scholarly journals Vertical profiles of lightning-produced NO<sub>2</sub> enhancements in the upper troposphere observed by OSIRIS

2007 ◽  
Vol 7 (2) ◽  
pp. 5013-5051 ◽  
Author(s):  
C. E. Sioris ◽  
C. A. McLinden ◽  
R. V. Martin ◽  
B. Sauvage ◽  
C. S. Haley ◽  
...  

Abstract. The purpose of this study is to perform a global search of the upper troposphere (z≥10 km) for enhancements of nitrogen dioxide and determine their sources. We have searched two years (May 2003–May 2005) of OSIRIS (Optical Spectrograph and Infrared Imager System) operational NO2 data (version 2.3/2.4) to find large enhancements in the observations by comparing concentrations with those predicted by a photochemical model and by identifying local maxima in NO2 volume mixing ratio. We find that lightning is the main production mechanism responsible for the large enhancements in OSIRIS NO2 observations as expected. Similar patterns in the abundances and spatial distribution of the NO2 enhancements are obtained by perturbing the lightning within the GEOS-Chem 3-dimensional chemical transport model. In most cases, the presence of lightning is confirmed with coincident imagery from LIS (Lightning Imaging Sensor) and the spatial extent of the NO2 enhancement is mapped using nadir observations of tropospheric NO2 at high spatial resolution from SCIAMACHY (Scanning Imaging Absorption Spectrometer for Atmospheric Chartography) and OMI (Ozone Monitoring Instrument). The combination of the lightning and chemical sensors allows us to investigate globally the role of lightning to the abundance of NO2 in the upper troposphere (UT). This is the first application of satellite-based limb scattering to study upper tropospheric NO2. The spatial and temporal distribution of NO2 enhancements from lightning (May 2003–May 2005) is investigated. The NO2 from lightning generally occurs at 12 to 13 km more frequently than at 10 to 11 km. This is consistent with the notion that most of the NO2 is forming and persisting near the cloud top altitude in the tropical upper troposphere. The latitudinal distribution is mostly as expected. In general, the thunderstorms exhibiting weaker vertical development (e.g. 11≤z≤13 km) extend latitudinally as far poleward as 45° but the thunderstorms with stronger vertical development (z≥14 km) tend to be located within 33° of the equator. There is also the expected hemispheric asymmetry in the frequency of the NO2 enhancements, as most were observed in the Northern Hemisphere for the period analyzed.

2007 ◽  
Vol 7 (16) ◽  
pp. 4281-4294 ◽  
Author(s):  
C. E. Sioris ◽  
C. A. McLinden ◽  
R. V. Martin ◽  
B. Sauvage ◽  
C. S. Haley ◽  
...  

Abstract. The purpose of this study is to perform a global search of the upper troposphere (z≥10 km) for enhancements of nitrogen dioxide and determine their sources. This is the first application of satellite-based limb scattering to study upper tropospheric NO2. We have searched two years (May 2003–May 2005) of OSIRIS (Optical Spectrograph and Infrared Imager System) operational NO2 concentrations (version 2.3/2.4) to find large enhancements in the observations by comparing with photochemical box model calculations and by identifying local maxima in NO2 volume mixing ratio. We find that lightning is the main production mechanism responsible for the large enhancements in OSIRIS NO2 observations as expected. Similar patterns in the abundances and spatial distribution of the NO2 enhancements are obtained by perturbing the lightning within the GEOS-Chem 3-dimensional chemical transport model. In most cases, the presence of lightning is confirmed with coincident imagery from LIS (Lightning Imaging Sensor) and the spatial extent of the NO2 enhancement is mapped using nadir observations of tropospheric NO2 at high spatial resolution from SCIAMACHY (Scanning Imaging Absorption Spectrometer for Atmospheric Chartography) and OMI (Ozone Monitoring Instrument). The combination of the lightning and chemical sensors allows us to investigate globally the role of lightning to the abundance of NO2 in the upper troposphere (UT). Lightning contributes 60% of the tropical upper tropospheric NO2 in GEOS-Chem simulations. The spatial and temporal distribution of NO2 enhancements from lightning (May 2003–May 2005) is investigated. The enhancements generally occur at 12 to 13 km more frequently than at 10 to 11 km. This is consistent with the notion that most of the NO2 is forming and persisting near the cloud top altitude in the tropical upper troposphere. The latitudinal distribution is mostly as expected. In general, the thunderstorms exhibiting weaker vertical development (e.g. 11≤z≤13 km) extend latitudinally as far poleward as 45° but the thunderstorms with stronger vertical development (z≥14 km) tend to be located within 33° of the equator. There is also the expected hemispheric asymmetry in the frequency of the NO2 enhancements, as most were observed in the northern hemisphere for the period analyzed.


