[Show abstract][Hide abstract] ABSTRACT: The vertical profile of aerosol is important for its radiative effects, but weakly constrained by observations on the global scale, and highly variable among different models. To investigate the controlling factors, we investigate the effects of individual processes in one particular model (HadGEM3–UKCA), and compare the resulting diversity of aerosol vertical profiles with the inter-model diversity from the AeroCom Phase
II control experiment.
In this way we show that (in this model at least) the vertical profile is controlled by a relatively small number of processes, although these vary among aerosol components and particle sizes. We also show that suffciently coarse variations in these processes can produce a similar diversity to that among different models in terms of the global mean profile and zonal-mean vertical position. However, there are features of certain models’ profiles that cannot be reproduced, suggesting the influence of further structural differences between models.
Convective transport is found to be very important in controlling the vertical profile of all aerosol components by mass. In-cloud scavenging is very important for all except mineral dust. Growth by condensation is important for sulphate and carbonaceous aerosol (along with aqueous oxidation for the former and ageing by soluble material for the latter). The vertical extent of biomass-burning emissions into the free troposphere
is also important for the profile of carbonaceous aerosol. Boundary-layer mixing plays a dominant role for sea-salt and mineral dust, which are emitted only from the surface. Dry deposition and below-cloud scavenging are important for the profile of mineral dust only.
In this model, the microphysical processes of nucleation, condensation and coagulation dominate the vertical profile of the smallest particles by number, while the profiles of larger particles are controlled by the same processes as the component mass profiles, plus the size distribution of primary emissions.
We also show that the processes that affect the AOD-normalised radiative forcing in
the model are predominantly those that affect the vertical mass distribution, in particular
convective transport, in-cloud scavenging, aqueous oxidation, ageing and the vertical
extent of biomass-burning emissions.
[Show abstract][Hide abstract] ABSTRACT: Aerosols have important impacts on air quality and climate, but the processes affecting their removal from the atmosphere are not fully understood and are poorly constrained by observations. This makes modelled aerosol lifetimes uncertain. In this study, we make use of an observational constraint on aerosol lifetimes provided by radionuclide measurements and investigate the causes of differences within a set of global models. During the Fukushima Dai-Ichi nuclear power plant accident of March 2011, the radioactive isotopes cesium-137 (137Cs) and xenon-133 (133Xe) were released in large quantities. Cesium attached to particles in the ambient air, approximately according to their available aerosol surface area. 137Cs size distribution measurements taken close to the power plant suggested that accumulation-mode (AM) sulphate aerosols were the main carriers for the cesium. Hence, 137Cs can be used as a proxy tracer for the AM sulphate aerosol's fate in the atmosphere. In contrast, the noble gas 133Xe behaves almost like a passive transport tracer. Global surface measurements of the two radioactive isotopes taken over several months after the release allow the derivation of a lifetime of the carrier aerosol. We compare this to the lifetimes simulated by 19 different atmospheric transport models initialized with identical emissions of 137Cs that were assigned to an aerosol tracer with each model's default properties of AM sulphate, and 133Xe emissions that were assigned to a passive tracer. We investigate to what extent the modelled sulphate tracer can reproduce the measurements, especially with respect to the observed loss of aerosol mass with time. Modelled 37Cs and 133Xe concentrations sampled at the same location and times as station measurements allow a direct comparison between measured and modelled aerosol lifetime. The e-folding lifetime τe, calculated from station measurement data taken between two and nine weeks after the start of the emissions, is 14.3 days (95 % confidence interval 13.1–15.7 days). The equivalent modelled τe lifetimes have a large spread, varying between 4.8 and 26.7 days with a model median of 9.4 ± 2.3 days, indicating too fast removal in most models. Because sufficient measurement data were only available from about two weeks after the release, the estimated lifetimes apply to aerosols that have undergone long-range transport, i.e. not for freshly emitted aerosol. However, modelled instantaneous lifetimes show that the initial removal in the first two weeks was quicker (lifetimes between 1–5 days) due to the emissions occurring at low altitudes and co-location of the fresh plume with strong precipitation. Deviations between measured and modelled aerosol lifetimes are largest for the northernmost stations and at later time periods, suggesting that models do not transport enough of the aerosol towards the Arctic. The models underestimate passive tracer (133Xe) concentrations in the Arctic as well but to a smaller extent than for the aerosol (137Cs) tracer. This indicates that in addition to too fast aerosol removal in the models, errors in simulated atmospheric transport towards the Arctic in most models also contribute to the Arctic aerosol underestimates.
