scholarly journals Nitrogen oxides in the global upper troposphere: interpreting cloud-sliced NO<sub>2</sub> observations from the OMI satellite instrument

2018 ◽  
Vol 18 (23) ◽  
pp. 17017-17027 ◽  
Author(s):  
Eloise A. Marais ◽  
Daniel J. Jacob ◽  
Sungyeon Choi ◽  
Joanna Joiner ◽  
Maria Belmonte-Rivas ◽  
...  

Abstract. Nitrogen oxides (NOx≡NO+NO2) in the upper troposphere (UT) have a large impact on global tropospheric ozone and OH (the main atmospheric oxidant). New cloud-sliced observations of UT NO2 at 450–280 hPa (∼6–9 km) from the Ozone Monitoring Instrument (OMI) produced by NASA and the Royal Netherlands Meteorological Institute (KNMI) provide global coverage to test our understanding of the factors controlling UT NOx. We find that these products offer useful information when averaged over coarse scales (20∘×32∘, seasonal), and that the NASA product is more consistent with aircraft observations of UT NO2. Correlation with Lightning Imaging Sensor (LIS) and Optical Transient Detector (OTD) satellite observations of lightning flash frequencies suggests that lightning is the dominant source of NOx to the upper troposphere except for extratropical latitudes in winter. The NO2 background in the absence of lightning is 10–20 pptv. We infer a global mean NOx yield of 280±80 moles per lightning flash, with no significant difference between the tropics and midlatitudes, and a global lightning NOx source of 5.9±1.7 Tg N a−1. There is indication that the NOx yield per flash increases with lightning flash footprint and with flash energy.

2018 ◽  
Author(s):  
Eloise A. Marais ◽  
Daniel J. Jacob ◽  
Sungyeon Choi ◽  
Joanna Joiner ◽  
Maria Belmonte-Rivas ◽  
...  

Abstract. Nitrogen oxides (NOx ≡ NO + NO2) in the upper troposphere (UT) have a large impact on global tropospheric ozone and OH (the main atmospheric oxidant). New cloud-sliced observations of UT NO2 at 450–280 hPa (~ 6–9 km) from the OMI satellite instrument produced by NASA and KNMI provide global coverage to test our understanding of the factors controlling UT NOx. We find that these products offer useful information when averaged over coarse scales (20° × 32°, seasonal), and that the NASA product is more consistent with aircraft observations of UT NO2. Correlation with LIS/OTD satellite observations of lightning flash frequencies shows that lightning is the dominant source of NOx to the upper troposphere except for extratropical latitudes in winter. We infer a global mean NOx yield of 280 moles per lightning flash, with no significant difference between the tropics and mid-latitudes, and a global lightning NOx source of 5.6 Tg N a−1. There is indication that the NOx yield per flash increases with lightning flash footprint and with flash energy.


2014 ◽  
Vol 2 (4) ◽  
pp. 2765-2787 ◽  
Author(s):  
S. Beirle ◽  
W. Koshak ◽  
R. Blakeslee ◽  
T. Wagner

Abstract. The satellite instruments Optical Transient Detector (OTD) and Lightning Imaging Sensor (LIS) provide unique empirical data about the frequency of lightning flashes around the globe (OTD), and the tropics (LIS), which have been used before to compile a well received global climatology of flash rate densities. Here we present a statistical analysis of various additional lightning properties derived from OTD/LIS, i.e. the number of so-called "events" and "groups" per flash, as well as the mean flash duration, footprint and radiance. These normalized quantities, which can be associated with the flash "strength", show consistent spatial patterns; most strikingly, oceanic flashes show higher values than continental flashes for all properties. Over land, regions with high (Eastern US) and low (India) flash strength can be clearly identified. We discuss possible causes and implications of the observed regional differences. Although a direct quantitative interpretation of the investigated flash properties is difficult, the observed spatial patterns provide valuable information for the interpretation and application of climatological flash rates. Due to the systematic regional variations of physical flash characteristics, viewing conditions, and/or measurement sensitivities, parametrisations of lightning NOx based on total flash rate densities alone are probably affected by regional biases.


2014 ◽  
Vol 14 (10) ◽  
pp. 2715-2726 ◽  
Author(s):  
S. Beirle ◽  
W. Koshak ◽  
R. Blakeslee ◽  
T. Wagner

Abstract. The satellite instruments Optical Transient Detector (OTD) and Lightning Imaging Sensor (LIS) provide unique empirical data about the frequency of lightning flashes around the globe (OTD), and the tropics (LIS), which have been used before to compile a well-received global climatology of flash rate densities. Here we present a statistical analysis of various additional lightning properties derived from OTD / LIS, i.e., the number of so-called "events" and "groups" per flash, as well as the mean flash duration, footprint and radiance. These normalized quantities, which can be associated with the flash "strength", show consistent spatial patterns; most strikingly, oceanic flashes show higher values than continental flashes for all properties. Over land, regions with high (eastern US) and low (India) flash strength can be clearly identified. We discuss possible causes for and implications of the observed regional differences. Although a direct quantitative interpretation of the investigated flash properties is difficult, the observed spatial patterns provide valuable information for the interpretation and application of climatological flash rates. Due to the systematic regional variations of physical flash characteristics, viewing conditions, and/or measurement sensitivities, parametrizations of lightning NOx based on total flash rate densities alone are probably affected by regional biases.


