scholarly journals New observations of NO<sub>2</sub> in the upper troposphere from TROPOMI

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 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 ° x 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. We find that synthetic cloud-sliced UT NO2 are spatially consistent (R = 0.64) with UT NO2 calculated across the same cloud pressure range and scenes as are cloud-sliced (“true” UT NO2), but the cloud-sliced UT NO2 is 11–22 % more than the "true" all-sky seasonal mean. The largest contributors to differences between synthetic cloud-sliced and “true” UT NO2 are target resolution of the cloud-sliced product and uniformity of overlying stratospheric NO2. 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 sites in 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 x 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 systematic altitude differences between the TROPOMI and OMI cloud products. 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.


2008 ◽  
Vol 8 (14) ◽  
pp. 4061-4068 ◽  
Author(s):  
D. Cariolle ◽  
M. J. Evans ◽  
M. P. Chipperfield ◽  
N. Butkovskaya ◽  
A. Kukui ◽  
...  

Abstract. We have studied the impact of the recently observed reaction NO+HO2→HNO3 on atmospheric chemistry. A pressure and temperature-dependent parameterisation of this minor channel of the NO+HO2→NO2+OH reaction has been included in both a 2-D stratosphere-troposphere model and a 3-D tropospheric chemical transport model (CTM). Significant effects on the nitrogen species and hydroxyl radical concentrations are found throughout the troposphere, with the largest percentage changes occurring in the tropical upper troposphere (UT). Including the reaction leads to a reduction in NOx everywhere in the troposphere, with the largest decrease of 25% in the tropical and Southern Hemisphere UT. The tropical UT also has a corresponding large increase in HNO3 of 25%. OH decreases throughout the troposphere with the largest reduction of over 20% in the tropical UT. The mean global decrease in OH is around 13%, which is very large compared to the impact that typical photochemical revisions have on this modelled quantity. This OH decrease leads to an increase in CH4 lifetime of 5%. Due to the impact of decreased NOx on the OH:HO2 partitioning, modelled HO2 actually increases in the tropical UT on including the new reaction. The impact on tropospheric ozone is a decrease in the range 5 to 12%, with the largest impact in the tropics and Southern Hemisphere. Comparison with observations shows that in the region of largest changes, i.e. the tropical UT, the inclusion of the new reaction tends to degrade the model agreement. Elsewhere the model comparisons are not able to critically assess the impact of including this reaction. Only small changes are calculated in the minor species distributions in the stratosphere.


2008 ◽  
Vol 8 (1) ◽  
pp. 2695-2713 ◽  
Author(s):  
D. Cariolle ◽  
M. J. Evans ◽  
M. P. Chipperfield ◽  
N. Butkovskaya ◽  
A. Kukui ◽  
...  

Abstract. We have studied the impact of the recently established reaction NO+HO2→HNO3 on atmospheric chemistry. A pressure and temperature-dependent parameterisation of this minor channel of the NO+HO2→NO2+OH reaction has been included in both a 2-D stratosphere-troposphere model and a 3-D tropospheric chemical transport model (CTM). Significant effects on the nitrogen species and hydroxyl radical concentrations are found throughout the troposphere, with the largest percentage changes occurring in the tropical upper troposphere (UT). Including the reaction leads to a reduction in NOx everywhere in the troposphere, with the largest decrease of 25% in the tropical and southern hemisphere UT. The tropical UT also has a corresponding large increase in HNO3 of 25%. OH decreases throughout the troposphere with the largest reduction of over 20% in the tropical UT. Mean global decreases in OH are around 13% which leads to a increase in CH4 lifetime of 5%. Due to the impact of decreased NOx on the OH:HO2 partitioning, modelled HO2 actually increases in the tropical UT on including the new reaction. The impact on tropospheric ozone is a decrease in the range 5 to 12%, with the largest impact in the tropics and southern hemisphere. Comparison with observations shows that in the region of largest changes, i.e. the tropical UT, the inclusion of the new reaction tends to degrade the model agreement. Elsewhere the model comparisons are not able to critically assess the impact of including this reaction. Only small changes are calculated in the minor species distributions in the stratosphere.


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.


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;


2011 ◽  
Vol 11 (1) ◽  
pp. 121-162 ◽  
Author(s):  
J. Aschmann ◽  
B.-M. Sinnhuber ◽  
M. P. Chipperfield ◽  
R. Hossaini

Abstract. Stratospheric bromine loading due to very short-lived substances is investigated with a three-dimensional chemical transport model over a period of 21 years using meteorological input data from the European Centre for Medium-Range Weather Forecasts ERA-Interim reanalysis from 1989 to the end of 2009. Within this framework we analyze the impact of dehydration and deep convection on the amount of stratospheric bromine using an idealized and a detailed full chemistry approach. We model the two most important brominated short-lived substances, bromoform (CHBr3) and dibromomethane (CH2Br2), assuming a uniform detrainment mixing ratio of 1 part per trillion by volume (pptv) for both species. The contribution of very short-lived substances to stratospheric bromine varies drastically with the applied dehydration mechanism and the associated scavenging of soluble species ranging from 3.4 pptv in the idealized setup up to 5 pptv using the full chemistry scheme. In the latter case virtually the entire amount of bromine originating from very short-lived source gases is able to reach the stratosphere thus rendering the impact of dehydration and scavenging on inorganic bromine in the tropopause insignificant. Furthermore, our long-term calculations show that the mixing ratios of very short-lived substances are strongly correlated to convective activity, i.e. intensified convection leads to higher amounts of very short-lived substances in the upper troposphere/lower stratosphere especially under extreme conditions like El Niño seasons. However, this does not apply to the inorganic brominated product gases whose concentrations are anti-correlated to convective activity mainly due to convective dilution and possible scavenging, depending on the applied approach.


