scholarly journals Inverse modeling of SO<sub>2</sub> and NO<sub><i>x</i></sub> emissions over China using multi-sensor satellite data: 1. formulation and sensitivity analysis

2019 ◽  
Author(s):  
Yi Wang ◽  
Jun Wang ◽  
Xiaoguang Xu ◽  
Daven K. Henze ◽  
Zhen Qu

Abstract. SO2 and NO2 observations from the Ozone Mapping and Profiler Suite (OMPS) sensor are used for the first time in conjunction with GEOS-Chem adjoint model to optimize both SO2 and NOx emission estimates over China for October 2013. OMPS SO2 and NO2 observations are first assimilated separately to optimize emissions of SO2 and NOx, respectively. Posterior emissions, compared to the prior, yield improvements in simulating columnar SO2 and NO2, in comparison to measurements from OMI and OMPS. The posterior SO2 and NOx emissions from separate inversions are 748 Gg S and 672 Gg N, which are 36 % and 6 % smaller than prior MIX emissions, respectively. In spite of the large reduction of SO2 emissions over the North China Plain, the simulated sulfate-nitrate-ammonium Aerosol Optical Depth (AOD) only decrease slightly, which can be attributed to (a) nitrate rather than sulfate as the dominant contributor to AOD and (b) replacement of ammonium sulfate with ammonium nitrate as SO2 emissions are reduced. Both data quality control and the weight given to SO2 relative to NO2 observations can affect the spatial distributions of the joint inversion results. When the latter is properly balanced, the posterior emissions from assimilating OMPS SO2 and NO2 jointly yield a difference of −3 % to 15 % with respect to the separate assimilations for total anthropogenic SO2 emissions and ± 2 % for total anthropogenic NOx emissions; but the differences can be up to 100 % for SO2 and 40 % for NO2 in some grid cells. Improvements on SO2 and NO2 simulations evaluated with OMPS and OMI measurements from the joint inversions are overall consistent with those from separate inversions. Moreover, the joint assimilations save ~ 50 % of the computational time than assimilating SO2 and NO2 separately when computational resources are limited to run one inversion at a time sequentially. The sensitivity analysis shows that a perturbation of NH3 to 50 % (20 %) of the prior emission inventory: (a) has negligible impact on the separate SO2 inversion, but can lead to decrease of posterior SO2 emissions over China by −2.4 % (−7.0 %) in total and up to −9.0 % (−27.7 %) in some grid cells in the joint inversion with NO2; (b) yield posterior NOx emissions over China decrease by −0.7 % (−2.8 %) for the separate NO2 inversion and by −2.7 % (−5.3 %) in total and up to −15.2 % (−29.4 %) in some grid cells for the joint inversion. The large reduction of SO2 between 2010 and 2013, however, only leads to ~ 10 % decrease of aerosol optical depth regionally; reducing surface aerosol concentration requires the reduction of emissions of NH3 as well.

2020 ◽  
Vol 20 (11) ◽  
pp. 6631-6650 ◽  
Author(s):  
Yi Wang ◽  
Jun Wang ◽  
Xiaoguang Xu ◽  
Daven K. Henze ◽  
Zhen Qu ◽  
...  

Abstract. SO2 and NO2 observations from the Ozone Mapping and Profiler Suite (OMPS) sensor are used for the first time in conjunction with the GEOS-Chem adjoint model to optimize both SO2 and NOx emission estimates over China for October 2013. Separate and joint (simultaneous) optimizations of SO2 and NO2 emissions are both conducted and compared. Posterior emissions, compared to the prior, yield improvements in simulating columnar SO2 and NO2, in comparison to measurements from the Ozone Monitoring Instrument (OMI) and OMPS. The posterior SO2 and NOx emissions from separate inversions are 748 Gg S and 672 Gg N, which are 36 % and 6 % smaller than prior MIX emissions (valid for 2010), respectively. In spite of the large reduction of SO2 emissions over the North China Plain, the simulated sulfate–nitrate–ammonium aerosol optical depth (AOD) only decrease slightly, which can be attributed to (a) nitrate rather than sulfate as the dominant contributor to AOD and (b) replacement of ammonium sulfate with ammonium nitrate as SO2 emissions are reduced. For joint inversions, both data quality control and the weight given to SO2 relative to NO2 observations can affect the spatial distributions of the posterior emissions. When the latter is properly balanced, the posterior emissions from assimilating OMPS SO2 and NO2 jointly yield a difference of −3 % to 15 % with respect to the separate assimilations for total anthropogenic SO2 emissions and ±2 % for total anthropogenic NOx emissions; but the differences can be up to 100 % for SO2 and 40 % for NO2 in some grid cells. Improvements on SO2 and NO2 simulations from the joint inversions are overall consistent with those from separate inversions. Moreover, the joint assimilations save ∼ 50 % of the computational time compared to assimilating SO2 and NO2 separately in a sequential manner of computation. The sensitivity analysis shows that a perturbation of NH3 to 50 % (20 %) of the prior emission inventory can (a) have a negligible impact on the separate SO2 inversion but can lead to a decrease in posterior SO2 emissions over China by −2.4 % (−7.0 %) in total and up to −9.0 % (−27.7 %) in some grid cells in the joint inversion with NO2 and (b) yield posterior NOx emission decreases over China by −0.7 % (−2.8 %) for the separate NO2 inversion and by −2.7 % (−5.3 %) in total and up to −15.2 % (−29.4 %) in some grid cells for the joint inversion. The large reduction of SO2 between 2010 and 2013, however, only leads to ∼ 10 % decrease in AOD regionally; reducing surface aerosol concentration requires the reduction of emissions of NH3 as well.


