Impact of different emission inventories on simulated tropospheric ozone over China: a regional chemical transport model evaluation

Abstract. The importance of emission inventory uncertainty on the simulation of summertime tropospheric Ozone over China has been analyzed using a regional chemical transport model. Three independent emissions inventories, that are (i) emission estimates from the Emission Database for Global Atmospheric Research (EDGAR) for the year 1995, (ii) a regional emission inventory used in the Transport and Chemical Evolution over the Pacific (TRACE-P) program with emissions for the year 2000 and (iii) a national emission inventory used in the China Ozone Research Program (CORP) with emission estimates for the year 1995, are used for model simulation over a summer period. Methods used for the development of the inventories are discussed and differences in simulated ozone and its precursors with these emission inventories are analyzed. Comparison of the emission inventories revealed large differences in the emission estimates (up to 50% for NOx, ~100% for NMVOC and ~1000% for CO). Application of the different emission inventories in three model simulations showed minor differences in both surface O3 in rather unpolluted areas in China and at higher altitudes (500 mbar). In polluted areas, differences in surface O3 are 30-50% between the different model simulations which seems rather small taking into account the large differences in the emission inventories. Additional sensitivity runs showed that the difference in NOx emissions as well NMVOC emissions is a dominant factor which controls the differences in simulated O3 concentrations while the impact of differences in CO emissions is relatively small. Although the CO emission estimate by CORP seems to be underestimated, there is no confidence to highlight one emission inventory better than the others.

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Impact of different emission inventories on simulated tropospheric ozone over China: a regional chemical transport model evaluation

Atmospheric Chemistry and Physics ◽

10.5194/acp-4-877-2004 ◽

2004 ◽

Vol 4 (4) ◽

pp. 877-887 ◽

Cited By ~ 39

Author(s):

J. Ma ◽

J. A. van Aardenne

Keyword(s):

Tropospheric Ozone ◽

Emission Inventory ◽

Transport Model ◽

Chemical Transport ◽

Dominant Factor ◽

Emission Inventories ◽

Chemical Transport Model ◽

Model Simulations ◽

The Impact ◽

Surface O3

Abstract. The importance of emission inventory uncertainty on the simulation of summertime tropospheric ozone over China has been analyzed using a regional chemical transport model. Three independent emissions inventories, that are (i) emission estimates from the Emission Database for Global Atmospheric Research (EDGAR) for the year 1995, (ii) a regional emission inventory used in the Transport and Chemical Evolution over the Pacific (TRACE-P) program with emissions for the year 2000 and (iii) a national emission inventory used in the China Ozone Research Program (CORP) with emission estimates for the year 1995, are used for model simulation over a summer period. Methods used for the development of the inventories are discussed and differences in simulated ozone and its precursors with these emission inventories are analyzed. Comparison of the emission inventories revealed large differences in the emission estimates (up to 50% for NOx, ~100% for NMVOC and ~1000% for CO). Application of the different emission inventories in three model simulations showed minor differences in both surface O3 in rather unpolluted areas in China and at higher altitudes (500mbar). In polluted areas, differences in surface O3 are 30-50% between the different model simulations which seem rather small taking into account the large differences in the emission inventories. Additional sensitivity runs showed that the difference in NOx emissions as well NMVOC emissions is a dominant factor which controls the differences in simulated O3 concentrations while the impact of differences in CO emissions is relatively small. Although the CO emission estimate by CORP seems to be underestimated, there is no confidence to highlight one emission inventory better than the others.

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Combined assimilation of IASI and MLS observations to constrain tropospheric and stratospheric ozone in a global chemical transport model

Atmospheric Chemistry and Physics Discussions ◽

10.5194/acpd-13-21455-2013 ◽

2013 ◽

Vol 13 (8) ◽

pp. 21455-21505

Author(s):

E. Emili ◽

B. Barret ◽

S. Massart ◽

E. Le Flochmoen ◽

A. Piacentini ◽

...

