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

2018 ◽  
Author(s):  
Eloise A. Marais ◽  
Daniel J. Jacob ◽  
Sungyeon Choi ◽  
Joanna Joiner ◽  
Maria Belmonte-Rivas ◽  
...  
Keyword(s):  
Nitrogen Oxides ◽  
Tropospheric Ozone ◽  
Lightning Flash ◽  
Upper Troposphere ◽  
Significant Difference ◽  
Aircraft Observations ◽  
Global Coverage ◽  
The Tropics ◽  
Lightning Nox ◽  
Global Mean

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.

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 ◽  
...  
Keyword(s):  
Nitrogen Oxides ◽  
Lightning Flash ◽  
Ozone Monitoring Instrument ◽  
Upper Troposphere ◽  
Significant Difference ◽  
Global Coverage ◽  
The Tropics ◽  
Imaging Sensor ◽  
Lightning Nox ◽  
Optical Transient

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.

scholarly journals Impact of the new HNO<sub>3</sub>-forming channel of the HO<sub>2</sub>+NO reaction on tropospheric HNO<sub>3</sub>, NO<sub>x</sub>, HO<sub>x</sub> and ozone

2008 ◽  
Vol 8 (14) ◽  
pp. 4061-4068 ◽  
Author(s):  
D. Cariolle ◽  
M. J. Evans ◽  
M. P. Chipperfield ◽  
N. Butkovskaya ◽  
A. Kukui ◽  
...  
Keyword(s):  
Southern Hemisphere ◽  
Atmospheric Chemistry ◽  
Tropospheric Ozone ◽  
Transport Model ◽  
Chemical Transport Model ◽  
Temperature Dependent ◽  
Upper Troposphere ◽  
The Mean ◽  
The Tropics ◽  
The Impact

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.

scholarly journals Impact of the new HNO<sub>3</sub>-forming channel of the HO<sub>2</sub>+NO reaction on tropospheric HNO<sub>3</sub>, NO<sub>x</sub>, HO<sub>x</sub> and ozone

2008 ◽  
Vol 8 (1) ◽  
pp. 2695-2713 ◽  
Author(s):  
D. Cariolle ◽  
M. J. Evans ◽  
M. P. Chipperfield ◽  
N. Butkovskaya ◽  
A. Kukui ◽  
...  
Keyword(s):  
Southern Hemisphere ◽  
Atmospheric Chemistry ◽  
Tropospheric Ozone ◽  
Transport Model ◽  
Chemical Transport Model ◽  
Temperature Dependent ◽  
Upper Troposphere ◽  
The Tropics ◽  
The Impact ◽  
Model Agreement

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.

scholarly journals Emission sources contributing to tropospheric ozone over equatorial Africa during the summer monsoon

2011 ◽  
Vol 11 (5) ◽  
pp. 13769-13827
Author(s):  
I. Bouarar ◽  
K. S. Law ◽  
M. Pham ◽  
C. Liousse ◽  
H. Schlager ◽  
...  
Keyword(s):  
West Africa ◽  
Atlantic Ocean ◽  
Summer Monsoon ◽  
Biomass Burning ◽  
Tropospheric Ozone ◽  
Anthropogenic Emissions ◽  
Model Calculations ◽  
Upper Troposphere ◽  
Sahel Region ◽  
Lightning Nox

