scholarly journals Spatial and temporal resolution of carbon flux estimates for 1983–2002

2007 ◽  
Vol 4 (6) ◽  
pp. 4697-4756 ◽  
Author(s):  
L. M. P. Bruhwiler ◽  
A. M. Michalak ◽  
P. P. Tans
Keyword(s):  
North America ◽  
Temporal Resolution ◽  
Carbon Flux ◽  
Seasonal Cycle ◽  
Transport Model ◽  
Spatial Scales ◽  
Carbon Fluxes ◽  
Chemical Transport Model ◽  
Data Product ◽  
Zonal Average

Abstract. We discuss the spatial and temporal resolution of monthly carbon flux estimates for the period 1983–2002 using a fixed-lag Kalman Smoother technique with a global chemical transport model, and the GLOBALVIEW data product. The observational network has expanded substantially over this period, and we the improvement in the constraints provided flux estimates by observations for the 1990's in comparison to the 1980's. The estimated uncertainties also decrease as observational coverage expands. In this study, we use the Globalview data product for a network that changes every 5 y, rather than using a small number of continually-operating sites (fewer observational constraints) or a large number of sites, some of which may consist almost entirely of extrapolated data. We show that the discontinuities resulting from network changes reflect uncertainty due to a sparse and variable network. This uncertainty effectively limits the resolution of trends in carbon fluxes. The ability of the inversion to distinguish, or resolve, carbon fluxes at various spatial scales is examined using a diagnostic known as the resolution kernel. We find that the global partition between land and ocean fluxes is well-resolved even for the very sparse network of the 1980's, although prior information makes a significant contribution to the resolution. The ability to distinguish zonal average fluxes has improved significantly since the 1980's, especially for the tropics, where the zonal ocean and land biosphere fluxes can be distinguished. Care must be taken when interpreting zonal average fluxes, however, since the lack of air samples for some regions in a zone may result in a large influence from prior flux estimates for these regions. We show that many of the TransCom 3 source regions are distinguishable throughout the period over which estimates are produced. Examples are Boreal and Temperate North America. The resolution of fluxes from Europe and Australia has greatly improved since the 1990's. Other regions, notably Tropical South America and the Equatorial Atlantic remain practically unresolved. Comparisons of the average seasonal cycle of the estimated carbon fluxes with the seasonal cycle of the prior flux estimates reveals a large adjustment of the summertime uptake of carbon for Boreal Eurasia, and an earlier onset of springtime uptake for Temperate North America. In addition, significantly larger seasonal cycles are obtained for some ocean regions, such as the Northern Ocean, North Pacific, North Atlantic and Western Equatorial Pacific, regions that appear to be well-resolved by the inversion.

scholarly journals Spatial and temporal resolution of carbon flux estimates for 1983–2002

2011 ◽  
Vol 8 (5) ◽  
pp. 1309-1331 ◽  
Author(s):  
L. M. P. Bruhwiler ◽  
A. M. Michalak ◽  
P. P. Tans
Keyword(s):  
North America ◽  
Temporal Resolution ◽  
Carbon Flux ◽  
Seasonal Cycle ◽  
Transport Model ◽  
Spatial Scales ◽  
Carbon Fluxes ◽  
Chemical Transport Model ◽  
Data Product ◽  
Zonal Average

