scholarly journals The zonal structure of tropical O<sub>3</sub> and CO as observed by the Tropospheric Emission Spectrometer in November 2004 – Part 1: Inverse modeling of CO emissions

2009 ◽  
Vol 9 (11) ◽  
pp. 3547-3562 ◽  
Author(s):  
D. B. A. Jones ◽  
K. W. Bowman ◽  
J. A. Logan ◽  
C. L. Heald ◽  
J. Liu ◽  
...  

Abstract. We conduct an inverse modeling analysis of measurements of atmospheric CO from the TES and MOPITT satellite instruments using the GEOS-Chem global chemical transport model to quantify emissions of CO in the tropics in November 2004. We also assess the consistency of the information provided by TES and MOPITT on surface emissions of CO. We focus on the tropics in November 2004, during the biomass burning season, because TES observations of CO and O3 and MOPITT observations of CO reveal significantly greater abundances of these gases than simulated by the GEOS-Chem model during that period. We find that both datasets suggest substantially greater emissions of CO from sub-equatorial Africa and the Indonesian/Australian region than in the climatological emissions in the model. The a posteriori emissions from sub-equatorial Africa based on TES and MOPITT data were 173 Tg CO/yr and 184 Tg CO/yr, respectively, compared to the a priori of 95 Tg CO/yr. In the Indonesian/Australian region, the a posteriori emissions inferred from TES and MOPITT data were 155 Tg CO/yr and 185 Tg CO/yr, respectively, whereas the a priori was 69 Tg CO/yr. The differences between the a posteriori emission estimates obtained from the two datasets are generally less than 20%. The a posteriori emissions significantly improve the simulated distribution of CO, however, large regional residuals remain, and are likely due to systematic errors in the analysis. Reducing these residuals and improving the accuracy of top-down emission estimates will require better characterization of systematic errors in the observations and the model (chemistry and transport).

2007 ◽  
Vol 7 (6) ◽  
pp. 17625-17662 ◽  
Author(s):  
D. B. A. Jones ◽  
K. W. Bowman ◽  
J. A. Logan ◽  
C. L. Heald ◽  
J. Liu ◽  
...  

Abstract. We conduct an inverse modeling analysis of measurements of atmospheric CO from the TES and MOPITT satellite instruments using the GEOS-Chem global chemical transport model. This is the first quantitative analysis of the consistency of the information provided by these two instruments on surface emissions of CO in an inverse modeling context. We focus on observations of CO for November 2004, when the climatological emission inventory in the GEOS-Chem model significantly underestimated the atmospheric abundance of CO as observed by TES and MOPITT. We find that both datasets suggest significantly greater emissions of CO from sub-equatorial Africa and the Indonesian/Australian region. The a posteriori emissions from sub-equatorial Africa based on TES and MOPITT data were 173 Tg CO/yr and 184 Tg CO/yr, respectively, compared to the a priori of 95 Tg CO/yr. In the Indonesian/Australian region, the a posteriori emissions inferred from TES and MOPITT data were 155 Tg CO/yr and 185 Tg CO/yr, respectively, whereas the a priori was 69 Tg CO/yr. The differences between the a posteriori emission estimates obtained from the two datasets are generally less than 20%, and are likely due to the different spatio-temporal sampling of the measurements. The a posteriori emissions significantly improve the simulated distribution of CO, however, large regional residuals remain, reflecting systematic errors in the analysis. For example, the a posteriori emissions obtained from both datasets do not completely reduce the underestimate in the model of CO column abundances over the southern tropical Atlantic, southern Africa, and over the Indian Ocean, where biases of 3–7% remain. Over eastern Asia the a posteriori emissions overestimate the CO column abundances by about 3–6%. These residuals reflect the sensitivity of the top-down source estimates to systematic errors in the analysis. Our results indicate that improving the accuracy of top-down emission estimates will require further characterization of model biases (chemical and transport) and the use of spatial-temporal inversion resolutions consistent with the information content of the observations.


2010 ◽  
Vol 10 (3) ◽  
pp. 855-876 ◽  
Author(s):  
M. Kopacz ◽  
D. J. Jacob ◽  
J. A. Fisher ◽  
J. A. Logan ◽  
L. Zhang ◽  
...  

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


2013 ◽  
Vol 13 (8) ◽  
pp. 21883-21926
Author(s):  
K. C. Wells ◽  
D. B. Millet ◽  
K. E. Cady-Pereira ◽  
M. W. Shephard ◽  
D. K. Henze ◽  
...  