Abstract. A global chemistry-climate model LMDz_INCA is used to investigate the contribution of African and Asian emissions to tropospheric ozone over central and West Africa during the summer monsoon. The model results show that ozone in this region is most sensitive to lightning NOx and to central African biomass burning emissions. However, other emission categories also contribute significantly to regional ozone. The maximum ozone changes due to lightning NOx occur in the upper troposphere between 400 hPa and 200 hPa over West Africa and downwind over the Atlantic Ocean. Biomass burning emissions mainly influence ozone in the lower and middle troposphere over central Africa, and downwind due to westward transport. Biogenic emissions of volatile organic compounds, which can be uplifted from the lower troposphere into higher altitudes by the deep convection that occurs over West Africa during the monsoon season, dominate the ozone changes in the upper troposphere and lower stratosphere region. Convective uplift of soil NOx emissions over the Sahel region also makes a significant contribution to ozone in the upper troposphere. Concerning African anthropogenic emissions, they make a lower contribution to ozone compared to the other emission categories. The model results indicate that most ozone changes due to African emissions occur downwind, especially over the Atlantic Ocean, far from the emission regions. The influence of Asian emissions should also be taken into account in studies of the ozone budget over Africa since they make a considerable contribution to ozone concentrations above 150 hPa. Using IPCC AR5 (Intergovernmental Panel on Climate Change; Fifth Assessment Report) estimates of anthropogenic emissions for 2030 over Africa and Asia, the model calculations suggest largest changes in ozone due to the growth of emissions over Asia than over Africa over the next 20 years.

scholarly journals Drivers of the tropospheric ozone budget throughout the 21st century under the medium-high climate scenario RCP 6.0

2015 ◽  
Vol 15 (10) ◽  
pp. 5887-5902 ◽  
Author(s):  
L. E. Revell ◽  
F. Tummon ◽  
A. Stenke ◽  
T. Sukhodolov ◽  
A. Coulon ◽  
...  
Keyword(s):  
Climate Change ◽  
21St Century ◽  
Tropospheric Ozone ◽  
Climate Scenario ◽  
Climate Impacts ◽  
Air Pollutant ◽  
Tropospheric Temperature ◽  
Ozone Precursor ◽  
Lightning Nox ◽  
Global Mean

Abstract. Because tropospheric ozone is both a greenhouse gas and harmful air pollutant, it is important to understand how anthropogenic activities may influence its abundance and distribution through the 21st century. Here, we present model simulations performed with the chemistry–climate model SOCOL, in which spatially disaggregated chemistry and transport tracers have been implemented in order to better understand the distribution and projected changes in tropospheric ozone. We examine the influences of ozone precursor emissions (nitrogen oxides (NOx), carbon monoxide (CO) and volatile organic compounds (VOCs)), climate change (including methane effects) and stratospheric ozone recovery on the tropospheric ozone budget, in a simulation following the climate scenario Representative Concentration Pathway (RCP) 6.0 (a medium-high, and reasonably realistic climate scenario). Changes in ozone precursor emissions have the largest effect, leading to a global-mean increase in tropospheric ozone which maximizes in the early 21st century at 23% compared to 1960. The increase is most pronounced at northern midlatitudes, due to regional emission patterns: between 1990 and 2060, northern midlatitude tropospheric ozone remains at constantly large abundances: 31% larger than in 1960. Over this 70-year period, attempts to reduce emissions in Europe and North America do not have an effect on zonally averaged northern midlatitude ozone because of increasing emissions from Asia, together with the long lifetime of ozone in the troposphere. A simulation with fixed anthropogenic ozone precursor emissions of NOx, CO and non-methane VOCs at 1960 conditions shows a 6% increase in global-mean tropospheric ozone by the end of the 21st century, with an 11 % increase at northern midlatitudes. This increase maximizes in the 2080s and is mostly caused by methane, which maximizes in the 2080s following RCP 6.0, and plays an important role in controlling ozone directly, and indirectly through its influence on other VOCs and CO. Enhanced flux of ozone from the stratosphere to the troposphere as well as climate change-induced enhancements in lightning NOx emissions also increase the tropospheric ozone burden, although their impacts are relatively small. Overall, the results show that under this climate scenario, ozone in the future is governed largely by changes in methane and NOx; methane induces an increase in tropospheric ozone that is approximately one-third of that caused by NOx. Climate impacts on ozone through changes in tropospheric temperature, humidity and lightning NOx remain secondary compared with emission strategies relating to anthropogenic emissions of NOx, such as fossil fuel burning. Therefore, emission policies globally have a critical role to play in determining tropospheric ozone evolution through the 21st century.

scholarly journals Emission sources contributing to tropospheric ozone over Equatorial Africa during the summer monsoon

