Climate Effects Of Aerosols Research Articles

The GAMIL3: Model Description and Evaluation

AbstractThe Grid‐point Atmospheric Model of the IAP LASG version 3 (GAMIL3) has been developed by upgrading the horizontal resolution, methods of parallel computation, boundary layer scheme, aerosol parameterization, convective parameterization, stratocumulus cloud fraction scheme, land component, and coupler, as well as tuning some moist physical parameters with large uncertainties. Its performance is evaluated, and the results show significant improvements compared with the previous version, GAMIL2. The simulated performance of mean states is notably enhanced, including the energy budget terms at the top of the atmosphere (TOA) and surface, shortwave/longwave cloud radiative forcing (SWCF/LWCF), precipitation, zonal wind, low‐level temperature, 500‐hPa geopotential height, and snow cover fraction in the Northern Hemisphere. The characteristics of internal variability are captured well, such as the frequency band and active areas of quasi‐biweekly (QBW) oscillation, spectral power of convectively coupled equatorial waves (CCEWs), Madden‐Julian Oscillation (MJO) eastward propagation, and heat flux response to El Niño‐Southern Oscillation (ENSO), and these variabilities are generally strengthened in GAMIL3. In addition, the anthropogenic aerosol climate effects are weakened when using the forcings recommended by CMIP6.

Characterization of Aerosol Type Over East Asia by 4.4 km MISR Product: First Insight and General Performance

AbstractThe lack of aerosol type information has largely hindered satellite products from further applications such as constraining model simulations and quantifying aerosol climate effects. The recent Version (V) 23 Multi‐angle Imaging Spectroradiometer (MISR) aerosol products with an enhanced spatial resolution at 4.4 km enable an unprecedented chance to explore aerosol types and associated processes in the regional scale. Here we provide a comprehensive insight into the characterization of MISR aerosol optical and microphysical properties, as well as their performance, over East Asia. Ground validation shows a remarkable improvement in the accuracy of V23 MISR aerosol optical depth (AOD) with ~80% of its retrieval bias within ±(0.05 + 20%AODAERONET). However, an underestimation of MISR AOD is still prevalent in the high‐AOD (>0.6) conditions, due to the surface‐atmosphere separation problem and insufficient absorbing aerosol mixtures being selected. MISR AOD of different size bins agrees well with AErosol RObotic NETwork (AERONET) results, demonstrating an evident advantage in discriminating natural dust from anthropogenic particles. Although MISR nonspherical and absorbing retrievals display a consistent variation with the AERONET inversions, their component AODs have a poor reliability over East Asia due to the inappropriate aerosol component models or their mixtures as in V22. In particular, the most striking problem is the sparse and discrete MISR absorbing retrievals with spatial discontinuity. Generally, the high‐resolution V23 MISR products exhibit a great potential in characterizing the regional variations of aerosol type, which can be further refined by considering the prior aerosol knowledge over East Asia.

Spatiotemporal Distribution of Major Aerosol Types over China Based on MODIS Products between 2008 and 2017

Knowledge of aerosol-type distribution is critical to the evaluation of aerosol–climate effects. However, research on aerosol-type distribution covering all is limited. This study characterized the spatiotemporal distribution of major aerosol types over China by using MODerate resolution Imaging Spectroradiometer (MODIS) products from 2008 to 2017. Two aerosol-type classification methods were combined to achieve this goal. One was for relatively high aerosol load (AOD ≥ 0.2) using aerosol optical depth (AOD) and aerosol relative optical depth (AROD) and the other was for low aerosol load (AOD < 0.2) using land use and population density information, which assumed that aerosols are closely related to local emissions. Results showed that the dominant aerosol-type distribution has a distinct spatial and temporal pattern. In western China, background aerosols (mainly dust/desert dust and continent aerosol) dominate with a combined occurrence ratio over 70% and they have slight variations on seasonal scale. While in eastern China, the dominant aerosols show strong seasonal variations. Spatially, mixed aerosols dominate most parts of eastern China in spring due to the influence of long-range transported dust from Taklamakan and Gobi desert and urban/industry aerosols take place in summer due to strong photochemical reactions. Temporally, mixed and urban/industry aerosols co-dominate eastern China.

