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From Low-Cost Sensors to High-Quality Data: A Review of Challenges and Summary of Best Practices for Effectively Using Low-Cost Particulate Matter Mass Sensors

Low-cost sensors for particulate matter mass (PM) enable spatially dense, high temporal resolution measurements of air quality that traditional reference monitoring cannot. Low-cost PM sensors are especially beneficial in low and middle-income countries where few, if any, reference grade measurements exist and in areas where the concentration fields of air pollutants have significant spatial gradients. Unfortunately, low-cost PM sensors also come with a number of challenges that must be addressed if their data products are to be used for anything more than a qualitative characterization of air quality. The various PM sensors used in low-cost monitors are all subject to biases and calibration dependencies, corrections for which range from relatively straightforward(e.g. meteorology, age of sensor) to complex (e.g. aerosol source, composition, refractive index). The methods for correcting and calibrating these biases and dependencies that have been used in the literature likewise range from simple linear and quadratic models to complex machine learning algorithms. Here we review the needs and challenges when trying to get high-quality data from low-cost sensors. We also present a set of best practices to follow to obtain high-quality data from these low-cost sensors.

low-cost sensors↗

What Controls the Vertical Distribution of Aerosol? Relationships Between Process Sensitivity in HadGEM3-UKCA and Inter-Model Variation from AeroCom Phase II

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 in one particular model, we investigate the effects of individual processes in 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 sufficiently coarse variations in these processes can produce a similar diversity to that among different models in terms of the global-mean profile and, to a lesser extent, the 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. In HadGEM3-UKCA, 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 sulfate 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 (e.g. total CN >3 nm), while the profiles of larger particles (e.g. CN>100 nm) 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.

dust↗

The Dark Target Algorithm for Observing the Global Aerosol System: Past, Present and Future

The Dark Target aerosol algorithm was developed to exploit the information content available from the observations of Moderate-Resolution Imaging Spectroradiometers (MODIS), to better characterize the global aerosol system. The algorithm is based on measurements of the light scattered by aerosols toward a space-borne sensor against the backdrop of relatively dark Earth scenes, thus giving rise to the name “Dark Target”. Development required nearly a decade of research that included application of MODIS airborne simulators to provide test beds for proto-algorithms and analysis of existing data to form realistic assumptions to constrain surface reflectance and aerosol optical properties. This research in itself played a significant role in expanding our understanding of aerosol properties, even before Terra MODIS launch. Contributing to that understanding were the observations and retrievals of the growing Aerosol Robotic Network (AERONET) of sun-sky radiometers, which has walked hand-in-hand with MODIS and the development of other aerosol algorithms, providing validation of the satellite-retrieved products after launch. The MODIS Dark Target products prompted advances in Earth science and applications across subdisciplines such as climate, transport of aerosols, air quality, and data assimilation systems. Then, as the Terra and Aqua MODIS sensors aged, the challenge was to monitor the effects of calibration drifts on the aerosol products and to differentiate physical trends in the aerosol system from artefacts introduced by instrument characterization. Our intention is to continue to adapt and apply the well-vetted Dark Target algorithms to new instruments, including both polar-orbiting and geosynchronous sensors. The goal is to produce an uninterrupted time series of an aerosol climate data record that begins at the dawn of the 21st century and continues indefinitely into the future.

Aerosol↗

Influence of plumes from biomass burning on atmospheric chemistry over the equatorial and tropical South Atlantic during CITE 3