2014 ◽  
Vol 14 (4) ◽  
pp. 2015-2038 ◽  
Author(s):  
J. M. Livingston ◽  
J. Redemann ◽  
Y. Shinozuka ◽  
R. Johnson ◽  
P. B. Russell ◽  
...  

Abstract. Airborne sunphotometer measurements acquired by the NASA Ames Airborne Tracking Sunphotometer (AATS-14) aboard the NASA P-3 research aircraft are used to evaluate dark-target over-land retrievals of extinction aerosol optical depth (AOD) from spatially and temporally near-coincident measurements by the Moderate Resolution Imaging Spectroradiometer (MODIS) during the summer 2008 Arctic Research of the Composition of the Troposphere from Aircraft and Satellites (ARCTAS) field campaign. The new MODIS Collection 6 aerosol data set includes retrievals of AOD at both 10 km × 10 km and 3 km × 3 km (at nadir) resolution. In this paper we compare MODIS and AATS AOD at 553 nm in 58 10 km and 134 3 km retrieval grid cells. These AOD values were derived from data collected over Canada on four days during short time segments of five (four Aqua and one Terra) satellite overpasses of the P-3 during low-altitude P-3 flight tracks. Three of the five MODIS–AATS coincidence events were dominated by smoke: one included a P-3 transect of a well-defined smoke plume in clear sky, but two were confounded by the presence of scattered clouds above smoke. The clouds limited the number of MODIS retrievals available for comparison, and led to MODIS AOD retrievals that underestimated the corresponding AATS values. This happened because the MODIS aerosol cloud mask selectively removed 0.5 km pixels containing smoke and clouds before the aerosol retrieval. The other two coincidences (one Terra and one Aqua) occurred during one P-3 flight on the same day and in the same general area, in an atmosphere characterized by a relatively low AOD (< 0.3), spatially homogeneous regional haze from smoke outflow with no distinguishable plume. For the ensemble data set for MODIS AOD retrievals with the highest-quality flag, MODIS AOD agrees with AATS AOD within the expected MODIS over-land AOD uncertainty in 60% of the retrieval grid cells at 10 km resolution and 69% at 3 km resolution. These values improve to 65 % and 74%, respectively, when the cloud-affected case with the strongest plume is excluded. We find that the standard MODIS dark-target over-land retrieval algorithm fails to retrieve AOD for thick smoke, not only in cloud-contaminated regions but also in clear sky. We attribute this to deselection, by the cloud and/or bright surface masks, of 0.5 km resolution pixels that contain smoke.


Atmosphere ◽  
2020 ◽  
Vol 11 (4) ◽  
pp. 360 ◽  
Author(s):  
Laura Palacios-Peña ◽  
Juan P. Montávez ◽  
José M. López-Romero ◽  
Sonia Jerez ◽  
Juan J. Gómez-Navarro ◽  
...  

