scholarly journals Source attribution of Arctic black carbon constrained by aircraft and surface measurements

2017 ◽  
Vol 17 (19) ◽  
pp. 11971-11989 ◽  
Author(s):  
Jun-Wei Xu ◽  
Randall V. Martin ◽  
Andrew Morrow ◽  
Sangeeta Sharma ◽  
Lin Huang ◽  
...  
Keyword(s):  
North America ◽  
Biomass Burning ◽  
Western Siberia ◽  
Transport Model ◽  
Chemical Transport ◽  
The Arctic ◽  
Anthropogenic Emissions ◽  
Chemical Transport Model ◽  
Northern Asia ◽  
Airborne Measurements

Abstract. Black carbon (BC) contributes to Arctic warming, yet sources of Arctic BC and their geographic contributions remain uncertain. We interpret a series of recent airborne (NETCARE 2015; PAMARCMiP 2009 and 2011 campaigns) and ground-based measurements (at Alert, Barrow and Ny-Ålesund) from multiple methods (thermal, laser incandescence and light absorption) with the GEOS-Chem global chemical transport model and its adjoint to attribute the sources of Arctic BC. This is the first comparison with a chemical transport model of refractory BC (rBC) measurements at Alert. The springtime airborne measurements performed by the NETCARE campaign in 2015 and the PAMARCMiP campaigns in 2009 and 2011 offer BC vertical profiles extending to above 6 km across the Arctic and include profiles above Arctic ground monitoring stations. Our simulations with the addition of seasonally varying domestic heating and of gas flaring emissions are consistent with ground-based measurements of BC concentrations at Alert and Barrow in winter and spring (rRMSE  < 13 %) and with airborne measurements of the BC vertical profile across the Arctic (rRMSE  = 17 %) except for an underestimation in the middle troposphere (500–700 hPa).Sensitivity simulations suggest that anthropogenic emissions in eastern and southern Asia have the largest effect on the Arctic BC column burden both in spring (56 %) and annually (37 %), with the largest contribution in the middle troposphere (400–700 hPa). Anthropogenic emissions from northern Asia contribute considerable BC (27 % in spring and 43 % annually) to the lower troposphere (below 900 hPa). Biomass burning contributes 20 % to the Arctic BC column annually.At the Arctic surface, anthropogenic emissions from northern Asia (40–45 %) and eastern and southern Asia (20–40 %) are the largest BC contributors in winter and spring, followed by Europe (16–36 %). Biomass burning from North America is the most important contributor to all stations in summer, especially at Barrow.Our adjoint simulations indicate pronounced spatial heterogeneity in the contribution of emissions to the Arctic BC column concentrations, with noteworthy contributions from emissions in eastern China (15 %) and western Siberia (6.5 %). Although uncertain, gas flaring emissions from oilfields in western Siberia could have a striking impact (13 %) on Arctic BC loadings in January, comparable to the total influence of continental Europe and North America (6.5 % each in January). Emissions from as far as the Indo-Gangetic Plain could have a substantial influence (6.3 % annually) on Arctic BC as well.

scholarly journals Source attribution of Arctic black carbon constrained by aircraft and surface measurements

2017 ◽  
Author(s):  
Junwei Xu ◽  
Randall V. Martin ◽  
Andrew Morrow ◽  
Sangeeta Sharma ◽  
Lin Huang ◽  
...  
Keyword(s):  
North America ◽  
Black Carbon ◽  
Biomass Burning ◽  
Western Siberia ◽  
The Arctic ◽  
Anthropogenic Emissions ◽  
Northern Asia ◽  
Airborne Measurements ◽  
Gas Flaring ◽  
Southern Asia