During all eight flights conducted over the equatorial and tropical South Atlantic in the course of the Chemical Instrumentation Test and Evaluation (CITE 3) experiment, we observed haze layers with elevated concentrations of aerosols, O3, CO, and other trace gases related to biomass burning emissions. They occurred at altitudes between 1000 and 5200 m and were usually only some 100-300 m thick. These layers extended horizontally over several 100 km and were marked by the presence of visible brownish haze. Air mass trajectories indicate that these layers originate in the biomass burning regions of Africa and South America and typically have aged at least 10 days since the time of emission. In the haze layers, O3 and CO concentrations up to 90 and 210 ppb were observed, respectively. The two species were highly correlated. The ratio concentrations in plume minus background concentrations of O3/CO is typically in the range 0.2-0.7, much higher than the ratios in the less aged plumes investigated previously in Amazonia. In most cases, aerosol (0.12-3 micrometer diameter) number concentrations were also elevated by up to 400/cu cm in the layers; aerosol enrichments were also strongly correlated with elevated CO levels. Clear correlations between CO and NO(x) enrichments were not apparent due to the age of the plumes, in which most NO(x) would have already reacted away within 1-2 days. Only in some of the plumes could clear correlations between NO(y) and CO be identified; the absence of a general correlation between NO(y) and CO may be due to instrumental limitations and to variable sinks for NO(y). The average enrichment of the ratio concentrations in plume minus background concentrations of NO(y)/CO was quite high, consistent with the efficient production of ozone observed in the plumes. The chemical characteristics of the haze layers, together with remote sensing information and trajectory calculations, suggest that fire emissions (in Africa and/or South America) are the primary source of the haze layer components.

Andreae, M. O.↗

Airborne Observations of Aerosol Properties in Southeast Asia: Overview of Emissions, Cloud Processing, and Long Range Transport during NASA CAMP2Ex

The Southwest Monsoon represents an important synoptic scale meteorological feature that modulates precipitation throughout Southeast Asia. In addition, southwesterly flow can funnel large amounts of biomass burning aerosol into heavily populated areas throughout the Philippines, mixing with urban emissions and representing a significant air quality issue. From a climate perspective, understanding interactions between these particles and clouds has important societal ramifications through frequent extreme periods of flood and drought. Here we present airborne observations made in support of the NASA CAMP2Ex (Cloud and Aerosol Monsoonal Processes-Philippines Experiment) mission aboard the Wallops Flight Facility P-3 research aircraft, based at Clark International Airport in the Luzon region of Northern Philippines. Nineteen research flights were conducted in August-October of 2019. An extensive suite of aerosol microphysical, optical, and chemical instrumentation was deployed, along with trace gas and remote sensing measurements, to characterize aerosol emissions and their vertical/spatial variability associated with moderately convective marine cloud systems in the region. Analysis will focus on characterizing disparate aerosol sources with respect to derived chemical and optical properties relevant to global circulation modeling. For example, higher than expected mass scattering efficiencies for aged biomass burning emissions, derived from a combination of nephelometer and aerosol mass spectrometer measurements, are attributed to increased particle size and decreased density. Results will also illustrate the evolution of aerosols from Indonesian agricultural biomass burning activities into the Philippines region, in comparison with urban emissions from the megacity Manila and transported air masses from mainland Asia.

Luke David Ziemba↗

Evaluation of Aerosol Mixing State Classes in the GISS Modele-matrix Climate Model Using Single-particle Mass Spectrometry Measurements

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 micron, are typically aged, such as coated dust or reacted sea-salt particles. Particles below 1 micron 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.

climate models↗

Observations of the Age of Air from the Northern Hemisphere Midlatitude Surface

Understanding and modeling the interhemispheric transport (IHT) of trace gases and aerosols is important for interpreting past (and projecting future) changes in atmospheric composition. One IHT measure -- the mean age since air was last at the Northern Hemisphere (NH) midlatitude surface – represents a fundamental property of tropospheric transport that can be estimated from measurements of sulfur hexafluoride (SF6). Here we use SF6 measurements obtained from the recent NASA Atmospheric Tomography Mission (ATom) to construct observational estimates of the mean age throughout the troposphere. We compare the ATom based ages, which span all four seasons during the period 2016-2018 over both the Pacific and Atlantic Oceans, with previous in situ-based estimates obtained from the HIAPER Pole‐to‐Pole Observations (HIPPO) project, which are available only for the Pacific. In order to interpret the observed variations in mean age and their relationship with the large-scale flow we use simulations of the Goddard Earth Observing System (GEOS) general circulation model, constrained with meteorological fields derived from the Modern-Era Retrospective analysis for Research and Applications, Version 2 (MERRA-2), performed over the entire MERRA-2 period (including ATom). We confirm results from previous studies showing that the model ages are biased old compared to the observational estimates. However, we also show that this model bias is reduced in more recent years, which we interpret in terms of changes in the latitudinal distribution of SF6 emissions over the 2000s.

