scholarly journals Multi-species inversion of CH<sub>4</sub>, CO and H<sub>2</sub> emissions from surface measurements

2008 ◽  
Vol 8 (6) ◽  
pp. 20687-20722 ◽  
Author(s):  
I. Pison ◽  
P. Bousquet ◽  
F. Chevallier ◽  
S. Szopa ◽  
D. Hauglustaine
Keyword(s):  
Transport Model ◽  
Regional Scale ◽  
Surface Concentration ◽  
Temporal Variations ◽  
Global Scale ◽  
Chemical Transport Model ◽  
Methyl Chloroform ◽  
Emission Fluxes ◽  
Surface Measurements ◽  
Oxidation Chain

Abstract. In order to study the spatial and temporal variations of the emissions of greenhouse gases and of their precursors, we developed a data assimilation system. It is based on the atmospheric chemical transport model LMDz and on a simplified scheme for the oxidation chain of hydrocarbons, including methane, formaldehyde, carbon monoxide and molecular hydrogen together with methyl chloroform. Inversions of the emission fluxes of CO, CH4 and H2 and concentrations of HCHO and OH were performed for the year 2004, using surface concentration measurements as constraints. Independent data from satellite retrievals are used to evaluate the realism of the results. The total emitted mass of CO is 30% higher after the inversion and the spatial distribution of emissions of CH4 is modified by an increase of fluxes in boreal areas. The comparison between mono- and multi-species inversions shows that the results are close at a global scale but may significantly differ at a regional scale because of the interactions between the various tracers during the inversion.

scholarly journals Multi-species inversion of CH<sub>4</sub>, CO and H<sub>2</sub> emissions from surface measurements

2009 ◽  
Vol 9 (14) ◽  
pp. 5281-5297 ◽  
Author(s):  
I. Pison ◽  
P. Bousquet ◽  
F. Chevallier ◽  
S. Szopa ◽  
D. Hauglustaine
Keyword(s):  
Transport Model ◽  
Regional Scale ◽  
Surface Concentration ◽  
Temporal Variations ◽  
Global Scale ◽  
Chemical Transport Model ◽  
Methyl Chloroform ◽  
Emission Fluxes ◽  
Surface Measurements ◽  
One Year

Abstract. In order to study the spatial and temporal variations of the emissions of greenhouse gases and of their precursors, we developed a data assimilation system and applied it to infer emissions of CH4, CO and H2 for one year. It is based on an atmospheric chemical transport model and on a simplified scheme for the oxidation chain of hydrocarbons, including methane, formaldehyde, carbon monoxide and molecular hydrogen together with methyl chloroform. The methodology is exposed and a first attempt at evaluating the inverted fluxes is made. Inversions of the emission fluxes of CO, CH4 and H2 and concentrations of HCHO and OH were performed for the year 2004, using surface concentration measurements of CO, CH4, H2 and CH3CCl3 as constraints. Independent data from ship and aircraft measurements and satellite retrievals are used to evaluate the results. The total emitted mass of CO is 30% higher after the inversion, due to increased fluxes by up to 35% in the Northern Hemisphere. The spatial distribution of emissions of CH4 is modified by a decrease of fluxes in boreal areas up to 60%. The comparison between mono- and multi-species inversions shows that the results are close at a global scale but may significantly differ at a regional scale because of the interactions between the various tracers during the inversion.

scholarly journals Clouds, photolysis and regional tropospheric ozone budgets

2009 ◽  
Vol 9 (3) ◽  
pp. 13889-13916 ◽  
Author(s):  
A. Voulgarakis ◽  
O. Wild ◽  
N. H. Savage ◽  
G. D. Carver ◽  
J. A. Pyle
Keyword(s):  
Tropospheric Ozone ◽  
Large Scale ◽  
Transport Model ◽  
Regional Scale ◽  
Three Dimensional ◽  
Global Scale ◽  
Chemical Production ◽  
Chemical Transport Model ◽  
Photolysis Rates ◽  
Boundary Layer Ozone

