scholarly journals Constraints on Asian ozone using Aura TES, OMI and Terra MOPITT

2014 ◽  
Vol 14 (13) ◽  
pp. 19515-19544
Author(s):  
Z. Jiang ◽  
J. R. Worden ◽  
D. B. A. Jones ◽  
J. T. Lin ◽  
W. W. Verstraeten ◽  
...  

Abstract. Rapid industrialization in Asia in the last two decades has resulted in a significant increase in Asian ozone (O3) pre-cursor emissions with likely a corresponding increase in the export of O3 and its pre-cursors. However, the relationship between this increasing O3, the chemical environment, O3 production efficiency, and the partitioning between anthropogenic and natural precursors is unclear. In this work, we use satellite measurements of O3, CO and NO2 from TES (Tropospheric Emission Spectrometer), MOPITT (Measurement of Pollution In The Troposphere) and OMI (Ozone Monitoring Instrument) to quantify O3 pre-cursor emissions for 2006 and their impact on free-tropospheric O3 over North-East Asia, where pollution is typically exported globally due to strong westerlies. Using the GEOS-Chem global chemical transport model, we show that the modeled seasonal variation of O3 based on these updated O3 pre-cursor emissions is consistent with the observed O3 variability and amount, after accounting for known biases in the TES O3 data. Using the adjoint of GEOS-Chem we then partition the relative contributions of natural and anthropogenic sources to free troposphere O3 in this region. We find that the influence of lightning NOx is important in summer. The contribution from anthropogenic NOx is dominant in other seasons. China is the major contributor of anthropogenic VOCs (Volatile Organic Compounds), whereas the influence of biogenic VOCs is mainly from Southeast Asia. Our result shows that the influence of India and Southeast Asia emissions on O3 pollution export is significant, comparable with Chinese emisisons in winter and about 50% of Chinese emissions in other seasons.

2015 ◽  
Vol 15 (1) ◽  
pp. 99-112 ◽  
Author(s):  
Z. Jiang ◽  
J. R. Worden ◽  
D. B. A. Jones ◽  
J.-T. Lin ◽  
W. W. Verstraeten ◽  
...  

Abstract. Rapid industrialization in Asia in the last two decades has resulted in a significant increase in Asian ozone (O3) precursor emissions with likely a corresponding increase in the export of O3 and its precursors. However, the relationship between this increasing O3, the chemical environment, O3 production efficiency, and the partitioning between anthropogenic and natural precursors is unclear. In this work, we use satellite measurements of O3, CO and NO2 from TES (Tropospheric Emission Spectrometer), MOPITT (Measurement of Pollution In The Troposphere) and OMI (Ozone Monitoring Instrument) to quantify O3 precursor emissions for 2006 and their impact on free tropospheric O3 over northeastern Asia, where pollution is typically exported globally due to strong westerlies. Using the GEOS-Chem (Goddard Earth Observing System Chemistry) global chemical transport model, we test the modeled seasonal and interannual variation of O3 based on prior and updated O3 precursor emissions where the updated emissions of CO and NOx are based on satellite measurements of CO and NO2. We show that the observed TES O3 variability and amount are consistent with the model for these updated emissions. However, there is little difference in the modeled ozone between the updated and prior emissions. For example, for the 2006 June time period, the prior and posterior NOx emissions were 14% different over China but the modeled ozone in the free troposphere was only 2.5% different. Using the adjoint of GEOS-Chem we partition the relative contributions of natural and anthropogenic sources to free troposphere O3 in this region. We find that the influence of lightning NOx in the summer is comparable to the contribution from surface emissions but smaller for other seasons. China is the primary contributor of anthropogenic CO, emissions and their export during the summer. While the posterior CO emissions improved the comparison between model and TES by 32%, on average, this change also had only a small effect on the free tropospheric ozone. Our results show that the influence of India and southeastern Asia emissions on O3 pollution export to the northwestern Pacific is sizeable, comparable with Chinese emissions in winter, about 50% of Chinese emissions in spring and fall, and approximately 20% of the emissions in the summer.