Abstract. We discuss the spatial and temporal resolution of monthly carbon flux estimates for the period 1983–2002 using a fixed-lag Kalman Smoother technique with a global chemical transport model, and the GLOBALVIEW data product. The observational network has expanded substantially over this period, and the flux estimates are better constrained provided by observations for the 1990's in comparison to the 1980's. The estimated uncertainties also decrease as observational coverage expands. In this study, we use the Globalview data product for a network that changes every 5 yr, rather than using a small number of continually-operating sites (fewer observational constraints) or a large number of sites, some of which may consist almost entirely of extrapolated data. We show that the discontinuities resulting from network changes reflect uncertainty due to a sparse and variable network. This uncertainty effectively limits the resolution of trends in carbon fluxes, and is a potentially significant source of noise in assimilation systems that allow changes in observation distribution between assimilation time steps. The ability of the inversion to distinguish, or resolve, carbon fluxes at various spatial scales is examined using a diagnostic known as the resolution kernel. We find that the global partition between land and ocean fluxes is well-resolved even for the very sparse network of the 1980's, although prior information makes a significant contribution to the resolution. The ability to distinguish zonal average fluxes has improved significantly since the 1980's, especially for the tropics, where the zonal ocean and land biosphere fluxes can be distinguished. Care must be taken when interpreting zonal average fluxes, however, since the lack of air samples for some regions in a zone may result in a large influence from prior flux estimates for these regions. We show that many of the TransCom 3 source regions are distinguishable throughout the period over which estimates are produced. Examples are Boreal and Temperate North America. The resolution of fluxes from Europe and Australia has greatly improved since the 1990's. Other regions, notably Tropical South America and the Equatorial Atlantic remain practically unresolved. Comparisons of the average seasonal cycle of the estimated carbon fluxes with the seasonal cycle of the prior flux estimates reveals a large adjustment of the summertime uptake of carbon for Boreal Eurasia, and an earlier onset of springtime uptake for Temperate North America. In addition, significantly larger seasonal cycles are obtained for some ocean regions, such as the Northern Ocean, North Pacific, North Atlantic and Western Equatorial Pacific, regions that appear to be well-resolved by the inversion.

scholarly journals A regional high-resolution carbon flux inversion of North America for 2004

2009 ◽  
Vol 6 (6) ◽  
pp. 10195-10241 ◽  
Author(s):  
A. E. Schuh ◽  
A. S. Denning ◽  
K. D. Corbin ◽  
I. T. Baker ◽  
M. Uliasz ◽  
...  
Keyword(s):  
United States ◽  
High Resolution ◽  
North America ◽  
Carbon Flux ◽  
Transport Model ◽  
Ecosystem Respiration ◽  
Carbon Fluxes ◽  
The United States ◽  
Mixing Ratio ◽  
Ratio Data

Abstract. Resolving the discrepancies between NEE estimates based upon (1) ground studies and (2) atmospheric inversion results, demands increasingly sophisticated techniques. In this paper we present a high-resolution inversion based upon a regional meteorology model (RAMS) and an underlying biosphere (SiB3) model, both running on an identical 40 km grid over most of North America. Previous papers have utilized inversion regions formed by collapsing biome-similar grid cells into large aggregated regions. The effect of this is that the NEE correction imposed on forested regions on the east coast of the United States might be the same as that imposed on forests on the west coast of the United States while, in reality, there likely exist subtle differences in the two areas, both natural and anthropogenic. Our current inversion framework utilizes a combination of previously employed inversion techniques while allowing carbon flux corrections to be biome independent. Temporally and spatially high-resolution results utilizing biome-independent corrections provide insight into carbon dynamics in North America. In particular, we analyze hourly CO2 mixing ratio data from a sparse network of eight towers in North America for 2004. A prior estimate of carbon fluxes due to gross primary productivity (GPP) and ecosystem respiration (ER) is constructed from the SiB3 biosphere model on a 40 km grid. A combination of transport from the RAMS and the parameterized chemical transport model (PCTM) models is used to forge a connection between upwind biosphere fluxes and downwind observed CO2 mixing ratio data. A Kalman filter procedure is used to estimate weekly corrections to biosphere fluxes based upon observed CO2. RMSE-weighted annual NEE estimates, over an ensemble of potential inversion parameter sets, show a mean estimate 0.57 Pg/yr sink in North America. We perform the inversion with two independently derived boundary inflow conditions and calculate jackknife-based statistics to test the robustness of the model results. We then compare final results to estimates obtained from the CarbonTracker inversion system and the Ameriflux network. Results are promising, showing the ability to correct carbon fluxes from the biosphere models over annual and seasonal time scales, as well as over the different GPP and ER components, and also providing interesting hypotheses for future work.