Abstract. We use a three-dimensional chemical transport model to examine the shortwave radiative effects of clouds on the tropospheric ozone budget. In addition to looking at changes in global concentrations as previous studies have done, we examine changes in ozone chemical production and loss caused by clouds and how these vary in different parts of the troposphere. On a global scale, we find that clouds have a modest effect on ozone chemistry, but on a regional scale their role is much more significant, with the size of the response dependent on the region. The largest averaged changes in chemical budgets (±10–14%) are found in the marine troposphere, where cloud optical depths are high. We demonstrate that cloud effects are small on average in the middle troposphere because this is a transition region between reduction and enhancement in photolysis rates. We show that increases in boundary layer ozone due to clouds are driven by large-scale changes in downward ozone transport from higher in the troposphere rather than by decreases in in-situ ozone chemical loss rates. Increases in upper tropospheric ozone are caused by higher production rates due to backscattering of radiation and consequent increases in photolysis rates, mainly J(NO2). The global radiative effect of clouds on isoprene is stronger than on ozone. Tropospheric isoprene lifetime increases by 7% when taking clouds into account. We compare the importance of clouds in contributing to uncertainties in the global ozone budget with the role of other radiatively-important factors. The budget is most sensitive to the overhead ozone column, while surface albedo and clouds have smaller effects. However, uncertainty in representing the spatial distribution of clouds may lead to a large sensitivity on regional scales.

scholarly journals Clouds, photolysis and regional tropospheric ozone budgets

2009 ◽  
Vol 9 (21) ◽  
pp. 8235-8246 ◽  
Author(s):  
A. Voulgarakis ◽  
O. Wild ◽  
N. H. Savage ◽  
G. D. Carver ◽  
J. A. Pyle
Keyword(s):  
Tropospheric Ozone ◽  
Large Scale ◽  
Transport Model ◽  
Regional Scale ◽  
Three Dimensional ◽  
Lower Troposphere ◽  
Global Scale ◽  
Chemical Production ◽  
Chemical Transport Model ◽  
Photolysis Rates

Abstract. We use a three-dimensional chemical transport model to examine the shortwave radiative effects of clouds on the tropospheric ozone budget. In addition to looking at changes in global concentrations as previous studies have done, we examine changes in ozone chemical production and loss caused by clouds and how these vary in different parts of the troposphere. On a global scale, we find that clouds have a modest effect on ozone chemistry, but on a regional scale their role is much more significant, with the size of the response dependent on the region. The largest averaged changes in chemical budgets (±10–14%) are found in the marine troposphere, where cloud optical depths are high. We demonstrate that cloud effects are small on average in the middle troposphere because this is a transition region between reduction and enhancement in photolysis rates. We show that increases in boundary layer ozone due to clouds are driven by large-scale changes in downward ozone transport from higher in the troposphere rather than by decreases in in-situ ozone chemical loss rates. Increases in upper tropospheric ozone are caused by higher production rates due to backscattering of radiation and consequent increases in photolysis rates, mainly J(NO2). The global radiative effect of clouds on isoprene, through decreases of OH in the lower troposphere, is stronger than on ozone. Tropospheric isoprene lifetime increases by 7% when taking clouds into account. We compare the importance of clouds in contributing to uncertainties in the global ozone budget with the role of other radiatively-important factors. The budget is most sensitive to the overhead ozone column, while surface albedo and clouds have smaller effects. However, uncertainty in representing the spatial distribution of clouds may lead to a large sensitivity of the ozone budget components on regional scales.

scholarly journals Simulation of radon-222 with the GEOS-Chem global model: emissions, seasonality, and convective transport

2021 ◽  
Vol 21 (3) ◽  
pp. 1861-1887
Author(s):  
Bo Zhang ◽  
Hongyu Liu ◽  
James H. Crawford ◽  
Gao Chen ◽  
T. Duncan Fairlie ◽  
...  
Keyword(s):  
Large Scale ◽  
Emission Scenario ◽  
Transport Model ◽  
Lower Troposphere ◽  
Chemical Transport ◽  
Surface Concentration ◽  
Convective Transport ◽  
Emission Flux ◽  
Chemical Transport Model ◽  
Emission Fluxes