2014 ◽  
Vol 14 (7) ◽  
pp. 3277-3305 ◽  
Author(s):  
K. Miyazaki ◽  
H. J. Eskes ◽  
K. Sudo ◽  
C. Zhang

Abstract. The global source of lightning-produced NOx (LNOx) is estimated by assimilating observations of NO2, O3, HNO3, and CO measured by multiple satellite measurements into a chemical transport model. Included are observations from the Ozone Monitoring Instrument (OMI), Microwave Limb Sounder (MLS), Tropospheric Emission Spectrometer (TES), and Measurements of Pollution in the Troposphere (MOPITT) instruments. The assimilation of multiple chemical data sets with different vertical sensitivity profiles provides comprehensive constraints on the global LNOx source while improving the representations of the entire chemical system affecting atmospheric NOx, including surface emissions and inflows from the stratosphere. The annual global LNOx source amount and NO production efficiency are estimated at 6.3 Tg N yr−1 and 310 mol NO flash−1, respectively. Sensitivity studies with perturbed satellite data sets, model and data assimilation settings lead to an error estimate of about 1.4 Tg N yr−1 on this global LNOx source. These estimates are significantly different from those estimated from a parameter inversion that optimizes only the LNOx source from NO2 observations alone, which may lead to an overestimate of the source adjustment. The total LNOx source is predominantly corrected by the assimilation of OMI NO2 observations, while TES and MLS observations add important constraints on the vertical source profile. The results indicate that the widely used lightning parameterization based on the C-shape assumption underestimates the source in the upper troposphere and overestimates the peak source height by up to about 1 km over land and the tropical western Pacific. Adjustments are larger over ocean than over land, suggesting that the cloud height dependence is too weak over the ocean in the Price and Rind (1992) approach. The significantly improved agreement between the analyzed ozone fields and independent observations gives confidence in the performance of the LNOx source estimation.


2014 ◽  
Vol 14 (5) ◽  
pp. 2679-2698 ◽  
Author(s):  
E. V. Fischer ◽  
D. J. Jacob ◽  
R. M. Yantosca ◽  
M. P. Sulprizio ◽  
D. B. Millet ◽  
...  

Abstract. Peroxyacetyl nitrate (PAN) formed in the atmospheric oxidation of non-methane volatile organic compounds (NMVOCs) is the principal tropospheric reservoir for nitrogen oxide radicals (NOx = NO + NO2). PAN enables the transport and release of NOx to the remote troposphere with major implications for the global distributions of ozone and OH, the main tropospheric oxidants. Simulation of PAN is a challenge for global models because of the dependence of PAN on vertical transport as well as complex and uncertain NMVOC sources and chemistry. Here we use an improved representation of NMVOCs in a global 3-D chemical transport model (GEOS-Chem) and show that it can simulate PAN observations from aircraft campaigns worldwide. The immediate carbonyl precursors for PAN formation include acetaldehyde (44% of the global source), methylglyoxal (30%), acetone (7%), and a suite of other isoprene and terpene oxidation products (19%). A diversity of NMVOC emissions is responsible for PAN formation globally including isoprene (37%) and alkanes (14%). Anthropogenic sources are dominant in the extratropical Northern Hemisphere outside the growing season. Open fires appear to play little role except at high northern latitudes in spring, although results are very sensitive to plume chemistry and plume rise. Lightning NOx is the dominant contributor to the observed PAN maximum in the free troposphere over the South Atlantic.


2013 ◽  
Vol 13 (10) ◽  
pp. 26841-26891 ◽  
Author(s):  
E. V. Fischer ◽  
D. J. Jacob ◽  
R. M. Yantosca ◽  
M. P. Sulprizio ◽  
D. B. Millet ◽  
...  

Abstract. Peroxyacetyl nitrate (PAN) formed in the atmospheric oxidation of non-methane volatile organic compounds (NMVOCs), is the principal tropospheric reservoir for nitrogen oxide radicals (NOx = NO + NO2). PAN enables the transport and release of NOx to the remote troposphere with major implications for the global distributions of ozone and OH, the main tropospheric oxidants. Simulation of PAN is a challenge for global models because of the dependence of PAN on vertical transport as well as complex and uncertain NMVOC sources and chemistry. Here we use an improved representation of NMVOCs in a global 3-D chemical transport model (GEOS-Chem) and show that it can simulate PAN observations from aircraft campaigns worldwide. The immediate carbonyl precursors for PAN formation include acetaldehyde (44% of the global source), methylglyoxal (30%), acetone (7%), and a suite of other isoprene and terpene oxidation products (19%). A diversity of NMVOC emissions is responsible for PAN formation globally including isoprene (37%) and alkanes (14%). Anthropogenic sources are dominant in the extratropical Northern Hemisphere outside the growing season. Open fires appear to play little role except at high northern latitudes in spring, although results are very sensitive to plume chemistry and plume rise. Lightning NOx is the dominant contributor to the observed PAN maximum in the free troposphere over the South Atlantic.