[Show abstract][Hide abstract] ABSTRACT: We examine the anthropogenically forced climate response for the 21st century representative concentration pathway (RCP) emission scenarios and their extensions for the period 2101-2500. The experiments were performed with ModelE2, a new version of the NASA Goddard Institute for Space Sciences (GISS) coupled general circulation model that includes three different versions for the atmospheric composition components: a noninteractive version (NINT) with prescribed composition and a tuned aerosol indirect effect (AIE), the TCAD version with fully interactive aerosols, whole-atmosphere chemistry, and the tuned AIE, and the TCADI version which further includes a parameterized first indirect aerosol effect on clouds. Each atmospheric version is coupled to two different ocean general circulation models: the Russell ocean model (GISS-E2-R) and HYCOM (GISS-E2-H). By 2100, global mean warming in the RCP scenarios ranges from 1.0 to 4.5°C relative to 1850-1860 mean temperature in the historical simulations. In the RCP2.6 scenario, the surface warming in all simulations stays below a 2°C threshold at the end of the 21st century. For RCP8.5, the range is 3.5-4.5°C at 2100. Decadally averaged sea ice area changes are highly correlated to global mean surface air temperature anomalies and show steep declines in both hemispheres, with a larger sensitivity during winter months. By the year 2500, there are complete recoveries of the globally averaged surface air temperature for all versions of the GISS climate model in the low-forcing scenario RCP2.6. TCADI simulations show enhanced warming due to greater sensitivity to CO2, aerosol effects, and greater methane feedbacks, and recovery is much slower in RCP2.6 than with the NINT and TCAD versions. All coupled models have decreases in the Atlantic overturning stream function by 2100. In RCP2.6, there is a complete recovery of the Atlantic overturning stream function by the year 2500 while with scenario RCP8.5, the E2-R climate model produces a complete shutdown of deep water formation in the North Atlantic.
Journal of Advances in Modeling Earth Systems 02/2015; 7(1). DOI:10.1002/2014MS000403 · 4.92 Impact Factor
[Show abstract][Hide abstract] ABSTRACT: Atmospheric black carbon (BC) absorbs solar ra-diation, and exacerbates global warming through exerting positive radiative forcing (RF). However, the contribution of BC to ongoing changes in global climate is under debate. Anthropogenic BC emissions, and the resulting distribution of BC concentration, are highly uncertain. In particular, long-range transport and processes affecting BC atmospheric life-time are poorly understood. Here we discuss whether recent assessments may have overestimated present-day BC radia-tive forcing in remote regions. We compare vertical profiles of BC concentration from four recent aircraft measurement campaigns to simulations by 13 aerosol models participating in the AeroCom Phase II intercomparison. An atmospheric lifetime of BC of less than 5 days is shown to be essential for reproducing observations in remote ocean regions, in line with other recent studies. Adjusting model results to mea-surements in remote regions, and at high altitudes, leads to a 25 % reduction in AeroCom Phase II median direct BC forc-ing, from fossil fuel and biofuel burning, over the industrial era. The sensitivity of modelled forcing to BC vertical pro-file and lifetime highlights an urgent need for further flight campaigns, close to sources and in remote regions, to pro-vide improved quantification of BC effects for use in climate policy.