interhemispheric transport (IHT)↗

GCM simulations of volcanic aerosol forcing. I - Climate changes induced by steady-state perturbations

The response of the climate system to a temporally and spatially constant amount of volcanic particles is simulated using a general circulation model (GCM). The optical depth of the aerosols is chosen so as to produce approximately the same amount of forcing as results from doubling the present CO2 content of the atmosphere and from the boundary conditions associated with the peak of the last ice age. The climate changes produced by long-term volcanic aerosol forcing are obtained by differencing this simulation and one made for the present climate with no volcanic aerosol forcing. The simulations indicate that a significant cooling of the troposphere and surface can occur at times of closely spaced multiple sulfur-rich volcanic explosions that span time scales of decades to centuries. The steady-state climate response to volcanic forcing includes a large expansion of sea ice, especially in the Southern Hemisphere; a resultant large increase in surface and planetary albedo at high latitudes; and sizable changes in the annually and zonally averaged air temperature.

Pollack, James B.↗

Overview of the 2010 Carbonaceous Aerosols and Radiative Effects Study (CARES)

Substantial uncertainties still exist in the scientific understanding of the possible interactions between urban and natural (biogenic) emissions in the production and transformation of atmospheric aerosol and the resulting impact on climate change. The US Department of Energy (DOE) Atmospheric Radiation Measurement (ARM) program's Carbonaceous Aerosol and Radiative Effects Study (CARES) carried out in June 2010 in Central Valley, California, was a comprehensive effort designed to improve this understanding. The primary objective of the field study was to investigate the evolution of secondary organic and black carbon aerosols and their climate-related properties in the Sacramento urban plume as it was routinely transported into the forested Sierra Nevada foothills area. Urban aerosols and trace gases experienced significant physical and chemical transformations as they mixed with the reactive biogenic hydrocarbons emitted from the forest. Two heavily-instrumented ground sites - one within the Sacramento urban area and another about 40 km to the northeast in the foothills area - were set up to characterize the evolution of meteorological variables, trace gases, aerosol precursors, aerosol size, composition, and climaterelated properties in freshly polluted and "aged" urban air. On selected days, the DOE G-1 aircraft was deployed to make similar measurements upwind and across the evolving Sacramento plume in the morning and again in the afternoon. The NASA B-200 aircraft, carrying remote sensing instruments, was also deployed to characterize the vertical and horizontal distribution of aerosols and aerosol optical properties within and around the plume. This overview provides: (a) the scientific background and motivation for the study, (b) the operational and logistical information pertinent to the execution of the study, (c) an overview of key observations and initial findings from the aircraft and ground-based sampling platforms, and (d) a roadmap of planned data analyses and focused modeling efforts that will facilitate the integration of new knowledge into improved representations of key aerosol processes and properties in climate models.

aerosols↗

Scattering and Radiative Properties of Morphologically Complex Carbonaceous Aerosols: A Systematic Modeling Study

This paper provides a thorough modeling-based overview of the scattering and radiative properties of a wide variety of morphologically complex carbonaceous aerosols. Using the numerically-exact superposition T-matrix method, we examine the absorption enhancement, absorption Angstroem exponent (AAE), backscattering linear depolarization ratio (LDR), and scattering matrix elements of black-carbon aerosols with 11 different model morphologies ranging from bare soot to completely embedded soot-sulfate and soot-brown carbon mixtures. Our size-averaged results show that fluffy soot particles absorb more light than compact bare-soot clusters. For the same amount of absorbing material, the absorption cross section of internally mixed soot can be more than twice that of bare soot. Absorption increases as soot accumulates more coating material and can become saturated. The absorption enhancement is affected by particle size, morphology, wavelength, and the amount of coating. We refute the conventional belief that all carbonaceous aerosols have AAEs close to 1.0. Although LDRs caused by bare soot and certain carbonaceous particles are rather weak, LDRs generated by other soot-containing aerosols can reproduce strong depolarization measured by Burton et al. for aged smoke. We demonstrate that multi-wavelength LDR measurements can be used to identify the presence of morphologically complex carbonaceous particles, although additional observations can be needed for full characterization. Our results show that optical constants of the host/coating material can significantly influence the scattering and absorption properties of soot-containing aerosols to the extent of changing the sign of linear polarization. We conclude that for an accurate estimate of black-carbon radiative forcing, one must take into account the complex morphologies of carbonaceous aerosols in remote sensing studies as well as in atmospheric radiation computations.

