scholarly journals The influence of biogenic emissions on upper-tropospheric methanol as revealed from space

2007 ◽  
Vol 7 (24) ◽  
pp. 6119-6129 ◽  
Author(s):  
G. Dufour ◽  
S. Szopa ◽  
D. A. Hauglustaine ◽  
C. D. Boone ◽  
C. P. Rinsland ◽  
...  
Keyword(s):  
Northern Hemisphere ◽  
Biomass Burning ◽  
Transport Model ◽  
Tropospheric Chemistry ◽  
Biogenic Emissions ◽  
Chemistry Transport Model ◽  
Mixing Ratios ◽  
Oxygenated Compounds ◽  
Global Space ◽  
The Impact

Abstract. The distribution and budget of oxygenated organic compounds in the atmosphere and their impact on tropospheric chemistry are still poorly constrained. Near-global space-borne measurements of seasonally resolved upper tropospheric profiles of methanol (CH3OH) by the ACE Fourier transform spectrometer provide a unique opportunity to evaluate our understanding of this important oxygenated organic species. ACE-FTS observations from March 2004 to August 2005 period are presented. These observations reveal the pervasive imprint of surface sources on upper tropospheric methanol: mixing ratios observed in the mid and high latitudes of the Northern Hemisphere reflect the seasonal cycle of the biogenic emissions whereas the methanol cycle observed in the southern tropics is highly influenced by biomass burning emissions. The comparison with distributions simulated by the state-of-the-art global chemistry transport model, LMDz-INCA, suggests that: (i) the background methanol (high southern latitudes) is correctly represented by the model considering the measurement uncertainties; (ii) the current emissions from the continental biosphere are underestimated during spring and summer in the Northern Hemisphere leading to an underestimation of modelled upper tropospheric methanol; (iii) the seasonal variation of upper tropospheric methanol is shifted to the fall in the model suggesting either an insufficient destruction of CH3OH (due to too weak chemistry and/or deposition) in fall and winter months or an unfaithful representation of transport; (iv) the impact of tropical biomass burning emissions on upper tropospheric methanol is rather well reproduced by the model. This study illustrates the potential of these first global profile observations of oxygenated compounds in the upper troposphere to improve our understanding of their global distribution, fate and budget.

scholarly journals The influence of biogenic emissions on upper-tropospheric methanol as revealed from space

2007 ◽  
Vol 7 (3) ◽  
pp. 9183-9202 ◽  
Author(s):  
G. Dufour ◽  
S. Szopa ◽  
D. A. Hauglustaine ◽  
C. D. Boone ◽  
C. P. Rinsland ◽  
...  
Keyword(s):  
Fourier Transform ◽  
Transport Model ◽  
State Of The Art ◽  
Tropospheric Chemistry ◽  
Biogenic Emissions ◽  
Fourier Transform Spectrometer ◽  
Satellite Measurements ◽  
Chemistry Transport Model ◽  
Organic Species ◽  
Global Space

Abstract. The distribution and budget of oxygenated organic compounds in the atmosphere and their impact on tropospheric chemistry are still poorly constrained. Near-global space-borne measurements of seasonally resolved upper tropospheric profiles of methanol by the ACE Fourier transform spectrometer provide a unique opportunity to evaluate our understanding of this important oxygenated organic species. The comparison with distributions simulated by a state-of-the-art chemistry transport model shows fair agreement during the March 2004 to August 2005 period with about 50% of the measurements reproduced by the model within 50%. However, in the northern hemisphere and during summertime, the satellite measurements reveal that the emissions from the continental biosphere lead to upper-tropospheric methanol concentrations significantly higher than expected.

scholarly journals Towards a representation of halogen chemistry within volcanic plumes in a chemistry transport model

2014 ◽  
Vol 7 (2) ◽  
pp. 2581-2650 ◽  
Author(s):  
L. Grellier ◽  
V. Marécal ◽  
B. Josse ◽  
P. D. Hamer ◽  
T. J. Roberts ◽  
...  
Keyword(s):  
Transport Model ◽  
Computational Cost ◽  
Ambient Air ◽  
Heterogeneous Reactions ◽  
Tropospheric Chemistry ◽  
Volcanic Plume ◽  
Large Set ◽  
Chemistry Transport Model ◽  
Volcanic Plumes ◽  
The Impact