Abstract. Black carbon (BC) contributes to both degraded air quality and Arctic warming, however sources of Arctic BC and their geographic contributions remain uncertain. We interpret a series of recent airborne and ground-based measurements with the GEOS-Chem global chemical transport model and its adjoint to attribute the sources of Arctic BC. The springtime airborne measurements performed by the NETCARE campaign in 2015 and the PAMARCMiP campaigns in 2009 and 2011 offer BC vertical profiles extending to > 6 km across the Arctic and include profiles above Arctic ground monitoring stations. Long-term ground-based measurements are examined from multiple methods (thermal, laser incandescence and light absorption) at Alert (2011–2013), Barrow (2009–2015) and Ny-Ålesund (2009–2014) stations. Our simulations with the addition of gas flaring emissions are consistent with ground-based measurements of BC concentrations at Alert and Barrow in winter and spring (rRMSE < 13 %), and with airborne measurements of BC vertical profile across the Arctic (rRMSE = 17 %). Sensitivity simulations suggest that anthropogenic emissions in eastern and southern Asia are the largest source of the Arctic BC column both in spring (56 %) and annually (37 %), with larger contributions aloft than near the surface (e.g. a contribution of 66 % between 400–700 hPa and of 46 % below 900 hPa in spring). Anthropogenic emissions from northern Asia contribute considerable BC to the lower troposphere (a contribution of 27 % in spring and of 43 % annually below 900 hPa). Biomass burning has a substantial contribution to Arctic BC below 400 hPa of 25 % annually, despite minor influence in spring ( 50 %) in winter and those from eastern and southern Asia are the largest in spring (~ 40 %). At Ny-Ålesund, anthropogenic emissions from Europe (~ 30 %) and northern Asia (~ 30 %) are major sources in winter and early spring. Biomass burning from North America is the most important contributor to surface BC at all stations in summer, especially at Barrow where North American biomass burning contributes more than 90 % of BC in July and August. Our adjoint simulations indicate pronounced spatial and seasonal heterogeneity in the contribution of emissions to the Arctic BC column concentrations with noteworthy contributions from emissions in eastern China (15 %) and western Siberia (6.5 %). Although uncertain, gas flaring emissions from oilfields in western Siberia could have a striking impact (13 %) on Arctic BC loadings in January, comparable to the total influence of continental Europe and North America (6.5 % each in January).

scholarly journals Biomass burning influence on high latitude tropospheric ozone and reactive nitrogen in summer 2008: a multi-model analysis based on POLMIP simulations

2014 ◽  
Vol 14 (17) ◽  
pp. 24573-24621 ◽  
Author(s):  
S. R. Arnold ◽  
L. K. Emmons ◽  
S. A. Monks ◽  
K. S. Law ◽  
D. A. Ridley ◽  
...  
Keyword(s):  
Biomass Burning ◽  
High Latitude ◽  
Tropospheric Ozone ◽  
Transport Model ◽  
Chemical Transport ◽  
Ozone Production ◽  
The Arctic ◽  
Vertical Position ◽  
Chemical Transport Model ◽  
Fire Emissions

Abstract. We have evaluated tropospheric ozone enhancement in air dominated by biomass burning emissions at high laititudes (> 50˚ N) in July 2008, using 10 global chemical transport model simulations from the POLMIP multi-model comparison exercise. In model air masses dominated by fire emissions, Δ O3/ΔCO values ranged between 0.039 and 0.196 ppbv ppbv−1 (mean: 0.113 ppbv ppbv−1) in freshly fire-influenced air, and between 0.140 and 0.261 ppbv ppbv−1 (mean: 0.193 ppbv) in more aged fire-influenced air. These values are in broad agreement with the range of observational estimates from the literature. Model ΔPAN/ΔCO enhancement ratios show distinct groupings according to the meteorological data used to drive the models. ECMWF-forced models produce larger ΔPAN/ΔCO values (4.44–6.28 pptv ppbv−1) than GEOS5-forced models (2.02–3.02 pptv ppbv−1), which we show is likely linked to differences efficiency of vertical transport during poleward export from mid-latitude source regions. Simulations of a large plume of biomass burning and anthropogenic emissions exported from Asia towards the Arctic using a Lagrangian chemical transport model show that 4 day net ozone change in the plume is sensitive to differences in plume chemical composition and plume vertical position among the POLMIP models. In particular, Arctic ozone evolution in the plume is highly sensitive to initial concentrations of PAN, as well as oxygenated VOCs (acetone, acetaldehyde), due to their role in producing the peroxyacetyl radical PAN precursor. Vertical displacement is also important due to its effects on the stability of PAN, and subsequent effect on NOx abundance. In plumes where net ozone production is limited, we find that the lifetime of ozone in the plume is sensitive to hydrogen peroxide loading, due to the production of HO2 from peroxide photolysis, and the key role of HO2 + O3 in controlling ozone loss. Overall, our results suggest that emissions from biomass burning lead to large-scale photochemical enhancement in high latitude tropospheric ozone during summer.

scholarly journals The TOMCAT global chemical transport model: Description of chemical mechanism and model evaluation