carbonaceous aerosols; scattering matrix; polariza↗

Semivolatile Particulate Organic Material Southern Africa during SAFARI 2000

During August and September 2000, the University of Washington's Cloud and Aerosol Research Group (CARG) with its Convair-580 research aircraft participated in the Southern African Fire-Atmosphere Research Initiative (SAFARI) 2000 field study in southern Africa. Aboard this aircraft was a Particle Concentrator-Brigham Young University Organic Sampling System (PC-BOSS), which was used to determine semivolatile particulate material with a diffusion denuder sampler. Denuded quartz filters and sorbent beds in series were used to measure nonvolatile and semivolatile materials, respectively. Results obtained with the PC-BOSS are compared to those obtained with conventional quartz-quartz and Teflon-quartz filter pack samplers. Various 10-120 min integrated samples were collected during flights through the h e troposphere, in the atmospheric boundary layer, and in plumes from savanna fires. Significant fine particulate semivolatile organic compounds (SVOC) were found in all samples. The SVOC was not collected by conventional filter pack samplers and therefore would not have been determined in previous studies that used only filter pack samplers. The SVOC averaged 24% of the fine particulate mass in emissions from the fires and 36% of the fine particulate mass in boundary layer samples heavily impacted by aged emissions from savanna fires. Concentrations of fine particulate material in the atmospheric mixed layer heavily impacted by aged savanna frre emissions averaged 130 micrograms per cubic meter. This aerosol was 85% carbonaceous mated.

Eatough, D. J.↗

Canadian and Alaskan Wildfire Smoke Particle Properties, Their Evolution and Controlling Factors, From Satellite Observations

The optical and chemical properties of biomass burning (BB) smoke particles greatly affect the impact that wildfires have on climate and air quality. Previous work has demonstrated some links between smoke properties and factors such as fuel type and meteorology. However, the factors controlling BB particle speciation at emission are not adequately understood nor are the factors driving particle aging during atmospheric transport. As such, modeling wildfire smoke impacts on climate and air quality remains challenging. The potential to provide robust, statistical characterizations of BB particles based on ecosystem type and ambient environmental conditions with remote sensing data is investigated here. Space-based Multi-angle Imaging SpectroRadiometer (MISR) observations, combined with the MISR Research Aerosol (RA) algorithm and the MISR Interactive Explorer (MINX) tool, are used to retrieve smoke plume aerosol optical depth (AOD) and to provide constraints on plume vertical extent; smoke age; and particle size, shape, light-absorption properties, and absorption spectral dependence. These tools are applied to numerous wildfire plumes in Canada and Alaska, across a range of conditions, to create a regional inventory of BB particle-type temporal and spatial distribution. We then statistically compare these results with satellite measurements of fire radiative power (FRP) and land cover characteristics, as well as short-term climate, meteorological, and drought information from the Modern-Era Retrospective analysis for Research and Applications (MERRA-2) reanalysis and the North American Drought Monitor. We find statistically significant differences in the retrieved smoke properties based on land cover type, with fires in forests producing the thickest plumes containing the largest, brightest particles and fires in savannas and grasslands exhibiting the opposite. Additionally, the inferred dominant aging mechanisms and the timescales over which they occur vary systematically between land types. This work demonstrates the potential of remote sensing to constrain BB particle properties and the mechanisms governing their evolution over entire ecosystems. It also begins to realize this potential, as a means of improving regional and global climate and air quality modeling in a rapidly changing world.