[Show abstract][Hide abstract] ABSTRACT: Accurately representing aerosol-cloud interactions in global climate models is challenging. As parameterizations evolve, it is important to evaluate their performance with appropriate use of observations. In this investigation we compare aerosols, clouds, and their interactions in three global climate models (GFDL-AM3, NCAR-CAM5, GISS-ModelE2) to MODIS satellite observations. Modeled cloud properties are diagnosed using a MODIS simulator. Cloud droplet number concentrations (N) are computed identically from satellite-simulated and MODIS-observed values of liquid cloud optical depth and droplet effective radius. We find that aerosol optical depth (τa) simulated by models is similar to observations in many regions around the globe. For N, AM3 and CAM5 capture the observed spatial pattern of higher values in coastal marine stratocumulus versus remote ocean regions, though modeled values in general are higher than observed. Aerosol-cloud interactions were computed as the sensitivity of ln(N) to ln(τa) for coastal marine liquid clouds near South Africa (SAF) and Southeast Asia (SEA) where τa varies in time. AM3 and CAM5 are more sensitive than observations, while the sensitivity for ModelE2 is statistically insignificant. This widely used sensitivity could be subject to misinterpretation due to the confounding influence of meteorology on both aerosols and clouds. A simple framework for assessing the sensitivity of ln(N) to ln(τa) at constant meteorology illustrates that observed sensitivity can change from positive to statistically insignificant when including the confounding influence of relative humidity. Satellite-simulated versus standard model values of N from CAM5 are compared in SAF; standard model values are significantly lower with a bias of 83 cm−3.
Journal of Geophysical Research Atmospheres 09/2014; DOI:10.1002/2014JD021722 · 3.43 Impact Factor
[Show abstract][Hide abstract] ABSTRACT: Atmospheric pollution over South Asia attracts special attention due to its effects on regional climate, the water cycle, and human health. These effects are potentially growing owing to rising trends of anthropogenic aerosol emissions found there. In this study, the spatio-temporal aerosol distributions over South Asia from 7 global models, for the period of 2000–2007, are evaluated systematically against aerosol retrievals of NASA satellite sensors and ground-based measurements. Overall, substantial underestimations of aerosol loading over South Asia are found systematically in 6 out of 7 models. Averaged over the entire South Asia, the annual mean Aerosol Optical Depth (AOD) is underestimated by a range of 18–45 % across models compared to MISR, which is the lowest bound among various satellite AOD retrievals (from MISR, SeaWiFS, MODIS Aqua and Terra). In particular at Kanpur located in northern India, AOD is underestimated even more by a factor of 4, and annual mean Aerosol Absorption Optical Depth (AAOD) is underestimated by about a factor of 2 in comparison with AERONET, during the post-monsoon and the wintertime periods (i.e. October–January) when agricultural waste burning and anthropogenic emissions dominate. The largest model underestimation of aerosol loading occurs in the lowest boundary layer (from surface to 2 km) based on the comparisons with aerosol extinction vertical distribution from CALIPSO. The possible causes for the common problems of model aerosol underestimation over south Asia are identified here, which are suggested as the following. During the winter, not only the columnar aerosol loading in models, but also surface concentrations of all aerosol components (sulfate, nitrate, organic aerosol and black carbon) are found lower than observations (ISRO-GBP, ICARB and CALIPSO), indicating that anthropogenic emissions, especially biofuel, are likely underestimated in this season. Nitrate, a major component of aerosols in South Asia, is either not considered in 4 out of 7 models or significantly lower than observations in other 2 models. Surprisingly, the near-surface relative humidity in these models is found significantly lower than observations in the winter, resulting in suppression of the hygroscopic growth of soluble aerosols and formations of sulfate and nitrate, and thereby underestimation of AOD. During the post-monsoon season, the deficiency of agricultural waste burning emissions in GFED2 biomass burning emission inventory, used by the models, partly contributes to the model underestimation of aerosol loading over South Asia in burning seasons.
[Show abstract][Hide abstract] ABSTRACT: Observations of climate change during the CMIP5 extended historical period (1850-2012) are compared to trends simulated by six versions of the NASA Goddard Institute for Space Studies ModelE2 Earth System Model. The six models are constructed from three versions of the ModelE2 atmospheric general circulation model, distinguished by their treatment of atmospheric composition and the aerosol indirect effect, combined with two ocean general circulation models, HYCOM and Russell. Forcings that perturb the model climate during the historical period are described. Five-member ensemble averages from each of the six versions of ModelE2 simulate trends of surface air temperature, atmospheric temperature, sea ice and ocean heat content that are in general agreement with observed trends, although simulated warming is slightly excessive within the past decade. Only simulations that include increasing concentrations of long-lived greenhouse gases match the warming observed during the twentieth century. Differences in twentieth-century warming among the six model versions can be attributed to differences in climate sensitivity, aerosol and ozone forcing, and heat uptake by the deep ocean. Coupled models with HYCOM export less heat to the deep ocean, associated with reduced surface warming in regions of deepwater formation, but greater warming elsewhere at high latitudes along with reduced sea ice. All ensembles show twentieth-century annular trends toward reduced surface pressure at southern high latitudes and a poleward shift of the midlatitude westerlies, consistent with observations.