2009 ◽  
Vol 9 (1) ◽  
pp. 2289-2317 ◽  
Author(s):  
C. Zhao ◽  
Y. Wang ◽  
Y. Choi ◽  
T. Zeng

Abstract. A 3-D regional chemical transport model (REAM) is applied to examine the uncertainties in modeling the effects of convective transport and lightning NOx production on upper tropospheric chemical tracer distributions. To assess the model uncertainties, two different cumulus convective parameterizations, KF-eta and Grell, are adopted in REAM from the respective meteorological models, WRF and MM5. The model simulations are evaluated using INTEX-NA aircraft measurements and satellite measurements of NO2 columns and cloud top pressure, and we find that mid and upper tropospheric trace gas concentrations are affected strongly by convection and lightning NOx productions. A major improvement of the KF-eta scheme is its inclusion of cloud entrainment and detrainment processes. KF-eta scheme simulates larger convective updraft mass fluxes below 150 hPa than the Grell scheme, resulting in more outflow of pollutants in the mid troposphere. The ratio of C2H6/C3H8 is found to be a sensitive parameter to convective outflow; the simulation by WRF-REAM is in closer agreement with INTEX-NA measurements than MM5-REAM, implying that convective mass fluxes by KF-eta scheme are more realistic. The inclusion of entrainment and detrainment processes in the KF-eta scheme also leads to lower cloud top heights (10–12 km) than the Grell scheme (up to 16 km), and hence smaller amounts of estimated (intra-cloud) lightning NOx and lower emission altitudes. WRF simulated cloud top heights are in better agreement with GOES satellite measurements than MM5. The model divergence on lightning NOx mostly is above 12 km. As a result, both models suggest that lightning NOx production enhances the concentrations of upper tropospheric NO2 by a factor of >5 (~100 pptv) and increases O3 by up to ~20 ppbv at 8–12 km.


2010 ◽  
Vol 10 (1) ◽  
pp. 1417-1456 ◽  
Author(s):  
L. Zhang ◽  
D. J. Jacob ◽  
X. Liu ◽  
J. A. Logan ◽  
K. Chance ◽  
...  

Abstract. We analyze three different methods to validate and intercompare satellite measurements of atmospheric composition, and apply them to tropospheric ozone retrievals from the Tropospheric Emission Spectrometer (TES) and the Ozone Monitoring Instrument (OMI). The first method (in situ method) uses in situ vertical profiles for absolute instrument validation; it is limited by the sparseness of in situ data. The second method (CTM method) uses a chemical transport model (CTM) as an intercomparison platform; it provides a globally complete intercomparison with relatively small noise added by model error. The third method (averaging kernel smoothing method) involves smoothing the retrieved profile from one instrument with the averaging kernel matrix of the other; it also provides a global intercomparison but dampens the actual difference between instruments and adds noise from the a priori. Application to a full year (2006) of TES and OMI data shows mean positive biases of 5.3 parts per billion volume (ppbv) (10%) for TES and 2.8 ppbv (5%) for OMI at 500 hPa relative to in situ data from ozonesondes. We show that the CTM method (using the GEOS-Chem CTM) closely approximates results from the in situ method while providing global coverage. It reveals that differences between TES and OMI are generally less than 10 ppbv (18%), except at northern mid-latitudes in summer and over tropical continents. The CTM method allows for well-constrained CTM evaluation in places where the satellite observations are consistent. We thus find that GEOS-Chem underestimates tropospheric ozone in the tropics, reflecting a combination of possible factors, and overestimates ozone in the northern subtropics and southern mid-latitudes, likely because of excessive stratospheric influx.


