daily air quality. Both gases and the secondary pollutants they produce (particulate matter, PM2.5, and tropospheric ozone) are among USEPA designated criteria pollutants, posing serious threats to human health and the environment (e.g., acid rain, plant damage, and reduced visibility). A new generation of the OMI standard SO2 and NO2 products (based on critically improved DOAS spectral fitting for NO2 and innovative Principal Component Analysis method for SO2) provides a valuable dataset for studying anthropogenic pollution on local to global scales. Here we highlight some of the OMI observed long-term changes in air quality over several regions. Over the US, average NO2 and SO2 pollution levels have decreased dramatically as a result of both technological improvements (e.g., catalytic converters on cars) and stricter regulations of emissions. We see continued decline in NO2 and SO2 pollution over Europe. Over China OMI observed a ~ 60% increase in NO2 pollution between 2005 and 2013, despite a temporary reversal of the growing trend due to both 2008 Olympic Games and the economic recession in 2009. Chinese SO2 pollution seems to have stabilized since peaking in 2007, probably due to government efforts to curb SO2 emissions from the power sector. We have also observed large increases in both SO2 and NO2 pollution particularly in Eastern India where a number of new large coal power plants have been built in recent years. We expect that further improvements in the OMI NO2 and SO2 products will allow more robust quantification of long-term trends in local to global air quality.

Upper tropospheric cloud systems determined from IR Sounders and their influence on the atmosphere

Science.gov (United States)

Stubenrauch, Claudia; Protopapadaki, Sofia; Feofilov, Artem; Velasco, Carola Barrientos

2017-02-01

Covering about 30% of the Earth, upper tropospheric clouds play a key role in the climate system by modulating the Earth's energy budget and heat transport. Infrared Sounders reliably identify cirrus down to an IR optical depth of 0.1. Recently LMD has built global cloud climate data records from AIRS and IASI observations, covering the periods from 2003-2015 and 2008-2015, respectively. Upper tropospheric clouds often form mesoscale systems. Their organization and properties are being studied by (1) distinguishing cloud regimes within 2° × 2° regions and (2) applying a spatial composite technique on adjacent cloud pressures, which estimates the horizontal extent of the mesoscale cloud systems. Convective core, cirrus anvil and thin cirrus of these systems are then distinguished by their emissivity. Compared to other studies of tropical mesoscale convective systems our data include also the thinner anvil parts, which make out about 30% of the area of tropical mesoscale convective systems. Once the horizontal and vertical structure of these upper tropospheric cloud systems is known, we can estimate their radiative effects in terms of top of atmosphere and surface radiative fluxes and by computing their heating rates.

Tropospheric ozone and biomass burning in intertropical Africa

International Nuclear Information System (INIS)

Cros, B.; Nganga, D.; Delmas, R.A.; Fontan, J.

1991-01-01

To obtain a better understanding of tropospheric ozone's behavior in the equatorial belt of Africa, surface ozone measurements were made in the northern Congo (forest region) and on the other side of the equator in a savanna area. The data show a seasonal cycle with maximum values during the dry season: January and February in the northern tropics and June to October in the southern ones. Satellite data are needed to explain the eventual disappearance or non-appearance of a maximum of total tropospheric ozone during the northern dry season

Estimation of black carbon content for biomass burning aerosols from multi-channel Raman lidar data

Science.gov (United States)

Talianu, Camelia; Marmureanu, Luminita; Nicolae, Doina

2015-04-01

Biomass burning due to natural processes (forest fires) or anthropical activities (agriculture, thermal power stations, domestic heating) is an important source of aerosols with a high content of carbon components (black carbon and organic carbon). Multi-channel Raman lidars provide information on the spectral dependence of the backscatter and extinction coefficients, embedding information on the black carbon content. Aerosols with a high content of black carbon have large extinction coefficients and small backscatter coefficients (strong absorption), while aerosols with high content of organic carbon have large backscatter coefficients (weak absorption). This paper presents a method based on radiative calculations to estimate the black carbon content of biomass burning aerosols from 3b+2a+1d lidar signals. Data is collected at Magurele, Romania, at the cross-road of air masses coming from Ukraine, Russia and Greece, where burning events are frequent during both cold and hot seasons. Aerosols are transported in the free troposphere, generally in the 2-4 km altitude range, and reaches the lidar location after 2-3 days. Optical data are collected between 2011-2012 by a multi-channel Raman lidar and follows the quality assurance program of EARLINET. Radiative calculations are made with libRadTran, an open source radiative model developed by ESA. Validation of the retrievals is made by comparison to a co-located C-ToF Aerosol Mass Spectrometer. Keywords: Lidar, aerosols, biomass burning, radiative model, black carbon Acknowledgment: This work has been supported by grants of the Romanian National Authority for Scientific Research, Programme for Research- Space Technology and Advanced Research - STAR, project no. 39/2012 - SIAFIM, and by Romanian Partnerships in priority areas PNII implemented with MEN-UEFISCDI support, project no. 309/2014 - MOBBE

Empirical validation and proof of added value of MUSICA's tropospheric δD remote sensing products

Science.gov (United States)

Schneider, M.; González, Y.; Dyroff, C.; Christner, E.; Wiegele, A.; Barthlott, S.; García, O. E.; Sepúlveda, E.; Hase, F.; Andrey, J.; Blumenstock, T.; Guirado, C.; Ramos, R.; Rodríguez, S.

2015-01-01

The project MUSICA (MUlti-platform remote Sensing of Isotopologues for investigating the Cycle of Atmospheric water) integrates tropospheric water vapour isotopologue remote sensing and in situ observations. This paper presents a first empirical validation of MUSICA's H2O and δD remote sensing products, generated from ground-based FTIR (Fourier transform infrared), spectrometer and space-based IASI (infrared atmospheric sounding interferometer) observation. The study is made in the area of the Canary Islands in the subtropical northern Atlantic. As reference we use well calibrated in situ measurements made aboard an aircraft (between 200 and 6800 m a.s.l.) by the dedicated ISOWAT instrument and on the island of Tenerife at two different altitudes (at Izaña, 2370 m a.s.l., and at Teide, 3550 m a.s.l.) by two commercial Picarro L2120-i water isotopologue analysers. The comparison to the ISOWAT profile measurements shows that the remote sensors can well capture the variations in the water vapour isotopologues, and the scatter with respect to the in situ references suggests a δD random uncertainty for the FTIR product of much better than 45‰ in the lower troposphere and of about 15‰ for the middle troposphere. For the middle tropospheric IASI δD product the study suggests a respective uncertainty of about 15‰. In both remote sensing data sets we find a positive δD bias of 30-70‰. Complementing H2O observations with δD data allows moisture transport studies that are not possible with H2O observations alone. We are able to qualitatively demonstrate the added value of the MUSICA δD remote sensing data. We document that the δD-H2O curves obtained from the different in situ and remote sensing data sets (ISOWAT, Picarro at Izaña and Teide, FTIR, and IASI) consistently identify two different moisture transport pathways to the subtropical north eastern Atlantic free troposphere.

Tropospheric Delay from VLBI and GNSS Measurements

Science.gov (United States)

Gubanov, V. S.

2018-02-01

Using an updated version of the QUASAR software package developed at the Institute of Applied Astronomy of the Russian Academy of Sciences, we have processed the VLBI observations within the international CONT14 program (May 6-20, 2014), in which a global network of 17 stations was involved (a total of 250 000 observations). The package update concerned the optimization of data structure and the refinement of stochastic models for the random variations in wet tropospheric delay and atomic clock difference. The main goal of this paper is to compare the VLBI determinations of the tropospheric delay with its independent determinations using global navigation satellite systems (GNSS). We show that both these determinations agree well between themselves only in the case of a global analysis of the VLBI observations, where the VLBI station coordinates are also refined, along with the tropospheric delay and the clock synchronization and Earth orientation parameters. If, alternatively, the station coordinates are insufficiently accurate and are not refined from VLBI observations, then it is appropriate not to determine the tropospheric delay from these observations, but to take it from the publicly accessible independent GNSS data. However, this requires that the VLBI and GNSS techniques operate simultaneously at a common observing site. We have established the shortcomings of the universally accepted method of stabilizing the global solution associated with the absence of a criterion for choosing reference stations and radio sources. Two ways of their elimination are proposed: (i) introducing a coordinated list of weight factors for the errors in the coordinates of such stations and sources into the stabilization algorithm and (ii) adopting a coordinated list of stations and sources the refinement of whose coordinates is not required at all for a certain time.

Tropospheric Ozone and Photochemical Smog

Science.gov (United States)

Sillman, S.