2011 ◽  
Vol 11 (6) ◽  
pp. 2671-2687 ◽  
Author(s):  
J. Aschmann ◽  
B.-M. Sinnhuber ◽  
M. P. Chipperfield ◽  
R. Hossaini

Abstract. Stratospheric bromine loading due to very short-lived substances is investigated with a three-dimensional chemical transport model over a period of 21 years using meteorological input data from the European Centre for Medium-Range Weather Forecasts ERA-Interim reanalysis from 1989 to the end of 2009. Within this framework we analyze the impact of dehydration and deep convection on the amount of stratospheric bromine using an idealized and a detailed full chemistry approach. We model the two most important brominated short-lived substances, bromoform (CHBr3) and dibromomethane (CH2Br2), assuming a uniform convective detrainment mixing ratio of 1 part per trillion by volume (pptv) for both species. The contribution of very short-lived substances to stratospheric bromine varies drastically with the applied dehydration mechanism and the associated scavenging of soluble species ranging from 3.4 pptv in the idealized setup up to 5 pptv using the full chemistry scheme. In the latter case virtually the entire amount of bromine originating from very short-lived source gases is able to reach the stratosphere thus rendering the impact of dehydration and scavenging on inorganic bromine in the tropopause insignificant. Furthermore, our long-term calculations show that the mixing ratios of very short-lived substances are strongly correlated to convective activity, i.e. intensified convection leads to higher amounts of very short-lived substances in the upper troposphere/lower stratosphere especially under extreme conditions like El Niño seasons. However, this does not apply to the inorganic brominated product gases whose concentrations are anti-correlated to convective activity mainly due to convective dilution and possible scavenging, depending on the applied approach.


2013 ◽  
Vol 13 (9) ◽  
pp. 23491-23548 ◽  
Author(s):  
A. T. Brown ◽  
M. P. Chipperfield ◽  
S. Dhomse ◽  
C. Boone ◽  
P. F. Bernath

Abstract. We present chlorine budgets calculated between 2004 and 2009 for four latitude bands (70° N–30° N, 30° N–0° N, 0° N–30° S, and 30° S–70° S). The budgets were calculated using ACE-FTS version 3.0 retrievals of the volume mixing ratios (VMRs) of 9 chlorine-containing species: CCl4, CFC-12 (CCl2F2), CFC-11 (CCl3F), COCl2, COClF, HCFC-22 (CHF2Cl), CH3Cl, HCl and ClONO2. These data were supplemented with calculated VMRs from the SLIMCAT 3-D chemical transport model (CFC-113, CFC-114, CFC-115, H-1211, H-1301, HCFC-141b, HCFC-142b, ClO and HOCl). The total chlorine profiles are dominated by chlorofluorocarbons (CFCs) and halons up to 24 km in the tropics and 19 km in the extra-tropics. In this altitude range CFCs and halons account for 58% of the total chlorine VMR. Above this altitude HCl increasingly dominates the total chlorine profile, reaching a maximum of 95% of total chlorine at 54 km. All total chlorine profiles exhibit a positive slope with altitude, suggesting that the total chlorine VMR is now decreasing with time. This conclusion is supported by the time series of the mean stratospheric total chlorine budgets which show mean decreases in total stratospheric chlorine of 0.38 ± 0.03% per year in the Northern Hemisphere extra-tropics, 0.35 ± 0.07% per year in the Northern Hemisphere tropical stratosphere, 0.54 ± 0.16% per year in the Southern Hemisphere tropics and 0.53 ± 0.12% per year in the Southern Hemisphere extra-tropical stratosphere for 2004–2009. Globally stratospheric chlorine is decreasing by 0.46 ± 0.02% per year. Both global warming potential-weighted chlorine and ozone depletion potential-weighted chlorine are decreasing at all latitudes. These results show that the Montreal Protocol has had a significant effect in reducing emissions of both ozone-depleting substances and greenhouse gases.


Author(s):  
S H Lee ◽  
M Le Dilosquer ◽  
R Singh ◽  
S E Hobbs ◽  
C Giannakopoulos ◽  
...  

The exhaust emissions from civil subsonic aircraft at cruise altitude are important man-made sources that pollute the upper troposphere and the lower stratosphere (8-12 km). The formation of NO y species from NO x, both before and after the exit nozzle, have created increasing environmental concerns. Flight histories of Boeing 747-400 aircraft during the cruise stage between selected city pairs have been simulated using a computer program developed at Cranfield University. The passive distribution of NO x and HNO3 is calculated using the UGAMP three-dimensional chemical transport model. The sink of NO x, which is HNO3, is parameterized using an exponential decay process with an altitude-dependent lifetime. The model also includes transport by advection, vertical diffusion and convection. These simulations for January and July are analysed in terms of the resulting mean volume mixing ratios for both NO x and HNO3.


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.


Sign in / Sign up

Export Citation Format

Share Document