Abstract. Volcanoes are a known source of halogens to the atmosphere. HBr volcanic emissions lead rapidly to the formation of BrO within volcanic plumes as shown by recent work based on observations and models. BrO, having a longer residence time in the atmosphere than HBr, is expected to have a significant impact on tropospheric chemistry, at least at the local and regional scales. The objective of this paper is to prepare a framework that will allow 3-D modelling of volcanic halogen emissions in order to determine their fate within the volcanic plume and then in the atmosphere at the regional and global scales. This work is based on a 1-D configuration of the chemistry transport model MOCAGE whose low computational cost allows us to perform a large set of sensitivity studies. This paper studies the Etna eruption on the 10 May 2008 that took place just before night time. Adaptations are made to MOCAGE to be able to produce the chemistry occurring within the volcanic plume. A simple sub-grid scale parameterization of the volcanic plume is implemented and tested. The use of this parameterization in a 0.5° × 0.5° configuration (typical regional resolution) has an influence on the partitioning between the various bromine compounds both during the eruption period and also during the night period immediately afterwards. During the day after the eruption, simulations both with and without parameterizations give very similar results that are consistent with the tropospheric column of BrO and SO2 in the volcanic plume derived from GOME-2 observations. Tests have been performed to evaluate the sensitivity of the results to the mixing between ambient air and the magmatic air at very high temperature at the crater vent that modifies the composition of the emission, and in particular the sulphate aerosol content that is key compound in the BrO production. Simulations show that the plume chemistry is not very sensitive to the assumptions used for the mixing parameter (relative quantity of ambient air mixed with magmatic air in the mixture) that is not well known. This is because there is no large change in the compounds limiting/favouring the BrO production in the plume. The impact of the model grid resolution is also tested in view of future 3-D-simulations at the global scale. A dilution of the emitted gases and aerosols is observed when using the typical global resolution (2°) as compared to a typical regional resolution (0.5°), as expected. Taking this into account, the results of the 2° resolution simulations are consistent with the GOME-2 observations. In general the simulations at 2° resolution are less efficient at producing BrO after the emission both with and without the subgrid-scale parameterization. The differences are mainly due to an interaction between concentration effects than stem from using a reduced volume in the 0.5° resolution combined with second order rate kinetics. The last series of tests were on the mean radius assumed for the sulphate aerosols that indirectly impacts the production of BrO by heterogeneous reactions. The simulations show that the BrO production is sensitive to this parameter with a stronger production when smaller aerosols are assumed. These results will be used to guide the implementation of volcanic halogen emissions in the 3-D configuration of MOCAGE.

scholarly journals Global upper-tropospheric formaldehyde: seasonal cycles observed by the ACE-FTS satellite instrument

2009 ◽  
Vol 9 (1) ◽  
pp. 1051-1095 ◽  
Author(s):  
G. Dufour ◽  
S. Szopa ◽  
M. P. Barkley ◽  
C. D. Boone ◽  
A. Perrin ◽  
...  
Keyword(s):  
Southern Hemisphere ◽  
Northern Hemisphere ◽  
Biomass Burning ◽  
Growing Season ◽  
Global Scale ◽  
Tropospheric Chemistry ◽  
Data Set ◽  
Mixing Ratios ◽  
Good Reproduction ◽  
Summer Maximum