Journal of Advances in Modeling Earth Systems 06/2014; 6(2-2):441-477. DOI:10.1002/2013MS000266 · 4.92 Impact Factor
[Show abstract][Hide abstract] ABSTRACT: This study evaluates model simulated dust aerosols over North Africa and the North Atlantic from five global models that participated in the AeroCom phase II model experiments. The model results are compared with satellite aerosol optical depth (AOD) data from MODIS, MISR, and SeaWiFS, dust optical depth (DOD) derived from MODIS and MISR, AOD and coarse-mode AOD (as a proxy of DOD) from ground-based AERONET sunphotometer measurements, and dust vertical distributions/centroid height from CALIOP and AIRS satellite AOD retrievals. We examine the following quantities of AOD and DOD: (1) the magnitudes over land and over ocean in our study domain, (2) the longitudinal gradient from the dust source region over North Africa to the western North Atlantic, (3) seasonal variations at different locations, and (4) the dust vertical profile shape and the AOD centroid height (altitude above or below which half of the AOD is located). The different satellite data show consistent features in most of these aspects, however the models display large diversity in all of them, with significant differences among the models and between models and observations. By examining dust emission, removal, and mass extinction efficiency in the five models, we also find remarkable differences among the models that all contribute to the discrepancies of model simulated dust amount and distribution. This study highlights the challenges in simulating the dust physical and optical processes, even in the best-known dust environment, and stresses the need for observable quantities to constrain the model processes.
Journal of Geophysical Research Atmospheres 05/2014; DOI:10.1002/2013JD021099 · 3.43 Impact Factor
[Show abstract][Hide abstract] ABSTRACT: Though many global aerosols models prognose surface deposition, only a few models have been used to di- rectly simulate the radiative effect from black carbon (BC) deposition to snow and sea ice. Here, we apply aerosol de- position fields from 25 models contributing to two phases of the Aerosol Comparisons between Observations and Mod- els (AeroCom) project to simulate and evaluate within-snow BC concentrations and radiative effect in the Arctic. We ac- complish this by driving the offline land and sea ice com- ponents of the Community Earth System Model with dif- ferent deposition fields and meteorological conditions from
2004 to 2009, during which an extensive field campaign of BC measurements in Arctic snow occurred. We find that models generally underestimate BC concentrations in snow in northern Russia and Norway, while overestimating BC amounts elsewhere in the Arctic. Although simulated BC distributions in snow are poorly correlated with measure- ments, mean values are reasonable. The multi-model mean (range) bias in BC concentrations, sampled over the same grid cells, snow depths, and months of measurements, are −4.4 (−13.2 to +10.7) ng g−1 for an earlier phase of Aero- Com models (phase I), and +4.1 (−13.0 to +21.4) ng g−1
for a more recent phase of AeroCom models (phase II), com- pared to the observational mean of 19.2 ng g−1. Factors de- termining model BC concentrations in Arctic snow include Arctic BC emissions, transport of extra-Arctic aerosols, pre- cipitation, deposition efficiency of aerosols within the Arc- tic, and meltwater removal of particles in snow. Sensitivity studies show that the model–measurement evaluation is only weakly affected by meltwater scavenging efficiency because most measurements were conducted in non-melting snow. The Arctic (60–90◦ N) atmospheric residence time for BC in phase II models ranges from 3.7 to 23.2 days, imply- ing large inter-model variation in local BC deposition effi- ciency. Combined with the fact that most Arctic BC depo- sition originates from extra-Arctic emissions, these results suggest that aerosol removal processes are a leading source of variation in model performance. The multi-model mean (full range) of Arctic radiative effect from BC in snow is 0.15 (0.07–0.25) W m−2 and 0.18 (0.06–0.28) W m−2 in phase I and phase II models, respectively. After correcting for model biases relative to observed BC concentrations in different re- gions of the Arctic, we obtain a multi-model mean Arctic radiative effect of 0.17 W m−2 for the combined AeroCom ensembles. Finally, there is a high correlation between mod- eled BC concentrations sampled over the observational sites and the Arctic as a whole, indicating that the field campaign provided a reasonable sample of the Arctic.