Aerosol-cloud interactions (ACI) represent one of the most important sources of uncertainties in climate modelling. In this sense, realistic simulations of ACI are needed for a better understanding of the complex interactions between air pollution and the climate system. This work quantifies the added value of including ACI in an online coupled climate/chemistry model (WRF-Chem, 0.44 ∘ horizontal resolution, years 2003 to 2010) in order to assess whether there is an improvement in the representation of aerosol optical depth (AOD). Modelling results for each species have been evaluated against the Copernicus Atmosphere Monitoring Service (CAMS) reanalysis, and AOD at 675 nm has been compared to AERONET data. Results indicate that the improvements of the monthly biases are around 8% for total AOD550 when including ACI, reaching 20% for the monthly bias in AOD550 coming from dust. Moreover, the temporal representation of AOD550 largely improves (increase in the Pearson time correlation coefficients), ranging from 6% to 20% depending on the chemical species considered. The benefits from this improvement overcome the problems derived from the high computational time required in ACI simulations (eight times higher with respect to simulations not including aerosol-cloud interactions).


2011 ◽  
Vol 11 (8) ◽  
pp. 21971-21993 ◽  
Author(s):  
S. Itahashi ◽  
I. Uno ◽  
K. Yumimoto ◽  
H. Irie ◽  
K. Osada ◽  
...  

Abstract. Anthropogenic SO2 emissions increased alongside economic development in China at a rate of 12.7 % yr−1 from 2000 to 2005. However, under new Chinese government policy, SO2 emissions declined by 3.9 % yr−1 between 2005 and 2009. Between 2000 and 2010, we found that the variability in the fine-mode (submicron) aerosol optical depth (AOD) over the oceans adjacent to East Asia increased by 4–8 % yr−1 to a peak around 2005–2006 and subsequently decreased by 4–7 % yr−1, based on observations by the Moderate Resolution Imaging Spectroradiometer (MODIS) on board NASA's Terra satellite and simulations by a chemical transport model. This trend is consistent with ground-based observations of the number-size distribution of aerosol particles at a mountainous background observation site in central Japan. These fluctuations in SO2 emission intensity and AOD are thought to reflect the widespread installation of fuel-gas desulfurization (FGD) devices in power plants in China because aerosol sulfate is a major determinant of the AOD in East Asia. Using a chemical transport model, we confirmed that the above-mentioned fluctuation in AOD is mainly caused by changes in SO2 emission rather than by varying meteorological conditions in East Asia. High correlation was also found between satellite-retrieved SO2 vertical column density and bottom-up SO2 emissions, both of which were also consistent with observed AOD trends. We proposed a simplified approach for evaluating changes in SO2 emissions in China, combining the use of modeled sensitivity coefficients that describe the variation of AOD with changes in SO2 emissions and satellite retrieval. Satellite measurements of the AOD above Sea of Japan marked the 4.1 % yr−1 declining between 2007 and 2010, and this correspond to the SO2 emissions from China decreased by ~9 % yr−1 between the same period.


2013 ◽  
Vol 13 (6) ◽  
pp. 15007-15059 ◽  
Author(s):  
J. M. Livingston ◽  
J. Redemann ◽  
Y. Shinozuka ◽  
R. Johnson ◽  
P. B. Russell ◽  
...  

Abstract. Airborne sunphotometer measurements acquired by the NASA Ames Airborne Tracking Sunphotometer (AATS-14) from the NASA P-3 research aircraft are used to evaluate dark-target over-land retrievals of extinction aerosol optical depth (AOD) from spatially and temporally near-coincident measurements by the Moderate Resolution Imaging Spectroradiometer (MODIS) during the summer 2008 Arctic Research of the Composition of the Troposphere from Aircraft and Satellites (ARCTAS) field campaign. The new MODIS Collection 6 aerosol data set includes retrievals of AOD at both 10 km × 10 km and 3 km × 3 km (at nadir) resolution. In this paper we compare MODIS and AATS AOD at 553 nm in 58 10 km and 134 3 km retrieval grid cells. These AOD values were derived from data collected over Canada on four days during short time segments of five (four Aqua and one Terra) satellite overpasses of the P-3 during low altitude P-3 flight tracks. Three of the five MODIS/AATS coincidence events were dominated by smoke: one included a P-3 transect of a well-defined smoke plume in clear sky, but two were confounded by the presence of scattered clouds above smoke. The clouds limited the number of MODIS retrievals available for comparison, and led to MODIS AOD retrievals that underestimated the corresponding AATS values. This happened because the MODIS aerosol cloud mask selectively removed 0.5 km pixels containing smoke and clouds before the aerosol retrieval. The other two coincidences (one Terra and one Aqua) occurred during one P-3 flight on the same day and in the same general area, in an atmosphere characterized by a relatively low AOD (< 0.3), and spatially homogeneous regional haze from smoke outflow with no distinguishable plume. For the ensemble data set for MODIS AOD retrievals with the highest-quality flag, MODIS AOD agrees with AATS AOD within the expected MODIS over-land AOD uncertainty in 60% of the retrieval grid cells at 10 km resolution and 69% at 3 km resolution. These values improve to 65% and 74%, respectively, when the cloud-contaminated case with the strongest plume is excluded. We find that the standard MODIS dark-target over-land retrieval algorithm fails to retrieve AOD for thick smoke, not only in cloud-contaminated regions, but also in clear sky. We attribute this to deselection, by the cloud and/or bright surface masks, of 0.5 km resolution pixels that contain smoke.