2016 ◽  
Author(s):  
Sarah A. Monks ◽  
Stephen R. Arnold ◽  
Michael J. Hollaway ◽  
Richard J. Pope ◽  
Chris Wilson ◽  
...  
Keyword(s):  
North America ◽  
Transport Model ◽  
Chemical Transport ◽  
Chemical Degradation ◽  
Chemical Mechanism ◽  
The Arctic ◽  
Model Description ◽  
Chemical Transport Model ◽  
Fire Emissions ◽  
Model Biases

Abstract. The TOMCAT 3-D chemical transport model has been updated with the emissions and chemical degradation of ethene, propene, toluene, butane and monoterpenes. The full tropospheric chemical mechanism is described and the model is evaluated against a range of surface, balloon, aircraft and satellite measurements. The model is generally able to capture the main spatial and seasonal features of high and low concentrations of carbon monoxide (CO), ozone (O3), volatile organic compounds (VOCs) and reactive nitrogen. However, model biases are found, some of which are common to chemistry models and some that are specific to TOMCAT and warrant further investigation. Simulated O3 is found to generally lie within the range of ozonesonde observations and shows good agreement with surface sites. The most notable exceptions to this are during winter at high latitudes, when O3 is underestimated, and during summer over North America, when O3 is overestimated. Global Ozone Monitoring Experiment-2 (GOME-2) comparisons suggest that TOMCAT sub-column tropospheric O3 in DJF may also be underestimated outside of the Arctic, particularly near tropical regions. TOMCAT CO is negatively biased during winter and spring in the Northern Hemisphere (NH) when compared to ground-based observations and MOPITT (Measurements Of Pollution In The Troposphere) satellite data. In contrast, CO is positively biased throughout the year in the Southern Hemisphere (SH). The negative bias in the NH is a common feature in chemistry models and TOMCAT lies well within the range of biases found in other models, while the TOMCAT SH positive bias is at the upper range of positive biases reported in other models. Using two simulations with different boundary conditions highlighted the sensitivity of model performance to the chosen emission dataset when simulating VOCs, nitrogen oxides (NOx) and peroxyacetyl nitrate (PAN). VOC measurements show winter/spring negative biases in C2-C3 alkanes and alkenes, which is likely driven by underestimated anthropogenic emissions. TOMCAT is able to capture the seasonal minima and maxima of PAN and HNO3. However, comparisons to an aircraft climatology show that PAN may be overestimated in winter and HNO3 may be overestimated in winter and spring in regions over North America. The model showed different biases in NOx, depending on location, with evidence of underestimated Asian emissions contributing to negative model biases over China and underestimated fire emissions contributing to negative biases in the SH. TOMCAT global mean tropospheric hydroxyl radical (OH) concentrations are higher than estimates inferred from observations of methyl chloroform, but similar to, or lower than, multi-model mean concentrations reported in recent model intercomparison studies. TOMCAT shows peak OH concentrations in the tropical lower troposphere, unlike other models, which show peak concentrations in the tropical upper troposphere. This is likely to affect the lifetime and transport of important trace gases and warrants further investigation.

scholarly journals Biomass burning influence on high-latitude tropospheric ozone and reactive nitrogen in summer 2008: a multi-model analysis based on POLMIP simulations

2015 ◽  
Vol 15 (11) ◽  
pp. 6047-6068 ◽  
Author(s):  
S. R. Arnold ◽  
L. K. Emmons ◽  
S. A. Monks ◽  
K. S. Law ◽  
D. A. Ridley ◽  
...  
Keyword(s):  
Biomass Burning ◽  
High Latitude ◽  
Tropospheric Ozone ◽  
Transport Model ◽  
Chemical Transport ◽  
Ozone Production ◽  
The Arctic ◽  
Vertical Position ◽  
Chemical Transport Model ◽  
Fire Emissions