Abstract. We employ new global space-based measurements of atmospheric methanol from the Tropospheric Emission Spectrometer (TES) with the adjoint of the GEOS-Chem chemical transport model to quantify terrestrial emissions of methanol to the atmosphere. Biogenic methanol emissions in the model are based on MEGANv2.1 emission algorithms, using MODIS leaf area and GEOS-5 assimilated meteorological fields. We first carry out a pseudo observation test to validate the overall approach, and find that the TES sampling density is sufficient to accurately quantify regional- to continental-scale methanol emissions using this method. A global inversion of two years of TES data yields an optimized annual global surface flux of 117 Tg yr−1 (including biogenic, pyrogenic, and anthropogenic sources), an increase of 56% from the a priori global flux of 75 Tg yr−1. Global terrestrial methanol emissions are thus approximately 25% those of isoprene (~540 Tg yr−1), and are comparable to the combined emissions of all anthropogenic volatile organic compounds (~100–200 Tg yr−1). Our a posteriori terrestrial methanol source leads to a strong improvement of the simulation relative to an ensemble of airborne observations, and corroborates two other recent top-down estimates (114–120 Tg yr−1) derived using in-situ and space-based measurements. The TES data imply a relatively modest revision of model emissions over most of the tropics, but a significant upward revision in midlatitudes, particularly over Europe and North America. We interpret the inversion results in terms of specific source types using the methanol:CO correlations measured by TES, and find that biogenic emissions are overestimated relative to biomass burning and anthropogenic emissions in central Africa and southeastern China, while they are underestimated in regions such as Brazil and the US. Based on our optimized emissions, methanol accounts for >25% of the photochemical source of CO and HCHO over many parts of the northern extratropics during springtime, and contributes ~6% of the global secondary source of those compounds annually.


2009 ◽  
Vol 9 (5) ◽  
pp. 19967-20018 ◽  
Author(s):  
M. Kopacz ◽  
D. J. Jacob ◽  
J. A. Fisher ◽  
J. A. Logan ◽  
L. Zhang ◽  
...  

Abstract. We combine CO column measurements from the MOPITT, AIRS, SCIAMACHY, and TES satellite instruments in a full-year (May 2004–April 2005) global inversion of CO sources at 4°×5° spatial resolution and monthly temporal resolution. The inversion uses the GEOS-Chem chemical transport model (CTM) and its adjoint applied to MOPITT, AIRS, and SCIAMACHY. Observations from TES, surface sites (NOAA/GMD), and aircraft (MOZAIC) are used for evaluation of the a posteriori solution. Global intercomparison of the different satellite datasets using GEOS-Chem as a common intercomparison platform shows consistency between the satellite datasets and with the in situ data. The majority of the differences between the datasets can be explained by different averaging kernels and a priori information. The global CO emission from combustion as constrained in the inversion is 1350 Tg a−1, with an additional 217 Tg a−1 from oxidation of co-emitted VOCs. This is much higher than current bottom-up emission inventories. Consistent with both the satellite and in situ data, a large fraction of the correction results from a seasonal underestimate of CO sources at northern mid-latitudes and suggests a larger-than-expected CO source from vehicle cold starts and residential heating. A posteriori emissions also indicate a general underestimation of biomass burning relative to the GFED2 inventory. However, the tropical biomass burning constraints are not consistent across the different datasets. Although the datasets reveal regional inconsistencies over tropical biomass burning regions, we find the global emission estimates to be a balance of information from all three instruments.


Atmosphere ◽  
2021 ◽  
Vol 12 (7) ◽  
pp. 900
Author(s):  
Ioanna Skoulidou ◽  
Maria-Elissavet Koukouli ◽  
Arjo Segers ◽  
Astrid Manders ◽  
Dimitris Balis ◽  
...  

In this work, we investigate the ability of a data assimilation technique and space-borne observations to quantify and monitor changes in nitrogen oxides (NOx) emissions over Northwestern Greece for the summers of 2018 and 2019. In this region, four lignite-burning power plants are located. The data assimilation technique, based on the Ensemble Kalman Filter method, is employed to combine space-borne atmospheric observations from the high spatial resolution Sentinel-5 Precursor (S5P) Tropospheric Monitoring Instrument (TROPOMI) and simulations using the LOTOS-EUROS Chemical Transport model. The Copernicus Atmosphere Monitoring Service-Regional European emissions (CAMS-REG, version 4.2) inventory based on the year 2015 is used as the a priori emissions in the simulations. Surface measurements of nitrogen dioxide (NO2) from air quality stations operating in the region are compared with the model surface NO2 output using either the a priori (base run) or the a posteriori (assimilated run) NOx emissions. Relative to the a priori emissions, the assimilation suggests a strong decrease in concentrations for the station located near the largest power plant, by 80% in 2019 and by 67% in 2018. Concerning the estimated annual a posteriori NOx emissions, it was found that, for the pixels hosting the two largest power plants, the assimilated run results in emissions decreased by ~40–50% for 2018 compared to 2015, whereas a larger decrease, of ~70% for both power plants, was found for 2019, after assimilating the space-born observations. For the same power plants, the European Pollutant Release and Transfer Register (E-PRTR) reports decreased emissions in 2018 and 2019 compared to 2015 (−35% and −38% in 2018, −62% and −72% in 2019), in good agreement with the estimated emissions. We further compare the a posteriori emissions to the reported energy production of the power plants during the summer of 2018 and 2019. Mean decreases of about −35% and−63% in NOx emissions are estimated for the two larger power plants in summer of 2018 and 2019, respectively, which are supported by similar decreases in the reported energy production of the power plants (~−30% and −70%, respectively).