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

<p>Natural and anthropogenic aerosol particles are major drivers of the Earth’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’ 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.</p><p>The European continent is a region of particular interest for studying atmospheric aerosol effects, because of the presence of  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’s surface, within the atmospheric column and at the top of the atmosphere (TOA), at high spatial and temporal resolution (36 × 36 km grids, 27 vertical layers, hourly), during June and July 2012.</p><p>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.</p>

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 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 Evaluating a 3-D transport model of atmospheric CO<sub>2</sub> using ground-based, aircraft, and space-borne data

2010 ◽  
Vol 10 (7) ◽  
pp. 18025-18061 ◽  
Author(s):  
L. Feng ◽  
P. I. Palmer ◽  
Y. Yang ◽  
R. M. Yantosca ◽  
S. R. Kawa ◽  
...  
Keyword(s):  
Boundary Layer ◽  
North America ◽  
Seasonal Cycle ◽  
Transport Model ◽  
Atmospheric Transport ◽  
Co2 Fluxes ◽  
A Posteriori ◽  
Upper Troposphere ◽  
Co2 Concentrations ◽  
Geographical Regions

Abstract. We evaluate the GEOS-Chem atmospheric transport model (v8-02-01) of CO2 over 2003–2006, driven by GEOS-4 and GEOS-5 meteorology from the NASA Goddard Global Modelling and Assimilation Office, using surface, aircraft and space-borne concentration measurements of CO2. We use an established ensemble Kalman filter to estimate a posteriori biospheric+biomass burning (BS+BB) and oceanic (OC) CO2 fluxes from 22 geographical regions, following the TransCom 3 protocol, using boundary layer CO2 data from a subset of GLOBALVIEW surface sites. Global annual net BS+BB+OC CO2 fluxes over 2004–2006 for GEOS-4 (GEOS-5) meteorology are −4.4±0.9 (−4.2±0.9), −3.9±0.9 (−4.5±0.9), and −5.2±0.9 (−4.9±0.9) Pg C yr−1 , respectively. The regional a posteriori fluxes are broadly consistent in the sign and magnitude of the TransCom-3 study for 1992–1996, but we find larger net sinks over northern and southern continents. We find large departures from our a priori over Europe during summer 2003, over temperate Eurasia during 2004, and over North America during 2005, reflecting an incomplete description of terrestrial carbon dynamics. We find GEOS-4 (GEOS-5) a posteriori CO2 concentrations reproduce the observed surface trend of 1.91–2.43 ppm yr−1, depending on latitude, within 0.15 ppm yr−1 (0.2 ppm yr−1) and the seasonal cycle within 0.2 ppm (0.2 ppm) at all latitudes. We find the a posteriori model reproduces the aircraft vertical profile measurements of CO2 over North America and Siberia generally within 1.5 ppm in the free and upper troposphere but can be biased by up to 4–5 ppm in the boundary layer at the start and end of the growing season. The model has a small negative bias in the free troposphere CO2 trend (1.95–2.19 ppm yr−1) compared to AIRS data which has a trend of 2.21–2.63 ppm yr−1 during 2004–2006, consistent with surface data. Model CO2 concentrations in the upper troposphere, evaluated using CONTRAIL (Comprehensive Observation Network for TRace gases by AIrLiner) aircraft measurements, reproduce the magnitude and phase of the seasonal cycle of CO2 in both hemispheres. We generally find that the GEOS meteorology reproduces much of the observed tropospheric CO2 variability, suggesting that these meteorological fields will help make significant progress in understanding carbon fluxes as more data become available.