2020 ◽  
Vol 20 (3) ◽  
pp. 1483-1495 ◽  
Author(s):  
Viral Shah ◽  
Daniel J. Jacob ◽  
Ke Li ◽  
Rachel F. Silvern ◽  
Shixian Zhai ◽  
...  

Abstract. Satellite observations of tropospheric NO2 columns are extensively used to infer trends in anthropogenic emissions of nitrogen oxides (NOx≡NO+NO2), but this may be complicated by trends in NOx lifetime. Here we use 2004–2018 observations from the Ozone Monitoring Instrument (OMI) satellite-based instrument (QA4ECV and POMINO v2 retrievals) to examine the seasonality and trends of tropospheric NO2 columns over central–eastern China, and we interpret the results with the GEOS-Chem chemical transport model. The observations show a factor of 3 increase in NO2 columns from summer to winter, which we explain in GEOS-Chem as reflecting a longer NOx lifetime in winter than in summer (21 h versus 5.9 h in 2017). The 2005–2018 summer trends of OMI NO2 closely follow the trends in the Multi-resolution Emission Inventory for China (MEIC), with a rise over the 2005–2011 period and a 25 % decrease since. We find in GEOS-Chem no significant trend of the NOx lifetime in summer, supporting the emission trend reported by the MEIC. The winter trend of OMI NO2 is steeper than in summer over the entire period, which we attribute to a decrease in NOx lifetime at lower NOx emissions. Half of the NOx sink in winter is from N2O5 hydrolysis, which counterintuitively becomes more efficient as NOx emissions decrease due to less titration of ozone at night. The formation of organic nitrates also becomes an increasing sink of NOx as NOx emissions decrease but emissions of volatile organic compounds (VOCs) do not.


2021 ◽  
Vol 14 (3) ◽  
pp. 2389-2408
Author(s):  
Eloise A. Marais ◽  
John F. Roberts ◽  
Robert G. Ryan ◽  
Henk Eskes ◽  
K. Folkert Boersma ◽  
...  