2003-12-01

emitted species, in a process that is driven by sunlight and is accelerated by warm temperatures. This smog is largely the product of gasoline-powered engines (especially automobiles), although coal-fired industry can also generate photochemical smog. The process of photochemical smog formation was first identified by Haagen-Smit and Fox (1954) in association with Los Angeles, a city whose geography makes it particularly susceptible to this type of smog formation. Sulfate aerosols and organic particulates are often produced concurrently with ozone, giving rise to a characteristic milky-white haze associated with this type of air pollution.Today ozone and particulates are recognized as the air pollutants that are most likely to affect human health adversely. In the United States, most major metropolitan areas have periodic air pollution events with ozone in excess of government health standards. Violations of local health standards also occur in major cities in Canada and in much of Europe. Other cities around the world (especially Mexico City) also experience very high ozone levels. In addition to urban-scale events, elevated ozone occurs in region-wide events in the eastern USA and in Western Europe, with excess ozone extending over areas of 1,000 km2 or more. Ozone plumes of similar extent are found in the tropics (especially in Central Africa) at times of high biomass burning (e.g., Jenkins et al., 1997; Chatfield et al., 1998). In some cases ozone associated with biomass burning has been identified at distances up to 104 km from its sources (Schultz et al., 1999).Ozone also has a significant impact on the global troposphere, and ozone chemistry is a major component of global tropospheric chemistry. Global background ozone concentrations are much lower than urban or regional concentrations during pollution events, but there is evidence that the global background has increased as a result of human activities (e.g., Wang and Jacob, 1998; Volz and Kley, 1988). A rise in

What You Need to Know About the OMI NO2 Data Product for Air Quality Studies

Science.gov (United States)

Celarier, E. A.; Gleason, J. F.; Bucsela, E. J.; Brinksma, E.; Veefkind, J. P.

2007-01-01

The standard nitrogen dioxide (NO2) data product, produced from measurements by the Ozone Monitoring Instrument (OMI), are publicly available online from the NASA GESDISC facility. Important data fields include total and tropospheric column densities, as well as collocated data for cloud fraction and cloud top height, surface albedo and snow/ice coverage, at the resolution of the OMI instrument (12 km x 26 km, at nadir). The retrieved NO2 data have been validated, principally under clear-sky conditions. The first public-release version has been available since September 2006. An improved version of the data product, which includes a number of new data fields, and improved estimates of the retrieval uncertainties will be released by the end of 2007. This talk will describe the standard NO2 data product, including details that are essential for the use of the data for air quality studies. We will also describe the principal improvements with the new version of the data product.

Trends of rural tropospheric ozone at the northwest of the Iberian Peninsula.

Science.gov (United States)

Saavedra, S; Rodríguez, A; Souto, J A; Casares, J J; Bermúdez, J L; Soto, B

2012-01-01

Tropospheric ozone levels around urban and suburban areas at Europe and North America had increased during 80's-90's, until the application of NO(x) reduction strategies. However, as it was expected, this ozone depletion was not proportional to the emissions reduction. On the other hand, rural ozone levels show different trends, with peaks reduction and average increments; this different evolution could be explained by either emission changes or climate variability in a region. In this work, trends of tropospheric ozone episodes at rural sites in the northwest of the Iberian Peninsula were analyzed and compared to others observed in different regions of the Atlantic European coast. Special interest was focused on the air quality sites characterization, in order to guarantee their rural character in terms of air quality. Both episodic local meteorological and air quality measurements along five years were considered, in order to study possible meteorological influences in ozone levels, different to other European Atlantic regions.

Catalytic Reduction of NO and NOx Content in Tobacco Smoke

Directory of Open Access Journals (Sweden)

Cvetkovic N

2014-12-01

Full Text Available In order to reduce the nitric oxide (NO and nitrogen oxides (NO content in mainstream tobacco smoke, a new class of catalyst based on Cu-ZSM-5 zeolite has been synthesized. The effectiveness of the new catalyst (degree of reduction and specific catalytic ability was tested both by adding Cu-ZSM-5 zeolite directly to the tobacco blend and by addition to the filter. We have determined that adding the catalyst to the tobacco blend does not cause any changes in the physical, chemical or organoleptic properties of the cigarette blend. But, the addition reduces the yield of nitrogen oxides while having no influence on nicotine and “tar” content in the tobacco smoke of the modified blend. The catalyst addition increases the static burning rate (SBR. The changes in the quantity of NO and NOmay be explained by changes in burning conditions due to the increase of Oobtained from catalytic degradation of NO and NO, and adsorptive and diffusive properties of the catalyst. The changes in mainstream smoke analytes are also given on a puff-by-puff basis.

Testing fast photochemical theory during TRACE-P based on measurements of OH, HO2, and CH2O

Science.gov (United States)

Olson, Jennifer R.; Crawford, J. H.; Chen, G.; Fried, A.; Evans, M. J.; Jordan, C. E.; Sandholm, S. T.; Davis, D. D.; Anderson, B. E.; Avery, M. A.; Barrick, J. D.; Blake, D. R.; Brune, W. H.; Eisele, F. L.; Flocke, F.; Harder, H.; Jacob, D. J.; Kondo, Y.; Lefer, B. L.; Martinez, M.; Mauldin, R. L.; Sachse, G. W.; Shetter, R. E.; Singh, H. B.; Talbot, R. W.; Tan, D.

2004-08-01

Measurements of several short-lived photochemical species (e.g., OH, HO2, and CH2O) were obtained from the DC-8 and P3-B aircraft during the NASA Transport and Chemical Evolution over the Pacific (TRACE-P) campaign. To assess fast photochemical theory over the east Asian coast and western Pacific, these measurements are compared to predictions using a photochemical time-dependent box model constrained by coincident measurements of long-lived tracers and physical parameters. Both OH and HO2 are generally overpredicted by the model throughout the troposphere, which is a different result from previous field campaigns. The calculated-to-observed ratio of OH shows an altitude trend, with OH overpredicted by 80% in the upper troposphere and by 40-60% in the middle troposphere. Boundary layer and lower tropospheric OH ratios decrease from middle tropospheric values to 1.07 for the DC-8 and to 0.70 for the P3-B. HO2 measured on the DC-8 is overpredicted by a median of 23% and shows no trend in the agreement with altitude. Three subsets of data which compose 12% of the HO2 measurements represent outliers with respect to calculated-to-observed ratios: stratospherically influenced air, upper tropospheric data with NO > 135 pptv, and data from within clouds. Pronounced underpredictions of both HO2 and OH were found for stratospherically influenced air, which is in contrast to previous studies showing good agreement of predicted and observed HOx in the stratosphere. Observational evidence of heterogeneous uptake of HO2 within low and middle tropospheric clouds is presented, though there is no indication of significant HO2 uptake within higher-altitude clouds. Model predictions of CH2O are in good agreement with observations in the median for background concentrations, but a large scatter exists. Factors contributing to this scatter are examined, including the limited availability of some important constraining measurements, particularly CH3OOH. Some high concentrations of CH2O

The Ozone Budget in the Upper Troposphere from Global Modeling Initiative (GMI)Simulations

Science.gov (United States)

Rodriquez, J.; Duncan, Bryan N.; Logan, Jennifer A.

2006-01-01

Ozone concentrations in the upper troposphere are influenced by in-situ production, long-range tropospheric transport, and influx of stratospheric ozone, as well as by photochemical removal. Since ozone is an important greenhouse gas in this region, it is particularly important to understand how it will respond to changes in anthropogenic emissions and changes in stratospheric ozone fluxes.. This response will be determined by the relative balance of the different production, loss and transport processes. Ozone concentrations calculated by models will differ depending on the adopted meteorological fields, their chemical scheme, anthropogenic emissions, and treatment of the stratospheric influx. We performed simulations using the chemical-transport model from the Global Modeling Initiative (GMI) with meteorological fields from (It)h e NASA Goddard Institute for Space Studies (GISS) general circulation model (GCM), (2) the atmospheric GCM from NASA's Global Modeling and Assimilation Office(GMAO), and (3) assimilated winds from GMAO . These simulations adopt the same chemical mechanism and emissions, and adopt the Synthetic Ozone (SYNOZ) approach for treating the influx of stratospheric ozone -. In addition, we also performed simulations for a coupled troposphere-stratosphere model with a subset of the same winds. Simulations were done for both 4degx5deg and 2degx2.5deg resolution. Model results are being tested through comparison with a suite of atmospheric observations. In this presentation, we diagnose the ozone budget in the upper troposphere utilizing the suite of GMI simulations, to address the sensitivity of this budget to: a) the different meteorological fields used; b) the adoption of the SYNOZ boundary condition versus inclusion of a full stratosphere; c) model horizontal resolution. Model results are compared to observations to determine biases in particular simulations; by examining these comparisons in conjunction with the derived budgets, we may pinpoint

MAX-DOAS measurements of NO2, HCHO and CHOCHO at a rural site in Southern China

Science.gov (United States)

Li, X.; Brauers, T.; Hofzumahaus, A.; Lu, K.; Li, Y. P.; Shao, M.; Wagner, T.; Wahner, A.

