scholarly journals Development and implementation of a new biomass burning emissions injection height scheme for the GEOSChem model

Author(s):  
Liye Zhu ◽  
Maria Val Martin ◽  
Arsineh Hecobian ◽  
Luciana V. Gatti ◽  
Ralph Kahn ◽  
...  

Abstract. Biomass burning is a significant source of trace gases and aerosols to the atmosphere, and the evolution of these species depends acutely on where they are injected into the atmosphere. GEOS-Chem is a chemical transport model driven by assimilated meteorological data that is used to probe a variety of scientific questions related to atmospheric composition, including the role of biomass burning. This paper presents the development and implementation of a new global biomass burning emissions injection scheme in the GEOS-Chem model. The new injection scheme is based on monthly gridded Multi-Angle Imaging Spectro Radiometer (MISR) global plume-height stereoscopic observations in 2008. To provide specific examples of the impact of the model updates, we compare the output from simulations with and without the new MISR-based injection height scheme to several sets of observations from regions with active fires. Our comparisons with ARCTAS aircraft observations show that the updated injection height scheme improves the ability of the model to simulate the vertical distribution of peroxyacetyl nitrate (PAN) and carbon monoxide (CO) over North American boreal regions in summer. We also compare a simulation for October 2010 and 2011 to vertical profiles of CO over the Amazon Basin. When coupled with larger emission factors for CO, a simulation that includes the new injection scheme also better matches selected observations in this region. Finally the improved injection height also improves the simulation of monthly mean surface CO over California during July 2008, a period with large fires.

2018 ◽  
Vol 11 (10) ◽  
pp. 4103-4116 ◽  
Author(s):  
Liye Zhu ◽  
Maria Val Martin ◽  
Luciana V. Gatti ◽  
Ralph Kahn ◽  
Arsineh Hecobian ◽  
...  

Abstract. Biomass burning is a significant source of trace gases and aerosols to the atmosphere, and the evolution of these species depends acutely on where they are injected into the atmosphere. GEOS-Chem is a chemical transport model driven by assimilated meteorological data that is used to probe a variety of scientific questions related to atmospheric composition, including the role of biomass burning. This paper presents the development and implementation of a new global biomass burning emissions injection scheme in the GEOS-Chem model. The new injection scheme is based on monthly gridded Multi-angle Imaging SpectroRadiometer (MISR) global plume-height stereoscopic observations in 2008. To provide specific examples of the impact of the model updates, we compare the output from simulations with and without the new MISR-based injection height scheme to several sets of observations from regions with active fires. Our comparisons with Arctic Research on the Composition of the Troposphere from Aircraft and Satellites (ARCTAS) aircraft observations show that the updated injection height scheme can improve the ability of the model to simulate the vertical distribution of peroxyacetyl nitrate (PAN) and carbon monoxide (CO) over North American boreal regions in summer. We also compare a simulation for October 2010 and 2011 to vertical profiles of CO over the Amazon Basin. When coupled with larger emission factors for CO, a simulation that includes the new injection scheme also better matches selected observations in this region. Finally, the improved injection height improves the simulation of monthly mean surface CO over California during July 2008, a period with large fires.


2017 ◽  
Vol 17 (11) ◽  
pp. 6663-6678 ◽  
Author(s):  
Shreeya Verma ◽  
Julia Marshall ◽  
Mark Parrington ◽  
Anna Agustí-Panareda ◽  
Sebastien Massart ◽  
...  

