scholarly journals Estimates of lightning NO<sub><i>x</i></sub> production based on high-resolution OMI NO<sub>2</sub> retrievals over the continental US

2020 ◽  
Vol 13 (4) ◽  
pp. 1709-1734 ◽  
Author(s):  
Xin Zhang ◽  
Yan Yin ◽  
Ronald van der A ◽  
Jeff L. Lapierre ◽  
Qian Chen ◽  
...  

Abstract. Lightning serves as the dominant source of nitrogen oxides (NOx=NO+NO2) in the upper troposphere (UT), with a strong impact on ozone chemistry and the hydroxyl radical production. However, the production efficiency (PE) of lightning nitrogen oxides (LNOx) is still quite uncertain (32–1100 mol NO per flash). Satellite measurements are a powerful tool to estimate LNOx directly compared to conventional platforms. To apply satellite data in both clean and polluted regions, a new algorithm for calculating LNOx has been developed that uses the Berkeley High-Resolution (BEHR) v3.0B NO2 retrieval algorithm and the Weather Research and Forecasting model coupled with chemistry (WRF-Chem). LNOx PE over the continental US is estimated using the NO2 product of the Ozone Monitoring Instrument (OMI) data and the Earth Networks Total Lightning Network (ENTLN) data. Focusing on the summer season during 2014, we find that the lightning NO2 (LNO2) PE is 32±15 mol NO2 per flash and 6±3 mol NO2 per stroke while LNOx PE is 90±50 mol NOx per flash and 17±10 mol NOx per stroke. Results reveal that our method reduces the sensitivity to the background NO2 and includes much of the below-cloud LNO2. As the LNOx parameterization varies in studies, the sensitivity of our calculations to the setting of the amount of lightning NO (LNO) is evaluated. Careful consideration of the ratio of LNO2 to NO2 is also needed, given its large influence on the estimation of LNO2 PE.

2019 ◽  
Author(s):  
Xin Zhang ◽  
Yan Yin ◽  
Ronald van der A ◽  
Jeff L. Lapierre ◽  
Qian Chen ◽  
...  

Abstract. Lightning serves as the dominant source of nitrogen oxides (NOx = NO + NO2) in the upper troposphere (UT), with strong impact on ozone chemistry and the hydroxyl radical production. However, the production efficiency (PE) of lightning nitrogen oxides (LNOx) is still quite uncertain (32–1100 mol NO per flash). Satellites measurements are a powerful tool to estimate LNOx directly as compared to conventional platforms. To apply satellite data in both clean and polluted regions, a new algorithm for calculating LNOx has been developed based on the program of new Berkeley High Resolution (BEHR) v3.0B NO2 product and the Weather Research and Forecasting-Chemistry (WRF-Chem) model. LNOx PE over the continental US is estimated using the NO2 product of the Ozone Monitoring Instrument (OMI) satellite and the Earth Networks Total Lightning Network (ENTLN) data. Focusing on the summer season during 2014, we find that the lightning NO2 (LNO2) PE is 44 ± 16 mol NO2 flash-1 and 8 ± 3 mol NO2 stroke-1 while LNOx PE is 120 ± 52 mol NOx flash-1 and 22 ± 9 mol NOx stroke-1. Results reveal that former methods are more sensitive to background NO2 and neglect much of the below-cloud LNO2. As the LNOx parameterization varies in studies, the sensitivity of our calculations to the setting of the amount of lightning NO (LNO) is evaluated. Careful consideration of the ratio of LNO2 to NO2 is also needed, given its large influence on the estimation of LNO2 PE.


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.


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.


2021 ◽  
Author(s):  
Xin Zhang ◽  
Yan Yin ◽  
Ronald van der A ◽  
Henk Eskes ◽  
Jos van Geffen ◽  
...  