2013-02-01

We performed MAX-DOAS measurements during the PRIDE-PRD2006 campaign in the Pearl River Delta region (PRD), China, for 4 weeks in July 2006 at a site located 60 km north of Guangzhou. The vertical distributions of NO2, HCHO, and CHOCHO were independently retrieved by an automated iteration method. The NO2 mixing ratios measured by MAX-DOAS showed reasonable agreement with the simultaneous, ground based in-situ data. The tropospheric NO2 vertical column densities (VCDs) observed by OMI on board EOS-Aura satellite were higher than with those by MAX-DOAS. The 3-D chemical transport model CMAQ overestimated the NO2 VCDs as well as the surface concentrations by about 65%. From this observation, a reduction of NOx emission strength in CMAQ seems to be necessary in order to well reproduce the NO2 observations. The average mixing ratios of HCHO and CHOCHO were 7 ppb and 0.4 ppb, respectively, higher than in other rural or semirural environments. The high ratio of 0.062 between CHOCHO and HCHO corresponds to the high VOCs reactivity and high HOx turnover rate consistent with other observations during the campaign.

The interhemispheric distribution and the budget of acetonitrile in the troposphere

International Nuclear Information System (INIS)

Hamm, S.; Warneck, P.

1990-01-01

Gas chromatography in conjunction with a thermionic nitrogen-specific detector was used to determine mixing ratios of acetonitrile in air samples collected in Europe and over the Atlantic Ocean. In the city of Mainz, values of the order of 340 pptv were observed with large variations indicating the vicinity of sources. In the rural community of Deuselbach the average mixing ratio was 147±28 pptv; over the North Sea the range was 65-196 pptv depending on wind direction. Over the open ocean, maximum mixing ratios were observed near 4 degree S with values of 175 pptv. At latitudes near 30 degree S the mixing ratio averaged 90.4 pptv, whereas at 30 degree N the average was 52.1 pptv. The lowest mixing ratios of 21 pptv were found near 50 degree N. The tropical maximum is attributed to the advection with the trade winds of continental air from Africa, enriched with acetonitrile form biomass burning. The mixing ratios north and south of the maximum correlate well with the surface temperature of seawater, indicating a gas-liquid equilibrium for CH 3 CN dissolved in seawater. From the observations and with the further assumption that CH 3 CN is vertically well mixed, its total mass content in the troposphere was estimated as 0.37-0.57 Tg. Global emission rates for various sources were estimated as follows: Automobiles 0.27 Tg/year, oil-fired power stations 0.0035 Tg/year, and biomass burning 0.80 Tg/year. The total estimated source strength is 1.1±0.5 Tg/year. The troposphere residence time of acetonitrile was calculated from these data as 0.23-0.90 year with a probable value of 0.45 year. Wet precipitation and reaction with OH radicals are known sinks for tropospheric CH 3 CN, but they can take up only 30% of the global emission rate. The authors suggest absorption in the ocean to be the major sink

Towards a Model Climatology of Relative Humidity in the Upper Troposphere for Estimation of Contrail and Contrail-Induced Cirrus

Science.gov (United States)

Selkirk, Henry B.; Manyin, M.; Ott, L.; Oman, L.; Benson, C.; Pawson, S.; Douglass, A. R.; Stolarski, R. S.

2011-01-01

The formation of contrails and contrail cirrus is very sensitive to the relative humidity of the upper troposphere. To reduce uncertainty in an estimate of the radiative impact of aviation-induced cirrus, a model must therefore be able to reproduce the observed background moisture fields with reasonable and quantifiable fidelity. Here we present an upper tropospheric moisture climatology from a 26-year ensemble of simulations using the GEOS CCM. We compare this free-running model's moisture fields to those obtained from the MLS and AIRS satellite instruments, our most comprehensive observational databases for upper tropospheric water vapor. Published comparisons have shown a substantial wet bias in GEOS-5 assimilated fields with respect to MLS water vapor and ice water content. This tendency is clear as well in the GEOS CCM simulations. The GEOS-5 moist physics in the GEOS CCM uses a saturation adjustment that prevents supersaturation, which is unrealistic when compared to in situ moisture observations from MOZAIC aircraft and balloon sondes as we will show. Further, the large-scale satellite datasets also consistently underestimate super-saturation when compared to the in-situ observations. We place these results in the context of estimates of contrail and contrail cirrus frequency.

Discussion on the tropospheric concentrations of FC21

Energy Technology Data Exchange (ETDEWEB)

Crescentini, G.; Mangani, F.; Mastrogiamcomo, A.R.; Cappiello, A.; Bruner, F.

1986-01-01

FC21 tropospheric mixing ratios measured in air samples collected at different locations in the world are presented. Results of a campaign carried out at two locations in the Sahara desert where FC21 and FC11 mixing ratios were simultaneously determined in 180 samples are also shown. Though scattered high values have been found, the average background concentration of FC21 ranged between 0 and 1 pptv. 9 references, 1 figure, 2 tables.

Seasonal behavior and long-term trends of tropospheric ozone, its precursors and chemical conditions over Iran: A view from space

Science.gov (United States)

Choi, Yunsoo; Souri, Amir Hossein

2015-04-01

To identify spatial and temporal variations over the Iranian region, this study analyzed tropospheric formaldehyde (HCHO) and nitrogen dioxide (NO2) columns from Ozone Monitoring Instrument (OMI), carbon monoxide (CO) columns from the Measurement of Pollution in the Troposphere (MOPITT), and tropospheric column O3 (TCO) from OMI/MLS (Microwave Limb Sounder) satellites from 2005 to 2012. The study discovered high levels of HCHO (∼12 × 1015 molec./cm2) from plant isoprene emissions in the air above parts of the northern forest of Iran during the summer and from the oxidation of HCHO precursors emitted from petrochemical industrial facilities and biomass burning in South West Iran. This study showed that maximum NO2 levels (∼18 × 1015 molec./cm2) were concentrated in urban cities, indicating the predominance of anthropogenic sources. The results indicate that maximum concentrations were found in the winter, mainly because of weaker local winds and higher heating fuel consumption, in addition to lower hydroxyl radicals (OH). The high CO concentrations (∼2 × 1018 molec./cm2) in the early spring were inferred to mainly originate from a strong continental air mass from anthropogenic CO "hotspots" including regions around Caspian Sea, Europe, and North America, although the external sources of CO were partly suppressed by the Arabian anticyclone and topographic barriers. Variations in the TCO were seen to peak during the summer (∼40 DU), due to intensive solar radiation and stratospheric sources. This study also examined long-term trends in TCO and its precursors over a period of eight years in five urban cities in Iran. To perform the analysis, we estimated seasonal changes and inter-seasonal variations using least-squares harmonic estimation (LS-HE), which reduced uncertainty in the trend by 5-15%. The results showed significant increases in the levels of HCHO (∼0.08 ± 0.06 × 1015 molec./cm2 yr-1), NO2 (∼0.08 ± 0.02 × 1015 molec./cm2 yr-1), and peak

Real-Time Tropospheric Delay Estimation using IGS Products

Science.gov (United States)

Stürze, Andrea; Liu, Sha; Söhne, Wolfgang

2014-05-01

The Federal Agency for Cartography and Geodesy (BKG) routinely provides zenith tropospheric delay (ZTD) parameter for the assimilation in numerical weather models since more than 10 years. Up to now the results flowing into the EUREF Permanent Network (EPN) or E-GVAP (EUMETNET EIG GNSS water vapour programme) analysis are based on batch processing of GPS+GLONASS observations in differential network mode. For the recently started COST Action ES1206 about "Advanced Global Navigation Satellite Systems tropospheric products for monitoring severe weather events and climate" (GNSS4SWEC), however, rapid updates in the analysis of the atmospheric state for nowcasting applications require changing the processing strategy towards real-time. In the RTCM SC104 (Radio Technical Commission for Maritime Services, Special Committee 104) a format combining the advantages of Precise Point Positioning (PPP) and Real-Time Kinematic (RTK) is under development. The so-called State Space Representation approach is defining corrections, which will be transferred in real-time to the user e.g. via NTRIP (Network Transport of RTCM via Internet Protocol). Meanwhile messages for precise orbits, satellite clocks and code biases compatible to the basic PPP mode using IGS products are defined. Consequently, the IGS Real-Time Service (RTS) was launched in 2013 in order to extend the well-known precise orbit and clock products by a real-time component. Further messages e.g. with respect to ionosphere or phase biases are foreseen. Depending on the level of refinement, so different accuracies up to the RTK level shall be reachable. In co-operation of BKG and the Technical University of Darmstadt the real-time software GEMon (GREF EUREF Monitoring) is under development. GEMon is able to process GPS and GLONASS observation and RTS product data streams in PPP mode. Furthermore, several state-of-the-art troposphere models, for example based on numerical weather prediction data, are implemented. Hence, it

Lidar Profiling In the lower Troposphere: experience from PECAN

Science.gov (United States)

Demoz, Belay B.; Delgado, Ruben; Caroll, Brian; Vermeesch, Kevin; Whiteman, David N.; Sakai, Ricardo; Tesfay, Sium; Cooper, Lorenza

2018-04-01

Results from the PECAN (Plains Elevated Convection at Night) campaign are discussed. In particular, the utility of simple backscatter lidars/ceilometers in quantifying atmospheric dynamics parameters and variables as well as evolution of the lower tropospheric dynamics are made. Cases of bore wave dynamics and the potential of these events in lofting of low level, moist, airmass and its consequence in thunderstorm initiation are made. A suite of thermodynamic profiling instruments are combined and compared to describe and visualize lower tropospheric dynamic evolution.