Abstract. Airborne observations of greenhouse gases are a very useful reference for validation of satellite-based column-averaged dry air mole fraction data. However, since the aircraft data are available only up to about 9–13 km altitude, these profiles do not fully represent the depth of the atmosphere observed by satellites and therefore need to be extended synthetically into the stratosphere. In the near future, observations of CO2 and CH4 made from passenger aircraft are expected to be available through the In-Service Aircraft for a Global Observing System (IAGOS) project. In this study, we analyse three different data sources that are available for the stratospheric extension of aircraft profiles by comparing the error introduced by each of them into the total column and provide recommendations regarding the best approach. First, we analyse CH4 fields from two different models of atmospheric composition – the European Centre for Medium-Range Weather Forecasts (ECMWF) Integrated Forecasting System for Composition (C-IFS) and the TOMCAT/SLIMCAT 3-D chemical transport model. Secondly, we consider scenarios that simulate the effect of using CH4 climatologies such as those based on balloons or satellite limb soundings. Thirdly, we assess the impact of using a priori profiles used in the satellite retrievals for the stratospheric part of the total column. We find that the models considered in this study have a better estimation of the stratospheric CH4 as compared to the climatology-based data and the satellite a priori profiles. Both the C-IFS and TOMCAT models have a bias of about −9 ppb at the locations where tropospheric vertical profiles will be measured by IAGOS. The C-IFS model, however, has a lower random error (6.5 ppb) than TOMCAT (12.8 ppb). These values are well within the minimum desired accuracy and precision of satellite total column XCH4 retrievals (10 and 34 ppb, respectively). In comparison, the a priori profile from the University of Leicester Greenhouse Gases Observing Satellite (GOSAT) Proxy XCH4 retrieval and climatology-based data introduce larger random errors in the total column, being limited in spatial coverage and temporal variability. Furthermore, we find that the bias in the models varies with latitude and season. Therefore, applying appropriate bias correction to the model fields before using them for profile extension is expected to further decrease the error contributed by the stratospheric part of the profile to the total column.


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 ◽  
...  

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.


2020 ◽  
Author(s):  
Nikos Daskalakis ◽  
Maria Kanakidou ◽  
Mihalis Vrekoussis ◽  
Laura Gallardo

<p>Carbon Monoxide (CO) is an important atmospheric trace gas, and among the key O<sub>3</sub> precursors in the troposphere, alongside NO<sub>x</sub> and VOCs. It is among the most important sinks of OH radical in the atmosphere, which controls lifetime of CH<sub>4</sub> — a major greenhouse gas. Biomass burning sources contribute about 25% to the global emissions of CO, with the remaining CO being either emitted from anthropogenic sources, or being chemically formed in the atmosphere. Because of CO tropospheric lifetime is about two months; it can be transported in the atmosphere thus its sources have a hemispheric impact on atmospheric composition.</p><p>The extent of the impact of biomass burning to remote areas of the world through long range transport is here investigated using the global 3-dimensional chemistry transport model TM4-ECPL. For this, tagged biomass burning CO tracers from the 13 different HTAP (land) source regions are used in the model in order to evaluate the contribution of each source region to the CO concentrations in the 170 HTAP receptor regions that originate from biomass burning. The global simulations cover the period 1994—2015 in order to derive climatological transport patterns for CO and assess the contribution of each of the source regions to each of the receptor regions in the global troposphere. The CO simulations are evaluated by comparison with satellite observations from MOPITT and ground based observations from WDCGG. We show the significant impact of biomass burning emissions to the most remote regions of the world.</p>


2016 ◽  
Vol 16 (4) ◽  
pp. 1937-1953 ◽  
Author(s):  
Gregory R. Wentworth ◽  
Jennifer G. Murphy ◽  
Betty Croft ◽  
Randall V. Martin ◽  
Jeffrey R. Pierce ◽  
...  

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.


2015 ◽  
Vol 15 (2) ◽  
pp. 1915-1952
Author(s):  
L. Molina ◽  
G. Broquet ◽  
P. Imbach ◽  
F. Chevallier ◽  
B. Poulter ◽  
...  