2018 ◽  
Author(s):  
Jerry R. Ziemke ◽  
Luke D. Oman ◽  
Sarah A. Strode ◽  
Anne R. Douglass ◽  
Mark A. Olsen ◽  
...  

Abstract. Past studies have suggested that ozone in the troposphere has increased globally throughout much of the 20th century due to increases in anthropogenic emissions and transport. We show by combining satellite measurements with a chemical transport model that during the last four decades tropospheric ozone does indeed indicate increases that are global in nature, yet still highly regional. Satellite ozone measurements from Nimbus-7 and Earth Probe Total Ozone Mapping Spectrometer (TOMS) are merged with ozone measurements from Aura Ozone Monitoring Instrument/Microwave Limb Sounder (OMI/MLS) to determine trends in tropospheric ozone for 1979–2016. Both TOMS (1979–2005) and OMI/MLS (2005–2016) depict large increases in tropospheric ozone from the Near East to India/East Asia and further eastward over the Pacific Ocean. The 38-year merged satellite record shows total net change over this region of about +6 to +7 Dobson Units (DU) (i.e., ~ 15–20 % of average background ozone), with the largest increase (~ 4 DU) occurring during the 2005–2016 Aura period. The Global Modeling Initiative (GMI) chemical transport model with time-varying emissions is included to evaluate tropospheric ozone trends for 1980–2016. The GMI simulation for the combined record also depicts greatest increases of +6 to +7 DU over India/east Asia, identical to the satellite measurements. In regions of significant increases in TCO the trends are a factor of 2–2.5 larger for the Aura record when compared to the earlier TOMS record; for India/east Asia the trends in TCO for both GMI and satellite measurements are ~ +3 DU-decade−1 or greater during 2005–2016 compared to about +1.2 to +1.4 DU-decade−1 for 1979–2016. The GMI simulation and satellite data also reveal a tropospheric ozone increase of ~ +4 to +5 DU for the 38-year record over central Africa and the tropical Atlantic Ocean. Both the GMI simulation and satellite-measured tropospheric ozone during the latter Aura time period show increases of ~ +3 DU-decade−1 over the NH Atlantic and NE Pacific.


2019 ◽  
Vol 19 (5) ◽  
pp. 3257-3269 ◽  
Author(s):  
Jerry R. Ziemke ◽  
Luke D. Oman ◽  
Sarah A. Strode ◽  
Anne R. Douglass ◽  
Mark A. Olsen ◽  
...  

Abstract. Past studies have suggested that ozone in the troposphere has increased globally throughout much of the 20th century due to increases in anthropogenic emissions and transport. We show, by combining satellite measurements with a chemical transport model, that during the last four decades tropospheric ozone does indeed indicate increases that are global in nature, yet still highly regional. Satellite ozone measurements from Nimbus-7 and Earth Probe Total Ozone Mapping Spectrometer (TOMS) are merged with ozone measurements from the Aura Ozone Monitoring Instrument/Microwave Limb Sounder (OMI/MLS) to determine trends in tropospheric ozone for 1979–2016. Both TOMS (1979–2005) and OMI/MLS (2005–2016) depict large increases in tropospheric ozone from the Near East to India and East Asia and further eastward over the Pacific Ocean. The 38-year merged satellite record shows total net change over this region of about +6 to +7 Dobson units (DU) (i.e., ∼15 %–20 % of average background ozone), with the largest increase (∼4 DU) occurring during the 2005–2016 Aura period. The Global Modeling Initiative (GMI) chemical transport model with time-varying emissions is used to aid in the interpretation of tropospheric ozone trends for 1980–2016. The GMI simulation for the combined record also depicts the greatest increases of +6 to +7 DU over India and East Asia, very similar to the satellite measurements. In regions of significant increases in tropospheric column ozone (TCO) the trends are a factor of 2–2.5 larger for the Aura record when compared to the earlier TOMS record; for India and East Asia the trends in TCO for both GMI and satellite measurements are ∼+3 DU decade−1 or greater during 2005–2016 compared to about +1.2 to +1.4 DU decade−1 for 1979–2005. The GMI simulation and satellite data also reveal a tropospheric ozone increases in ∼+4 to +5 DU for the 38-year record over central Africa and the tropical Atlantic Ocean. Both the GMI simulation and satellite-measured tropospheric ozone during the latter Aura time period show increases of ∼+3 DU decade−1 over the N Atlantic and NE Pacific.