Abstract. We have evaluated tropospheric ozone enhancement in air dominated by biomass burning emissions at high latitudes (> 50° N) in July 2008, using 10 global chemical transport model simulations from the POLMIP multi-model comparison exercise. In model air masses dominated by fire emissions, ΔO3/ΔCO values ranged between 0.039 and 0.196 ppbv ppbv−1 (mean: 0.113 ppbv ppbv−1) in freshly fire-influenced air, and between 0.140 and 0.261 ppbv ppbv−1 (mean: 0.193 ppbv) in more aged fire-influenced air. These values are in broad agreement with the range of observational estimates from the literature. Model ΔPAN/ΔCO enhancement ratios show distinct groupings according to the meteorological data used to drive the models. ECMWF-forced models produce larger ΔPAN/ΔCO values (4.47 to 7.00 pptv ppbv−1) than GEOS5-forced models (1.87 to 3.28 pptv ppbv−1), which we show is likely linked to differences in efficiency of vertical transport during poleward export from mid-latitude source regions. Simulations of a large plume of biomass burning and anthropogenic emissions exported from towards the Arctic using a Lagrangian chemical transport model show that 4-day net ozone change in the plume is sensitive to differences in plume chemical composition and plume vertical position among the POLMIP models. In particular, Arctic ozone evolution in the plume is highly sensitive to initial concentrations of PAN, as well as oxygenated VOCs (acetone, acetaldehyde), due to their role in producing the peroxyacetyl radical PAN precursor. Vertical displacement is also important due to its effects on the stability of PAN, and subsequent effect on NOx abundance. In plumes where net ozone production is limited, we find that the lifetime of ozone in the plume is sensitive to hydrogen peroxide loading, due to the production of HOx from peroxide photolysis, and the key role of HO2 + O3 in controlling ozone loss. Overall, our results suggest that emissions from biomass burning lead to large-scale photochemical enhancement in high-latitude tropospheric ozone during summer.

scholarly journals Source attributions of pollution to the Western Arctic during the NASA ARCTAS field campaign

2013 ◽  
Vol 13 (9) ◽  
pp. 4707-4721 ◽  
Author(s):  
H. Bian ◽  
P. R. Colarco ◽  
M. Chin ◽  
G. Chen ◽  
J. M. Rodriguez ◽  
...  
Keyword(s):  
Biomass Burning ◽  
Field Experiments ◽  
Transport Model ◽  
Background Level ◽  
Anthropogenic Emissions ◽  
Airborne Measurements ◽  
Ch4 Production ◽  
Regional Sources ◽  
Western Arctic ◽  
Co Concentrations

Abstract. We use the NASA GEOS-5 transport model with tagged tracers to investigate the contributions of different regional sources of CO and black carbon (BC) to their concentrations in the Western Arctic (i.e., 50–90° N and 190–320° E) in spring and summer 2008. The model is evaluated by comparing the results with airborne measurements of CO and BC from the NASA Arctic Research of the Composition of the Troposphere from Aircraft and Satellites (ARCTAS) field campaigns to demonstrate the strengths and limitations of our simulations. We also examine the reliability of tagged CO tracers in characterizing air mass origins using the measured fossil fuel tracer of dichloromethane and the biomass burning tracer of acetonitrile. Our tagged CO simulations suggest that most of the enhanced CO concentrations (above background level from CH4 production) observed during April originate from Asian anthropogenic emissions. Boreal biomass burning emissions and Asian anthropogenic emissions are of similar importance in July domain wise, although the biomass burning CO fraction is much larger in the area of the ARCTAS field experiments. The fraction of CO from Asian anthropogenic emissions is larger in spring than in summer. European sources make up no more than 10% of CO levels in the campaign domain during either period. Comparisons of CO concentrations along the flight tracks with regional averages from GEOS-5 show that the along-track measurements are representative of the concentrations within the large domain of the Western Arctic in April but not in July.

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.

High resolution Aerosol Radiative Effects over Europe using detailed optical properties from the Chemical Transport Model PMCAMx

2020 ◽  
Author(s):  
Marios Bruno Korras Carraca ◽  
Dimitris Manetas ◽  
David Patoulias ◽  
Spyros Pandis ◽  
Nikolaos Hatzianastassiou ◽  
...  
Keyword(s):  
Optical Properties ◽  
Temporal Resolution ◽  
Biomass Burning ◽  
Transport Model ◽  
Aerosol Particles ◽  
Chemical Transport ◽  
Chemical Transport Model ◽  
Aerosol Optical Properties ◽  
The Earth ◽  
Spatio Temporal