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.

scholarly journals Long range transport of mercury to the Arctic and across Canada

2010 ◽  
Vol 10 (2) ◽  
pp. 4673-4717 ◽  
Author(s):  
D. Durnford ◽  
A. Dastoor ◽  
D. Figueras-Nieto ◽  
A. Ryjkov
Keyword(s):  
North America ◽  
Long Range ◽  
Transport Model ◽  
Extensive Study ◽  
Atmospheric Mercury ◽  
The Arctic ◽  
Long Range Transport ◽  
Chemical Transport Model ◽  
Transport Pathways ◽  
Range Transport

Abstract. This study is the most extensive study to date on the transport of mercury to the Arctic. Moreover, it is the first such study to use a fully-coupled, online chemical transport model, Environment Canada's Global/Regional Atmospheric Heavy Metals model (GRAHM), where the meteorology and mercury processes are fully integrated. It is also the only study to date on the transport of mercury across Canada. We determined source attribution from Asia, North America, Russia and Europe at six arctic verification stations, as well as three subarctic and eight midlatitude Canadian stations. We have found that Asia, despite having transport efficiencies that were almost always lower than those of North America and often lower than those of Russia, was the dominant source of gaseous atmospheric mercury at all verification stations: it contributed the most mercury (29–37% at all stations, seasons and levels considered), its concentrations frequently explained nearly 100% of the variability in the concentrations produced by the simulation performed with full global emissions, particularly in the absence of local sources, and it generated the most long range transport (LRT) events, causing 43%, 67% and 75% of the events at the arctic, subarctic and midlatitude stations, respectively. For the Arctic, Russian transport efficiencies tended to be the strongest, as expected, while European and Asian efficiencies were lower and higher, respectively, than those found in the literature. This disagreement is likely produced by mercury's long lifetime relative to that of other pollutants. The accepted springtime preference for the trans-Pacific transport of Asian pollution was evident only in the midlatitude group of stations, being masked in the arctic and subarctic groups by the occurrence of atmospheric mercury depletion events. Some neighbouring arctic stations recorded dissimilar numbers of LRT events; despite their proximity, the behaviour of mercury at these stations was governed by different dynamics and transport pathways. The column burden of GEM in the lowest 5 km of the Northern Hemisphere was largest in summer from Asia, North America and Russia, but in winter from Europe. In the vertical, transport of mercury from all source regions occurred principally in the mid-troposphere.

scholarly journals Interpretation of measured aerosol mass scattering efficiency over North America using a chemical transport model

2019 ◽  
Vol 19 (4) ◽  
pp. 2635-2653 ◽  
Author(s):  
Robyn N. C. Latimer ◽  
Randall V. Martin
Keyword(s):  
North America ◽  
Transport Model ◽  
Geometric Mean ◽  
Chemical Transport ◽  
Hygroscopic Growth ◽  
Chemical Transport Model ◽  
Scattering Efficiency ◽  
Alternative Representation ◽  
Aerosol Mass ◽  
Dry Conditions

Abstract. Aerosol mass scattering efficiency affects climate forcing calculations, atmospheric visibility, and the interpretation of satellite observations of aerosol optical depth. We evaluated the representation of aerosol mass scattering efficiency (αsp) in the GEOS-Chem chemical transport model over North America using collocated measurements of aerosol scatter and mass from IMPROVE network sites between 2000 and 2010. We found a positive bias in mass scattering efficiency given current assumptions of aerosol size distributions and particle hygroscopicity in the model. We found that overestimation of mass scattering efficiency was most significant in dry (RH <35 %) and midrange humidity (35 % < RH <65 %) conditions, with biases of 82 % and 40 %, respectively. To address these biases, we investigated assumptions surrounding the two largest contributors to fine aerosol mass, organic (OA) and secondary inorganic aerosols (SIA). Inhibiting hygroscopic growth of SIA below 35 % RH and decreasing the dry geometric mean radius, from 0.069 µm for SIA and 0.073 µm for OA to 0.058 µm for both aerosol types, significantly decreased the overall bias observed at IMPROVE sites in dry conditions from 82 % to 9 %. Implementation of a widely used alternative representation of hygroscopic growth following κ-Kohler theory for secondary inorganic (hygroscopicity parameter κ=0.61) and organic (κ=0.10) aerosols eliminated the remaining overall bias in αsp. Incorporating these changes in aerosol size and hygroscopicity into the GEOS-Chem model resulted in an increase of 16 % in simulated annual average αsp over North America, with larger increases of 25 % to 45 % in northern regions with high RH and hygroscopic aerosol fractions, and decreases in αsp up to 15 % in the southwestern U.S. where RH is low.

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