Abstract. Nitrogen oxides (NOx≡NO+NO2) in the NOx-limited upper troposphere (UT) are long-lived and so have a large influence on the oxidizing capacity of the troposphere and formation of the greenhouse gas ozone. Models misrepresent NOx in the UT, and observations to address deficiencies in models are sparse. Here we obtain a year of near-global seasonal mean mixing ratios of NO2 in the UT (450–180 hPa) at 1∘×1∘ by applying cloud-slicing to partial columns of NO2 from TROPOMI. This follows refinement of the cloud-slicing algorithm with synthetic partial columns from the GEOS-Chem chemical transport model. TROPOMI, prior to cloud-slicing, is corrected for a 13 % underestimate in stratospheric NO2 variance and a 50 % overestimate in free-tropospheric NO2 determined by comparison to Pandora total columns at high-altitude free-tropospheric sites at Mauna Loa, Izaña, and Altzomoni and MAX-DOAS and Pandora tropospheric columns at Izaña. Two cloud-sliced seasonal mean UT NO2 products for June 2019 to May 2020 are retrieved from corrected TROPOMI total columns using distinct TROPOMI cloud products that assume clouds are reflective boundaries (FRESCO-S) or water droplet layers (ROCINN-CAL). TROPOMI UT NO2 typically ranges from 20–30 pptv over remote oceans to >80 pptv over locations with intense seasonal lightning. Spatial coverage is mostly in the tropics and subtropics with FRESCO-S and extends to the midlatitudes and polar regions with ROCINN-CAL, due to its greater abundance of optically thick clouds and wider cloud-top altitude range. TROPOMI UT NO2 seasonal means are spatially consistent (R=0.6–0.8) with an existing coarser spatial resolution (5∘ latitude × 8∘ longitude) UT NO2 product from the Ozone Monitoring Instrument (OMI). UT NO2 from TROPOMI is 12–26 pptv more than that from OMI due to increase in NO2 with altitude from the OMI pressure ceiling (280 hPa) to that for TROPOMI (180 hPa), but possibly also due to altitude differences in TROPOMI and OMI cloud products and NO2 retrieval algorithms. The TROPOMI UT NO2 product offers potential to evaluate and improve representation of UT NOx in models and supplement aircraft observations that are sporadic and susceptible to large biases in the UT.


2020 ◽  
Author(s):  
Eloise Marais ◽  
Joanna Joiner ◽  
Sungyeon Choi

&lt;p&gt;Nitrogen oxides (NO&lt;sub&gt; x&lt;/sub&gt; = NO + NO&lt;sub&gt;2&lt;/sub&gt;) in the upper troposphere (~10-12 km) are effective at producing ozone in the upper troposphere where ozone is a potent greenhouse gas. Observations of NO&lt;sub&gt;x&lt;/sub&gt; in the upper troposphere are limited in time to a few intensive research aircraft campaigns and in space to commercial aircraft campaigns. There are satellite-derived observations of NO&lt;sub&gt;2&lt;/sub&gt; in the upper troposphere from the Ozone Monitoring Instrument (OMI), but these are at very coarse resolutions (seasonal, &gt; 2,000 km). The high-resolution Sentinel-5P/TROPOMI instrument offers higher spatial resolution and better cloud-resolving capability than OMI. Here we use synthetic columns of NO&lt;sub&gt;2&lt;/sub&gt; from the GEOS-Chem chemical transport model to assess feasibility of deriving NO&lt;sub&gt;2&lt;/sub&gt; in the upper troposphere using partial columns of NO&lt;sub&gt;2&lt;/sub&gt; above cloudy scenes (the so-called cloud-slicing technique). The model is also used to quantify errors induced by uncertainties in cloud-top height and to determine whether NO&lt;sub&gt;2&lt;/sub&gt; over cloudy scenes is representative of all-sky conditions (the &quot;truth&quot;). We find that the cloud-slicing approach is spatially consistent (R =0.5) with the &quot;truth&quot;, but with a small (10 pptv) bias in background NO&lt;sub&gt;2&lt;/sub&gt;. Cloud-slicing is then applied to TROPOMI total columns of NO&lt;sub&gt;2&lt;/sub&gt; to derive near-global observations of NO&lt;sub&gt;2&lt;/sub&gt; in the upper troposphere and assessed against the existing OMI products and aircraft observations from NASA DC8 aircraft campaigns.&lt;/p&gt;


Sensors ◽  
2018 ◽  
Vol 18 (9) ◽  
pp. 2893 ◽  
Author(s):  
Willem W. Verstraeten ◽  
Klaas Folkert Boersma ◽  
John Douros ◽  
Jason E. Williams ◽  
Henk Eskes ◽  
...  