2011 ◽  
Vol 11 (24) ◽  
pp. 13395-13419 ◽  
Author(s):  
I. Bouarar ◽  
K. S. Law ◽  
M. Pham ◽  
C. Liousse ◽  
H. Schlager ◽  
...  
Keyword(s):  
West Africa ◽  
Atlantic Ocean ◽  
Summer Monsoon ◽  
Biomass Burning ◽  
Tropospheric Ozone ◽  
Lower Troposphere ◽  
Anthropogenic Emissions ◽  
Upper Troposphere ◽  
Sahel Region ◽  
Lightning Nox

Abstract. A global chemistry-climate model LMDz_INCA is used to investigate the contribution of African and Asian emissions to tropospheric ozone over Central and West Africa during the summer monsoon. The model results show that ozone in this region is most sensitive to lightning NOx and to Central African biomass burning emissions. However, other emission categories also contribute significantly to regional ozone. The maximum ozone changes due to lightning NOx occur in the upper troposphere between 400 hPa and 200 hPa over West Africa and downwind over the Atlantic Ocean. Biomass burning emissions mainly influence ozone in the lower and middle troposphere over Central Africa, and downwind due to westward transport. Biogenic emissions of volatile organic compounds, which can be uplifted from the lower troposphere to higher altitudes by the deep convection that occurs over West Africa during the monsoon season, lead to maximum ozone changes in the lower stratosphere region. Soil NOx emissions over the Sahel region make a significant contribution to ozone in the lower troposphere. In addition, convective uplift of these emissions and subsequent ozone production are also an important source of ozone in the upper troposphere over West Africa. Concerning African anthropogenic emissions, they only make a small contribution to ozone compared to the other emission categories. The model results indicate that most ozone changes due to African emissions occur downwind, especially over the Atlantic Ocean, far from the emission regions. The import of Asian emissions also makes a considerable contribution to ozone concentrations above 150 hPa and has to be taken into account in studies of the ozone budget over Africa. Using IPCC AR5 (Intergovernmental Panel on Climate Change; Fifth Assessment Report) estimates of anthropogenic emissions for 2030 over Africa and Asia, model calculations show larger changes in ozone over Africa due to growth in Asian emissions compared to African emissions over the next 20 yr.

scholarly journals Drivers of the tropospheric ozone budget throughout the 21st century under the medium-high climate scenario RCP 6.0

2015 ◽  
Vol 15 (1) ◽  
pp. 481-519
Author(s):  
L. E. Revell ◽  
F. Tummon ◽  
A. Stenke ◽  
T. Sukhodolov ◽  
A. Coulon ◽  
...  
Keyword(s):  
Climate Change ◽  
21St Century ◽  
Tropospheric Ozone ◽  
Climate Scenario ◽  
Climate Impacts ◽  
Air Pollutant ◽  
Tropospheric Temperature ◽  
Ozone Precursor ◽  
Lightning Nox ◽  
Global Mean

Abstract. Because tropospheric ozone is both a~greenhouse gas and harmful air pollutant, it is important to understand how anthropogenic activities may influence its abundance and distribution through the 21st century. Here, we present model simulations performed with the chemistry-climate model SOCOL, in which spatially disaggregated chemistry and transport tracers have been implemented in order to better understand the distribution and projected changes in tropospheric ozone. We examine the influences of ozone precursor emissions (nitrogen oxides (NOx), carbon monoxide (CO) and volatile organic compounds (VOCs)), climate change and stratospheric ozone recovery on the tropospheric ozone budget, in a~simulation following the climate scenario Representative Concentration Pathway (RCP) 6.0. Changes in ozone precursor emissions have the largest effect, leading to a global-mean increase in tropospheric ozone which maximises in the early 21st century at 23%. The increase is most pronounced at northern midlatitudes, due to regional emission patterns: between 1990 and 2060, northern midlatitude tropospheric ozone remains at constantly large abundances: 31% larger than in 1960. Over this 70 year period, attempts to reduce emissions in Europe and North America do not have an effect on zonally-averaged northern midlatitude ozone because of increasing emissions from Asia, together with the longevity of ozone in the troposphere. A~simulation with fixed anthropogenic ozone precursor emissions of NOx, CO and non-methane VOCs at 1960 conditions shows a 6 % increase in global-mean tropospheric ozone, and an 11% increase at northern midlatitudes. This increase maximises in the 2080s, and is mostly caused by methane, which maximises in the 2080s following RCP 6.0, and plays an important role in controlling ozone directly, and indirectly through its influence on other VOCs and CO. Enhanced flux of ozone from the stratosphere to the troposphere as well as climate change-induced enhancements in lightning NOx emissions also increase the tropospheric ozone burden, although their impacts are relatively small. Overall, the results show that ozone in the future is governed largely by changes in methane and NOx; methane induces an increase in tropospheric ozone that is approximately one-third of that caused by NOx. Climate impacts on ozone through changes in tropospheric temperature, humidity and lightning NOx remain secondary compared with emission strategies relating to anthropogenic emissions of NOx, such as fossil fuel burning. Therefore, emission policies globally have a critical role to play in determining tropospheric ozone evolution through the 21st century.