The Total Electron Content From InSAR and GNSS: A Midlatitude Study

DEFF Research Database (Denmark)

Musico, Elvira; Cesaroni, Claudio; Spogli, Luca

2018-01-01

The total electron content (TEC) measured from the interferometric synthetic aperture radar (InSAR) and froma dense network of global navigation satellite system (GNSS) receivers are used to assess the capability of InSAR to retrieve ionospheric information, when the tropospheric contribution...

submitter Technical Note: Using DEG-CPCs at upper tropospheric temperatures

CERN Document Server

Wimmer, D; Nieminen, T; Duplissy, J; Ehrhart, S; Almeida, J; Rondo, L; Franchin, A; Kreissl, F; Bianchi, F; Manninen, H E; Kulmala, M; Curtius, J; Petäjä, T

2015-01-01

Over the last few years, several condensation particle counters (CPCs) capable of measuring in the sub-3 nm size range have been developed. Here we study the performance of CPCs based on diethylene glycol (DEG) at different temperatures during Cosmics Leaving OUtdoor Droplets (CLOUD) measurements at CERN. The data shown here are the first set of verification measurements for sub-3 nm CPCs under upper tropospheric temperatures using atmospherically relevant aerosol particles. To put the results in perspective we calibrated the DEG-CPC at room temperature, resulting in a cut-off diameter of 1.4 nm. All diameters refer to mobility equivalent diameters in this paper. At upper tropospheric temperatures ranging from 246.15 K to 207.15 K, we found cut-off sizes relative to a particle size magnifier in the range of 2.5 to 2.8 nm. Due to low number concentration after size classification, the cut-off diameters have a high uncertainty (±0.3 nm) associated with them. Operating two laminar flow DEG-CPCs with different c...

Elevated carbon dioxide and ozone alter productivity and ecosystem carbon content in northern temperate forests.

Science.gov (United States)

Talhelm, Alan F; Pregitzer, Kurt S; Kubiske, Mark E; Zak, Donald R; Campany, Courtney E; Burton, Andrew J; Dickson, Richard E; Hendrey, George R; Isebrands, J G; Lewin, Keith F; Nagy, John; Karnosky, David F

2014-08-01

Three young northern temperate forest communities in the north-central United States were exposed to factorial combinations of elevated carbon dioxide (CO2 ) and tropospheric ozone (O3 ) for 11 years. Here, we report results from an extensive sampling of plant biomass and soil conducted at the conclusion of the experiment that enabled us to estimate ecosystem carbon (C) content and cumulative net primary productivity (NPP). Elevated CO2 enhanced ecosystem C content by 11%, whereas elevated O3 decreased ecosystem C content by 9%. There was little variation in treatment effects on C content across communities and no meaningful interactions between CO2 and O3 . Treatment effects on ecosystem C content resulted primarily from changes in the near-surface mineral soil and tree C, particularly differences in woody tissues. Excluding the mineral soil, cumulative NPP was a strong predictor of ecosystem C content (r(2) = 0.96). Elevated CO2 enhanced cumulative NPP by 39%, a consequence of a 28% increase in canopy nitrogen (N) content (g N m(-2) ) and a 28% increase in N productivity (NPP/canopy N). In contrast, elevated O3 lowered NPP by 10% because of a 21% decrease in canopy N, but did not impact N productivity. Consequently, as the marginal impact of canopy N on NPP (∆NPP/∆N) decreased through time with further canopy development, the O3 effect on NPP dissipated. Within the mineral soil, there was less C in the top 0.1 m of soil under elevated O3 and less soil C from 0.1 to 0.2 m in depth under elevated CO2 . Overall, these results suggest that elevated CO2 may create a sustained increase in NPP, whereas the long-term effect of elevated O3 on NPP will be smaller than expected. However, changes in soil C are not well-understood and limit our ability to predict changes in ecosystem C content. © 2014 The Authors Global Change Biology Published by John Wiley & Sons Ltd.

Elevated carbon dioxide and ozone alter productivity and ecosystem carbon content in northern temperate forests

Science.gov (United States)

Talhelm, Alan F; Pregitzer, Kurt S; Kubiske, Mark E; Zak, Donald R; Campany, Courtney E; Burton, Andrew J; Dickson, Richard E; Hendrey, George R; Isebrands, J G; Lewin, Keith F; Nagy, John; Karnosky, David F

2014-01-01

Three young northern temperate forest communities in the north-central United States were exposed to factorial combinations of elevated carbon dioxide (CO2) and tropospheric ozone (O3) for 11 years. Here, we report results from an extensive sampling of plant biomass and soil conducted at the conclusion of the experiment that enabled us to estimate ecosystem carbon (C) content and cumulative net primary productivity (NPP). Elevated CO2 enhanced ecosystem C content by 11%, whereas elevated O3 decreased ecosystem C content by 9%. There was little variation in treatment effects on C content across communities and no meaningful interactions between CO2 and O3. Treatment effects on ecosystem C content resulted primarily from changes in the near-surface mineral soil and tree C, particularly differences in woody tissues. Excluding the mineral soil, cumulative NPP was a strong predictor of ecosystem C content (r2 = 0.96). Elevated CO2 enhanced cumulative NPP by 39%, a consequence of a 28% increase in canopy nitrogen (N) content (g N m−2) and a 28% increase in N productivity (NPP/canopy N). In contrast, elevated O3 lowered NPP by 10% because of a 21% decrease in canopy N, but did not impact N productivity. Consequently, as the marginal impact of canopy N on NPP (ΔNPP/ΔN) decreased through time with further canopy development, the O3 effect on NPP dissipated. Within the mineral soil, there was less C in the top 0.1 m of soil under elevated O3 and less soil C from 0.1 to 0.2 m in depth under elevated CO2. Overall, these results suggest that elevated CO2 may create a sustained increase in NPP, whereas the long-term effect of elevated O3 on NPP will be smaller than expected. However, changes in soil C are not well-understood and limit our ability to predict changes in ecosystem C content. PMID:24604779

Aura OMI Observations of Global SO2 and NO2 Pollution from 2005 to 2013

Science.gov (United States)

Krotkov, Nickolay; Li, Can; Lamsal, Lok; Celarier, Edward; Marchenko, Sergey; Swartz, William H.; Bucsela, Eric; Fioletov, Vitali; McLinden, Chris; Joiner, Joanna;

Accomplishments of the MUSICA project to provide accurate, long-term, global and high-resolution observations of tropospheric {H2O,δD} pairs - a review

Science.gov (United States)

Schneider, Matthias; Wiegele, Andreas; Barthlott, Sabine; González, Yenny; Christner, Emanuel; Dyroff, Christoph; García, Omaira E.; Hase, Frank; Blumenstock, Thomas; Sepúlveda, Eliezer; Mengistu Tsidu, Gizaw; Takele Kenea, Samuel; Rodríguez, Sergio; Andrey, Javier

2016-07-01

In the lower/middle troposphere, {H2O,δD} pairs are good proxies for moisture pathways; however, their observation, in particular when using remote sensing techniques, is challenging. The project MUSICA (MUlti-platform remote Sensing of Isotopologues for investigating the Cycle of Atmospheric water) addresses this challenge by integrating the remote sensing with in situ measurement techniques. The aim is to retrieve calibrated tropospheric {H2O,δD} pairs from the middle infrared spectra measured from ground by FTIR (Fourier transform infrared) spectrometers of the NDACC (Network for the Detection of Atmospheric Composition Change) and the thermal nadir spectra measured by IASI (Infrared Atmospheric Sounding Interferometer) aboard the MetOp satellites. In this paper, we present the final MUSICA products, and discuss the characteristics and potential of the NDACC/FTIR and MetOp/IASI {H2O,δD} data pairs. First, we briefly resume the particularities of an {H2O,δD} pair retrieval. Second, we show that the remote sensing data of the final product version are absolutely calibrated with respect to H2O and δD in situ profile references measured in the subtropics, between 0 and 7 km. Third, we reveal that the {H2O,δD} pair distributions obtained from the different remote sensors are consistent and allow distinct lower/middle tropospheric moisture pathways to be identified in agreement with multi-year in situ references. Fourth, we document the possibilities of the NDACC/FTIR instruments for climatological studies (due to long-term monitoring) and of the MetOp/IASI sensors for observing diurnal signals on a quasi-global scale and with high horizontal resolution. Fifth, we discuss the risk of misinterpreting {H2O,δD} pair distributions due to incomplete processing of the remote sensing products.