Abstract. Seasonally-resolved upper tropospheric profiles of formaldehyde (HCHO) observed by the ACE Fourier transform spectrometer (ACE-FTS) on a near-global scale are presented for the time period from March 2004 to November 2006. Large upper tropospheric HCHO mixing ratios (>150 pptv) are observed during the growing season of the terrestrial biosphere in the Northern Hemisphere and during the biomass burning season in the Southern Hemisphere. The total errors estimated for the retrieved mixing ratios range from 30 to 40% in the upper troposphere and increase in the lower stratosphere. The sampled HCHO concentrations are in satisfactory agreement with previous aircraft and satellite observations with a negative bias (<25%) within observation errors. An overview of the seasonal cycle of the upper tropospheric HCHO is given for different latitudes. A maximum is observed during summer, i.e. during the growing season, in the northern mid- and high latitudes. The influence of biomass burning is visible in HCHO upper tropospheric concentrations during the September-to-October period in the southern tropics and subtropics. Comparisons with two state-of-the-art models (GEOS-Chem and LMDz-INCA) show that the models fail to reproduce the seasonal variations observed in the southern tropics and subtropics but they capture well the variations observed in the Northern Hemisphere (correlation >0.9). Both models underestimate the summer maximum over Europe and Russia and differences in the emissions used for North America result in a good reproduction of the summer maximum by GEOS-Chem but in an underestimate by LMDz-INCA. Globally, GEOS-Chem reproduces well the observations on average over one year but has some difficulties in reproducing the spatial variability of the observations. LMDz-INCA shows significant bias in the Southern Hemisphere, likely related to an underestimation of methane, but better reproduces the temporal and spatial variations. The differences between the models underline the large uncertainties that remain in the emissions of HCHO precursors. Observations of the HCHO upper tropospheric profile provided by the ACE-FTS represent a unique data set for investigating and improving our current understanding of the formaldehyde budget and upper tropospheric chemistry.

scholarly journals Assimilation of IASI satellite CO fields into a global chemistry transport model for validation against aircraft measurements

2012 ◽  
Vol 12 (10) ◽  
pp. 4493-4512 ◽  
Author(s):  
A. Klonecki ◽  
M. Pommier ◽  
C. Clerbaux ◽  
G. Ancellet ◽  
J.-P. Cammas ◽  
...  
Keyword(s):  
Transport Model ◽  
Source Region ◽  
Specific Treatment ◽  
Arctic Region ◽  
The Arctic ◽  
Chemistry Transport Model ◽  
Mixing Ratios ◽  
High Concentrations ◽  
The Impact

Abstract. This work evaluates the IASI CO product against independent in-situ aircraft data from the MOZAIC program and the POLARCAT aircraft campaign. The validation is carried out by analysing the impact of assimilation of eight months of IASI CO columns retrieved for the period of May to December 2008 into the global chemistry transport model LMDz-INCA. A modelling system based on a sub-optimal Kalman filter was developed and a specific treatment that takes into account the representativeness of observations at the scale of the model grid is applied to the IASI CO columns and associated errors before their assimilation in the model. Comparisons of the assimilated CO profiles with in situ CO measurements indicate that the assimilation leads to a considerable improvement of the model simulations in the middle troposphere as compared with a control run with no assimilation. Model biases in the simulation of background values are reduced and improvement in the simulation of very high concentrations is observed. The improvement is due to the transport by the model of the information present in the IASI CO retrievals. Our analysis also shows the impact of assimilation of CO on the representation of transport into the Arctic region during the POLARCAT summer campaign. A considerable increase in CO mixing ratios over the Asian source region was observed when assimilation was used leading to much higher values of CO during the cross-pole transport episode. These higher values are in good agreement with data from the POLARCAT flights that sampled this plume.

scholarly journals Reactive nitrogen, ozone and ozone production in the Arctic troposphere and the impact of stratosphere-troposphere exchange

2011 ◽  
Vol 11 (4) ◽  
pp. 10721-10767 ◽  
Author(s):  
Q. Liang ◽  
J. M. Rodriguez ◽  
A. R. Douglass ◽  
J. H. Crawford ◽  
E. Apel ◽  
...  
Keyword(s):  
Biomass Burning ◽  
Arctic Region ◽  
Tropospheric Chemistry ◽  
Ozone Production ◽  
The Arctic ◽  
Source Attribution ◽  
Air Masses ◽  
Upper Troposphere ◽  
Mixing Ratios ◽  
The Impact