scholarly journals Cloud-resolving chemistry simulation of a Hector thunderstorm

2012 ◽  
Vol 12 (7) ◽  
pp. 16701-16761 ◽  
Author(s):  
K. A. Cummings ◽  
T. L. Huntemann ◽  
K. E. Pickering ◽  
M. C. Barth ◽  
W. C. Skamarock ◽  
...  
Keyword(s):  
Early Morning ◽  
Primary Objective ◽  
Convective Transport ◽  
No Production ◽  
Lightning Flash ◽  
Mean Values ◽  
Mixing Ratios ◽  
Aircraft Observations ◽  
Cloud Resolving Model ◽  
Lightning Nox

Abstract. Cloud chemistry simulations are performed for a Hector storm observed on 16 November 2005 during the SCOUT-O3/ACTIVE campaigns based in Darwin, Australia, with the primary objective of estimating the average production of NO per lightning flash during the storm which occurred in a tropical environment. The 3-D WRF-AqChem model (Barth et al., 2007a) containing the WRF nonhydrostatic cloud-resolving model, online gas- and aqueous-phase chemistry, and a lightning-NOx production algorithm is used for these calculations. An idealized early morning sounding of temperature, water vapor, and winds is used to initialize the model. Surface heating of the Tiwi Islands is simulated in the model to induce convection. Aircraft observations from air undisturbed by the storm are used to construct composite initial condition chemical profiles. The idealized model storm has many characteristics similar to the observed storm. Convective transport in the idealized simulated storm is evaluated using tracer species, such as CO and O3. The convective transport of CO from the boundary layer to the anvil region was well represented in the model, with a small overestimate of the increase of CO at anvil altitudes. Lightning flashes observed by the LIghtning detection NETwork (LINET) are input to the model and a lightning placement scheme is used to inject the resulting NO into the simulated cloud. We find that a lightning NO production scenario of 500 moles per flash for both CG and IC flashes yields anvil NOx mixing ratios that match aircraft observations well for this storm. These values of NO production nearly match the mean values for CG and IC flashes obtained from similar modeling analyses conducted for several midlatitude and subtropical convective events and are larger than most other estimates for tropical thunderstorms. Approximately 85% of the lightning NOx mass was located at altitudes greater than 7 km in the later stages of the storm, which is an amount greater than found for subtropical and midlatitude storms. Upper tropospheric NO2 partial columns computed from the model output are also considerably greater than observed by satellite for most tropical marine convective events, as tropical island convection, such as Hector, is more vigorous and more productive of lightning NOx.

scholarly journals Comparison of ISS–CATS and CALIPSO–CALIOP Characterization of High Clouds in the Tropics

2020 ◽  
Vol 12 (23) ◽  
pp. 3946
Author(s):  
Pasquale Sellitto ◽  
Silvia Bucci ◽  
Bernard Legras
Keyword(s):  
Optical Properties ◽  
Space Station ◽  
Satellite Observation ◽  
Observation Data ◽  
Upper Troposphere ◽  
Cloud Properties ◽  
Synchronous Orbit ◽  
The Tropics ◽  
High Clouds

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.

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