Verification and Validation of Tropospheric Model/Database

National Research Council Canada - National Science Library

Junho, choi

1998-01-01

A verification and validation of tropospheric models and databases has been performed based on ray tracing algorithm, statistical analysis, test on real time system operation, and other technical evaluation process...

Ozone Depletion in Tropospheric Volcanic Plumes: From Halogen-Poor to Halogen-Rich Emissions

Directory of Open Access Journals (Sweden)

Tjarda J. Roberts

2018-02-01

Full Text Available Volcanic halogen emissions to the troposphere undergo a rapid plume chemistry that destroys ozone. Quantifying the impact of volcanic halogens on tropospheric ozone is challenging, only a few observations exist. This study presents measurements of ozone in volcanic plumes from Kīlauea (HI, USA, a low halogen emitter. The results are combined with published data from high halogen emitters (Mt Etna, Italy; Mt Redoubt, AK, USA to identify controls on plume processes. Ozone was measured during periods of relatively sustained Kīlauea plume exposure, using an Aeroqual instrument deployed alongside Multi-Gas SO2 and H2S sensors. Interferences were accounted for in data post-processing. The volcanic H2S/SO2 molar ratio was quantified as 0.03. At Halema‘uma‘u crater-rim, ozone was close to ambient in the emission plume (at 10 ppmv SO2. Measurements in grounding plume (at 5 ppmv SO2 about 10 km downwind of Pu‘u ‘Ō‘ō showed just slight ozone depletion. These Kīlauea observations contrast with substantial ozone depletion reported at Mt Etna and Mt Redoubt. Analysis of the combined data from these three volcanoes identifies the emitted Br/S as a strong but non-linear control on the rate of ozone depletion. Model simulations of the volcanic plume chemistry highlight that the proportion of HBr converted into reactive bromine is a key control on the efficiency of ozone depletion. This underlines the importance of chemistry in the very near-source plume on the fate and atmospheric impacts of volcanic emissions to the troposphere.

Impact of lightning-NO on eastern United States photochemistry during the summer of 2006 as determined using the CMAQ model

Directory of Open Access Journals (Sweden)

D. J. Allen

2012-02-01

Full Text Available A lightning-nitrogen oxide (NO algorithm is implemented in the Community Multiscale Air Quality Model (CMAQ and used to evaluate the impact of lightning-NO emissions (LNO_x on tropospheric photochemistry over the United States during the summer of 2006.

For a 500 mole per flash lightning-NO source, the mean summertime tropospheric NO₂ column agrees with satellite-retrieved columns to within −5 to +13%. Temporal fluctuations in the column are moderately well simulated; however, the addition of LNO_x does not lead to a better simulation of day-to-day variability. The contribution of lightning-NO to the model column ranges from ∼10% in the northern US to >45% in the south-central and southeastern US. Lightning-NO adds up to 20 ppbv to upper tropospheric model ozone and 1.5–4.5 ppbv to 8-h maximum surface layer ozone, although, on average, the contribution of LNO_x to model surface ozone is 1–2 ppbv less on poor air quality days. LNO_x increases wet deposition of oxidized nitrogen by 43% and total deposition of nitrogen by 10%. This additional deposition reduces the mean magnitude of the CMAQ low-bias in nitrate wet deposition with respect to National Atmospheric Deposition monitors to near zero.

Differences in urban/rural biases between model and satellite-retrieved NO₂ columns were examined to identify possible problems in model chemistry and/or transport. CMAQ columns were too large over urban areas. Biases at other locations were minor after accounting for the impacts of lightning-NO emissions and the averaging kernel on model columns.

In order to obtain an upper bound on the contribution of uncertainties in NO_y chemistry to upper tropospheric NO_x low biases, sensitivity calculations with updated chemistry were run for the time period of the Intercontinental Chemical Transport Experiment (INTEX-A field campaign (summer 2004

Effects of tropospheric aerosols on radiative flux calculations at UV and visible wavelengths

International Nuclear Information System (INIS)

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

1994-08-01

The surface fluxes in the wavelength range 175 to 735nm have been calculated for an atmosphere which contains a uniformly mixed aerosol layer of thickness 1km at the earth's surface. Two different aerosol types were considered, a rural aerosol, and an urban aerosol. The visibility range for the aerosol layers was 95 to 15 km. Surface flux ratios (15km/95km) were in agreement with previously published results for the rural aerosol layer to within about 2%. The surface flux ratios vary from 7 to 14% for the rural aerosol layer and from 13 to 23% for the urban aerosol layer over the wavelength range. A tropospheric radiative forcing of about 1.3% of the total tropospheric flux was determined for the 95km to 15km visibility change in the rural aerosol layer, indicating the potential of tropospheric feedback effects on the surface flux changes. This effect was found to be negligible for the urban aerosol layer. Stratospheric layer heating rate changes due to visibility changes in either the rural or urban aerosol layer were found to be negligible

Tropospheric ozone over Equatorial Africa: regional aspects from the MOZAIC data

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B. Sauvage

2005-01-01

Full Text Available We analyze ozone observations recorded over Equatorial Africa between April 1997 and March 2003 by the MOZAIC programme, providing the first ozone climatology deriving from continental in-situ data over this region. Three-dimensional streamlines strongly suggests connections between the characteristics of the ozone monthly mean vertical profiles, the most persistent circulation patterns in the troposphere over Equatorial Africa (on a monthly basis such as the Harmattan, the African Easterly Jet, the Trades and the regions of ozone precursors emissions by biomass burning. During the biomass burning season in each hemisphere, the lower troposphere exhibits layers of enhanced ozone (i.e. 70 ppbv over the coast of Gulf of Guinea in December-February and 85 ppbv over Congo in June-August. The characteristics of the ozone monthly mean vertical profiles are clearly connected to the regional flow regime determined by seasonal dynamic forcing. The mean ozone profile over the coast of Gulf of Guinea in the burning season is characterized by systematically high ozone below 650hPa ; these are due to the transport by the Harmattan and the AEJ of the pollutants originating from upwind fires. The confinement of high ozone to the lower troposphere is due to the high stability of the Harmattan and the blocking Saharan anticyclone which prevents efficient vertical mixing. In contrast, ozone enhancements observed over Central Africa during the local dry season (June-August are not only found in the lower troposphere but throughout the troposphere. Moreover, this study highlights a connection between the regions of the coast of Gulf of Guinea and regions of Congo to the south that appears on a semi annual basis. Vertical profiles in wet-season regions exhibit ozone enhancements in the lower troposphere due to biomass burning products transport from fires situated in the opposite dry-season hemisphere.

Autoregressive Processes in Homogenization of GNSS Tropospheric Data

Science.gov (United States)

Klos, A.; Bogusz, J.; Teferle, F. N.; Bock, O.; Pottiaux, E.; Van Malderen, R.

2016-12-01

Offsets due to changes in hardware equipment or any other artificial event are all a subject of a task of homogenization of tropospheric data estimated within a processing of Global Navigation Satellite System (GNSS) observables. This task is aimed at identifying exact epochs of offsets and estimate their magnitudes since they may artificially under- or over-estimate trend and its uncertainty delivered from tropospheric data and used in climate studies. In this research, we analysed a common data set of differences of Integrated Water Vapour (IWV) from GPS and ERA-Interim (1995-2010) provided for a homogenization group working within ES1206 COST Action GNSS4SWEC. We analysed daily IWV records of GPS and ERA-Interim in terms of trend, seasonal terms and noise model with Maximum Likelihood Estimation in Hector software. We found that this data has a character of autoregressive process (AR). Basing on this analysis, we performed Monte Carlo simulations of 25 years long data with two different noise types: white as well as combination of white and autoregressive and also added few strictly defined offsets. This synthetic data set of exactly the same character as IWV from GPS and ERA-Interim was then subjected to a task of manual and automatic/statistical homogenization. We made blind tests and detected possible epochs of offsets manually. We found that simulated offsets were easily detected in series with white noise, no influence of seasonal signal was noticed. The autoregressive series were much more problematic when offsets had to be determined. We found few epochs, for which no offset was simulated. This was mainly due to strong autocorrelation of data, which brings an artificial trend within. Due to regime-like behaviour of AR it is difficult for statistical methods to properly detect epochs of offsets, which was previously reported by climatologists.

