scholarly journals Satellite constraint for emissions of nitrogen oxides from anthropogenic, lightning and soil sources over East China on a high-resolution grid

2012 ◽  
Vol 12 (6) ◽  
pp. 2881-2898 ◽  
Author(s):  
J.-T. Lin

Abstract. Vertical column densities (VCDs) of tropospheric nitrogen dioxide (NO2) retrieved from space provide valuable information to estimate emissions of nitrogen oxides (NOx) inversely. Accurate emission attribution to individual sources, important both for understanding the global biogeochemical cycling of nitrogen and for emission control, remains difficult. This study presents a regression-based multi-step inversion approach to estimate emissions of NOx from anthropogenic, lightning and soil sources individually for 2006 over East China on a 0.25° long × 0.25° lat grid, employing the DOMINO product version 2 retrieved from the Ozone Monitoring Instrument. The inversion is done gridbox by gridbox to derive the respective emissions, taking advantage of differences in seasonality between anthropogenic and natural sources. Lightning and soil emissions are combined together for any given gridbox due to their similar seasonality; and their different spatial distributions are used implicitly for source separation to some extent. The nested GEOS-Chem model for East Asia is used to simulate the seasonal variations of different emission sources and impacts on VCDs of NO2 for the inversion purpose. Sensitivity tests are conducted to evaluate key assumptions embedded in the inversion process. The inverse estimate suggests annual budgets of about 7.1 TgN (±39%), 0.21 TgN (±61%), and 0.38 TgN (±65%) for the a posteriori anthropogenic, lightning and soil emissions, respectively, about 18–23% higher than the respective a priori values. The enhancements in anthropogenic emissions are largest in cities and areas with extensive use of coal, particularly in the north in winter, as evident on the high-resolution grid. Derived soil emissions are consistent with recent bottom-up estimates. They are less than 6% of anthropogenic emissions annually, increasing to about 13% for July. Derived lightning emissions are about 3% of anthropogenic emissions annually and about 10% in July. Overall, anthropogenic emissions are found to be the dominant source of NOx over East China with important implications for nitrogen control.

2011 ◽  
Vol 11 (11) ◽  
pp. 29807-29843 ◽  
Author(s):  
J.-T. Lin

Abstract. Vertical column densities (VCDs) of tropospheric nitrogen dioxide (NO2) retrieved from space provide valuable information to estimate emissions of nitrogen oxides (NOx) inversely. Accurate emission attribution to individual sources, important both for understanding the global biogeochemical cycling of nitrogen and for emission control, remains difficult. This study presents a regression-based multi-step inversion approach to estimate emissions of NOx from anthropogenic, lightning and soil sources individually for 2006 over East China on a 0.25° long × 0.25° lat grid, employing the DOMINO product version 2 retrieved from the Ozone Monitoring Instrument. The nested GEOS-Chem model for East Asia is used to simulate the seasonal variations of different emission sources and impacts on VCDs of NO2 for the inversion purpose. Sensitivity tests are conducted to evaluate key assumptions embedded in the inversion process. The inverse estimate suggests annual budgets of about 7.1 TgN (±38%), 0.22 TgN (±46%), and 0.40 TgN (±48%) for the a posteriori anthropogenic, lightning and soil emissions, respectively, each about 24% higher than the respective a priori values. The enhancements in anthropogenic emissions are largest in cities and areas with extensive use of coal, particularly in the north in winter, as evident on the high-resolution grid. Derived soil emissions are consistent with recent bottom-up estimates. They are each less than 6% of anthropogenic emissions annually, increasing to about 13% for July. Overall, anthropogenic emissions are found to be the dominant source of NOx over East China with important implications for nitrogen control.


2009 ◽  
Vol 9 (5) ◽  
pp. 19205-19241 ◽  
Author(s):  
J.-T. Lin ◽  
M. B. McElroy ◽  
K. F. Boersma

Abstract. A new methodology is developed to constrain Chinese anthropogenic emissions of nitrogen oxides (NOx) from four major sectors (industry, power plants, mobile and residential) in July 2008. It combines tropospheric NO2 column retrievals from GOME-2 and OMI, taking advantage of their different passing time over China (9:30 a.m. local time versus 1:30 p.m.), and explicitly accounts for diurnal variations in anthropogenic emissions of NOx as well as their tropospheric lifetime and column concentrations. The approach is based on the daytime variation of NOx (when its lifetime is relatively short) alone; and potential errors in inverse modeling by neglecting horizontal transport are minimized. Separation of anthropogenic sectors relies on the estimated diurnal profiles and budget uncertainties. Our best top-down estimate suggests a national budget of 6.8 Tg N/yr (5.5 Tg N/yr for East China), close to the a priori bottom-up emission estimate from the INTEX-B mission. The top-down emissions are lower than the a priori near Beijing, in the northeastern provinces and along the east coast; yet they exceed the a priori over many inland regions. Systematic errors in satellite retrievals are estimated to lead to underestimation of top-down emissions by at most 17% (most likely 10%). Effects of other factors on the top-down estimate are typically less than 15%, including lightning, soil emissions, mixing in planetary boundary layer, anthropogenic emissions of carbon monoxide and volatile organic compounds, assumptions on emission diurnal variations, and uncertainties in the four sectors. The a posteriori emission budget is 5.7 Tg N/yr for East China.


