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

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.

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

2009 ◽  
Vol 9 (3) ◽  
pp. 831-848 ◽  
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.

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

2004 ◽  
Vol 4 (1) ◽  
pp. 507-532 ◽  
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 (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.

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

2004 ◽  
Vol 4 (4) ◽  
pp. 877-887 ◽  
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.

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

2012 ◽  
Vol 12 (15) ◽  
pp. 7073-7085 ◽  
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.

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

2011 ◽  
Vol 11 (24) ◽  
pp. 12773-12786 ◽  
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.

scholarly journals Ammonia in the summertime Arctic marine boundary layer: sources, sinks, and implications

2016 ◽  
Vol 16 (4) ◽  
pp. 1937-1953 ◽  
Author(s):  
Gregory R. Wentworth ◽  
Jennifer G. Murphy ◽  
Betty Croft ◽  
Randall V. Martin ◽  
Jeffrey R. Pierce ◽  
...  
Keyword(s):  
Boundary Layer ◽  
Transport Model ◽  
Canadian Arctic ◽  
Atmospheric Composition ◽  
Chemical Transport Model ◽  
Data Set ◽  
Baffin Bay ◽  
Melt Ponds ◽  
Ambient Nh3 ◽  
The Impact

Abstract. Continuous hourly measurements of gas-phase ammonia (NH3(g)) were taken from 13 July to 7 August 2014 on a research cruise throughout Baffin Bay and the eastern Canadian Arctic Archipelago. Concentrations ranged from 30 to 650 ng m−3 (40–870 pptv) with the highest values recorded in Lancaster Sound (74°13′ N, 84°00′ W). Simultaneous measurements of total ammonium ([NHx]), pH and temperature in the ocean and in melt ponds were used to compute the compensation point (χ), which is the ambient NH3(g) concentration at which surface–air fluxes change direction. Ambient NH3(g) was usually several orders of magnitude larger than both χocean and χMP (< 0.4–10 ng m3) indicating these surface pools are net sinks of NH3. Flux calculations estimate average net downward fluxes of 1.4 and 1.1 ng m−2 s−1 for the open ocean and melt ponds, respectively. Sufficient NH3(g) was present to neutralize non-sea-salt sulfate (nss-SO42−) in the boundary layer during most of the study. This finding was corroborated with a historical data set of PM2.5 composition from Alert, Nunavut (82°30′ N, 62°20′ W) wherein the median ratio of NH4+/nss-SO42− equivalents was greater than 0.75 in June, July and August. The GEOS-Chem chemical transport model was employed to examine the impact of NH3(g) emissions from seabird guano on boundary-layer composition and nss-SO42− neutralization. A GEOS-Chem simulation without seabird emissions underestimated boundary layer NH3(g) by several orders of magnitude and yielded highly acidic aerosol. A simulation that included seabird NH3 emissions was in better agreement with observations for both NH3(g) concentrations and nss-SO42− neutralization. This is strong evidence that seabird colonies are significant sources of NH3 in the summertime Arctic, and are ubiquitous enough to impact atmospheric composition across the entire Baffin Bay region. Large wildfires in the Northwest Territories were likely an important source of NH3, but their influence was probably limited to the Central Canadian Arctic. Implications of seabird-derived N-deposition to terrestrial and aquatic ecosystems are also discussed.

scholarly journals Statistical diagnostic and correction of a chemistry-transport model for the prediction of total column ozone

2006 ◽  
Vol 6 (2) ◽  
pp. 525-537 ◽  
Author(s):  
S. Guillas ◽  
G. C. Tiao ◽  
D. J. Wuebbles ◽  
A. Zubrow
Keyword(s):  
Transport Model ◽  
Chemical Transport ◽  
Satellite System ◽  
Chemical Transport Model ◽  
Quasi Biennial Oscillation ◽  
Data Set ◽  
Total Column Ozone ◽  
Noise Component ◽  
Column Ozone ◽  
Total Column

Abstract. In this paper, we introduce a statistical method for examining and adjusting chemical-transport models. We illustrate the findings with total column ozone predictions, based on the University of Illinois at Urbana-Champaign 2-D (UIUC 2-D) chemical-transport model of the global atmosphere. We propose a general diagnostic procedure for the model outputs in total ozone over the latitudes ranging from 60° South to 60° North to see if the model captures some typical patterns in the data. The method proceeds in two steps to avoid possible collinearity issues. First, we regress the measurements given by a cohesive data set from the SBUV(/2) satellite system on the model outputs with an autoregressive noise component. Second, we regress the residuals of this first regression on the solar flux, the annual cycle, the Antarctic or Arctic Oscillation, and the Quasi Biennial Oscillation. If the coefficients from this second regression are statistically significant, then they mean that the model did not simulate properly the pattern associated with these factors. Systematic anomalies of the model are identified using data from 1979 to 1995, and statistically corrected afterwards. The 1996–2003 validation sample confirms that the combined approach yields better predictions than the direct UIUC 2-D outputs.