Keyword(s):

Tropospheric Ozone ◽

Radiative Forcing ◽

Transport Model ◽

Stratospheric Ozone ◽

Chemical Transport ◽

Free Troposphere ◽

Chemical Transport Model ◽

Ozone Monitoring Instrument ◽

Global Chemical Transport Model ◽

The Impact

Abstract. Accurate and temporally resolved fields of free-troposphere ozone are of major importance to quantify the intercontinental transport of pollution and the ozone radiative forcing. In this study we examine the impact of assimilating ozone observations from the Microwave Limb Sounder (MLS) and the Infrared Atmospheric Sounding Interferometer (IASI) in a global chemical transport model (MOdèle de Chimie Atmosphérique à Grande Échelle, MOCAGE). The assimilation of the two instruments is performed by means of a variational algorithm (4-D-VAR) and allows to constrain stratospheric and tropospheric ozone simultaneously. The analysis is first computed for the months of August and November 2008 and validated against ozone-sondes measurements to verify the presence of observations and model biases. It is found that the IASI Tropospheric Ozone Column (TOC, 1000–225 hPa) should be bias-corrected prior to assimilation and MLS lowermost level (215 hPa) excluded from the analysis. Furthermore, a longer analysis of 6 months (July–August 2008) showed that the combined assimilation of MLS and IASI is able to globally reduce the uncertainty (Root Mean Square Error, RMSE) of the modeled ozone columns from 30% to 15% in the Upper-Troposphere/Lower-Stratosphere (UTLS, 70–225 hPa) and from 25% to 20% in the free troposphere. The positive effect of assimilating IASI tropospheric observations is very significant at low latitudes (30° S–30° N), whereas it is not demonstrated at higher latitudes. Results are confirmed by a comparison with additional ozone datasets like the Measurements of OZone and wAter vapour by aIrbus in-service airCraft (MOZAIC) data, the Ozone Monitoring Instrument (OMI) total ozone columns and several high-altitude surface measurements. Finally, the analysis is found to be little sensitive to the assimilation parameters and the model chemical scheme, due to the high frequency of satellite observations compared to the average life-time of free-troposphere/low-stratosphere ozone.

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Combined assimilation of IASI and MLS observations to constrain tropospheric and stratospheric ozone in a global chemical transport model

Atmospheric Chemistry and Physics ◽

10.5194/acp-14-177-2014 ◽

2014 ◽

Vol 14 (1) ◽

pp. 177-198 ◽

Cited By ~ 18

Author(s):

E. Emili ◽

B. Barret ◽

S. Massart ◽

E. Le Flochmoen ◽

A. Piacentini ◽

...

Keyword(s):

Tropospheric Ozone ◽

Radiative Forcing ◽

Transport Model ◽

Stratospheric Ozone ◽

Chemical Transport ◽

Chemical Transport Model ◽

Ozone Monitoring Instrument ◽

Intercontinental Transport ◽

Global Chemical Transport Model ◽

The Impact

Abstract. Accurate and temporally resolved fields of free-troposphere ozone are of major importance to quantify the intercontinental transport of pollution and the ozone radiative forcing. We consider a global chemical transport model (MOdèle de Chimie Atmosphérique à Grande Échelle, MOCAGE) in combination with a linear ozone chemistry scheme to examine the impact of assimilating observations from the Microwave Limb Sounder (MLS) and the Infrared Atmospheric Sounding Interferometer (IASI). The assimilation of the two instruments is performed by means of a variational algorithm (4D-VAR) and allows to constrain stratospheric and tropospheric ozone simultaneously. The analysis is first computed for the months of August and November 2008 and validated against ozonesonde measurements to verify the presence of observations and model biases. Furthermore, a longer analysis of 6 months (July–December 2008) showed that the combined assimilation of MLS and IASI is able to globally reduce the uncertainty (root mean square error, RMSE) of the modeled ozone columns from 30 to 15% in the upper troposphere/lower stratosphere (UTLS, 70–225 hPa). The assimilation of IASI tropospheric ozone observations (1000–225 hPa columns, TOC – tropospheric O3 column) decreases the RMSE of the model from 40 to 20% in the tropics (30° S–30° N), whereas it is not effective at higher latitudes. Results are confirmed by a comparison with additional ozone data sets like the Measurements of OZone and wAter vapour by aIrbus in-service airCraft (MOZAIC) data, the Ozone Monitoring Instrument (OMI) total ozone columns and several high-altitude surface measurements. Finally, the analysis is found to be insensitive to the assimilation parameters. We conclude that the combination of a simplified ozone chemistry scheme with frequent satellite observations is a valuable tool for the long-term analysis of stratospheric and free-tropospheric ozone.

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A global stratospheric bromine monoxide climatology based on the BASCOE chemical transport model

Atmospheric Chemistry and Physics Discussions ◽

10.5194/acpd-8-17581-2008 ◽

2008 ◽

Vol 8 (5) ◽

pp. 17581-17629

Author(s):

N. Theys ◽

M. Van Roozendael ◽

Q. Errera ◽

F. Hendrick ◽

F. Daerden ◽

...