Top-down estimates of surface NOX emissions were derived for 23 European cities based on the downwind plume decay of tropospheric nitrogen dioxide (NO2) columns from the LOTOS-EUROS (Long Term Ozone Simulation-European Ozone Simulation) chemistry transport model (CTM) and from Ozone Monitoring Instrument (OMI) satellite retrievals, averaged for the summertime period (April–September) during 2013. Here we show that the top-down NOX emissions derived from LOTOS-EUROS for European urban areas agree well with the bottom-up NOX emissions from the MACC-III inventory data (R2 = 0.88) driving the CTM demonstrating the potential of this method. OMI top-down NOX emissions over the 23 European cities are generally lower compared with the MACC-III emissions and their correlation is slightly lower (R2 = 0.79). The uncertainty on the derived NO2 lifetimes and NOX emissions are on average ~55% for OMI and ~63% for LOTOS-EUROS data. The downwind NO2 plume method applied on both LOTOS-EUROS and OMI tropospheric NO2 columns allows to estimate NOX emissions from urban areas, demonstrating that this is a useful method for real-time updates of urban NOX emissions with reasonable accuracy.


2009 ◽  
Vol 9 (5) ◽  
pp. 18511-18543 ◽  
Author(s):  
J. Aschmann ◽  
B. M. Sinnhuber ◽  
E. L. Atlas ◽  
S. M. Schauffler

Abstract. The transport of very short-lived substances into the tropical upper troposphere and lower stratosphere is investigated by a three-dimensional chemical transport model using archived convective updraft mass fluxes (or detrainment rates) from the European Centre for Medium-Range Weather Forecast's ERA-Interim reanalysis. Large-scale vertical velocities are calculated from diabatic heating rates. With this approach we explicitly model the large scale subsidence in the tropical troposphere with convection taking place in fast and isolated updraft events. The model calculations agree generally well with observations of bromoform and methyl iodide from aircraft campaigns and with ozone and water vapor from sonde and satellite observations. Using a simplified treatment of dehydration and bromine product gas washout we give a range of 1.6 to 3 ppt for the contribution of bromoform to stratospheric bromine, assuming a uniform source in the boundary layer of 1 ppt. We show that the most effective region for VSLS transport into the stratosphere is the West Pacific, accounting for about 55% of the bromine from bromoform transported into the stratosphere under the supposition of a uniformly distributed source.


2016 ◽  
Vol 9 (9) ◽  
pp. 4355-4373 ◽  
Author(s):  
Swagata Payra ◽  
Philippe Ricaud ◽  
Rachid Abida ◽  
Laaziz El Amraoui ◽  
Jean-Luc Attié ◽  
...  

Abstract. The present analysis deals with one of the most debated aspects of the studies on the upper troposphere/lower stratosphere (UTLS), namely the budget of water vapour (H2O) at the tropical tropopause. Within the French project “Multiscale water budget in the upper troposphere and lower stratosphere in the TROpics” (TRO-pico), a global-scale analysis has been set up based on space-borne observations, models and assimilation techniques. The MOCAGE-VALENTINA assimilation tool has been used to assimilate the Aura Microwave Limb Sounder (MLS) version 3.3 H2O measurements within the 316–5 hPa range from August 2011 to March 2013 with an assimilation window of 1 h. Diagnostics based on observations minus analysis and forecast are developed to assess the quality of the assimilated H2O fields. Comparison with an independent source of H2O measurements in the UTLS based on the space-borne Michelson Interferometer for Passive Atmospheric Sounding (MIPAS) observations and with meteorological ARPEGE analyses is also shown. Sensitivity studies of the analysed fields have been performed by (1) considering periods when no MLS measurements are available and (2) using H2O data from another MLS version (4.2). The studies have been performed within three different spaces in time and space coincidences with MLS (hereafter referred to as MLS space) and MIPAS (MIPAS space) observations and with the model (model space) outputs and at three different levels: 121 hPa (upper troposphere), 100 hPa (tropopause) and 68 hPa (lower stratosphere) in January and February 2012. In the MLS space, the analyses behave consistently with the MLS observations from the upper troposphere to the lower stratosphere. In the model space, the analyses are wetter than the reference atmosphere as represented by ARPEGE and MLS in the upper troposphere (121 hPa) and around the tropopause (100 hPa), but are consistent with MLS and MIPAS in the lower stratosphere (68 hPa). In the MIPAS space, the sensitivity and the vertical resolution of the MIPAS data set at 121 and 100 hPa prevent assessment of the behaviour of the analyses at 121 and 100 hPa, particularly over intense convective areas as the South American, the African and the Maritime continents but, in the lower stratosphere (68 hPa), the analyses are very consistent with MIPAS. Sensitivity studies show the improvement on the H2O analyses in the tropical UTLS when assimilating space-borne measurements of better quality, particularly over the convective areas.