2018 ◽  
Author(s):  
Jin Liao ◽  
Thomas F. Hanisco ◽  
Glenn M. Wolfe ◽  
Jason St. Clair ◽  
Jose L. Jimenez ◽  
...  

Abstract. Organic aerosol (OA) is one of the main components of the global particulate burden and intimately links natural and anthropogenic emissions with air quality and climate. It is challenging to accurately represent OA in global models. Direct quantification of global OA abundance is not possible with current remote sensing technology; however, it may be possible to exploit correlations of OA with remotely observable quantities to infer OA spatiotemporal variability. In particular, formaldehyde (HCHO) and OA share common sources via both primary emissions and secondary production from oxidation of volatile organic compounds (VOCs). We examine OA-HCHO correlations using data from summer-time airborne campaigns investigating biogenic (NASA SEAC4RS and DC3), biomass burning (NASA SEAC4RS) and anthropogenic conditions (NOAA CalNex and NASA KORUS-AQ). In situ OA correlates well with HCHO (r = 0.59–0.97) but the slope and intercept of this relationship vary with chemical regime. For biogenic and anthropogenic regions, the OA-vs-HCHO slope is higher in low NOx conditions, where HCHO yields are lower and aerosol yields are likely higher. The OA-vs-HCHO slope of wild fires is more than 9 times higher than that associated with biogenic and anthropogenic sources. An estimate of near-surface OA is derived by combining observed in situ relationships with HCHO column retrievals from NASA’s Ozone Monitoring Instrument (OMI). We evaluate this OA estimate against OA observations from the US EPA IMPROVE network and simulated OA from the GEOS-Chem global chemical transport model. The OA estimate compares well with IMPROVE data obtained over summer months (e.g. slope = 0.62, r = 0.56 for August 2013), comparable to intensively validated GEOS-Chem performance (e.g. slope = 0.57, r = 0.56) and superior to the correlation with satellite-derived total aerosol extinction (r = 0.41). Improving the detection limit of satellite HCHO and expanding in situ airborne HCHO and OA coverage in future missions will improve the quality and spatiotemporal coverage of this OA estimate, potentially enabling constraints on the global OA distribution.


2010 ◽  
Vol 10 (10) ◽  
pp. 4725-4739 ◽  
Author(s):  
L. Zhang ◽  
D. J. Jacob ◽  
X. Liu ◽  
J. A. Logan ◽  
K. Chance ◽  
...  

Abstract. We analyze the theoretical basis of three different methods to validate and intercompare satellite measurements of atmospheric composition, and apply them to tropospheric ozone retrievals from the Tropospheric Emission Spectrometer (TES) and the Ozone Monitoring Instrument (OMI). The first method (in situ method) uses in situ vertical profiles for absolute instrument validation; it is limited by the sparseness of in situ data. The second method (CTM method) uses a chemical transport model (CTM) as an intercomparison platform; it provides a globally complete intercomparison with relatively small noise from model error. The third method (averaging kernel smoothing method) involves smoothing the retrieved profile from one instrument with the averaging kernel matrix of the other; it also provides a global intercomparison but dampens the actual difference between instruments and adds noise from the a priori. We apply the three methods to a full year (2006) of TES and OMI data. Comparison with in situ data from ozonesondes shows mean positive biases of 5.3 parts per billion volume (ppbv) (10%) for TES and 2.8 ppbv (5%) for OMI at 500 hPa. We show that the CTM method (using the GEOS-Chem CTM) closely approximates results from the in situ method while providing global coverage. It reveals that differences between TES and OMI are generally less than 10 ppbv (18%), except at northern mid-latitudes in summer and over tropical continents. The CTM method further allows for CTM evaluation using both satellite observations. We thus find that GEOS-Chem underestimates tropospheric ozone in the tropics due to possible underestimates of biomass burning, soil, and lightning emissions. It overestimates ozone in the northern subtropics and southern mid-latitudes, likely because of excessive stratospheric influx of ozone.


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