Abstract. Thunderstorms can significantly influence the air composition via strong updraft and lightning nitrogen oxides (LNOx). In this study, the ozonesondes and TROPOMI nitrogen dioxide (NO2) observations for two cases are combined with model to investigate the effects of typical strong convection on vertical redistribution of air pollutants in Nanjing, southeastern China. The ozonesonde observations show higher O3 and water vapor mixing ratios in the upper troposphere (UT) after convection, indicating the strong updraft transporting lower-level airmass into the UT, and the possible downward O3-rich air near the top of UT over the convective period. During the whole convection life cycle, the UT O3 production is driven by the chemistry (> 87 %) and reduced by the LNOx (−40 %). Sensitivity tests demonstrate that neglecting LNOx in standard TROPOMI NO2 products causes overestimated air mass factors over fresh lightning regions and the opposite for outflow and aged lightning areas. Therefore, a new high-resolution retrieval algorithm is applied to estimate the LNOx production efficiency. Our work shows the demand for high-resolution modeling and satellite observations on LNOx emissions of both active and dissipated convection, especially small-scale storms.


2011 ◽  
Vol 4 (9) ◽  
pp. 1905-1928 ◽  
Author(s):  
K. F. Boersma ◽  
H. J. Eskes ◽  
R. J. Dirksen ◽  
R. J. van der A ◽  
J. P. Veefkind ◽  
...  

Abstract. We present an improved tropospheric nitrogen dioxide column retrieval algorithm (DOMINO v2.0) for OMI based on better air mass factors (AMFs) and a correction for across-track stripes resulting from calibration errors in the OMI backscattered reflectances. Since October 2004, NO2 retrievals from the Ozone Monitoring Instrument (OMI), a UV/Vis nadir spectrometer onboard NASA's EOS-Aura satellite, have been used with success in several scientific studies focusing on air quality monitoring, detection of trends, and NOx emission estimates. Dedicated evaluations of previous DOMINO tropospheric NO2 retrievals indicated their good quality, but also suggested that the tropospheric columns were susceptible to high biases (by 0–40%), probably because of errors in the air mass factor calculations. Here we update the DOMINO air mass factor approach. We calculate a new look-up table (LUT) for altitude-dependent AMFs based on more realistic atmospheric profile parameters, and include more surface albedo and surface pressure reference points than before. We improve the sampling of the TM4 model, resulting in a priori NO2 profiles that are better mixed throughout the boundary layer. We evaluate the NO2 profiles simulated with the improved TM4 sampling as used in the AMF calculations and show that they are highly consistent with in situ NO2 measurements from aircraft during the INTEX-A and INTEX-B campaigns in 2004 and 2006. Our air mass factor calculations are further updated by the implementation of a high-resolution terrain height and a high-resolution surface albedo climatology based on OMI measurements. Together with a correction for across-track stripes, the overall impact of the improved terrain height and albedo descriptions is modest (<5%) on average over large polluted areas, but still causes significant changes locally. The main changes in the DOMINO v2.0 algorithm follow from the new LUT and the improved TM4 sampling that results in more NO2 simulated aloft, where sensitivity to NO2 is higher, and amount to reductions in tropospheric NO2 columns of up to 20% in winter, and 10% in summer over extended polluted areas. We investigate the impact of aerosols on the NO2 retrieval, and based on a comparison of concurrent retrievals of clouds from OMI and aerosols from MODIS Aqua, we find empirical evidence that OMI cloud retrievals are sensitive to the presence of scattering aerosols. It follows that an implicit correction for the effects of aerosols occurs through the aerosol-induced cloud parameters in DOMINO, and we show that such an empirical correction amounts to a 20 %AMF reduction in summer and ±10% changes in winter over the eastern United States.


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.


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.


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.


2013 ◽  
Vol 13 (11) ◽  
pp. 29203-29261 ◽  
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. 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 datasets 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 350 mol NO flash−1, respectively. Sensitivity studies with perturbed satellite datasets, model and data assimilation settings leads to an error estimate of about 1.4 Tg N yr−1 on this global LNOx source. These estimates are significantly different from those derived 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 analysed ozone fields and independent observations gives confidence in the performance of the LNOx source estimation.


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.


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