scholarly journals Intercomparison methods for satellite measurements of atmospheric composition: application to tropospheric ozone from TES and OMI

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.

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.


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.


2013 ◽  
Vol 13 (4) ◽  
pp. 8901-8937 ◽  
Author(s):  
P. S. Kim ◽  
D. J. Jacob ◽  
X. Liu ◽  
J. X. Warner ◽  
K. Yang ◽  
...  

Abstract. We present a global data set of free tropospheric ozone–CO correlations with 2° × 2.5° spatial resolution from the Ozone Monitoring Instrument (OMI) and Atmospheric Infrared Sounder (AIRS) satellite instruments for each season of 2008. OMI and AIRS have near daily global coverage of ozone and CO respectively and observe coincident scenes with similar vertical sensitivities. The resulting ozone–CO correlations are highly statistically significant (positive or negative) in most regions of the world, and are less noisy than previous satellite-based studies that used sparser data. We interpret the observed ozone–CO correlations with the GEOS-Chem chemical transport model to infer constraints on ozone sources. Driving GEOS-Chem with different meteorological fields generally shows consistent ozone–CO correlation patterns, except in some tropical regions where the correlations are strongly sensitive to model transport error associated with deep convection. GEOS-Chem reproduces the general structure of the observed ozone–CO correlations and regression slopes (dO3/dCO), although there are some large regional discrepancies. We examine the model sensitivity of dO3/dCO to different ozone sources (combustion, biosphere, stratosphere, and lightning NOx) by correlating the ozone change from that source to CO from the standard simulation. The model reproduces the observed positive dO3/dCO in the extratropical Northern Hemisphere in spring–summer, driven by combustion sources. Stratospheric influence there is also associated with a positive dO3/dCO because of the interweaving of stratospheric downwelling with continental outflow. The well-known ozone maximum over the tropical South Atlantic is associated with negative dO3/dCO in the observations; this feature is reproduced in GEOS-Chem and supports a dominant contribution from lightning to the ozone maximum. A~major model discrepancy is found over the Northeast Pacific in summer-fall where dO3/dCO is positive in the observations but negative in the model, for all ozone sources. We suggest that this reflects a model overestimate of lightning at northern mid-latitudes combined with an underestimate of the East Asian CO source.


2013 ◽  
Vol 13 (8) ◽  
pp. 21455-21505
Author(s):  
E. Emili ◽  
B. Barret ◽  
S. Massart ◽  
E. Le Flochmoen ◽  
A. Piacentini ◽  
...  

Abstract. Accurate and temporally resolved fields of free-troposphere ozone are of major importance to quantify the intercontinental transport of pollution and the ozone radiative forcing. In this study we examine the impact of assimilating ozone observations from the Microwave Limb Sounder (MLS) and the Infrared Atmospheric Sounding Interferometer (IASI) in a global chemical transport model (MOdèle de Chimie Atmosphérique à Grande Échelle, MOCAGE). The assimilation of the two instruments is performed by means of a variational algorithm (4-D-VAR) and allows to constrain stratospheric and tropospheric ozone simultaneously. The analysis is first computed for the months of August and November 2008 and validated against ozone-sondes measurements to verify the presence of observations and model biases. It is found that the IASI Tropospheric Ozone Column (TOC, 1000–225 hPa) should be bias-corrected prior to assimilation and MLS lowermost level (215 hPa) excluded from the analysis. Furthermore, a longer analysis of 6 months (July–August 2008) showed that the combined assimilation of MLS and IASI is able to globally reduce the uncertainty (Root Mean Square Error, RMSE) of the modeled ozone columns from 30% to 15% in the Upper-Troposphere/Lower-Stratosphere (UTLS, 70–225 hPa) and from 25% to 20% in the free troposphere. The positive effect of assimilating IASI tropospheric observations is very significant at low latitudes (30° S–30° N), whereas it is not demonstrated at higher latitudes. Results are confirmed by a comparison with additional ozone datasets like the Measurements of OZone and wAter vapour by aIrbus in-service airCraft (MOZAIC) data, the Ozone Monitoring Instrument (OMI) total ozone columns and several high-altitude surface measurements. Finally, the analysis is found to be little sensitive to the assimilation parameters and the model chemical scheme, due to the high frequency of satellite observations compared to the average life-time of free-troposphere/low-stratosphere ozone.


2020 ◽  
Author(s):  
Alice Drinkwater ◽  
Tim Arnold ◽  
Paul Palmer

<p>Changes in atmospheric methane (CH<sub>4</sub>) are mainly driven by natural, anthropogenic and pyrogenic emissions and oxidation by OH.</p><p>There is no consensus about the underlying explanations about hemispheric-scale changes in atmospheric methane (CH<sub>4</sub>). This is partly due to sparse data that do not exclusively identify individual changes in surface emissions and surface and atmospheric losses of CH<sub>4</sub>. This challenge represents a major scientific weakness in our understanding of this potent greenhouse gas, with implications for meeting global climate policy obligations.  A confounding challenge is that the regional importance of individual emission sources change with time due to, for example, innovations in agricultural practices, climate-sensitive wetlands, and political decisions associated with climate friendlier transitional fuels.  </p><p><br>Here we use bulk isotope ratios δ<sup>13</sup>C and δD of CH<sub>4</sub> that have been previously shown to provide effective constraints on source apportionment: different CH<sub>4</sub> sources have characteristic isotope ratios. One of the key challenges associated with using these data is that region-specific isotope ratios change with time due to varying source prevalance, in addition to source signatures having inherent uncertainties. We use the GEOS-Chem global 3-D chemical transport model to describe the spatial and temporal isotopic behaviour of atmospheric CH<sub>4</sub>. We develop a Maximum A-Posteriori inverse method to simultaneously infer time dependent CH<sub>4</sub> emissions and isotope ratios from in situ data. </p><p>We will report the magnitude, distribution and source attribution of CH<sub>4</sub> emissions from 2004 to 2017, inferred from in situ measurements of total atmospheric CH<sub>4</sub> mole fraction and the corresponding measurements of δ<sup>13</sup>C and δD. We will compare our results with previous studies.</p>


2016 ◽  
Author(s):  
Whitney Bader ◽  
Benoît Bovy ◽  
Stephanie Conway ◽  
Kimberly Strong ◽  
Dan Smale ◽  
...  