Keyword(s):

Transport Model ◽

Chemical Transport ◽

Atmospheric Dynamics ◽

Chemical Transport Model ◽

Output Data ◽

Data Set ◽

Chemistry Transport Model ◽

Model Simulations ◽

Chemical Indicators ◽

The Impact

Abstract. A new climatology of stratospheric BrO profiles based on dynamical and chemical indicators has been developed, with the aim to apply it to the retrieval of tropospheric BrO columns from space nadir measurements. The suitability of the adopted parameterization is evaluated based on three years of output data from the 3-D chemistry transport model BASCOE. The impact of the atmospheric dynamics on the stratospheric BrO distribution is treated by means of Bry/ozone correlations build from 3-D-CTM model results, while photochemical effects are taken into account using stratospheric NO2 columns as an indicator of the BrO/Bry ratio. The model simulations have been optimized for bromine chemistry and budget, and validated through comparisons using an extensive data set of ground-based, balloon-borne and satellite limb (SCIAMACHY) stratospheric BrO observations.

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A global stratospheric bromine monoxide climatology based on the BASCOE chemical transport model

Atmospheric Chemistry and Physics ◽

10.5194/acp-9-831-2009 ◽

2009 ◽

Vol 9 (3) ◽

pp. 831-848 ◽

Cited By ~ 50

Author(s):

N. Theys ◽

M. Van Roozendael ◽

Q. Errera ◽

F. Hendrick ◽

F. Daerden ◽

...

Keyword(s):

Transport Model ◽

Chemical Transport ◽

Atmospheric Dynamics ◽

Chemical Transport Model ◽

Output Data ◽

Data Set ◽

Chemistry Transport Model ◽

Model Simulations ◽

Chemical Indicators ◽

The Impact

Abstract. A new climatology of stratospheric BrO profiles based on a parameterization using dynamical and chemical indicators has been developed, with the aim to apply it to the retrieval of tropospheric BrO columns from space nadir measurements. The adopted parameterization is based on three years of output data from the 3-D chemistry transport model BASCOE. The impact of the atmospheric dynamics on the stratospheric BrO distribution is treated by means of Bry/ozone correlations built from 3-D-CTM model results, while photochemical effects are taken into account using stratospheric NO2 columns as an indicator of the BrO/Bry ratio. The model simulations have been optimized for bromine chemistry and budget, and validated through comparisons using an extensive data set of ground-based, balloon-borne and satellite limb (SCIAMACHY) stratospheric BrO observations.

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Record-breaking ozone loss in the Arctic winter 2010/2011: comparison with 1996/1997

Atmospheric Chemistry and Physics ◽

10.5194/acp-12-7073-2012 ◽

2012 ◽

Vol 12 (15) ◽

pp. 7073-7085 ◽

Cited By ~ 34

Author(s):

J. Kuttippurath ◽

S. Godin-Beekmann ◽

F. Lefèvre ◽

G. Nikulin ◽

M. L. Santee ◽

...

Keyword(s):

Transport Model ◽

Chemical Transport ◽

The Arctic ◽

Altitude Range ◽

Chemical Transport Model ◽

Model Simulations ◽

Ozone Loss ◽

Elevated Ozone ◽

Record Value ◽

First Time

Abstract. We present a detailed discussion of the chemical and dynamical processes in the Arctic winters 1996/1997 and 2010/2011 with high resolution chemical transport model (CTM) simulations and space-based observations. In the Arctic winter 2010/2011, the lower stratospheric minimum temperatures were below 195 K for a record period of time, from December to mid-April, and a strong and stable vortex was present during that period. Simulations with the Mimosa-Chim CTM show that the chemical ozone loss started in early January and progressed slowly to 1 ppmv (parts per million by volume) by late February. The loss intensified by early March and reached a record maximum of ~2.4 ppmv in the late March–early April period over a broad altitude range of 450–550 K. This coincides with elevated ozone loss rates of 2–4 ppbv sh−1 (parts per billion by volume/sunlit hour) and a contribution of about 30–55% and 30–35% from the ClO-ClO and ClO-BrO cycles, respectively, in late February and March. In addition, a contribution of 30–50% from the HOx cycle is also estimated in April. We also estimate a loss of about 0.7–1.2 ppmv contributed (75%) by the NOx cycle at 550–700 K. The ozone loss estimated in the partial column range of 350–550 K exhibits a record value of ~148 DU (Dobson Unit). This is the largest ozone loss ever estimated in the Arctic and is consistent with the remarkable chlorine activation and strong denitrification (40–50%) during the winter, as the modeled ClO shows ~1.8 ppbv in early January and ~1 ppbv in March at 450–550 K. These model results are in excellent agreement with those found from the Aura Microwave Limb Sounder observations. Our analyses also show that the ozone loss in 2010/2011 is close to that found in some Antarctic winters, for the first time in the observed history. Though the winter 1996/1997 was also very cold in March–April, the temperatures were higher in December–February, and, therefore, chlorine activation was moderate and ozone loss was average with about 1.2 ppmv at 475–550 K or 42 DU at 350–550 K, as diagnosed from the model simulations and measurements.