2018 ◽  
Vol 10 (4) ◽  
pp. 2069-2095 ◽  
Author(s):  
Joshua L. Laughner ◽  
Qindan Zhu ◽  
Ronald C. Cohen

Abstract. We describe upgrades to the Berkeley High Resolution (BEHR) NO2 satellite retrieval product. BEHR v3.0B builds on the NASA version 3 standard Ozone Monitoring Instrument (OMI) tropospheric NO2 product to provide a high spatial resolution product for a domain covering the continental United States and lower Canada that is consistent with daily variations in the 12 km a priori NO2 profiles. Other improvements to the BEHR v3.0 product include surface reflectance and elevation, and factors affecting the NO2 a priori profiles such as lightning and anthropogenic emissions.We describe the retrieval algorithm in detail and evaluate the impact of changes to the algorithm between v2.1C and v3.0B on the retrieved NO2 vertical column densities (VCDs). Not surprisingly, we find that, on average, the changes to the a priori NO2 profiles and the update to the new NASA slant column densities have the greatest impact on the retrieved VCDs. More significantly, we find that using daily a priori profiles results in greater average VCDs than using monthly profiles in regions and times with significant lightning activity.The BEHR product is available as four subproducts on the University of California DASH repository, using monthly a priori profiles at native OMI pixel resolution (https://doi.org/10.6078/D1N086) and regridded to 0.05° × 0.05° (https://doi.org/10.6078/D1RQ3G) and using daily a priori profiles at native OMI (https://doi.org/10.6078/D1WH41) and regridded (https://doi.org/10.6078/D12D5X) resolutions. The subproducts using monthly profiles are currently available from January 2005 to July 2017, and will be expanded to more recent years. The subproducts using daily profiles are currently available for years 2005–2010 and 2012–2014; 2011 and 2015 on will be added as the necessary input data are simulated for those years.


2018 ◽  
Author(s):  
Joshua L. Laughner ◽  
Qindan Zhu ◽  
Ronald C. Cohen

Abstract. We describe upgrades to the Berkeley High Resolution (BEHR) NO2 satellite retrieval product. BEHR v3.0 builds on the NASA version 3 standard Ozone Monitoring Instrument (OMI) tropospheric NO2 product to provide a high spatial resolution product that is consistent with daily variations in the 12 km a priori NO2 profiles. Other improvements to the BEHR v3.0 product include surface reflectance and elevation, and factors affecting the NO2 a priori profiles such as lightning and anthropogenic emissions. We describe the retrieval algorithm in detail and evaluate the impact of changes to the algorithm between v2.1C and v3.0B has on the retrieved NO2 vertical column densities (VCDs). Not surprisingly, we find that, on average, the changes to the a priori NO2 profiles and the update to the new NASA slant column densities have the greatest impact on the retrieved VCDs. More significantly, we find that using daily a priori profiles results in greater average VCDs than using monthly profiles in regions and times with significant lightning activity. The BEHR product is available as four subproducts on the University of California DASH repository: using monthly a priori profiles at native OMI pixel resolution (https://doi.org/10.6078/D1N086) and regridded to 0.05° × 0.05° (https://doi.org/10.6078/D1RQ3G) and using daily a priori profiles at native OMI ( https://doi.org/10.6078/D1WH41) and regridded (https: //doi.org/10.6078/D12D5X) resolutions.


2019 ◽  
Vol 12 (11) ◽  
pp. 6091-6111 ◽  
Author(s):  
Laura M. Judd ◽  
Jassim A. Al-Saadi ◽  
Scott J. Janz ◽  
Matthew G. Kowalewski ◽  
R. Bradley Pierce ◽  
...  