Abstract. The exchanges of carbon, water, and energy between the atmosphere and the Amazon Basin have global implications for current and future climate. Here, the global atmospheric inversion system of the Monitoring of Atmospheric Composition and Climate service (MACC) was used to further study the seasonal and interannual variations of biogenic CO2 fluxes in Amazonia. The system assimilated surface measurements of atmospheric CO2 mole fractions made over more than 100 sites over the globe into an atmospheric transport model. This study added four surface stations located in tropical South America, a region poorly covered by CO2 observations. The estimates of net ecosystem exchange (NEE) optimized by the inversion were compared to independent estimates of NEE upscaled from eddy-covariance flux measurements in Amazonia, and against reports on the seasonal and interannual variations of the land sink in South America from the scientific literature. We focused on the impact of the interannual variation of the strong droughts in 2005 and 2010 (due to severe and longer-than-usual dry seasons), and of the extreme rainfall conditions registered in 2009. The spatial variations of the seasonal and interannual variability of optimized NEE were also investigated. While the inversion supported the assumption of strong spatial heterogeneity of these variations, the results revealed critical limitations that prevent global inversion frameworks from capturing the data-driven seasonal patterns of fluxes across Amazonia. In particular, it highlighted issues due to the configuration of the observation network in South America and the lack of continuity of the measurements. However, some robust patterns from the inversion seemed consistent with the abnormal moisture conditions in 2009.


2017 ◽  
Vol 17 (19) ◽  
pp. 11707-11726 ◽  
Author(s):  
Sarah J. Lawson ◽  
Martin Cope ◽  
Sunhee Lee ◽  
Ian E. Galbally ◽  
Zoran Ristovski ◽  
...  

Abstract. We have tested the ability of a high-resolution chemical transport model (CTM) to reproduce biomass burning (BB) plume strikes and ozone (O3) enhancements observed at Cape Grim in Tasmania, Australia, from the Robbins Island fire. The CTM has also been used to explore the contribution of near-field BB emissions and background sources to O3 observations under conditions of complex meteorology. Using atmospheric observations, we have tested model sensitivity to meteorology, BB emission factors (EFs) corresponding to low, medium, and high modified combustion efficiency (MCE), and spatial variability. The use of two different meteorological models (TAPM–CTM and CCAM–CTM) varied the first (BB1) plume strike time by up to 15 h and the duration of impact between 12 and 36 h, and it varied the second (BB2) plume duration between 50 and 57 h. Meteorology also had a large impact on simulated O3, with one model (TAPM–CTM) simulating four periods of O3 enhancement, while the other model (CCAM) simulating only one period. Varying the BB EFs, which in turn varied the non-methane organic compound (NMOC) ∕ oxides of nitrogen (NOx) ratio, had a strongly non-linear impact on simulated O3 concentration, with either destruction or production of O3 predicted in different simulations. As shown in previous work (Lawson et al., 2015), minor rainfall events have the potential to significantly alter EF due to changes in combustion processes. Models that assume fixed EF for O3 precursor species in an environment with temporally or spatially variable EF may be unable to simulate the behaviour of important species such as O3. TAPM–CTM is used to further explore the contribution of the Robbins Island fire to the observed O3 enhancements during BB1 and BB2. Overall, TAPM–CTM suggests that the dominant source of O3 observed at Cape Grim was aged urban air (age  = 2 days), with a contribution of O3 formed from local BB emissions. This work shows the importance of assessing model sensitivity to meteorology and EF and the large impact these variables can have in particular on simulated destruction or production of O3 in regional atmospheric chemistry simulations. This work also shows the importance of using models to elucidate the contribution from different sources to atmospheric composition, where this is difficult using observations alone.


2020 ◽  
Author(s):  
Georgia N. Theodoritsi ◽  
Giancarlo Ciarelli ◽  
Spyros N. Pandis

Abstract. A source-resolved three-dimensional chemical transport model, PMCAMx-SR, was applied in the continental U.S. to investigate the contribution of the various components (primary and secondary) of biomass burning organic aerosol (bbOA) to organic aerosol levels. Two different schemes based on the volatility basis set were used for the simulation of the bbOA during different seasons. The first is the default scheme of PMCAMx-SR and the second is a recently developed scheme based on laboratory experiments of the bbOA evolution. The simulations with the alternative bbOA scheme predict much higher total bbOA concentrations when compared with the base case ones. This is mainly due to the high emissions of intermediate volatility organic compounds (IVOCs) assumed in the alternative scheme. The oxidation of these compounds is predicted to be a significant source of secondary organic aerosol. The impact of the other parameters that differ in the two schemes is low to negligible. The monthly average maximum predicted concentrations of the alternative bbOA scheme were approximately an order of magnitude higher than those of the default scheme during all seasons. The performance of the two schemes was evaluated against observed total organic aerosol concentrations from several measurement sites across the US. The results were mixed. The default scheme performed better during July and September while the alternative scheme performed a little better during April. These results illustrate the uncertainty of the corresponding predictions, the need to quantify the emissions and reactions of IVOCs from specific biomass sources, and to better constrain the total (primary and secondary) bbOA levels.