Abstract. We analyze the aircraft observations obtained during the Arctic Research of the Composition of the Troposphere from Aircraft and Satellite (ARCTAS) mission together with the GEOS-5 CO simulation to examine O3 and NOy in the Arctic and sub-Arctic region and their source attribution. Using a number of marker tracers and their probability density distributions, we distinguish various air masses from the background troposphere and examine their contribution to NOx, O3, and O3 production in the Arctic troposphere. The background Arctic troposphere has mean O3 of ~60 ppbv and NOx of ~25 pptv throughout spring and summer with CO decreases from ~145 ppbv in spring to ~100 ppbv in summer. These observed CO, NOx and O3 mixing ratios are not notably different from the values measured during the 1988 ABLE-3A and the 2002 TOPSE field campaigns despite the significant changes in the past two decades in processes that could have changed the Arctic tropospheric composition. Air masses associated with stratosphere-troposphere exchange are present throughout the mid and upper troposphere during spring and summer. These air masses with mean O3 concentration of 140–160 ppbv are the most important direct sources of O3 in the Arctic troposphere. In addition, air of stratospheric origin is the only notable driver of net O3 formation in the Arctic due to its sustainable high NOx (75 pptv in spring and 110 pptv in summer) and NOy (~800 pptv in spring and ~1100 pptv in summer) levels. The ARCTAS measurements present observational evidence suggesting significant conversion of nitrogen from HNO3 to NOx and then to PAN (a net formation of ~120 pptv PAN) in summer when air of stratospheric origin is mixed with tropospheric background during stratosphere-to-troposphere transport. These findings imply that an adequate representation of stratospheric O3 and NOy input are essential in accurately simulating O3 and NOx photochemistry as well as the atmospheric budget of PAN in tropospheric chemistry transport models of the Arctic. Anthropogenic and biomass burning pollution plumes observed during ARCTAS show highly elevated hydrocarbons and NOy (mostly in the form of NOx and PAN), but do not contribute significantly to O3 in the Arctic troposphere except in some of the aged biomass burning plumes sampled during spring. Convection and/or lightning influences are negligible sources of O3 in the Arctic troposphere but can have significant impacts in the upper troposphere in the continental sub-Arctic during summer.

scholarly journals Interaction of anthropogenic and natural emission sources during a wild-land fire event – influence on ozone formation

2012 ◽  
Vol 12 (1) ◽  
pp. 3467-3507
Author(s):  
E. Bossioli ◽  
M. Tombrou ◽  
A. Karali ◽  
A. Dandou ◽  
D. Paronis ◽  
...  
Keyword(s):  
Eastern Europe ◽  
Transport Model ◽  
Biogenic Emissions ◽  
Fire Event ◽  
Chemistry Transport Model ◽  
Fire Emissions ◽  
Natural Emission ◽  
Lower Ratio ◽  
The Impact ◽  
Surface O3

Abstract. The objective of this study is to investigate the contribution of biomass burning in the formation of tropospheric O3. Furthermore, the impact of biogenic emissions under fire and no fire conditions is examined. This is achieved by applying the CAMx chemistry transport model for a wild-land fire event over Western Russia (24 April–10 May 2006). The model results are compared with O3 and isoprene observations from 117 and 9 stations of the EMEP network, respectively. Model computations show that the fire episode altered the O3 sensitivity in the area. In particular, the fire emissions increased surface O3 over Northern and Eastern Europe by up to 80% (40–45 ppb). In case of adopting a high fire NOx/CO emission ratio (0.06), the area (Eastern Europe and Western Russia) is characterized by VOC-sensitive O3 production and the impact of biogenic emissions is proven significant, contributing up to 8 ppb. Under a lower ratio (0.025), total surface O3 is almost doubled due to higher O3 production at the fire spots and lower fires' NO emissions. In this case as well as in the absence of fires, the impact of biogenic emissions is almost negligible. Injection height of the fire emissions accounted for O3 differences of the order of 10%, both at surface and over the planetary boundary layer (PBL).

scholarly journals A new version of the CNRM Chemistry-Climate Model, CNRM-CCM: description and improvements from the CCMVal-2 simulations

2011 ◽  
Vol 4 (4) ◽  
pp. 873-900 ◽  
Author(s):  
M. Michou ◽  
D. Saint-Martin ◽  
H. Teyssèdre ◽  
A. Alias ◽  
F. Karcher ◽  
...  
Keyword(s):  
Climate Model ◽  
Transport Model ◽  
Chemistry Transport Model ◽  
Mixing Ratios ◽  
Tropical Tropopause ◽  
On Line ◽  
Volcanic Aerosols ◽  
Chemical Fields ◽  
The Impact ◽  
Radiation Scheme