Abstract. Radon-222 (222Rn) is a short-lived radioactive gas naturally emitted from land surfaces and has long been used to assess convective transport in atmospheric models. In this study, we simulate 222Rn using the GEOS-Chem chemical transport model to improve our understanding of 222Rn emissions and surface concentration seasonality and characterize convective transport associated with two Goddard Earth Observing System (GEOS) meteorological products, the Modern-Era Retrospective analysis for Research and Applications (MERRA) and GEOS Forward Processing (GEOS-FP). We evaluate four global 222Rn emission scenarios by comparing model results with observations at 51 surface sites. The default emission scenario in GEOS-Chem yields a moderate agreement with surface observations globally (68.9 % of data within a factor of 2) and a large underestimate of winter surface 222Rn concentrations at Northern Hemisphere midlatitudes and high latitudes due to an oversimplified formulation of 222Rn emission fluxes (1 atom cm−2 s−1 over land with a reduction by a factor of 3 under freezing conditions). We compose a new global 222Rn emission scenario based on Zhang et al. (2011) and demonstrate its potential to improve simulated surface 222Rn concentrations and seasonality. The regional components of this scenario include spatially and temporally varying emission fluxes derived from previous measurements of soil radium content and soil exhalation models, which are key factors in determining 222Rn emission flux rates. However, large model underestimates of surface 222Rn concentrations still exist in Asia, suggesting unusually high regional 222Rn emissions. We therefore propose a conservative upscaling factor of 1.2 for 222Rn emission fluxes in China, which was also constrained by observed deposition fluxes of 210Pb (a progeny of 222Rn). With this modification, the model shows better agreement with observations in Europe and North America (> 80 % of data within a factor of 2) and reasonable agreement in Asia (close to 70 %). Further constraints on 222Rn emissions would require additional concentration and emission flux observations in the central United States, Canada, Africa, and Asia. We also compare and assess convective transport in model simulations driven by MERRA and GEOS-FP using observed 222Rn vertical profiles in northern midlatitude summer and from three short-term airborne campaigns. While simulations with both GEOS products are able to capture the observed vertical gradient of 222Rn concentrations in the lower troposphere (0–4 km), neither correctly represents the level of convective detrainment, resulting in biases in the middle and upper troposphere. Compared with GEOS-FP, MERRA leads to stronger convective transport of 222Rn, which is partially compensated for by its weaker large-scale vertical advection, resulting in similar global vertical distributions of 222Rn concentrations between the two simulations. This has important implications for using chemical transport models to interpret the transport of other trace species when these GEOS products are used as driving meteorology.

scholarly journals Influence of the aerosol solar extinction on photochemistry during the 2010 Russian wildfires episode

2015 ◽  
Vol 15 (19) ◽  
pp. 10983-10998 ◽  
Author(s):  
J. C. Péré ◽  
B. Bessagnet ◽  
V. Pont ◽  
M. Mallet ◽  
F. Minvielle
Keyword(s):  
Transport Model ◽  
Regional Scale ◽  
Model Performance ◽  
Surface Concentration ◽  
Near Surface ◽  
Aerosol Mass ◽  
Aerosol Mass Concentration ◽  
Air Quality Measurements ◽  
Photolysis Rates ◽  
Optical Module

Abstract. In this work, impact of aerosol solar extinction on the photochemistry over eastern Europe during the 2010 wildfires episode is discussed for the period from 5 to 12 August 2010, which coincides to the peak of fire activity. The methodology is based on an online coupling between the chemistry-transport model CHIMERE (extended by an aerosol optical module) and the radiative transfer code TUV. Results of simulations indicate an important influence of the aerosol solar extinction, in terms of intensity and spatial extent, with a reduction of the photolysis rates of NO2 and O3 up to 50 % (in daytime average) along the aerosol plume transport. At a regional scale, these changes in photolysis rates lead to a 3–15 % increase in the NO2 daytime concentration and to an ozone reduction near the surface of 1–12 %. The ozone reduction is shown to occur over the entire boundary layer, where aerosols are located. Also, the total aerosol mass concentration (PM10) is shown to be decreased by 1–2 %, on average during the studied period, caused by a reduced formation of secondary aerosols such as sulfates and secondary organics (4–10 %) when aerosol impact on photolysis rates is included. In terms of model performance, comparisons of simulations with air quality measurements at Moscow indicate that an explicit representation of aerosols interaction with photolysis rates tend to improve the estimation of the near-surface concentration of ozone and nitrogen dioxide as well as the formation of inorganic aerosol species such as ammonium, nitrates and sulfates.