Katherine T. Junghenn Noyes↗

Radiative Effects of Aerosols

During the Atlantic Stratocumulus Transition Experiment (ASTEX) in June 1992, two descents in cloud-free regions allowed comparison of the change in aerosol optical depth as determined by an onboard total-direct-diffuse radiometer (TDDR) to the change calculated from measured size-resolved aerosol microphysics and chemistry. Both profiles included a pollution haze from Europe but the second also included the effect of a Saharan dust layer above the haze. The separate contributions of supermicrometer (coarse) and submicrometer (fine) aerosol were determined and thermal analysis of the pollution haze indicated that the fine aerosol was composed primarily of a sulfate/water mixture with a refractory soot-like core. The soot core increased the calculated extinction by about 10% in the most polluted drier layer relative to a pure sulfate aerosol but had significantly less effect at higher humidities. A 3 km descent through a boundary layer air mass dominated by pollutant aerosol with relative humidities (RH) 10-77% yielded a close agreement between the measured and calculated aerosol optical depths (550 nm) of 0.160 (+/- 0.07) and 0. 157 (+/- 0.034) respectively. During descent the aerosol mass scattering coefficient per unit sulfate mass varied from about 5 to 16 m(exp 2)/g and primarily dependent upon ambient RH. However, the total scattering coefficient per total fine mass was far less variable at about 4+/- 0.7 m(exp 2)/g. A subsequent descent through a Saharan dust layer located above the pollution aerosol layer revealed that both layers contributed similarly to aerosol optical depth. The scattering per unit mass of the coarse aged dust was estimated at 1.1 +/- 0.2 m(exp 2)/g. The large difference (50%) in measured and calculated optical depth for the dust layer exceeded measurements.

Valero, Francisco P. J.↗

Initial Results from the Kwajalein Micrometeorite Collections

Micrometeorites are constantly arriving at the Earth's surface, however, they are quickly diluted by the natural and anthropogenic back-ground dust. The successful collection of micromete-orites requires either the employment of a separation technique (e.g. using magnets to separate metal-bearing micrometeorites from deepsea sediments [e.g. 1,2] and dissolved pre-historic limestones and salts [e.g. 3,4]), or an approach that limits contamination by terrestrial dust (e.g. collecting from ice, snow and well water in polar regions - locations where the terrestrial dust flux is so low that micrometeorites repre-sent the major dust component [e.g. 5-7]). We have recently set up a micrometeorite collection station on Kwajalein Island in the Republic of the Marshall Is-lands in the Pacific Ocean, using high volume air samplers to collect particles directly from the atmosphere. Collecting at this location exploits the considerably reduced anthropogenic background; Kwajalein is >1000 miles from the nearest continent and for much of the year, trade winds blow from the northeast at 15 to 20 knots providing a continuous stream of oceanic aerosol for sampling. By collecting directly from the atmosphere, the terrestrial age of the particles, and hence weathering they experience, is minimal. We therefore anticipate that the Kwajalein col-lection may include particles that are highly susceptible to weathering and either not preserved well or not found at all in other collections. In addition, this collection method allows for particle arrival times to be constrained so that collections can be timed to correlate with celestial events (e.g. meteor showers). Here we describe the collections and their preparation and report on the initial results.

Wozniakiewicz, P. J.↗

New Particle Formation and Growth to Climate‐Relevant Aerosols at a Background Remote Site in the Western Himalaya

New particle formation (NPF) can influence the Earth's radiative budget when the newly formed particles grow to climate‐relevant sizes. Here, we present analysis of 21 months of continuous aerosol size distribution measurements at a background remote site in the western Himalaya and provide observational evidence that newly formed particles grow to cloud condensation nuclei (CCN)‐active sizes (i.e., >20–100 nm in diameter). Out of total 55 NPF events, 38 (66%) events occurred in the pre‐monsoon season (March–May). NPF events were classified into those with and without pollution influence as polluted and cleaner, respectively, using black carbon data. The analysis of air mass age, based on the ratio of number concentration of Aitken to accumulation mode aerosols, indicated that NPF occurred in the relatively cleaner air masses reaching to the site. The median formation rate of 10 nm particles and particle growth rates for cleaner events were three‐fold and two‐fold, respectively, higher than polluted events. We present the first estimates of the survival probability of newly formed particles to 50 and 100 nm size, which was not attempted in an Indian environment previously. The survival probability to 50 nm particles ranged from 44% to 98%, with a mean and standard deviation of 82 ± 18%. On average, ∼60% of the particles surviving to 50 nm survived to 100 nm, making the overall survival probability of 100 nm to 53 ± 31%. This indicates that the probability of nucleated particles growing to CCN‐active sizes under a large source of condensing vapor (transported from nearby lower‐altitude regions) and low pre‐existing particle concentrations (background mountain site) is high compared to the previous studies. These findings highlight the importance of the efficiency of nucleation events for producing CCN, which is a critical basis of aerosol indirect effects.