Abstract. This paper presents a new version of the Météo-France CNRM Chemistry-Climate Model, so-called CNRM-CCM. It includes some fundamental changes from the previous version (CNRM-ACM) which was extensively evaluated in the context of the CCMVal-2 validation activity. The most notable changes concern the radiative code of the GCM, and the inclusion of the detailed stratospheric chemistry of our Chemistry-Transport model MOCAGE on-line within the GCM. A 47-yr transient simulation (1960–2006) is the basis of our analysis. CNRM-CCM generates satisfactory dynamical and chemical fields in the stratosphere. Several shortcomings of CNRM-ACM simulations for CCMVal-2 that resulted from an erroneous representation of the impact of volcanic aerosols as well as from transport deficiencies have been eliminated. Remaining problems concern the upper stratosphere (5 to 1 hPa) where temperatures are too high, and where there are biases in the NO2, N2O5 and O3 mixing ratios. In contrast, temperatures at the tropical tropopause are too cold. These issues are addressed through the implementation of a more accurate radiation scheme at short wavelengths. Despite these problems we show that this new CNRM CCM is a useful tool to study chemistry-climate applications.

scholarly journals A new version of the CNRM Chemistry-Climate Model, CNRM-CCM: description and improvements from the CCMVal-2 simulations

2011 ◽  
Vol 4 (2) ◽  
pp. 1129-1183 ◽  
Author(s):  
M. Michou ◽  
D. Saint-Martin ◽  
H. Teyssèdre ◽  
A. Alias ◽  
F. Karcher ◽  
...  
Keyword(s):  
Climate Model ◽  
Transport Model ◽  
Chemistry Transport Model ◽  
Mixing Ratios ◽  
Tropical Tropopause ◽  
On Line ◽  
Volcanic Aerosols ◽  
Chemical Fields ◽  
The Impact ◽  
Radiation Scheme

Abstract. This paper presents a new version of the Météo-France CNRM Chemistry-Climate Model, so-called CNRM-CCM. It includes some fundamental changes from the previous version (CNRM-ACM) which was extensively evaluated in the context of the CCMVal-2 validation activity. The most notable changes concern the radiative code of the GCM, and the inclusion of the detailed stratospheric chemistry of our Chemistry-Transport model MOCAGE on-line within the GCM. A 47-yr transient simulation (1960–2006) is the basis of our analysis. CNRM-CCM generates satisfactory dynamical and chemical fields in the stratosphere. Several shortcomings of CNRM-ACM simulations for CCMVal-2 that resulted from an erroneous representation of the impact of volcanic aerosols as well as from transport deficiencies have been eliminated. Remaining problems concern the upper stratosphere (5 to 1 hPa) where temperatures are too high, and where there are biases in the NO2, N2O5 and O3 mixing ratios. In contrast, temperatures at the tropical tropopause are too cold. These issues are addressed through the implementation of a more accurate radiation scheme at short wavelengths. Despite these problems we show that this new CNRM CCM is a useful tool to study chemistry-climate applications.

scholarly journals Modeling anthropogenically controlled secondary organic aerosols in a megacity: a simplified framework for global and climate models

2011 ◽  
Vol 4 (4) ◽  
pp. 901-917 ◽  
Author(s):  
A. Hodzic ◽  
J. L. Jimenez
Keyword(s):  
Mexico City ◽  
Biomass Burning ◽  
Climate Models ◽  
Transport Model ◽  
Anthropogenic Pollution ◽  
Temporal Variations ◽  
Anthropogenic Sources ◽  
Organic Vapors ◽  
Chemistry Transport Model ◽  
Evolution Of Oxygen