2012 ◽  
Vol 12 (5) ◽  
pp. 2631-2640 ◽  
Author(s):  
S. Itahashi ◽  
I. Uno ◽  
K. Yumimoto ◽  
H. Irie ◽  
K. Osada ◽  
...  

Abstract. Anthropogenic SO2 emissions increased alongside economic development in China at a rate of 12.7% yr−1 from 2000 to 2005. However, under new Chinese government policy, SO2 emissions declined by 3.9% yr−1 between 2005 and 2009. Between 2000 and 2010, we found that the variability in the fine-mode (submicron) aerosol optical depth (AOD) over the oceans adjacent to East Asia increased by 3–8% yr−1 to a peak around 2005–2006 and subsequently decreased by 2–7% yr−1, based on observations by the Moderate Resolution Imaging Spectroradiometer (MODIS) on board NASA's Terra satellite and simulations by a chemical transport model. This trend is consistent with ground-based observations of aerosol particles at a mountainous background observation site in central Japan. These fluctuations in SO2 emission intensity and fine-mode AOD are thought to reflect the widespread installation of fuel-gas desulfurization (FGD) devices in power plants in China, because aerosol sulfate is a major determinant of the fine-mode AOD in East Asia. Using a chemical transport model, we confirmed that the contribution of particulate sulfate to the fine-mode AOD is more than 70% of the annual mean and that the abovementioned fluctuation in fine-mode AOD is caused mainly by changes in SO2 emission rather than by other factors such as varying meteorological conditions in East Asia. A strong correlation was also found between satellite-retrieved SO2 vertical column density and bottom-up SO2 emissions, both of which were also consistent with observed fine-mode AOD trends. We propose a simplified approach for evaluating changes in SO2 emissions in China, combining the use of modeled sensitivity coefficients that describe the variation of fine-mode AOD with changes in SO2 emissions and satellite retrieval. Satellite measurements of fine-mode AOD above the Sea of Japan marked a 4.1% yr−1 decline between 2007 and 2010, which corresponded to the 9% yr−1 decline in SO2 emissions from China during the same period.


2012 ◽  
Vol 69 (3) ◽  
pp. 1037-1053 ◽  
Author(s):  
Omar Torres ◽  
Hiren Jethva ◽  
P. K. Bhartia

Abstract A large fraction of the atmospheric aerosol load reaching the free troposphere is frequently located above low clouds. Most commonly observed aerosols above clouds are carbonaceous particles generally associated with biomass burning and boreal forest fires, and mineral aerosols originating in arid and semiarid regions and transported across large distances, often above clouds. Because these aerosols absorb solar radiation, their role in the radiative transfer balance of the earth–atmosphere system is especially important. The generally negative (cooling) top-of-the-atmosphere direct effect of absorbing aerosols may turn into warming when the light-absorbing particles are located above clouds. The actual effect depends on the aerosol load and the single scattering albedo, and on the geometric cloud fraction. In spite of its potential significance, the role of aerosols above clouds is not adequately accounted for in the assessment of aerosol radiative forcing effects due to the lack of measurements. This paper discusses the basis of a simple technique that uses near-UV observations to simultaneously derive the optical depth of both the aerosol layer and the underlying cloud for overcast conditions. The two-parameter retrieval method described here makes use of the UV aerosol index and reflectance measurements at 388 nm. A detailed sensitivity analysis indicates that the measured radiances depend mainly on the aerosol absorption exponent and aerosol–cloud separation. The technique was applied to above-cloud aerosol events over the southern Atlantic Ocean, yielding realistic results as indicated by indirect evaluation methods. An error analysis indicates that for typical overcast cloudy conditions and aerosol loads, the aerosol optical depth can be retrieved with an accuracy of approximately 54% whereas the cloud optical depth can be derived within 17% of the true value.


Sign in / Sign up

Export Citation Format

Share Document