Abstract. NASA deployed the GeoTASO airborne UV–visible spectrometer in May–June 2017 to produce high-resolution (approximately 250 m×250 m) gapless NO2 datasets over the western shore of Lake Michigan and over the Los Angeles Basin. The results collected show that the airborne tropospheric vertical column retrievals compare well with ground-based Pandora spectrometer column NO2 observations (r2=0.91 and slope of 1.03). Apparent disagreements between the two measurements can be sensitive to the coincidence criteria and are often associated with large local variability, including rapid temporal changes and spatial heterogeneity that may be observed differently by the sunward-viewing Pandora observations. The gapless mapping strategy executed during the 2017 GeoTASO flights provides data suitable for averaging to coarser areal resolutions to simulate satellite retrievals. As simulated satellite pixel area increases to values typical of TEMPO (Tropospheric Emissions: Monitoring Pollution), TROPOMI (TROPOspheric Monitoring Instrument), and OMI (Ozone Monitoring Instrument), the agreement with Pandora measurements degraded, particularly for the most polluted columns as localized large pollution enhancements observed by Pandora and GeoTASO are spatially averaged with nearby less-polluted locations within the larger area representative of the satellite spatial resolutions (aircraft-to-Pandora slope: TEMPO scale =0.88; TROPOMI scale =0.77; OMI scale =0.57). In these two regions, Pandora and TEMPO or TROPOMI have the potential to compare well at least up to pollution scales of 30×1015 molecules cm−2. Two publicly available OMI tropospheric NO2 retrievals are found to be biased low with respect to these Pandora observations. However, the agreement improves when higher-resolution a priori inputs are used for the tropospheric air mass factor calculation (NASA V3 standard product slope =0.18 and Berkeley High Resolution product slope =0.30). Overall, this work explores best practices for satellite validation strategies with Pandora direct-sun observations by showing the sensitivity to product spatial resolution and demonstrating how the high-spatial-resolution NO2 data retrieved from airborne spectrometers, such as GeoTASO, can be used with high-temporal-resolution ground-based column observations to evaluate the influence of spatial heterogeneity on validation results.


2011 ◽  
Vol 11 (15) ◽  
pp. 8171-8188 ◽  
Author(s):  
J.-T. Lin ◽  
M. B. McElroy

Abstract. Rapid economic and industrial development in China and relatively weak emission controls have resulted in significant increases in emissions of nitrogen oxides (NOx) in recent years, with the exception of late 2008 to mid 2009 when the economic downturn led to emission reductions detectable from space. Here vertical column densities (VCDs) of tropospheric NO2 retrieved from satellite observations by SCIAMACHY, GOME-2 and OMI (both by KNMI and by NASA) are used to evaluate changes in emissions of NOx from October 2004 to February 2010 identifying impacts of the economic downturn. Data over polluted regions of Northern East China suggest an increase of 27–33 % in 12-month mean VCD of NO2 prior to the downturn, consistent with an increase of 49 % in thermal power generation (TPG) reflecting the economic growth. More detailed analysis is used to quantify changes in emissions of NOx in January over the period 2005–2010 when the effect of the downturn was most evident. The GEOS-Chem model is employed to evaluate the effect of changes in chemistry and meteorology on VCD of NO2. This analysis indicates that emissions decreased by 20 % from January 2008 to January 2009, close to the reduction of 18 % in TPG that occurred over the same interval. A combination of three independent approaches indicates that the economic downturn was responsible for a reduction in emissions by 9–11 % in January 2009 with an additional decrease of 10 % attributed to the slow-down in industrial activity associated with the coincident celebration of the Chinese New Year; errors in the estimate are most likely less than 3.4 %.


2011 ◽  
Vol 11 (1) ◽  
pp. 193-223 ◽  
Author(s):  
J.-T. Lin ◽  
M. B. McElroy

Abstract. Rapid economic and industrial development in China and relatively weak emission controls have resulted in significant increases in emissions of nitrogen oxides (NOx) in recent years, with the exception of late 2008 to mid 2009 when the economic downturn led to emission reductions detectable from space. Here vertical column densities (VCDs) of tropospheric NO2 retrieved from satellite observations by SCIAMACHY, GOME-2 and OMI (both by KNMI and by NASA) are used to evaluate changes in emissions of NOx from October 2004 to February 2010 identifying impacts of the economic downturn. Data over polluted regions of Northern East China suggest an increase of 27–33% in annual mean VCD of NO2 prior to the downturn, consistent with an increase of 49% in thermal power generation (TPG) reflecting the economic growth. More detailed analysis is used to quantify changes in emissions of NOx in January over the period 2005–2010 when the effect of the downturn was most evident. The GEOS-Chem model is employed to evaluate the effect of changes in chemistry and meteorology on VCD of NO2. This analysis indicates that emissions decreased by 20% from January 2008 to January 2009, close to the reduction of 18% in TPG that occurred over the same interval. A combination of three relatively independent approaches indicates that the economic downturn was responsible for a~reduction in emissions by 9–11% in January 2009 with an additional decrease of 10% attributed to the slow-down in industrial activity associated with the coincident celebration of the Chinese New Year.