Abstract. A simplified parameterization for secondary organic aerosol (SOA) formation in polluted air and biomass burning smoke is tested and optimized in this work, towards the goal of a computationally inexpensive method to calculate pollution and biomass burning SOA mass and hygroscopicity in global and climate models. A regional chemistry-transport model is used as the testbed for the parameterization, which is compared against observations from the Mexico City metropolitan area during the MILAGRO 2006 field experiment. The empirical parameterization is based on the observed proportionality of SOA concentrations to excess CO and photochemical age of the airmass. The approach consists in emitting an organic gas as lumped SOA precursor surrogate proportional to anthropogenic or biomass burning CO emissions according to the observed ratio between SOA and CO in aged air, and reacting this surrogate with OH into a single non-volatile species that condenses to form SOA. An emission factor of 0.08 g of the lumped SOA precursor per g of CO and a rate constant with OH of 1.25 × 10−11 cm3 molecule−1 s−1 reproduce the observed average SOA mass within 30 % in the urban area and downwind. When a 2.5 times slower rate is used (5 × 10−12 cm3 molecule−1 s−1) the predicted SOA amount and temporal evolution is nearly identical to the results obtained with SOA formation from semi-volatile and intermediate volatility primary organic vapors according to the Robinson et al. (2007) formulation. Our simplified method has the advantage of being much less computationally expensive than Robinson-type methods, and can be used in regions where the emissions of SOA precursors are not yet available. As the aged SOA/ΔCO ratios are rather consistent globally for anthropogenic pollution, this parameterization could be reasonably tested in and applied to other regions. The evolution of oxygen-to-carbon ratio was also empirically modeled and the predicted levels were found to be in reasonable agreement with observations. The potential enhancement of biogenic SOA by anthropogenic pollution, which has been suggested to play a major role in global SOA formation, is also tested using two simple parameterizations. Our results suggest that the pollution enhancement of biogenic SOA could provide additional SOA, but does not however explain the concentrations or the spatial and temporal variations of measured SOA mass in the vicinity of Mexico City, which appears to be controlled by anthropogenic sources. The contribution of the biomass burning to the predicted SOA is less than 10% during the studied period.

scholarly journals What could have caused pre-industrial biomass burning emissions to exceed current rates?

2013 ◽  
Vol 9 (1) ◽  
pp. 289-306 ◽  
Author(s):  
G. R. van der Werf ◽  
W. Peters ◽  
T. T. van Leeuwen ◽  
L. Giglio
Keyword(s):  
Population Density ◽  
Biomass Burning ◽  
Transport Model ◽  
Ice Core ◽  
Ice Cores ◽  
Fire Emissions ◽  
Core Data ◽  
Mixing Ratios ◽  
The Past ◽  
Co Concentrations

Abstract. Recent studies based on trace gas mixing ratios in ice cores and charcoal data indicate that biomass burning emissions over the past millennium exceeded contemporary emissions by up to a factor of 4 for certain time periods. This is surprising because various sources of biomass burning are linked with population density, which has increased over the past centuries. We have analysed how emissions from several landscape biomass burning sources could have fluctuated to yield emissions that are in correspondence with recent results based on ice core mixing ratios of carbon monoxide (CO) and its isotopic signature measured at South Pole station (SPO). Based on estimates of contemporary landscape fire emissions and the TM5 chemical transport model driven by present-day atmospheric transport and OH concentrations, we found that CO mixing ratios at SPO are more sensitive to emissions from South America and Australia than from Africa, and are relatively insensitive to emissions from the Northern Hemisphere. We then explored how various landscape biomass burning sources may have varied over the past centuries and what the resulting emissions and corresponding CO mixing ratio at SPO would be, using population density variations to reconstruct sources driven by humans (e.g., fuelwood burning) and a new model to relate savanna emissions to changes in fire return times. We found that to match the observed ice core CO data, all savannas in the Southern Hemisphere had to burn annually, or bi-annually in combination with deforestation and slash and burn agriculture exceeding current levels, despite much lower population densities and lack of machinery to aid the deforestation process. While possible, these scenarios are unlikely and in conflict with current literature. However, we do show the large potential for increased emissions from savannas in a pre-industrial world. This is mainly because in the past, fuel beds were probably less fragmented compared to the current situation; satellite data indicates that the majority of savannas have not burned in the past 10 yr, even in Africa, which is considered "the burning continent". Although we have not considered increased charcoal burning or changes in OH concentrations as potential causes for the elevated CO concentrations found at SPO, it is unlikely they can explain the large increase found in the CO concentrations in ice core data. Confirmation of the CO ice core data would therefore call for radical new thinking about causes of variable global fire rates over recent centuries.

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