2019 ◽  
Author(s):  
Emanuele Emili ◽  
Brice Barret ◽  
Eric Le Flochmoën ◽  
Daniel Cariolle

Abstract. The prior information used for Level 2 (L2) retrievals in the thermal infrared can influence the quality of the retrievals themselves and, therefore, their further assimilation in atmospheric composition models. In this study we evaluate the differences between assimilating L2 ozone profiles and Level 1 (L1) radiances from the Infrared Atmospheric Sounding Interferometer (IASI). We minimized potential differences between the two approaches by employing the same radiative transfer code (RTTOV) and a very similar setup for both the L2 retrievals (1D-Var) and the L1 assimilation (3D-Var). We computed hourly 3D-Var reanalyses assimilating respectively L1 and L2 data in the chemical transport model MOCAGE and compared the resulting O3 fields among each other and against ozonesondes. We also evaluated the joint assimilation of limb measurements from the Microwave Limb Sounder (MLS) on top of IASI to assess the impact of stratospheric O3 on tropospheric reanalyses. Results indicate that significant differences can arise between L2 and L1 assimilation, especially in regions where the L2 prior is biased (at the tropics and in the southern hemisphere in this study). L1 and L2 assimilation give instead very similar results in the northern hemisphere, especially when MLS measurements are used to constrain the stratospheric O3 column. We conclude this study by listing remaining issues that are common to both the L1 and L2 approaches and that deserve further research.


2016 ◽  
Author(s):  
Shreeya Verma ◽  
Julia Marshall ◽  
Mark Parrington ◽  
Anna Agusti-Panareda ◽  
Sebastien Massart ◽  
...  

Abstract. Airborne observations of greenhouse gases are a very useful reference for validation of satellite-based column-averaged dry air mole fraction data. However, since the aircraft data are available only up to about 9–13 km altitude, these profiles do not fully represent the depth of the atmosphere observed by satellites and therefore need to be extended synthetically into the stratosphere. In the near future, observations of CO2 and CH4 made from passenger aircraft are expected to be available through the In-Service Aircraft for a Global Observing System (IAGOS) project. In this study, we analyse three different data sources that are available for the stratospheric extension of aircraft profiles by comparing the error introduced by each of them into the total column and provide recommendations regarding the best approach. First, we analyse CH4 fields from two different models of atmospheric composition – the European Centre for Medium-Range Weather Forecasts (ECMWF) Integrated Forecasting System for Composition (C-IFS) and the TOMCAT/SLIMCAT 3-D chemical transport model. Secondly, we consider scenarios that simulate the effect of using CH4 climatologies such as those based on balloons or satellite limb soundings. Thirdly, we assess the impact of using a-priori profiles used in the satellite retrievals for the stratospheric part of the total column. We find that the models considered in this study have a better estimation of the stratospheric CH4 as compared to the climatology-based data and the satellite a-priori profiles. Both the C-IFS and TOMCAT models have a bias of about −9 ppb at the locations where tropospheric vertical profiles will be measured by IAGOS. The C-IFS model, however, has a lower random error (6.5 ppb) than TOMCAT (12.8 ppb). These values are well within the minimum desired accuracy and precision of satellite total column XCH4 retrievals (10 ppb and 34 ppb, respectively). In comparison, the a-priori profile from the University of Leicester Greenhouse Gases Observing Satellite (GOSAT) Proxy XCH4 retrieval and climatology-based data introduce larger random errors in the total column, being limited in spatial coverage and temporal variability. Furthermore, we find that the bias in the models varies with latitude and season. Therefore, applying appropriate bias correction to the model fields before using them for profile extension is expected to further decrease the error contributed by the stratospheric part of the profile to the total column.


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