A joint data record of tropospheric ozone from Aura-TES and MetOp-IASI

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H. Oetjen

2016-08-01

Full Text Available The Tropospheric Emission Spectrometer (TES on Aura and Infrared Atmospheric Sounding Interferometer (IASI on MetOp-A together provide a time series of 10 years of free-tropospheric ozone with an overlap of 3 years. We characterise the differences between TES and IASI ozone measurements and find that IASI's coarser vertical sensitivity leads to a small (< 5 ppb low bias relative to TES for the free troposphere. The TES-IASI differences are not dependent on season or any other factor and hence the measurements from the two instruments can be merged, after correcting for the offset, in order to study decadal-scale changes in tropospheric ozone. We calculate time series of regional monthly mean ozone in the free troposphere over eastern Asia, the western United States (US, and Europe, carefully accounting for differences in spatial sampling between the instruments. We show that free-tropospheric ozone over Europe and the western US has remained relatively constant over the past decade but that, contrary to expectations, ozone over Asia in recent years does not continue the rapid rate of increase observed from 2004 to 2010.

Evaluating A Priori Ozone Profile Information Used in TEMPO Tropospheric Ozone Retrievals

Science.gov (United States)

Johnson, Matthew S.; Sullivan, John T.; Liu, Xiong; Newchurch, Mike; Kuang, Shi; McGee, Thomas J.; Langford, Andrew O'Neil; Senff, Christoph J.; Leblanc, Thierry; Berkoff, Timothy;

Evaluating A Priori Ozone Profile Information Used in TEMPO Tropospheric Ozone Retrievals

Science.gov (United States)

Johnson, M. S.; Sullivan, J. T.; Liu, X.; Newchurch, M.; Kuang, S.; McGee, T. J.; Langford, A. O.; Senff, C. J.; Leblanc, T.; Berkoff, T.; Gronoff, G.; Chen, G.; Strawbridge, K. B.

2016-12-01

Ozone (O3) is a greenhouse gas and toxic pollutant which plays a major role in air quality. Typically, monitoring of surface air quality and O3 mixing ratios is primarily conducted using in situ measurement networks. This is partially due to high-quality information related to air quality being limited from space-borne platforms due to coarse spatial resolution, limited temporal frequency, and minimal sensitivity to lower tropospheric and surface-level O3. The Tropospheric Emissions: Monitoring of Pollution (TEMPO) satellite is designed to address these limitations of current space-based platforms and to improve our ability to monitor North American air quality. TEMPO will provide hourly data of total column and vertical profiles of O3 with high spatial resolution to be used as a near-real-time air quality product. TEMPO O3 retrievals will apply the Smithsonian Astrophysical Observatory profile algorithm developed based on work from GOME, GOME-2, and OMI. This algorithm uses a priori O3 profile information from a climatological data-base developed from long-term ozone-sonde measurements (tropopause-based (TB) O3 climatology). It has been shown that satellite O3 retrievals are sensitive to a priori O3 profiles and covariance matrices. During this work we investigate the climatological data to be used in TEMPO algorithms (TB O3) and simulated data from the NASA GMAO Goddard Earth Observing System (GEOS-5) Forward Processing (FP) near-real-time (NRT) model products. These two data products will be evaluated with ground-based lidar data from the Tropospheric Ozone Lidar Network (TOLNet) at various locations of the US. This study evaluates the TB climatology, GEOS-5 climatology, and 3-hourly GEOS-5 data compared to lower tropospheric observations to demonstrate the accuracy of a priori information to potentially be used in TEMPO O3 algorithms. Here we present our initial analysis and the theoretical impact on TEMPO retrievals in the lower troposphere.

Tropospheric ozone seasonal and long-term variability as seen by lidar and surface measurements at the JPL-Table Mountain Facility, California

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M. J. Granados-Muñoz

2016-07-01

Full Text Available A combined surface and tropospheric ozone climatology and interannual variability study was performed for the first time using co-located ozone photometer measurements (2013–2015 and tropospheric ozone differential absorption lidar measurements (2000–2015 at the Jet Propulsion Laboratory Table Mountain Facility (TMF; elev. 2285 m, in California. The surface time series were investigated both in terms of seasonal and diurnal variability. The observed surface ozone is typical of high-elevation remote sites, with small amplitude of the seasonal and diurnal cycles, and high ozone values, compared to neighboring lower altitude stations representative of urban boundary layer conditions. The ozone mixing ratio ranges from 45 ppbv in the winter morning hours to 65 ppbv in the spring and summer afternoon hours. At the time of the lidar measurements (early night, the seasonal cycle observed at the surface is similar to that observed by lidar between 3.5 and 9 km. Above 9 km, the local tropopause height variation with time and season impacts significantly the ozone lidar observations. The frequent tropopause folds found in the vicinity of TMF (27 % of the time, mostly in winter and spring produce a dual-peak vertical structure in ozone within the fold layer, characterized by higher-than-average values in the bottom half of the fold (12–14 km, and lower-than-averaged values in the top half of the fold (14–18 km. This structure is consistent with the expected origin of the air parcels within the fold, i.e., mid-latitude stratospheric air folding down below the upper tropospheric sub-tropical air. The influence of the tropopause folds extends down to 5 km, increasing the ozone content in the troposphere. No significant signature of interannual variability could be observed on the 2000–2015 de-seasonalized lidar time series, with only a statistically non-significant positive anomaly during the years 2003–2007. Our trend analysis

Lidar Profiling In the lower Troposphere: experience from PECAN

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Demoz Belay B.

2018-01-01

Full Text Available Results from the PECAN (Plains Elevated Convection at Night campaign are discussed. In particular, the utility of simple backscatter lidars/ceilometers in quantifying atmospheric dynamics parameters and variables as well as evolution of the lower tropospheric dynamics are made. Cases of bore wave dynamics and the potential of these events in lofting of low level, moist, airmass and its consequence in thunderstorm initiation are made. A suite of thermodynamic profiling instruments are combined and compared to describe and visualize lower tropospheric dynamic evolution.

Transport and build-up of tropospheric trace gases during the MINOS campaign: comparision of GOME, in situ aircraft measurements and MATCH-MPIC-data

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A. Ladstätter-Weißenmayer

2003-01-01

Full Text Available The MINOS (Mediterranean INtensive Oxidant Study campaign was an international, multi-platform field campaign to measure long-range transport of air-pollution and aerosols from South East Asia and Europe towards the Mediterranean basin during August 2001. High pollution events were observed during this campaign. For the Mediterranean region enhanced tropospheric nitrogen dioxide (NO2 and formaldehyde (HCHO, which are precursors of tropospheric ozone (O3, were detected by the satellite based GOME (Global Ozone Monitoring Experiment instrument and compared with airborne in situ measurements as well as with the output from the global 3D photochemistry-transport model MATCH-MPIC (Model of Atmospheric Transport and CHemistry - Max Planck Institute for Chemistry. The increase of pollution in that region leads to severe air quality degradation with regional and global implications.

Soil water content plays an important role in soil-atmosphere exchange of carbonyl sulfide (OCS)

Science.gov (United States)

Yi, Zhigang; Behrendt, Thomas; Bunk, Rüdiger; Wu, Dianming; Kesselmeier, Jürgen

2016-04-01

Carbonyl sulfide (OCS) is a quite stable gas in the troposphere and is transported up to the stratosphere, where it contributes to the sulfate aerosol layer (Crutzen 1976). The tropospheric concentration seems to be quite constant, indicating a balance between sinks and sources. Recent work by Sandoval-Soto et al. (2005) demonstrated the enormous strength of the vegetation sink and the urgent needs to understand the sinks and sources. The role of soils is a matter of discussion (Kesselmeier et al., 1999; Van Diest and Kesselmeier, 2008; Maseyk et al., 2014; Whelan et al., 2015). To better understand the influence of soil water content and OCS mixing ratio on OCS fluxes, we used an OCS analyzer (LGR COS/CO Analyzer 907-0028, Los Gatos, CA, USA) coupled with automated soil chamber system (Behrendt et al., 2014) to measure the OCS fluxes with a slow drying of four different types of soil (arable wheat soil in Mainz, blueberry soil in Waldstein, spruce soil in Waldstein and needle forest soil in Finland). Results showed that OCS fluxes as well as the optimum soil water content for OCS uptake varied significantly for different soils. The net production rates changed significantly with the soil drying out from 100% to about 5% water holding capacity (WHC), implying that soil water content play an important role in the uptake processes. The production and uptake processes were distinguished by the regression of OCS fluxes under different OCS mixing ratios. OCS compensation points (CP) were found to differ significantly for different soil types and water content, with the lowest CP at about 20% WHC, implying that when estimating the global budgets of OCS, especially for soils fluxes, soil water content should be taken into serious consideration. References Crutzen, P. J. 1976, Geophys. Res. Lett., 3, 73-76. Sandoval-Soto, L. et al., 2005, Biogeosciences, 2, 125-132. Kesselmeier, J. et al., 1999, J. Geophys. Res., 104, 11577-11584. Van Diest, H. and Kesselmeier, J. 2008

The Tropospheric Products of the International VLBI Service for Geodesy and Astrometry

Science.gov (United States)

Heinkelmann, Robert; Schwatke, Christian

2010-01-01

The IVS runs two tropospheric products: The IVS tropospheric parameter rapid combination monitors the zenith wet delay (ZWD) and zenith total delay (ZTD) of the rapid turnaround sessions R1 and R4. Goal of the combination is the identification and the exclusion of outliers by comparison and the assessment of the precision of current VLBI solutions in terms of tropospheric parameters. The rapid combination is done on a weekly basis four weeks after the observation files are released on IVS Data Centers. Since tropospheric and geodetic parameters, such as vertical station components, can significantly correlate, the consistency of the ZTD can be a measure of the consistency of the corresponding TRF as well. The ZWD mainly rely on accurate atmospheric pressure data. Thus, besides estimation techniques, modeling and analyst s noise, ZWD reflects differences in the atmospheric pressure data applied to the VLBI analysis. The second product, called tropospheric parameter long-term combination, aims for an accurate determination of climatological signals, such as trends of the atmospheric water vapor observed by VLBI. Therefore, the long-term homogeneity of atmospheric pressure data plays a crucial role for this product. The paper reviews the methods applied and results achieved so far and describes the new maintenance through DGFI.