2017 ◽  
Vol 17 (11) ◽  
pp. 6663-6678 ◽  
Author(s):  
Shreeya Verma ◽  
Julia Marshall ◽  
Mark Parrington ◽  
Anna Agustí-Panareda ◽  
Sebastien Massart ◽  
...  

Abstract. Airborne observations of greenhouse gases are a very useful reference for validation of satellite-based column-averaged dry air mole fraction data. However, since the aircraft data are available only up to about 9–13 km altitude, these profiles do not fully represent the depth of the atmosphere observed by satellites and therefore need to be extended synthetically into the stratosphere. In the near future, observations of CO2 and CH4 made from passenger aircraft are expected to be available through the In-Service Aircraft for a Global Observing System (IAGOS) project. In this study, we analyse three different data sources that are available for the stratospheric extension of aircraft profiles by comparing the error introduced by each of them into the total column and provide recommendations regarding the best approach. First, we analyse CH4 fields from two different models of atmospheric composition – the European Centre for Medium-Range Weather Forecasts (ECMWF) Integrated Forecasting System for Composition (C-IFS) and the TOMCAT/SLIMCAT 3-D chemical transport model. Secondly, we consider scenarios that simulate the effect of using CH4 climatologies such as those based on balloons or satellite limb soundings. Thirdly, we assess the impact of using a priori profiles used in the satellite retrievals for the stratospheric part of the total column. We find that the models considered in this study have a better estimation of the stratospheric CH4 as compared to the climatology-based data and the satellite a priori profiles. Both the C-IFS and TOMCAT models have a bias of about −9 ppb at the locations where tropospheric vertical profiles will be measured by IAGOS. The C-IFS model, however, has a lower random error (6.5 ppb) than TOMCAT (12.8 ppb). These values are well within the minimum desired accuracy and precision of satellite total column XCH4 retrievals (10 and 34 ppb, respectively). In comparison, the a priori profile from the University of Leicester Greenhouse Gases Observing Satellite (GOSAT) Proxy XCH4 retrieval and climatology-based data introduce larger random errors in the total column, being limited in spatial coverage and temporal variability. Furthermore, we find that the bias in the models varies with latitude and season. Therefore, applying appropriate bias correction to the model fields before using them for profile extension is expected to further decrease the error contributed by the stratospheric part of the profile to the total column.


2014 ◽  
Vol 7 (2) ◽  
pp. 1645-1689
Author(s):  
E. Hache ◽  
J.-L. Attié ◽  
C. Tourneur ◽  
P. Ricaud ◽  
L. Coret ◽  
...  

Abstract. Ozone is a tropospheric pollutant and plays a key role in determining the air quality that affects human wellbeing. In this study, we compare the capability of two hypothetical grating spectrometers onboard a geostationary (GEO) satellite to sense ozone in the lowermost troposphere (surface and the 0–1 km column). We consider one week during the Northern Hemisphere summer simulated by a chemical transport model, and use the two GEO instrument configurations to measure ozone concentration (1) in the thermal infrared (GEO TIR) and (2) in the thermal infrared and the visible (GEO TIR+VIS). These configurations are compared against each other, and also against an ozone reference state and a priori ozone information. In a first approximation, we assume clear sky conditions neglecting the influence of aerosols and clouds. A number of statistical tests are used to assess the performance of the two GEO configurations. We consider land and sea pixels and whether differences between the two in the performance are significant. Results show that the GEO TIR+VIS configuration provides a better representation of the ozone field both for surface ozone and the 0–1 km ozone column during the daytime especially over land.