[Show abstract][Hide abstract] ABSTRACT: This paper evaluates the current status of global modeling of the organic aerosol (OA) in the troposphere and analyzes the differences between models as well as between models and observations. Thirty-one global chemistry transport models (CTMs) and general circulation models (GCMs) have participated in this intercomparison, in the framework of AeroCom phase II. The simulation of OA varies greatly between models in terms of the magnitude of primary emissions, secondary OA (SOA) formation, the number of OA species used (2 to 62), the complexity of OA parameterizations (gas-particle partitioning, chemical aging, multiphase chemistry, aerosol microphysics), and the OA physical, chemical and optical properties. The diversity of the global OA simulation results has increased since earlier AeroCom experiments, mainly due to the increasing complexity of the SOA parameterization in models, and the implementation of new, highly uncertain, OA sources. Diversity of over one order of magnitude exists in the modeled vertical distribution of OA concentrations that deserves a dedicated future study. Furthermore, although the OA/OC ratio depends on OA sources and atmospheric processing, and is important for model evaluation against OA and OC observations, it is resolved only by a few global models. The median global primary OA (POA) source strength is 56 Tg a(-1) (range 34-144 Tg a(-1)) and the median SOA source strength (natural and anthropogenic) is 19 Tg a(-1) (range 13-121 Tg a(-1)). Among the models that take into account the semi-volatile SOA nature, the median source is calculated to be 51 Tg a(-1) (range 16-121 Tg a(-1)), much larger than the median value of the models that calculate SOA in a more simplistic way (19 Tg a(-1); range 13-20 Tg a(-1), with one model at 37 Tg a(-1)). The median atmospheric burden of OA is 1.4 Tg (24 models in the range of 0.6-2.0 Tg and 4 between 2.0 and 3.8 Tg), with a median OA lifetime of 5.4 days (range 3.8-9.6 days). In models that reported both OA and sulfate burdens, the median value of the OA/sulfate burden ratio is calculated to be 0.77; 13 models calculate a ratio lower than 1, and 9 models higher than 1. For 26 models that reported OA deposition fluxes, the median wet removal is 70 Tg a(-1) (range 28-209 Tg a(-1)), which is on average 85% of the total OA deposition. Fine aerosol organic carbon (OC) and OA observations from continuous monitoring networks and individual field campaigns have been used for model evaluation. At urban locations, the model-observation comparison indicates missing knowledge on anthropogenic OA sources, both strength and seasonality. The combined model-measurements analysis suggests the existence of increased OA levels during summer due to biogenic SOA formation over large areas of the USA that can be of the same order of magnitude as the POA, even at urban locations, and contribute to the measured urban seasonal pattern. Global models are able to simulate the high secondary character of OA observed in the atmosphere as a result of SOA formation and POA aging, although the amount of OA present in the atmosphere remains largely underestimated, with a mean normalized bias (MNB) equal to -0.62 (-0.51) based on the comparison against OC (OA) urban data of all models at the surface, -0.15 (+0.51) when compared with remote measurements, and -0.30 for marine locations with OC data. The mean temporal correlations across all stations are low when compared with OC (OA) measurements: 0.47 (0.52) for urban stations, 0.39 (0.37) for remote stations, and 0.25 for marine stations with OC data. The combination of high (negative) MNB and higher correlation at urban stations when compared with the low MNB and lower correlation at remote sites suggests that knowledge about the processes that govern aerosol processing, transport and removal, on top of their sources, is important at the remote stations. There is no clear change in model skill with increasing model complexity with regard to OC or OA mass concentration. However, the complexity is needed in models in order to distinguish between anthropogenic and natural OA as needed for climate mitigation, and to calculate the impact of OA on climate accurately.