scholarly journals Carbon monoxide (CO) and ethane (C<sub>2</sub>H<sub>6</sub>) trends from ground-based solar FTIR measurements at six European stations, comparison and sensitivity analysis with the EMEP model

2011 ◽  
Vol 11 (17) ◽  
pp. 9253-9269 ◽  
Author(s):  
J. Angelbratt ◽  
J. Mellqvist ◽  
D. Simpson ◽  
J. E. Jonson ◽  
T. Blumenstock ◽  
...  
Keyword(s):  
Transport Model ◽  
Global Scale ◽  
Global Model ◽  
Scale Model ◽  
Chemical Transport Model ◽  
Suitable Alternative ◽  
European Model ◽  
Time Period ◽  
Volatile Organic ◽  
Made In

Abstract. Trends in the CO andC2H6 partial columns ~0–15 km) have been estimated from four European ground-based solar FTIR (Fourier Transform InfraRed) stations for the 1996–2006 time period. The CO trends from the four stations Jungfraujoch, Zugspitze, Harestua and Kiruna have been estimated to −0.45 ± 0.16% yr−1, −1.00 ± 0.24% yr−1, −0.62 ± 0.19 % yr−1 and −0.61 ± 0.16% yr−1, respectively. The corresponding trends for C2H6 are −1.51 ± 0.23% yr−1, −2.11 ± 0.30% yr−1, −1.09 ± 0.25% yr−1 and −1.14 ± 0.18% yr−1. All trends are presented with their 2-σ confidence intervals. To find possible reasons for the CO trends, the global-scale EMEP MSC-W chemical transport model has been used in a series of sensitivity scenarios. It is shown that the trends are consistent with the combination of a 20% decrease in the anthropogenic CO emissions seen in Europe and North America during the 1996–2006 period and a 20% increase in the anthropogenic CO emissions in East Asia, during the same time period. The possible impacts of CH4 and biogenic volatile organic compounds (BVOCs) are also considered. The European and global-scale EMEP models have been evaluated against the measured CO and C2H6 partial columns from Jungfraujoch, Zugspitze, Bremen, Harestua, Kiruna and Ny-Ålesund. The European model reproduces, on average the measurements at the different sites fairly well and within 10–22% deviation for CO and 14–31% deviation for C2H6. Their seasonal amplitude is captured within 6–35% and 9–124% for CO and C2H6, respectively. However, 61–98% of the CO and C2H6 partial columns in the European model are shown to arise from the boundary conditions, making the global-scale model a more suitable alternative when modeling these two species. In the evaluation of the global model the average partial columns for 2006 are shown to be within 1–9% and 37–50% of the measurements for CO and C2H6, respectively. The global model sensitivity for assumptions made in this paper is also analyzed.

scholarly journals Sensitivity of the recent methane budget to LMDz sub-grid scale physical parameterizations

2015 ◽  
Vol 15 (8) ◽  
pp. 11853-11888
Author(s):  
R. Locatelli ◽  
P. Bousquet ◽  
M. Saunois ◽  
F. Chevallier ◽  
C. Cressot
Keyword(s):  
Satellite Data ◽  
Transport Model ◽  
Deep Convection ◽  
Chemical Transport ◽  
Global Scale ◽  
Methane Emissions ◽  
Inverse Modelling ◽  
Chemical Transport Model ◽  
Methane Budget ◽  
Physical Parameterizations