scholarly journals On the ability of chemical transport models to simulate the vertical structure of the N<sub>2</sub>O, NO<sub>2</sub> and HNO<sub>3</sub> species in the mid-latitude stratosphere

2005 ◽  
Vol 5 (6) ◽  
pp. 12373-12401
Author(s):  
G. Berthet ◽  
N. Huret ◽  
F. Lefèvre ◽  
G. Moreau ◽  
C. Robert ◽  
...  
Keyword(s):  
Transport Model ◽  
Three Dimensional ◽  
Chemical Transport ◽  
Chemical Transport Model ◽  
Transport Models ◽  
One Dimensional ◽  
Chemical Transport Models ◽  
Dimensional Version ◽  
The Impact

Abstract. In this paper we study the impact of the modelling of N2O on the simulation of NO2 and HNO3 by comparing in situ vertical profiles measured at mid-latitudes with the results of the Reprobus 3-D CTM (Three-dimensional Chemical Transport Model) computed with the kinetic parameters from the JPL recommendation in 2002. The analysis of the measured in situ profile of N2O shows particular features indicating different air mass origins. The measured N2O, NO2 and HNO3 profiles are not satisfyingly reproduced by the CTM when computed using the current 6-hourly ECMWF operational analysis. Improving the simulation of N2O transport allows us to calculate quantities of NO2 and HNO3 in reasonable agreement with observations. This is achieved using 3-hourly winds obtained from ECMWF forecasts. The best agreement is obtained by constraining a one-dimensional version of the model with the observed N2O. This study shows that modelling the NOy partitioning with better accuracy relies at least on a correct simulation of N2O and thus of total NOy.

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

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.

scholarly journals ML-TOMCAT: machine-learning-based satellite-corrected global stratospheric ozone profile data set from a chemical transport model

2021 ◽  
Vol 13 (12) ◽  
pp. 5711-5729
Author(s):  
Sandip S. Dhomse ◽  
Carlo Arosio ◽  
Wuhu Feng ◽  
Alexei Rozanov ◽  
Mark Weber ◽  
...  
Keyword(s):  
Transport Model ◽  
Stratospheric Ozone ◽  
Chemical Transport ◽  
Data Sets ◽  
Chemical Transport Model ◽  
Profile Data ◽  
Data Set ◽  
Ozone Profile ◽  
Satellite Instruments

Abstract. High-quality stratospheric ozone profile data sets are a key requirement for accurate quantification and attribution of long-term ozone changes. Satellite instruments provide stratospheric ozone profile measurements over typical mission durations of 5–15 years. Various methodologies have then been applied to merge and homogenise the different satellite data in order to create long-term observation-based ozone profile data sets with minimal data gaps. However, individual satellite instruments use different measurement methods, sampling patterns and retrieval algorithms which complicate the merging of these different data sets. In contrast, atmospheric chemical models can produce chemically consistent long-term ozone simulations based on specified changes in external forcings, but they are subject to the deficiencies associated with incomplete understanding of complex atmospheric processes and uncertain photochemical parameters. Here, we use chemically self-consistent output from the TOMCAT 3-D chemical transport model (CTM) and a random-forest (RF) ensemble learning method to create a merged 42-year (1979–2020) stratospheric ozone profile data set (ML-TOMCAT V1.0). The underlying CTM simulation was forced by meteorological reanalyses, specified trends in long-lived source gases, solar flux and aerosol variations. The RF is trained using the Stratospheric Water and OzOne Satellite Homogenized (SWOOSH) data set over the time periods of the Microwave Limb Sounder (MLS) from the Upper Atmosphere Research Satellite (UARS) (1991–1998) and Aura (2005–2016) missions. We find that ML-TOMCAT shows excellent agreement with available independent satellite-based data sets which use pressure as a vertical coordinate (e.g. GOZCARDS, SWOOSH for non-MLS periods) but weaker agreement with the data sets which are altitude-based (e.g. SAGE-CCI-OMPS, SCIAMACHY-OMPS). We find that at almost all stratospheric levels ML-TOMCAT ozone concentrations are well within uncertainties of the observational data sets. The ML-TOMCAT (V1.0) data set is ideally suited for the evaluation of chemical model ozone profiles from the tropopause to 0.1 hPa and is freely available via https://doi.org/10.5281/zenodo.5651194 (Dhomse et al., 2021).

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