[Show abstract][Hide abstract] ABSTRACT: We present a description of the ModelE2 version of the Goddard Institute for Space Studies (GISS) General Circulation Model (GCM) and the configurations used in the simulations performed for the Coupled Model Intercomparison Project Phase 5 (CMIP5). We use six variations related to the treatment of the atmospheric composition, the calculation of aerosol indirect effects, and ocean model component. Specifically, we test the difference between atmospheric models that have noninteractive composition, where radiatively important aerosols and ozone are prescribed from precomputed decadal averages, and interactive versions where atmospheric chemistry and aerosols are calculated given decadally varying emissions. The impact of the first aerosol indirect effect on clouds is either specified using a simple tuning, or parameterized using a cloud microphysics scheme. We also use two dynamic ocean components: the Russell and HYbrid Coordinate Ocean Model (HYCOM) which differ significantly in their basic formulations and grid. Results are presented for the climatological means over the satellite era (1980-2004) taken from transient simulations starting from the preindustrial (1850) driven by estimates of appropriate forcings over the 20th Century. Differences in base climate and variability related to the choice of ocean model are large, indicating an important structural uncertainty. The impact of interactive atmospheric composition on the climatology is relatively small except in regions such as the lower stratosphere, where ozone plays an important role, and the tropics, where aerosol changes affect the hydrological cycle and cloud cover. While key improvements over previous versions of the model are evident, these are not uniform across all metrics. Key Points Description of the GISS ModelE2 contribution to CMIP5 Impact on evaluation of structural changes in composition and ocean treatment Ocean model choice is an important structural uncertainty
Journal of Advances in Modeling Earth Systems 03/2014; 6(1):141-184. DOI:10.1002/2013MS000265 · 4.92 Impact Factor
[Show abstract][Hide abstract] ABSTRACT: Many of the next generation of global climate models will include aerosol schemes which explicitly simulate the microphysical processes that determine the particle size distribution. These models enable aerosol optical properties and cloud condensation nuclei (CCN) concentrations to be determined by fundamental aerosol processes, which should lead to a more physically based simulation of aerosol direct and indirect radiative forcings. This study examines the global variation in particle size distribution simulated by 12 global aerosol microphysics models to quantify model diversity and to identify any common biases against observations. Evaluation against size distribution measurements from a new European network of aerosol supersites shows that the mean model agrees quite well with the observations at many sites on the annual mean, but there are some seasonal biases common to many sites. In particular, at many of these European sites, the accumulation mode number concentration is biased low during winter and Aitken mode concentrations tend to be overestimated in winter and underestimated in summer. At high northern latitudes, the models strongly underpredict Aitken and accumulation particle concentrations compared to the measurements, consistent with previous studies that have highlighted the poor performance of global aerosol models in the Arctic. In the marine boundary layer, the models capture the observed meridional variation in the size distribution, which is dominated by the Aitken mode at high latitudes, with an increasing concentration of accumulation particles with decreasing latitude. Considering vertical profiles, the models reproduce the observed peak in total particle concentrations in the upper troposphere due to new particle formation, although modelled peak concentrations tend to be biased high over Europe. Overall, the multimodel-mean data set simulates the global variation of the particle size distribution with a good degree of skill, suggesting that most of the individual global aerosol microphysics models are performing well, although the large model diversity indicates that some models are in poor agreement with the observations. Further work is required to better constrain size-resolved primary and secondary particle number sources, and an improved understanding of nucleation and growth (e. g. the role of nitrate and secondary organics) will improve the fidelity of simulated particle size distributions.