Relationship between changes in the upper and lower tropospheric water vapor: A revisit

Science.gov (United States)

Yang, M.; Sun, D. Z.; Zhang, G. J.

2017-12-01

Upper tropospheric water vapor response to enhanced greenhouse gas forcing is as important as the lower tropospheric water vapor response in determining climate sensitivity. Early studies using older versions of climate models have suggested that the upper- and lower-troposphere water vapor changes are more strongly coupled in the climate models than in the observations. Here we reexamine this issue using a state-of-the-art climate model—the NCAR community model CAM5. Specifically, we have calculated the correlations between interannual variations of specific humidity in all levels of the troposphere with that at the surface in CAM5 and in the observations (as represented by the updated ERA-Interim and NCEP reanalysis). It is found that the previously noted biases in how strongly upper tropospheric water vapor and lower troposphere water vapor are linked still exist in CAM5—the change in the tropical averaged upper tropospheric water vapor is more strongly correlated with the change in the surface. However, this bias disappears in the averaged correlation obtained by averaging the point-by-point correlations over the tropics. The spatial pattern of the point-by-point correlations reveals that the better agreement between the model and the observations is related to the opposite model biases in different regions: the correlation is weaker in the model in the western Pacific, but stronger in the central and eastern Pacific. Further analysis of precipitation fields suggests that the weaker (stronger) coupling between tropospheric water vapor and surface moisture over western (central-eastern) Pacific in model is related to weaker (stronger) simulated convective activities in these regions. More specifically, during El Nino, the model has excessive deep convection in the central Pacific, but too littler deep convection in western Pacific. Implications of the results are discussed in the context of climate change as well as in the context of how to improve the model

HYDROLOGIC CONDITIONS AFFECTING THE TROPOSPHERIC FLUX OF VINCLOZOLIN AND ITS DEGRADATION PRODUCTS

Science.gov (United States)

A laboratory chamber was used to determine hydrologic conditions that lead to the tropospheric flux of a suspected anti-androgenic dicarboximide fungicide, vinclozolin (3-(3,5-dichlorophenyl)-5-methyl-5-vinyl-oxzoli-dine-2,4-dione) and three degradation products from sterilized...

Characteristics of tropospheric ozone depletion events in the Arctic spring: analysis of the ARCTAS, ARCPAC, and ARCIONS measurements and satellite BrO observations

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J.-H. Koo

2012-10-01

Full Text Available Arctic ozone depletion events (ODEs are caused by halogen catalyzed ozone loss. In situ chemistry, advection of ozone-poor air mass, and vertical mixing in the lower troposphere are important factors affecting ODEs. To better characterize the ODEs, we analyze the combined set of surface, ozonesonde, and aircraft in situ measurements of ozone and bromine compounds during the Arctic Research of the Composition of the Troposphere from Aircraft and Satellites (ARCTAS, the Aerosol, Radiation, and Cloud Processes affecting Arctic Climate (ARCPAC, and the Arctic Intensive Ozonesonde Network Study (ARCIONS experiments (April 2008. Tropospheric BrO columns retrieved from satellite measurements and back trajectory calculations are also used to investigate the characteristics of observed ODEs. In situ observations from these field experiments are inadequate to validate tropospheric BrO columns derived from satellite measurements. In view of this difficulty, we construct an ensemble of tropospheric column BrO estimates from two satellite (OMI and GOME-2 measurements and with three independent methods of calculating stratospheric BrO columns. Furthermore, we select analysis methods that do not depend on the absolute magnitude of column BrO, such as time-lagged correlation analysis of ozone and tropospheric column BrO, to understand characteristics of ODEs. Time-lagged correlation analysis between in situ (surface and ozonesonde measurements of ozone and satellite derived tropospheric BrO columns indicates that the ODEs are due to either local halogen-driven ozone loss or short-range (∼1 day transport from nearby regions with ozone depletion. The effect of in situ ozone loss is also evident in the diurnal variation difference between low (10th and 25th percentiles and higher percentiles of surface ozone concentrations at Alert, Canada. Aircraft observations indicate low-ozone air mass transported from adjacent high-BrO regions. Correlation analyses of ozone

Transportable lidar for the measurement of ozone concentration and flux profiles in the lower troposphere

International Nuclear Information System (INIS)

Zhao, Yanzeng; Howell, J.N.; Hardesty, R.M.

1992-01-01

In many areas of the United States, as well as in other industrial areas (such as Europe), elevated and potentially harmful levels of ozone are being measured during summer. Most of this ozone is photochemically produced. The relatively long lifetime of ozone allows industrially produced ozone to be transported on a hemispheric scale. Since the trends of tropospheric ozone are very likely dependent on the source strengths and distributions of the pollutants and the chemical/ transport process involved, a predictive understanding of tropospheric ozone climatology requires a focus on the chemical and transport processes that link regional emissions to hemispheric ozone trends and distributions. Of critical importance to these studies is a satisfactory data base of tropospheric ozone distribution from which global and regional tropospheric ozone climatology can be derived, and the processes controlling tropospheric ozone can be better understood. A transportable lidar for measuring ozone concentration and flux profiles in the lower troposphere is needed. One such system is being developed at the National Oceanic and Atmospheric Administration/Earth Resources Laboratory (NOAA/ERL) Wave Propagation Laboratory (WPL)

Evaluating the lower-tropospheric COSMIC GPS radio occultation sounding quality over the Arctic

Science.gov (United States)

Yu, Xiao; Xie, Feiqin; Ao, Chi O.

2018-04-01

Lower-tropospheric moisture and temperature measurements are crucial for understanding weather prediction and climate change. Global Positioning System radio occultation (GPS RO) has been demonstrated as a high-quality observation technique with high vertical resolution and sub-kelvin temperature precision from the upper troposphere to the stratosphere. In the tropical lower troposphere, particularly the lowest 2 km, the quality of RO retrievals is known to be degraded and is a topic of active research. However, it is not clear whether similar problems exist at high latitudes, particularly over the Arctic, which is characterized by smooth ocean surface and often negligible moisture in the atmosphere. In this study, 3-year (2008-2010) GPS RO soundings from COSMIC (Constellation Observing System for Meteorology, Ionosphere, and Climate) over the Arctic (65-90° N) show uniform spatial sampling with average penetration depth within 300 m above the ocean surface. Over 70 % of RO soundings penetrate deep into the lowest 300 m of the troposphere in all non-summer seasons. However, the fraction of such deeply penetrating profiles reduces to only about 50-60 % in summer, when near-surface moisture and its variation increase. Both structural and parametric uncertainties of GPS RO soundings were also analyzed. The structural uncertainty (due to different data processing approaches) is estimated to be within ˜ 0.07 % in refractivity, ˜ 0.72 K in temperature, and ˜ 0.05 g kg-1 in specific humidity below 10 km, which is derived by comparing RO retrievals from two independent data processing centers. The parametric uncertainty (internal uncertainty of RO sounding) is quantified by comparing GPS RO with near-coincident radiosonde and European Centre for Medium-Range Weather Forecasts (ECMWF) ERA-Interim profiles. A systematic negative bias up to ˜ 1 % in refractivity below 2 km is only seen in the summer, which confirms the moisture impact on GPS RO quality.

Improvement of OMI Ozone Profile Retrievals in the Troposphere and Lower Troposphere by the Use of the Tropopause-Based Ozone Profile Climatology

Science.gov (United States)

Bak, Juseon; Liu, X.; Wei, J.; Kim, J. H.; Chance, K.; Barnet, C.