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A new diagnostic for tropospheric ozone production

10.5194/acp-2017-378 ◽

2017 ◽

Author(s):

Peter M. Edwards ◽

Mathew J. Evans

Keyword(s):

Air Quality ◽

Tropospheric Ozone ◽

Transport Model ◽

Chemical Transport ◽

Ozone Production ◽

Chemical Transport Model ◽

Organic Species ◽

Earth’S Climate ◽

Oxidation Of Organics

Abstract. Tropospheric ozone is important for the Earth’s climate and air quality. It is produced during the oxidation of organics in the presence of nitrogen oxides. Due to the range of organic species emitted and the chain like nature of their oxidation, this chemistry is complex and understanding the role of different processes (emission, deposition, chemistry) is difficult. We demonstrate a new methodology for diagnosing ozone production based on the processing of bonds contained within emitted molecules, the fate of which is determined by the conservation of spin of the bonding electrons. Using this methodology to diagnose ozone production in the GEOS-Chem chemical transport model, we demonstrate its advantages over the standard diagnostic. We show that the number of bonds emitted, their chemistry and lifetime, and feedbacks on OH are all important in determining the ozone production within the model and its sensitivity to changes. This insight may allow future model-model comparisons to better identify the root causes of model differences.

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Solar response in tropical stratospheric ozone: a 3-D chemical transport model study using ERA reanalyses

Atmospheric Chemistry and Physics ◽

10.5194/acp-11-12773-2011 ◽

2011 ◽

Vol 11 (24) ◽

pp. 12773-12786 ◽

Cited By ~ 23

Author(s):

S. Dhomse ◽

M. P. Chipperfield ◽

W. Feng ◽

J. D. Haigh

Keyword(s):

Standard Model ◽

Transport Model ◽

Stratospheric Ozone ◽

Chemical Transport ◽

Stratospheric Aerosol ◽

Data Sets ◽

Chemical Transport Model ◽

Model Simulations ◽

Model Study ◽

Significant Difference

Abstract. We have used an off-line 3-D chemical transport model (CTM) to investigate the 11-yr solar cycle response in tropical stratospheric ozone. The model is forced with European Centre for Medium-Range Weather Forecasts (ECMWF) (re)analysis (ERA-40/operational and ERA-Interim) data for the 1979–2005 time period. We have compared the modelled solar response in ozone to observation-based data sets that are constructed using satellite instruments such as Total Ozone Mapping Spectrometer (TOMS), Solar Backscatter UltraViolet instrument (SBUV), Stratospheric Aerosol and Gas Experiment (SAGE) and Halogen Occultation Experiment (HALOE). A significant difference is seen between simulated and observed ozone during the 1980s, which is probably due to inhomogeneities in the ERA-40 reanalyses. In general, the model with ERA-Interim dynamics shows better agreement with the observations from 1990 onwards than with ERA-40. Overall both standard model simulations are partially able to simulate a "double peak"-structured ozone solar response with a minimum around 30 km, and these are in better agreement with HALOE than SAGE-corrected SBUV (SBUV/SAGE) or SAGE-based data sets. In the tropical lower stratosphere (TLS), the modelled solar response with time-varying aerosols is amplified through aliasing with a volcanic signal, as the model overestimates ozone loss during high aerosol loading years. However, the modelled solar response with fixed dynamics and constant aerosols shows a positive signal which is in better agreement with SBUV/SAGE and SAGE-based data sets in the TLS. Our model simulations suggests that photochemistry contributes to the ozone solar response in this region. The largest model-observation differences occur in the upper stratosphere where SBUV/SAGE and SAGE-based data show a significant (up to 4%) solar response whereas the standard model and HALOE do not. This is partly due to a positive solar response in the ECMWF upper stratospheric temperatures which reduces the modelled ozone signal. The large positive upper stratospheric solar response seen in SBUV/SAGE and SAGE-based data can be reproduced in model runs with fixed dynamical fields (i.e. no inter-annual meteorological changes). As these runs effectively assume no long-term temperature changes (solar-induced or otherwise), it should provide an upper limit of the ozone solar response. Overall, full quantification of the solar response in stratospheric ozone is limited by differences in the observed data sets and by uncertainties in the solar response in stratospheric temperatures.

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