2014 ◽  
Vol 14 (7) ◽  
pp. 3277-3305 ◽  
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 into a chemical transport model. 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 data sets 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 310 mol NO flash−1, respectively. Sensitivity studies with perturbed satellite data sets, model and data assimilation settings lead to an error estimate of about 1.4 Tg N yr−1 on this global LNOx source. These estimates are significantly different from those estimated from a parameter inversion that optimizes only the LNOx source 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 analyzed ozone fields and independent observations gives confidence in the performance of the LNOx source estimation.


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.


2019 ◽  
Vol 11 (2) ◽  
pp. 137 ◽  
Author(s):  
Yapeng Wang ◽  
Jinhua Tao ◽  
Liangxiao Cheng ◽  
Chao Yu ◽  
Zifeng Wang ◽  
...  

East China is the ‘hotspot’ of glyoxal (CHOCHO), especially over the Pearl River Delta (PRD) region, where glyoxal is yielded from the oxidation of aromatics. To better understand the glyoxal spatial-temporal characteristics over China and evaluate the effectiveness of atmospheric prevention efforts on the reduction of volatile organic compound (VOC) emissions, we present an algorithm for glyoxal retrieval using the Ozone Monitoring instrument (OMI) over China. The algorithm is based on the differential optical absorption spectroscopy (DOAS) and accounts for the interference of the tropospheric nitrogen dioxide (NO2) spatial-temporal distribution on glyoxal retrieval. We conduct a sensitively test based on a synthetic spectrum to optimize the fitting parameters set. It shows that the fitting interval of 430–458 nm and a 4th order polynomial are optimal for glyoxal retrieval when using the daily mean value of the earthshine spectrum in the Pacific region as a reference. In addition, tropospheric NO2 pre-fitted during glyoxal retrieval is first proposed and tested, which shows a ±10% variation compared with the reference scene. The interference of NO2 on glyoxal was further investigated based on the OMI observations, and the spatial distribution showed that changes in the NO2 concentration can affect the glyoxal result depending on the NO2 spatial distribution. A method to prefix NO2 during glyoxal retrieval is proposed in this study and is referred to as OMI-CAS. We perform an intercomparison of the glyoxal from the OMI-CAS with the seasonal datasets provided by different institutions for North China (NC), South China (SC), the Yangtze River Delta (YRD) and the ChuanYu (CY) region in southwestern China in the year 2005. The results show that our algorithm can obtain the glyoxal spatial and temporal variations in different regions over China. OMI-CAS has the best correlations with other datasets in summer, with the correlations between OMI-CAS and OMI-Harvard, OMI-CAS and OMI-IUP, and OMI-CAS and Sciamachy-IUP being 0.63, 0.67 and 0.67, respectively. Autumn results followed, with the correlations of 0.58, 0.36 and 0.48, respectively, over China. However, the correlations are less or even negative for spring and winter. From the regional perspective, SC has the best correlation compared with other regions, with R reaching 0.80 for OMI-CAS and OMI-IUP in summer. The discrepancies between different glyoxal datasets can be attributed to the fitting parameters and larger glyoxal retrieval uncertainties. Finally, useful recommendations are given based on the results comparison according to region and season.


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