&lt;p&gt;Natural and anthropogenic aerosol particles are major drivers of the Earth&amp;#8217;s radiation budget, which they affect directly (through scattering and absorption) and indirectly (through modification of cloud scattering and precipitation properties), while they semi-directly influence atmospheric stability and convection, mainly through modification of solar radiation absorption by the atmosphere. Despite the important climatic role of aerosols, large uncertainties in their radiative effects remain due to limited knowledge of the aerosol spatio-temporal distribution and physico-chemical properties. The interaction of aerosols with radiation is strongly dependent on their optical properties, which in turn are controlled by the particles&amp;#8217; size distribution, shape, chemical composition and mixing state. In order to accurately estimate the magnitude of the aerosol direct radiative effect (DRE), detailed knowledge of their optical properties with high spatial and temporal resolution is required.&lt;/p&gt;&lt;p&gt;The European continent is a region of particular interest for studying atmospheric aerosol effects, because of the presence of&amp;#160; numerous and varying sources of particles and their precursors, such as industries, large urban centers and biomass burning, especially when combined with high levels of solar insolation during summer. In this study, the aerosol DRE over Europe is examined using the FORTH deterministic spectral radiative transfer model (RTM) and aerosol data from the chemical transport model PMCAMx. Chemically and size resolved aerosol concentrations predicted by PMCAMx are combined with a Mie model to calculate key aerosol optical properties (i.e. vertically resolved aerosol optical depth, single scattering albedo and asymmetry parameter) that are necessary to compute aerosol DRE using the RTM. The Mie model takes into account concentrations of organics, black carbon, sulfate, nitrate, ammonium, chlorine, sodium, water, and crustal material, and calculates aerosol optical properties assuming that the aerosol particles of the same size are internally mixed. The DRE is estimated at the Earth&amp;#8217;s surface, within the atmospheric column and at the top of the atmosphere (TOA), at high spatial and temporal resolution (36 &amp;#215; 36 km grids, 27 vertical layers, hourly), during June and July 2012.&lt;/p&gt;&lt;p&gt;Initial modelling results reveal that DREs exhibit significant spatio-temporal variability, due to the heterogeneity of source emissions rates, mostly with regard to wildfires, and the varying synoptic conditions. Emphasis is thus given to biomass burning aerosols, which are among the most significant radiative forcing agents in Europe during summer. Their relative forcing is computed by performing model computations with and without biomass burning emissions.&lt;/p&gt;

scholarly journals Pollution transport from North America to Greenland during summer 2008

2013 ◽  
Vol 13 (7) ◽  
pp. 3825-3848 ◽  
Author(s):  
J. L. Thomas ◽  
J.-C. Raut ◽  
K. S. Law ◽  
L. Marelle ◽  
G. Ancellet ◽  
...  
Keyword(s):  
North America ◽  
Transport Model ◽  
Ozone Production ◽  
The Arctic ◽  
Pollution Transport ◽  
Chemical Transport Model ◽  
Fire Emissions ◽  
Fire Plumes ◽  
Ozone Levels ◽  
Pollution Plumes

Abstract. Ozone pollution transported to the Arctic is a significant concern because of the rapid, enhanced warming in high northern latitudes, which is caused, in part, by short-lived climate forcers, such as ozone. Long-range transport of pollution contributes to background and episodic ozone levels in the Arctic. However, the extent to which plumes are photochemically active during transport, particularly during the summer, is still uncertain. In this study, regional chemical transport model simulations are used to examine photochemical production of ozone in air masses originating from boreal fire and anthropogenic emissions over North America and during their transport toward the Arctic during early July 2008. Model results are evaluated using POLARCAT aircraft data collected over boreal fire source regions in Canada (ARCTAS-B) and several days downwind over Greenland (POLARCAT-France and POLARCAT-GRACE). Model results are generally in good agreement with the observations, except for certain trace gas species over boreal fire regions, in some cases indicating that the fire emissions are too low. Anthropogenic and biomass burning pollution (BB) from North America was rapidly uplifted during transport east and north to Greenland where pollution plumes were observed in the mid- and upper troposphere during POLARCAT. A model sensitivity study shows that CO levels are in better agreement with POLARCAT measurements (fresh and aged fire plumes) upon doubling CO emissions from fires. Analysis of model results, using ΔO3/ΔCO enhancement ratios, shows that pollution plumes formed ozone during transport towards the Arctic. Fresh anthropogenic plumes have average ΔO3/ΔCO enhancement ratios of 0.63 increasing to 0.92 for aged anthropogenic plumes, indicating additional ozone production during aging. Fresh fire plumes are only slightly enhanced in ozone (ΔO3/ΔCO=0.08), but form ozone downwind with ΔO3/ΔCO of 0.49 for aged BB plumes (model-based run). We estimate that aged anthropogenic and BB pollution together made an important contribution to ozone levels with an average contribution for latitudes >55° N of up to 6.5 ppbv (18%) from anthropogenic pollution and 3 ppbv (5.2%) from fire pollution in the model domain in summer 2008.

scholarly journals The sensitivity of CO and aerosol transport to the temporal and vertical distribution of North American boreal fire emissions