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.


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.


2020 ◽  
Vol 12 (23) ◽  
pp. 3946
Author(s):  
Pasquale Sellitto ◽  
Silvia Bucci ◽  
Bernard Legras

Clouds in the tropics have an important role in the energy budget, atmospheric circulation, humidity, and composition of the tropical-to-global upper-troposphere–lower-stratosphere. Due to its non-sun-synchronous orbit, the Cloud–Aerosol Transport System (CATS) onboard the International Space Station (ISS) provided novel information on clouds from space in terms of overpass time in the period of 2015–2017. In this paper, we provide a seasonally resolved comparison of CATS characterization of high clouds (between 13 and 18 km altitude) in the tropics with well-established CALIPSO (Cloud–Aerosol Lidar and Infrared Pathfinder Satellite Observation) data, both in terms of clouds’ occurrence and cloud optical properties (optical depth). Despite the fact that cloud statistics for CATS and CALIOP are generated using intrinsically different local overpass times, the characterization of high clouds occurrence and optical properties in the tropics with the two instruments is very similar. Observations from CATS underestimate clouds occurrence (up to 80%, at 18 km) and overestimate the occurrence of very thick clouds (up to 100% for optically very thick clouds, at 18 km) at higher altitudes. Thus, the description of stratospheric overshoots with CATS and CALIOP might be different. While this study hints at the consistency of CATS and CALIOP clouds characterizaton, the small differences highlighted in this work should be taken into account when using CATS for estimating cloud properties and their variability in the tropics.


2020 ◽  
Author(s):  
Timothy J Lang ◽  
Richard Blakeslee ◽  
William J. Koshak ◽  
Dennis E. Buechler ◽  
Patrick Gatlin ◽  
...  

2017 ◽  
Vol 10 (11) ◽  
pp. 4403-4419 ◽  
Author(s):  
Joshua L. Laughner ◽  
Ronald C. Cohen

Abstract. Space-borne measurements of tropospheric nitrogen dioxide (NO2) columns are up to 10x more sensitive to upper tropospheric (UT) NO2 than near-surface NO2 over low-reflectivity surfaces. Here, we quantify the effect of adding simulated lightning NO2 to the a priori profiles for NO2 observations from the Ozone Monitoring Instrument (OMI) using modeled NO2 profiles from the Weather Research and Forecasting–Chemistry (WRF-Chem) model. With observed NO2 profiles from the Deep Convective Clouds and Chemistry (DC3) aircraft campaign as observational truth, we quantify the bias in the NO2 column that occurs when lightning NO2 is not accounted for in the a priori profiles. Focusing on late spring and early summer in the central and eastern United States, we find that a simulation without lightning NO2 underestimates the air mass factor (AMF) by 25 % on average for common summer OMI viewing geometry and 35 % for viewing geometries that will be encountered by geostationary satellites. Using a simulation with 500 to 665 mol NO flash−1 produces good agreement with observed NO2 profiles and reduces the bias in the AMF to  <  ±4 % for OMI viewing geometries. The bias is regionally dependent, with the strongest effects in the southeast United States (up to 80 %) and negligible effects in the central US. We also find that constraining WRF meteorology to a reanalysis dataset reduces lightning flash counts by a factor of 2 compared to an unconstrained run, most likely due to changes in the simulated water vapor profile.


2008 ◽  
Vol 8 (1) ◽  
pp. 1589-1634 ◽  
Author(s):  
D. B. Considine ◽  
J. A. Logan ◽  
M. A. Olsen

Abstract. The NASA Global Modeling Initiative has developed a combined stratosphere/troposphere chemistry and transport model which fully represents the processes governing atmospheric composition near the tropopause. We evaluate model ozone distributions near the tropopause, using two high vertical resolution monthly mean ozone profile climatologies constructed with ozonesonde data, one by averaging on pressure levels and the other relative to the thermal tropopause. Model ozone is high-biased at the SH tropical and NH midlatitude tropopause by ~45% in a 4° latitude × 5° longitude model simulation. Increasing the resolution to 2°×2.5&amp;deg increases the NH tropopause high bias to ~60%, but decreases the tropical tropopause bias to ~30%, an effect of a better-resolved residual circulation. The tropopause ozone biases appear not to be due to an overly vigorous residual circulation or excessive stratosphere/troposphere exchange, but are more likely due to insufficient vertical resolution or excessive vertical diffusion near the tropopause. In the upper troposphere and lower stratosphere, model/measurement intercomparisons are strongly affected by the averaging technique. NH and tropical mean model lower stratospheric biases are <20%. In the upper troposphere, the 2°×2.5&amp;deg simulation exhibits mean high biases of ~20% and~35% during April in the tropics and NH midlatitudes, respectively, compared to the pressure-averaged climatology. However, relative-to-tropopause averaging produces upper troposphere high biases of ~30% and 70% in the tropics and NH midlatitudes. This is because relative-to-tropopause averaging better preserves large cross-tropopause O3 gradients, which are seen in the daily sonde data, but not in daily model profiles. The relative annual cycle of ozone near the tropopause is reproduced very well in the model Northern Hemisphere midlatitudes. In the tropics, the model amplitude of the near-tropopause annual cycle is weak. This is likely due to the annual amplitude of mean vertical upwelling near the tropopause, which analysis suggests is ~30% weaker than in the real atmosphere.


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