1995 ◽  
Vol 166 ◽  
pp. 372-372
Author(s):  
L. G. Taff ◽  
J. E. Morrison ◽  
R. L. Smart

As better precision is achieved and more sophisticated reduction methods are created previously invisible biases surface. This has been especially true in astrometric Schmidt plate work. The problem of their amelioration is not fully solved and precision per se is meaningless in the presence of poor accuracy of comparable amplitude. Continuing to benignly neglect this issue puts us in the position of standing on only one statistical leg. New techniques have been designed to further minimize systematic errors. Of especial interest to star catalog analysis is the method of infinitely overlapping circles (Taff, Bucciarelli & Lattanzi, ApJ 361, 667, 1990; Taff, Bucciarelli & Lattanzi, ApJ 392, 746 1992; Bucciarelli, Taff & Lattanzi, J. Stat. Comp. and Sim. 48, 29 1993). With it almost complete success has occurred with regard to the removal of systematic errors which creep into compilation catalogs as a result of inadequate treatment of catalog-to-catalog systematic errors; they can essentially be eliminated a priori or a posteriori (Bucciarelli, Lattanzi & Taff, in press in ApJ 1994; Taff & Bucciarelli, in press in ApJ 1994). What infinitely overlapping circles does can be briefly described as follows: Let X (x) be the measured (true) value of a standard coordinate, S(x,y) (ε) be the systematic (random) error in x at this point, let w∞ be the infinitely overlapping circle weight, a be the standard deviation of the random error in x, N be the total number of stars in this circle which has radius R, and x0,y0 be the coordinates of the center of this circle.


2009 ◽  
Vol 9 (19) ◽  
pp. 7313-7323 ◽  
Author(s):  
H. Wang ◽  
D. J. Jacob ◽  
M. Kopacz ◽  
D. B. A. Jones ◽  
P. Suntharalingam ◽  
...  

Abstract. Inverse modeling of CO2 satellite observations to better quantify carbon surface fluxes requires a chemical transport model (CTM) to relate the fluxes to the observed column concentrations. CTM transport error is a major source of uncertainty. We show that its effect can be reduced by using CO satellite observations as additional constraint in a joint CO2-CO inversion. CO is measured from space with high precision, is strongly correlated with CO2, and is more sensitive than CO2 to CTM transport errors on synoptic and smaller scales. Exploiting this constraint requires statistics for the CTM transport error correlation between CO2 and CO, which is significantly different from the correlation between the concentrations themselves. We estimate the error correlation globally and for different seasons by a paired-model method (comparing GEOS-Chem CTM simulations of CO2 and CO columns using different assimilated meteorological data sets for the same meteorological year) and a paired-forecast method (comparing 48- vs. 24-h GEOS-5 CTM forecasts of CO2 and CO columns for the same forecast time). We find strong error correlations (r2>0.5) between CO2 and CO columns over much of the extra-tropical Northern Hemisphere throughout the year, and strong consistency between different methods to estimate the error correlation. Application of the averaging kernels used in the retrieval for thermal IR CO measurements weakens the correlation coefficients by 15% on average (mostly due to variability in the averaging kernels) but preserves the large-scale correlation structure. We present a simple inverse modeling application to demonstrate that CO2-CO error correlations can indeed significantly reduce uncertainty on surface carbon fluxes in a joint CO2-CO inversion vs. a CO2-only inversion.


2019 ◽  
Vol 19 (21) ◽  
pp. 13569-13579 ◽  
Author(s):  
Helen M. Worden ◽  
A. Anthony Bloom ◽  
John R. Worden ◽  
Zhe Jiang ◽  
Eloise A. Marais ◽  
...  

Abstract. Biogenic non-methane volatile organic compounds (NMVOCs) emitted from vegetation are a primary source for the chemical production of carbon monoxide (CO) in the atmosphere, and these biogenic emissions account for about 18 % of the global CO burden. Partitioning CO fluxes to different source types in top-down inversion methods is challenging; typically a simple scaling of the posterior flux to prior flux values for fossil fuel, biogenic and biomass burning sources is used. Here we show top-down estimates of biogenic CO fluxes using a Bayesian inference approach, which explicitly accounts for both posterior and a priori CO flux uncertainties. This approach re-partitions CO fluxes following inversion of Measurements Of Pollution In The Troposphere (MOPITT) CO observations with the GEOS-Chem model, a global chemical transport model driven by assimilated meteorology from the NASA Goddard Earth Observing System (GEOS). We compare these results to the prior information for CO used to represent biogenic NMVOCs from GEOS-Chem, which uses the Model of Emissions of Gases and Aerosols from Nature (MEGAN) for biogenic emissions. We evaluate the a posteriori biogenic CO fluxes against top-down estimates of isoprene fluxes using Ozone Monitoring Instrument (OMI) formaldehyde observations. We find similar seasonality and spatial consistency in the posterior CO and top-down isoprene estimates globally. For the African savanna region, both top-down CO and isoprene seasonality vary significantly from the MEGAN a priori inventory. This method for estimating biogenic sources of CO will provide an independent constraint on modeled biogenic emissions and has the potential for diagnosing decadal-scale changes in emissions due to land-use change and climate variability.


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