2009 ◽  
Vol 9 (3) ◽  
pp. 11951-12006 ◽  
Author(s):  
Y. Chen ◽  
Q. Li ◽  
J. T. Randerson ◽  
E. A. Lyons ◽  
R. A. Kahn ◽  
...  
Keyword(s):  
North America ◽  
Biomass Burning ◽  
Forest Fires ◽  
Transport Model ◽  
Source Region ◽  
Fire Season ◽  
Height Distribution ◽  
Chemical Transport Model ◽  
Fire Emissions ◽  
Fire Source

Abstract. Forest fires in Alaska and West Canada represent important sources of aerosols and trace gases in North America. Among the largest uncertainties when modeling forest fire effects are the timing and injection height of biomass burning emissions. Here we simulate CO and aerosols over North America during the 2004 fire season, using the GEOS-Chem chemical transport model. We apply different temporal distributions and injection height profiles to the biomass burning emissions, and compare model results with satellite-, aircraft-, and ground-based measurements. We find that averaged over the fire season, the use of finer temporal resolved biomass burning emissions usually decreases CO and aerosol concentrations near the fire source region, and often enhances long-range transport. Among the individual temporal constraints, switching from monthly to 8-day time intervals for emissions has the largest effect on CO and aerosol distributions, and shows better agreement with measured day-to-day variability. Injection height substantially modifies the surface concentrations and vertical profiles of pollutants near the source region. In comparison with CO, the simulation of black carbon aerosol is more sensitive to the temporal and injection height distribution of emissions. The use of MISR-derived injection height improves agreement with surface aerosol measurements near the fire source. Our results indicate that the discrepancies between model simulations and MOPITT CO measurements near the Hudson Bay can not be attributed solely to the representation of injection height within the model. Frequent occurrence of strong convection in North America during summer tends to limit the influence of injection height distribution of fire emissions in Alaska and West Canada on CO and aerosol distributions over eastern North America.

scholarly journals Composite study of aerosol export events from East Asia and North America

2012 ◽  
Vol 12 (8) ◽  
pp. 21977-22022 ◽  
Author(s):  
Y. Luan ◽  
L. Jaeglé
Keyword(s):  
Boundary Layer ◽  
North America ◽  
East Asia ◽  
Transport Model ◽  
Lower Troposphere ◽  
Temporal Variations ◽  
The Arctic ◽  
Chemical Transport Model ◽  
Mean Values ◽  
Warm Conveyor Belts

Abstract. We use satellite observations of aerosol optical depth (AOD) from the Moderate Resolution Imaging Spectrometer (MODIS) together with the GEOS-Chem global chemical transport model to contrast export of aerosols from East Asia and North America during 2004–2010. The GEOS-Chem model reproduces the spatial distribution and temporal variations of Asian aerosol outflow generally well, although a low bias (−30%) is found in the model fine mode AOD. We use the model to identify 244 aerosol pollution export events from E. Asia and 251 export events from N. America over our 7-yr study period. When these events are composited by season, we find that the AOD in the outflow is enhanced by 50–100% relative to seasonal mean values. The composite Asian plume splits into one branch going poleward towards the Arctic, with the other crossing the Pacific in 6–8 days. A fraction of the aerosols is trapped in the subtropical Pacific High. The N. American plume travels to the northeast Atlantic, reaching Europe after 4–5 days. Part of the composite plume turns anticyclonically in the Azores High, where it slowly decays. Both the Asian and N. American export events are favored by a dipole structure in sea-level pressure anomalies, associated with mid-latitude cyclone activity over the respective source regions. The observed AOD in the E. Asian outflow exhibits stronger seasonality, with a spring maximum, than the N. American outflow, with a weak summer maximum. The large spring AOD in the Asian outflow is the result of enhanced sulfate and dust aerosol concentrations, but is also due to a larger export efficiency of sulfate and SO2 from the Asian boundary layer relative to the N. American boundary layer. While the N. American sulfate outflow is mostly found in the lower troposphere (1–3 km altitude), the Asian sulfate outflow occurs at higher altitudes (2–6 km). In the Asian outflow 42–59% of the sulfate column is present above 2 km altitude, with only 24–35% in the N. American outflow. We link this to the factor of 2–5 lower precipitation in the warm conveyor belts (WCB) of midlatitude cyclones over E. Asia compared to N. America. This relative lack of precipitation makes Asian WCB very efficient for injecting aerosols in the middle troposphere.

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