2020 ◽  
Author(s):  
Can Li ◽  
Nickolay A. Krotkov ◽  
Peter J. T. Leonard ◽  
Simon Carn ◽  
Joanna Joiner ◽  
...  

Abstract. The Ozone Monitoring Instrument (OMI) has been providing global observations of SO2 pollution since 2004. Here we introduce the new anthropogenic SO2 vertical column density (VCD) dataset in the version 2 OMI SO2 product (OMSO2 V2). As with the previous version (OMSO2 V1.3), the new dataset is generated with an algorithm based on principal component analysis of OMI radiances, but features several updates. The most important among those is the use of expanded lookup tables and model a priori profiles to estimate SO2 Jacobians for individual OMI pixels, in order to better characterize pixel-to-pixel variations in SO2 sensitivity, including over snow and ice. Additionally, new data screening and spectral fitting schemes have been implemented to improve the quality of the spectral fit. As compared with the planetary boundary layer SO2 dataset in OMSO2 V1.3, the new dataset has substantially better data quality, especially over areas that are relatively clean or affected by the south Atlantic anomaly. The updated retrievals over snow/ice yield more realistic seasonal changes in SO2 at high latitudes and offer enhanced sensitivity to sources during wintertime. An error analysis has been conducted to assess uncertainties in SO2 VCDs from both the spectral fit and Jacobian calculations. The uncertainties from spectral fitting are reflected in SO2 slant column densities (SCDs) and largely depend on the signal-to-noise ratio of the measured radiances, as implied by the generally smaller SCD uncertainties over clouds or for lower solar zenith angles. The SCD uncertainties for individual pixels are estimated to be ~ 0.15–0.3 DU (Dobson Units) between ~ 40° S and ~ 40° N and to be ~ 0.2–0.5 DU at higher latitudes. The uncertainties from the Jacobians are approximately ~ 50–100 % over polluted areas, and primarily attributed to errors in SO2 a priori profiles and cloud pressures, as well as the lack of explicit treatment for aerosols. Finally, the daily mean and median SCDs over the presumably SO2-free equatorial East Pacific have increased by only ~ 0.0035 DU and ~ 0.003 DU respectively over the entire 15-year OMI record; while the standard deviation of SCDs has grown by only ~ 0.02 DU or ~ 10 %. Such remarkable long-term stability makes the new dataset particularly suitable for detecting regional changes in SO2 pollution.


2021 ◽  
Author(s):  
Jianfeng Li ◽  
Yuhang Wang ◽  
Ruixiong Zhang ◽  
Charles Smeltzer ◽  
Andrew Weinheimer ◽  
...  

Abstract. Nitrogen oxides (NOx = NO + NO2) play a crucial role in the formation of ozone and secondary inorganic and organic aerosols, thus affecting human health, global radiation budget, and climate. The diurnal and spatial variations of NO2 are functions of emissions, advection, deposition, vertical mixing, and chemistry. Their observations, therefore, provide useful constraints in our understanding of these factors. We employ a Regional chEmical and trAnsport model (REAM) to analyze the observed temporal (diurnal cycles) and spatial distributions of NO2 concentrations and tropospheric vertical column densities (TVCDs) using aircraft in situ measurements, surface EPA Air Quality System (AQS) observations, as well as the measurements of TVCDs by satellite instruments (OMI: the Ozone Monitoring Instrument; and GOME-2A: Global Ozone Monitoring Experiment – 2A), ground-based Pandora, and the Airborne Compact Atmospheric Mapper (ACAM) instrument, in July 2011 during the DISCOVER-AQ campaign over the Baltimore-Washington region. The model simulations at 36- and 4-km resolutions are in reasonably good agreement with the temporospatial NO2 observations in the daytime. However, nighttime mixing in the model needs to be enhanced to reproduce the observed NO2 diurnal cycle in the model. Another discrepancy is that Pandora measured NO2 TVCDs show much less variation in the late afternoon than simulated in the model. Relative to the 36-km model simulations, the 4-km model results show larger biases compared to the observations due largely to the larger spatial variations of NO2 in the model when the spatial resolution is increased from 36 to 4 km, although the biases are often comparable to the ranges of the observations. The high-resolution aircraft ACAM observations show a more dispersed distribution of NO2 vertical column densities (VCDs) and lower VCDs in urban regions than 4-km model simulations, reflecting likely the spatial distribution bias of NOx emissions in the National Emissions Inventory (NEI) 2011 at high resolution.


2017 ◽  
Vol 10 (9) ◽  
pp. 3133-3149 ◽  
Author(s):  
Nickolay A. Krotkov ◽  
Lok N. Lamsal ◽  
Edward A. Celarier ◽  
William H. Swartz ◽  
Sergey V. Marchenko ◽  
...  

Abstract. 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.


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