cloud condensation nuclei↗

On Improving the Dust Lidar Ratios for Version 5 of CALIOP by Using Measurements with Source-tagged Model Results

Vertically resolved retrievals of aerosol backscatter and extinction have been available since 2006 from global measurements acquired by the space borne lidar CALIOP onboard the CALIPSO satellite. These retrievals depend crucially upon the ratio of extinction to backscatter (i.e., lidar ratio) which typically has to be assumed for the various aerosol species for an elastic backscatter lidar like CALIOP. For all CALIPSO data releases up until now (version 4.2), these lidar ratios have been taken as constant both spatially and temporally. However, it is well established that the aerosol lidar ratios can vary significantly regionally, seasonally, and also as a function of age and relative humidity. In particular, the dust lidar ratios show significant variation depending upon their source regions, which is related to the mineral composition of dust in that region. In this paper, we shall present a scheme to obtain the regionally and seasonally dependent lidar ratios of dust. In this scheme, which may be implemented in a forthcoming version of CALIOP aerosol extinction retrievals, we first derive lidar ratios of aerosol layers globally, classified as dust by CALIOP, by using the backscatter measurements constrained by collocated MODIS aerosol optical depths. Since this dust will frequently be a mixture of dust from various source regions, we obtain the corresponding regional contributions from the dust simulations using the GEOS model tagged to nine source regions. Finally, combining information from both measurements and models, we obtain the lidar ratios of dust corresponding to the nine source regions. The lidar ratio of the mixed dust anywhere can now be obtained from the tagged model fractions and the corresponding regional lidar ratio. We shall show the application of this scheme for various regions and seasons.

CALIPSO↗

Impact of Nonabsorbing Anthropogenic Aerosols on Clear-Sky Atmospheric Absorption

Absorption of solar radiation by atmospheric aerosol has become recognized as important in regional and global climate. Nonabsorbing, hydrophilic aerosols, such as sulfate, potentially affect atmospheric absorption in opposing ways: first, decreasing absorption through aging initially hydrophobic black carbon (BC) to a hydrophilic state, enhancing its removal by wet scavenging, and consequently decreasing BC lifetime and abundance, and second, increasing absorption through enhancement of the BC absorption efficiency by internal mixing as well as through increasing the amount of diffuse solar radiation in the atmosphere. On the basis of General Circulation Model studies with an embedded microphysical aerosol module we systematically demonstrate the significance of these mechanisms both on the global and regional scales. In remote transport regions, the first mechanism prevails, reducing atmospheric absorption, whereas in the vicinity of source regions, despite enhanced wet scavenging, absorption is enhanced owing to the prevalence of the second mechanisms. Our findings imply that the sulfur to BC emission ratio plays a key role in aerosol absorption.

Stier, Philip↗

Organic Aerosol Volatility Parameterizations and Their Impact on Atmospheric Composition and Climate

Despite their importance and ubiquity in the atmosphere, organic aerosols are still very poorly parameterized in global models. This can be explained by two reasons: first, a very large number of unconstrained parameters are involved in accurate parameterizations, and second, a detailed description of semi-volatile organics is computationally very expensive. Even organic aerosol properties that are known to play a major role in the atmosphere, namely volatility and aging, are poorly resolved in global models, if at all. Studies with different models and different parameterizations have not been conclusive on whether the additional complexity improves model simulations, but the added diversity of the different host models used adds an unnecessary degree of variability in the evaluation of results that obscures solid conclusions. Aerosol microphysics do not significantly alter the mean OA vertical profile or comparison with surface measurements. This might not be the case for semi-volatile OA with microphysics.

Aerosols↗