Abstract. With the densification of surface observing networks and the development of remote sensing of greenhouse gases from space, estimations of methane (CH4) sources and sinks by inverse modelling face new challenges. Indeed, the chemical transport model used to link the flux space with the mixing ratio space must be able to represent these different types of constraints for providing consistent flux estimations. Here we quantify the impact of sub-grid scale physical parameterization errors on the global methane budget inferred by inverse modelling using the same inversion set-up but different physical parameterizations within one chemical-transport model. Two different schemes for vertical diffusion, two others for deep convection, and one additional for thermals in the planetary boundary layer are tested. Different atmospheric methane datasets are used as constraints (surface observations or satellite retrievals). At the global scale, methane emissions differ, on average, from 4.1 Tg CH4 per year due to the use of different sub-grid scale parameterizations. Inversions using satellite total-column retrieved by GOSAT satellite are less impacted, at the global scale, by errors in physical parameterizations. Focusing on large-scale atmospheric transport, we show that inversions using the deep convection scheme of Emanuel (1991) derive smaller interhemispheric gradient in methane emissions. At regional scale, the use of different sub-grid scale parameterizations induces uncertainties ranging from 1.2 (2.7%) to 9.4% (14.2%) of methane emissions in Africa and Eurasia Boreal respectively when using only surface measurements from the background (extended) surface network. When using only satellite data, we show that the small biases found in inversions using GOSAT-CH4 data and a coarser version of the transport model were actually masking a poor representation of the stratosphere–troposphere gradient in the model. Improving the stratosphere–troposphere gradient reveals a larger bias in GOSAT-CH4 satellite data, which largely amplifies inconsistencies between surface and satellite inversions. A simple bias correction is proposed. The results of this work provide the level of confidence one can have for recent methane inversions relatively to physical parameterizations included in chemical-transport models.

scholarly journals Analysis of a Regional Scale Chemical-Transport Model to Investigate the Potential Capability of Satellites for Identifying a Widespread Air Pollution Event

2017 ◽  
Author(s):  
Jason Welsh ◽  
Jack Fishman
Keyword(s):  
Transport Model ◽  
Regional Scale ◽  
Ozone Production ◽  
Metropolitan Region ◽  
Trace Gas ◽  
Chemical Transport Model ◽  
Satellite Measurements ◽  
Pollution Event ◽  
Surface O3 ◽  
Good Agreement

We use a regional scale photochemical transport model to investigate the surface concentrations and column integrated amounts of ozone (O3) and nitrogen dioxide (NO2) during a pollution event that occurred in the St. Louis metropolitan region in 2012. These trace gases will be two of the primary constituents that will be measured by TEMPO, an instrument on a geostationary platform, which will result in a dataset that has hourly temporal resolution during the daytime and ~4 km spatial resolution. Although air quality managers are most concerned with surface concentrations, satellite measurements provide a quantity that reflects a column amount, which may or may not be directly relatable to what is measured at the surface. The model results provide good agreement with observed surface O3 concentrations, which is the only trace gas dataset that can be used for verification. The model shows that a plume of O3 extends downwind from St. Louis and contains an integrated amount of ozone of ~ 16 DU (1 DU = 2.69 x 1016 mol. cm-2), a quantity that is two to three times lower than what was observed by satellite measurements during two massive pollution episodes in the 1980s. Based on the smaller isolatable emissions coming from St. Louis, this quantity is not unreasonable, but may also reflect the reduction of photochemical ozone production due to the implementation of emission controls that have gone into effect in the past few decades.

scholarly journals Evaluating the performance of pyrogenic and biogenic emission inventories against one decade of space-based formaldehyde columns

2008 ◽  
Vol 8 (5) ◽  
pp. 16981-17036 ◽  
Author(s):  
T. Stavrakou ◽  
J.-F. Müller ◽  
I. De Smedt ◽  
M. Van Roozendael ◽  
G. R. van der Werf ◽  
...  
Keyword(s):  
Biomass Burning ◽  
Amazon Basin ◽  
Transport Model ◽  
Correlation Coefficients ◽  
Global Scale ◽  
Chemical Mechanism ◽  
Emission Inventories ◽  
Chemical Transport Model ◽  
Emissions Inventory ◽  
Fire Emissions