2011-01-01

An advance algorithm based on the optimal estimation technique has beeen developed to derive ozone profile from GOME UV radiances and have adapted it to OMI UV radiances. OMI vertical resolution : 7-11 km in the troposphere and 10-14 km in the stratosphere. Satellite ultraviolet measurements (GOME, OMI) contain little vertical information for the small scale of ozone, especially in the upper troposphere (UT) and lower stratosphere (LS) where the sharp O3 gradient across the tropopause and large ozone variability are observed. Therefore, retrievals depend greatly on the a-priori knowledge in the UTLS

MUSICA MetOp/IASI {H2O,δD} pair retrieval simulations for validating tropospheric moisture pathways in atmospheric models

Science.gov (United States)

Schneider, Matthias; Borger, Christian; Wiegele, Andreas; Hase, Frank; García, Omaira E.; Sepúlveda, Eliezer; Werner, Martin

2017-02-01

The project MUSICA (MUlti-platform remote Sensing of Isotopologues for investigating the Cycle of Atmospheric water) has shown that the sensor IASI aboard the satellite MetOp can measure the free tropospheric {H2O,δD} pair distribution twice per day on a quasi-global scale. Such data are very promising for investigating tropospheric moisture pathways, however, the complex data characteristics compromise their usage in the context of model evaluation studies. Here we present a tool that allows for simulating MUSICA MetOp/IASI {H2O,δD} pair remote sensing data for a given model atmosphere, thereby creating model data that have the remote sensing data characteristics assimilated. This model data can then be compared to the MUSICA data. The retrieval simulation method is based on the physical principles of radiative transfer and we show that the uncertainty of the simulations is within the uncertainty of the MUSICA MetOp/IASI products, i.e. the retrieval simulations are reliable enough. We demonstrate the working principle of the simulator by applying it to ECHAM5-wiso model data. The few case studies clearly reveal the large potential of the MUSICA MetOp/IASI {H2O,δD} data pairs for evaluating modelled moisture pathways. The tool is made freely available in form of MATLAB and Python routines and can be easily connected to any atmospheric water vapour isotopologue model.

In situ measurements of the NO{sub x} distribution and variability over the eastern North Atlantic

Energy Technology Data Exchange (ETDEWEB)

Ziereis, H.; Schlager, H.; Schulte, P.; Koehler, I.; Marquardt, R.; Feigl, C.

1998-11-01

Between 1994 and 1996 the research aircraft Falcon of the ``Deutsches Zentrum fuer Luft- und Raumfahrt (DLR)`` was used to probe the upper troposphere and lowermost stratosphere over the eastern North Atlantic. In situ measurements of NO, NO{sub 2}, and O{sub 3} were performed during 32 flights. The measurements were carried out during five aircraft campaigns in summer and late autumn, respectively, based from Shannon/Ireland and Prestwick/Scotland. Most of the flights were conducted in the region of the North Atlantic flight corridor. Main objectives of these measurements included the study of the large scale distribution of NO and NO{sub x} and the development of a ``climatology`` of NO{sub x} in a region of the atmosphere that is strongly affected by aircraft emissions. Substantial variability of NO and NO{sub x} volume mixing ratios was observed in the upper troposphere and lowermost stratosphere. In spite of this variability a significant seasonal dependence was found. NO mean values (averages over all measurements made during one campaign) at altitudes between 10,500 and 11,500 m, where most of the data have been obtained, ranged between about 0.1 and 0.14 ppbv in summer and 0.03 and 0.10 ppbv in late autumn. NO and NO{sub x} did not show a significant gradient across the tropopause. The correlation between NO{sub x} and O{sub 3} in the upper troposphere and lowermost stratosphere was only very weak. The present measurements represent a suitable data set for comparison with predictions of the NO{sub x} distribution in the upper troposphere over the eastern North Atlantic by three dimensional models. A comparison with the NO{sub x} fields simulated with the climate model ECHAM 3 extended by a simplified NO{sub x} chemistry reveals good agreement for summer and autumn conditions. (orig.) 44 refs.

Chemical and climatic drivers of radiative forcing due to changes in stratospheric and tropospheric ozone over the 21st century

Science.gov (United States)

Banerjee, Antara; Maycock, Amanda C.; Pyle, John A.

2018-02-01

The ozone radiative forcings (RFs) resulting from projected changes in climate, ozone-depleting substances (ODSs), non-methane ozone precursor emissions and methane between the years 2000 and 2100 are calculated using simulations from the UM-UKCA chemistry-climate model (UK Met Office's Unified Model containing the United Kingdom Chemistry and Aerosols sub-model). Projected measures to improve air-quality through reductions in non-methane tropospheric ozone precursor emissions present a co-benefit for climate, with a net global mean ozone RF of -0.09 W m-2. This is opposed by a positive ozone RF of 0.05 W m-2 due to future decreases in ODSs, which is driven by an increase in tropospheric ozone through stratosphere-to-troposphere transport of air containing higher ozone amounts. An increase in methane abundance by more than a factor of 2 (as projected by the RCP8.5 scenario) is found to drive an ozone RF of 0.18 W m-2, which would greatly outweigh the climate benefits of non-methane tropospheric ozone precursor reductions. A small fraction (˜ 15 %) of the ozone RF due to the projected increase in methane results from increases in stratospheric ozone. The sign of the ozone RF due to future changes in climate (including the radiative effects of greenhouse gases, sea surface temperatures and sea ice changes) is shown to be dependent on the greenhouse gas emissions pathway, with a positive RF (0.05 W m-2) for RCP4.5 and a negative RF (-0.07 W m-2) for the RCP8.5 scenario. This dependence arises mainly from differences in the contribution to RF from stratospheric ozone changes. Considering the increases in tropopause height under climate change causes only small differences (≤ |0.02| W m-2) for the stratospheric, tropospheric and whole-atmosphere RFs.

Interferences in photolytic NO2 measurements: explanation for an apparent missing oxidant?

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C. Reed

2016-04-01

Full Text Available Measurement of NO2 at low concentrations (tens of ppts is non-trivial. A variety of techniques exist, with the conversion of NO2 into NO followed by chemiluminescent detection of NO being prevalent. Historically this conversion has used a catalytic approach (molybdenum; however, this has been plagued with interferences. More recently, photolytic conversion based on UV-LED irradiation of a reaction cell has been used. Although this appears to be robust there have been a range of observations in low-NOx environments which have measured higher NO2 concentrations than might be expected from steady-state analysis of simultaneously measured NO, O3, jNO2, etc. A range of explanations exist in the literature, most of which focus on an unknown and unmeasured “compound X” that is able to convert NO to NO2 selectively. Here we explore in the laboratory the interference on the photolytic NO2 measurements from the thermal decomposition of peroxyacetyl nitrate (PAN within the photolysis cell. We find that approximately 5 % of the PAN decomposes within the instrument, providing a potentially significant interference. We parameterize the decomposition in terms of the temperature of the light source, the ambient temperature, and a mixing timescale ( ∼ 0.4 s for our instrument and expand the parametric analysis to other atmospheric compounds that decompose readily to NO2 (HO2NO2, N2O5, CH3O2NO2, IONO2, BrONO2, higher PANs. We apply these parameters to the output of a global atmospheric model (GEOS-Chem to investigate the global impact of this interference on (1 the NO2 measurements and (2 the NO2 : NO ratio, i.e. the Leighton relationship. We find that there are significant interferences in cold regions with low NOx concentrations such as the Antarctic, the remote Southern Hemisphere, and the upper troposphere. Although this interference is likely instrument-specific, the thermal decomposition to NO2 within the instrument's photolysis

Software for Generating Troposphere Corrections for InSAR Using GPS and Weather Model Data

Science.gov (United States)

Moore, Angelyn W.; Webb, Frank H.; Fishbein, Evan F.; Fielding, Eric J.; Owen, Susan E.; Granger, Stephanie L.; Bjoerndahl, Fredrik; Loefgren, Johan; Fang, Peng; Means, James D.;

The distribution and speciation of mercury in the free troposphere of the Pacific Northwest

Science.gov (United States)

Swartzendruber, Philip C.

2009-12-01

suggests that upper tropospheric influence is not a controlling factor. There was no mean vertical trend in total Hg (GEM + RGM) up to 5 km. The only factor common to all high RGM, was low aerosol scattering (<2 M/m).

Influence of char texture and volatile matter content on NO emissions

Energy Technology Data Exchange (ETDEWEB)

Arenillas, A.; Rubiera, F.; Parra, J.B.; Moreno, A.H.; Pis, J.J. [Inst. National Vacional del Carbon, Oviedo (Spain)

1997-12-31

A low volatile bituminous coal was pyrolysed in a quartz reactor under nitrogen at different heating rates (5, 10, 50 and 150 C/min) up to a final temperature of 850 C. Textural characterisation (mercury porosimetry, adsorption isotherms of N{sub 2} and CO{sub 2}, ASA) of the chars was carried out in order to study the influence of textural properties on char reactivity and NO emissions. The role of volatile matter content in the emission of nitrogen compounds was also investigated. A thermogravimetric analyser linked to a quadrupole mass spectrometer (TG-MS) was used to study the compounds evolved during pyrolysis and combustion. (orig.)