[Show abstract][Hide abstract] ABSTRACT: Atmospheric measurements from the Arctic Summer Cloud Ocean Study (ASCOS) are used to evaluate the performance of three atmospheric reanalyses (European Centre for Medium Range Weather Forecasting (ECMWF)-Interim reanalysis, National Center for Environmental Prediction (NCEP)-National Center for Atmospheric Research (NCAR) reanalysis, and NCEP-DOE (Department of Energy) reanalysis) and two global climate models (CAM5 (Community Atmosphere Model 5) and NASA GISS (Goddard Institute for Space Studies) ModelE2) in simulation of the high Arctic environment. Quantities analyzed include near surface meteorological variables such as temperature, pressure, humidity and winds, surface-based estimates of cloud and precipitation properties, the surface energy budget, and lower atmospheric temperature structure. In general, the models perform well in simulating large-scale dynamical quantities such as pressure and winds. Near-surface temperature and lower atmospheric stability, along with surface energy budget terms, are not as well represented due largely to errors in simulation of cloud occurrence, phase and altitude. Additionally, a development version of CAM5, which features improved handling of cloud macro physics, has demonstrated to improve simulation of cloud properties and liquid water amount. The ASCOS period additionally provides an excellent example of the benefits gained by evaluating individual budget terms, rather than simply evaluating the net end product, with large compensating errors between individual surface energy budget terms that result in the best net energy budget.
[Show abstract][Hide abstract] ABSTRACT: Aerosol particles in the atmosphere are composed of multiple chemical
species. The aerosol mixing state, which describes how chemical species
are mixed at the single-particle level, provides critical information on
microphysical characteristics that determine the interaction of aerosols
with the climate system. The evaluation of mixing state has become the
next challenge. This study uses aerosol time-of-flight mass spectrometry
(ATOFMS) data and compares the results to those of the Goddard Institute
for Space Studies modelE-MATRIX (Multiconfiguration Aerosol TRacker of
mIXing state) model, a global climate model that includes a detailed
aerosol microphysical scheme. We use data from field campaigns that
examine a variety of air mass regimens (urban, rural, and maritime). At
all locations, polluted areas in California (Riverside, La Jolla, and
Long Beach), a remote location in the Sierra Nevada Mountains (Sugar
Pine) and observations from Jeju (South Korea), the majority of aerosol
species are internally mixed. Coarse aerosol particles, those above 1
µm, are typically aged, such as coated dust or reacted sea-salt
particles. Particles below 1 µm contain large fractions of organic
material, internally mixed with sulfate and black carbon, and few
external mixtures. We conclude that observations taken over multiple
weeks characterize typical air mass types at a given location well;
however, due to the instrumentation, we could not evaluate mass budgets.
These results represent the first detailed comparison of single-particle
mixing states in a global climate model with real-time single-particle
mass spectrometry data, an important step in improving the
representation of mixing state in global climate models.
Journal of Geophysical Research Atmospheres 09/2013; 118(17):9834-9844. DOI:10.1002/jgrd.50700 · 3.43 Impact Factor
[Show abstract][Hide abstract] ABSTRACT: core measurements in conjunction with climate model simulations are of
tremendous value when examining anthropogenic and natural aerosol loads
and their role in past and future climates. Refractory black carbon (BC)
records from the Arctic, the Antarctic, and the Himalayas are analyzed
using three transient climate simulations performed with the Goddard
Institute for Space Studies ModelE. Simulations differ in aerosol
schemes (bulk aerosols vs. aerosol microphysics) and ocean couplings
(fully coupled vs. prescribed ocean). Regional analyses for past
(1850-2005) and future (2005-2100) carbonaceous aerosol simulations
focus on the Antarctic, Greenland, and the Himalayas. Measurements from
locations in the Antarctic show clean conditions with no detectable
trend over the past 150 years. Historical atmospheric deposition of BC
and sulfur in Greenland shows strong trends and is primarily influenced
by emissions from early twentieth century agricultural and domestic
practices. Models fail to reproduce observations of a sharp eightfold BC
increase in Greenland at the beginning of the twentieth century that
could be due to the only threefold increase in the North American
emission inventory. BC deposition in Greenland is about 10 times greater
than in Antarctica and 10 times less than in Tibet. The Himalayas show
the most complicated transport patterns, due to the complex terrain and
dynamical regimes of this region. Projections of future climate based on
the four CMIP5 Representative Concentration Pathways indicate further
dramatic advances of pollution to the Tibetan Plateau along with
decreasing BC deposition fluxes in Greenland and the Antarctic.
Journal of Geophysical Research Atmospheres 07/2013; 118(14):7948-7961. DOI:10.1002/jgrd.50612 · 3.43 Impact Factor