Abstract. A new one-decade dataset of formaldehyde (HCHO) columns retrieved from GOME and SCIAMACHY is compared with HCHO columns simulated by an updated version of the IMAGES global chemical transport model. This model version includes an optimized chemical scheme with respect to HCHO production, where the short-term and final HCHO yields from pyrogenically emitted non-methane volatile organic compounds (NMVOCs) are estimated from the Master Chemical Mechanism (MCM) and an explicit speciation profile of pyrogenic emissions. The model is driven by the Global Fire Emissions Database (GFED) version 1 or 2 for biomass burning, whereas biogenic emissions are provided either by the Global Emissions Inventory Activity (GEIA), or by a newly developed inventory based on the Model of Emissions of Gases and Aerosols from Nature (MEGAN) algorithms driven by meteorological fields from the European Centre for Medium-Range Weather Forecasts (ECMWF). The comparisons focus on tropical ecosystems, North America and China, which experience strong biogenic and biomass burning NMVOC emissions reflected in the enhanced measured HCHO columns. These comparisons aim at testing the ability of the model to reproduce the observed features of the HCHO distribution on the global scale and at providing a first assessment of the performance of the current emission inventories. The high correlation coefficients (r>0.8) between the observed and simulated columns over most regions indicate a very good consistency between the model, the implemented inventories and the HCHO dataset. The use of the MEGAN-ECMWF inventory improves the model/data agreement in almost all regions, but biases persist over parts of Africa and the Northern Australia. Although neither GFED version is consistent with the data over all regions, a better match is achieved over Indonesia and Southern Africa when GFEDv2 is used, but GFEDv1 succeeds better in getting the correct seasonal patterns and intensities of the fire episodes over the Amazon basin, as reflected by the higher correlations calculated in this region.

scholarly journals Evaluation of water vapour assimilation in the tropical upper troposphere and lower stratosphere by a chemical transport model

2016 ◽  
Vol 9 (9) ◽  
pp. 4355-4373 ◽  
Author(s):  
Swagata Payra ◽  
Philippe Ricaud ◽  
Rachid Abida ◽  
Laaziz El Amraoui ◽  
Jean-Luc Attié ◽  
...  
Keyword(s):  
Water Vapour ◽  
Lower Stratosphere ◽  
Transport Model ◽  
Michelson Interferometer ◽  
Model Space ◽  
Global Scale ◽  
Chemical Transport Model ◽  
Data Set ◽  
Upper Troposphere ◽  
Sensitivity Studies

Abstract. The present analysis deals with one of the most debated aspects of the studies on the upper troposphere/lower stratosphere (UTLS), namely the budget of water vapour (H2O) at the tropical tropopause. Within the French project “Multiscale water budget in the upper troposphere and lower stratosphere in the TROpics” (TRO-pico), a global-scale analysis has been set up based on space-borne observations, models and assimilation techniques. The MOCAGE-VALENTINA assimilation tool has been used to assimilate the Aura Microwave Limb Sounder (MLS) version 3.3 H2O measurements within the 316–5 hPa range from August 2011 to March 2013 with an assimilation window of 1 h. Diagnostics based on observations minus analysis and forecast are developed to assess the quality of the assimilated H2O fields. Comparison with an independent source of H2O measurements in the UTLS based on the space-borne Michelson Interferometer for Passive Atmospheric Sounding (MIPAS) observations and with meteorological ARPEGE analyses is also shown. Sensitivity studies of the analysed fields have been performed by (1) considering periods when no MLS measurements are available and (2) using H2O data from another MLS version (4.2). The studies have been performed within three different spaces in time and space coincidences with MLS (hereafter referred to as MLS space) and MIPAS (MIPAS space) observations and with the model (model space) outputs and at three different levels: 121 hPa (upper troposphere), 100 hPa (tropopause) and 68 hPa (lower stratosphere) in January and February 2012. In the MLS space, the analyses behave consistently with the MLS observations from the upper troposphere to the lower stratosphere. In the model space, the analyses are wetter than the reference atmosphere as represented by ARPEGE and MLS in the upper troposphere (121 hPa) and around the tropopause (100 hPa), but are consistent with MLS and MIPAS in the lower stratosphere (68 hPa). In the MIPAS space, the sensitivity and the vertical resolution of the MIPAS data set at 121 and 100 hPa prevent assessment of the behaviour of the analyses at 121 and 100 hPa, particularly over intense convective areas as the South American, the African and the Maritime continents but, in the lower stratosphere (68 hPa), the analyses are very consistent with MIPAS. Sensitivity studies show the improvement on the H2O analyses in the tropical UTLS when assimilating space-borne measurements of better quality, particularly over the convective areas.

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