Abstract. Changes of atmospheric methane (CH4) since 2005 have been evaluated using Fourier Transform Infrared (FTIR) solar observations performed at ten ground-based sites, all members of the Network for Detection of Atmospheric Composition Change (NDACC). From this, we find an increase of atmospheric methane total columns that amounts to 0.31 ± 0.03 % year−1 (2-sigma level of uncertainty) for the 2005–2014 period. Comparisons with in situ methane measurements at both local and global scales show good agreement. We used the GEOS-Chem Chemical Transport Model tagged simulation that accounts for the contribution of each emission source and one sink in the total methane, simulated over the 2005–2012 time period and based on emissions inventories and transport. After regridding according to NDACC vertical layering using a conservative regridding scheme and smoothing by convolving with respective FTIR seasonal averaging kernels, the GEOS-Chem simulation shows an increase of atmospheric methane of 0.35 ± 0.03 % year−1 between 2005 and 2012, which is in agreement with NDACC measurements over the same time period (0.30 ± 0.04 % year−1, averaged over ten stations). Analysis of the GEOS-Chem tagged simulation allows us to quantify the contribution of each tracer to the global methane change since 2005. We find that natural sources such as wetlands and biomass burning contribute to the inter-annual variability of methane. However, anthropogenic emissions such as coal mining, and gas and oil transport and exploration, which are mainly emitted in the Northern Hemisphere and act as secondary contributors to the global budget of methane, have played a major role in the increase of atmospheric methane observed since 2005. Based on the GEOS-Chem tagged simulation, we discuss possible cause(s) for the increase of methane since 2005, which is still unexplained.


2008 ◽  
Vol 8 (1) ◽  
pp. 1505-1548 ◽  
Author(s):  
K. W. Bowman ◽  
D. Jones ◽  
J. Logan ◽  
H. Worden ◽  
F. Boersma ◽  
...  

Abstract. The chemical and dynamical processes governing the zonal variability of tropical tropospheric ozone and carbon monoxide are investigated for November 2004 using satellite observations, in-situ measurements, and chemical transport models in conjunction with inverse-estimated surface emissions. Vertical ozone profile estimates from the Tropospheric Emission Spectrometer (TES) and ozone sonde measurements from the Southern Hemisphere Additional Ozonesondes (SHADOZ) network show the so-called zonal "wave-one" pattern, which is characterized by peak ozone concentrations (70–80 ppb) centered over the Atlantic, as well as elevated concentrations of ozone over Indonesia and Australia (60–70 ppb) in the lower troposphere. 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., 2007). 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% and led to changes in GEOS-Chem upper tropospheric ozone of up to 40% over Indonesia. The remaining residual differences can be explained in part by upper tropospheric ozone produced from lightning NOx in the South Atlantic. Furthermore, model simulations from GEOS-Chem indicate that ozone over Indonesian/Australian is more sensitive to changes in surface emissions of NOx than ozone over the tropical Atlantic.


2014 ◽  
Vol 14 (1) ◽  
pp. 177-198 ◽  
Author(s):  
E. Emili ◽  
B. Barret ◽  
S. Massart ◽  
E. Le Flochmoen ◽  
A. Piacentini ◽  
...  

Abstract. Accurate and temporally resolved fields of free-troposphere ozone are of major importance to quantify the intercontinental transport of pollution and the ozone radiative forcing. We consider a global chemical transport model (MOdèle de Chimie Atmosphérique à Grande Échelle, MOCAGE) in combination with a linear ozone chemistry scheme to examine the impact of assimilating observations from the Microwave Limb Sounder (MLS) and the Infrared Atmospheric Sounding Interferometer (IASI). The assimilation of the two instruments is performed by means of a variational algorithm (4D-VAR) and allows to constrain stratospheric and tropospheric ozone simultaneously. The analysis is first computed for the months of August and November 2008 and validated against ozonesonde measurements to verify the presence of observations and model biases. Furthermore, a longer analysis of 6 months (July–December 2008) showed that the combined assimilation of MLS and IASI is able to globally reduce the uncertainty (root mean square error, RMSE) of the modeled ozone columns from 30 to 15% in the upper troposphere/lower stratosphere (UTLS, 70–225 hPa). The assimilation of IASI tropospheric ozone observations (1000–225 hPa columns, TOC – tropospheric O3 column) decreases the RMSE of the model from 40 to 20% in the tropics (30° S–30° N), whereas it is not effective at higher latitudes. Results are confirmed by a comparison with additional ozone data sets like the Measurements of OZone and wAter vapour by aIrbus in-service airCraft (MOZAIC) data, the Ozone Monitoring Instrument (OMI) total ozone columns and several high-altitude surface measurements. Finally, the analysis is found to be insensitive to the assimilation parameters. We conclude that the combination of a simplified ozone chemistry scheme with frequent satellite observations is a valuable tool for the long-term analysis of stratospheric and free-tropospheric ozone.


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.


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