A framework for setting up a country-wide network of regional surface PM2.5 sampling sites utilising a satellite-derived proxy – The COALESCE project, India

Abstract Air quality management and assessment of aerosol climate effects over a large area require the strategic placement of regionally representative monitoring sites (RRMS) to capture the required information. Ground-based, fine particulate matter (PM2.5) concentrations measured for a long duration at high spatial resolution i.e. at several potential locations in a region help identify an optimal regionally representative site for the monitoring network. However, in the absence of long-term PM2.5 concentrations with high spatial resolution, identification of RRMS is a challenge. To identify for such situations, a novel methodology utilising satellite-derived PM2.5 is presented in this study. High spatial resolution (1 km × 1 km) daily aerosol optical depth (AOD) over several years (2004–2011) is used to derive surface PM2.5 using appropriate conversion factors. PM2.5 concentrations thus derived for a potential site and its nearby cells in the region are subjected to statistical analysis, to quantify linear/non-linear relationships between the respective PM2.5 time-series. Metrics such as coefficient of divergence (CoD), Pearson correlation coefficient (PCC) and Mutual information (MI) are calculated to assess the regional representativeness of a site. These criteria combined with physical criteria such as proximity of the site to local sources, local meteorology analysis and clustered air parcel back-trajectory analysis, are used in a weight-of-evidence approach to establish site adequacy. The selection and validation of eleven sites for the COALESCE project, is used as an illustrative example, to demonstrate the effectiveness of the site-selection methodology developed in this study.

High-humidity tandem differential mobility analyzer for accurate determination of aerosol hygroscopic growth, microstructure, and activity coefficients over a wide range of relative humidity

Abstract. Interactions with water are crucial for the properties, transformation, and climate effects of atmospheric aerosols. Here we present the high-humidity tandem differential hygroscopicity analyzer (HHTDMA) and a new method to measure the hygroscopic growth of aerosol particles with in situ restructuring to minimize the influence of particle shape. With this approach, growth factors can be measured with an uncertainty of 0.3 %–0.9 % over a relative humidity (RH) range of 2 %–99.6 % and with an RH measurement accuracy better than 0.4 %. The HHTDMA instrument can be used in hydration, dehydration, and restructuring modes of operation. The restructuring mode allows us to investigate the effects of drying conditions on the initial microstructure of aerosol particles and specifies the optimal parameters that provide their rearrangements into compact structures with a nearly spherical shape. These optimal parameters were used in hygroscopic growth experiments by combining the restructuring mode with a conventional hydration or dehydration mode. The tandem of two modes allowed us to measure the particle growth factors with high precision as well as to determine the thickness of the water adsorption layer on the surface of compact crystalline particles. To verify the HHTDMA instrument we compared the measured ammonium sulfate growth factors with those obtained from the E-AIM-based Köhler model (E-AIM: Extended Aerosol Inorganics Model). Averaged over the range of 38 %–96 % RH, the mean relative deviations between measurements and model results is less than 0.5 %. We demonstrate this precision by presenting data for glucose, for which bulk thermodynamic coefficients are available. The HHTDMA-derived activity coefficients of water and glucose were obtained for both dilute and supersaturated solutions and are in good agreement with those reported in the literature. The average deviation between the measured activity coefficients and those obtained by the bulk method is less than 4 %. For dilute solution in water with an activity range of 0.98–0.99, the hygroscopicity parameter of glucose and the molal osmotic coefficient were obtained with an uncertainty of 0.4 % and 2.5 %, respectively.

Climate effects of aerosols reduce economic inequality

The climate effects of anthropogenic aerosols have masked some of the warming induced by GHGs1 along with some impacts of that warming2. These temperature effects may be beneficial but are almost certainly overwhelmed by aerosols’ negative health impacts3. Recent analyses of economic impacts have concluded that warming harms economies in warm climates, but provides economic benefits in cold climates4. Here we investigate whether aerosol-induced cooling would have a positive effect on less wealthy economies in hotter regions and a negative effect on wealthier economies in colder regions. Climate simulations over the historical period both with and without anthropogenic aerosol emissions, using a fully coupled ocean and atmosphere climate model, indicate that in year 2010 anthropogenic aerosol emissions were cooling the Earth by 0.72 ± 0.02 °C relative to a scenario without such emissions. Due to opposing economic impacts in different regions, the net economic impact of aerosol-induced cooling is likely to be small at the global scale. However, these results suggest that the cooling effects of anthropogenic aerosols benefit developing tropical economies while harming developed high-latitude economies, and thus the temperature effects of past aerosol emissions have probably diminished global economic inequality. Anthropogenic aerosols mask some greenhouse warming via radiation scattering and cloud interactions. Research suggests the economic impact of this aerosol-induced cooling was small globally, although it benefitted developing countries in warm climates and harmed high-latitude developed countries.

A Comprehensive Nontarget Analysis for the Molecular Reconstruction of Organic Aerosol Composition from Glacier Ice Cores.

Ice cores are climate archives suitable for the reconstruction of past atmospheric composition changes. Ice core analysis provides valuable insight into the chemical nature of aerosols and enables constraining emission inventories of primary emissions and of gas-phase precursors. Changes in the emissions of volatile organic compounds (VOCs) can affect formation rates and mechanisms as well as chemical composition of aerosols during the preindustrial era, key information for understanding aerosol climate effects. Here, we present an analytical method for the reconstruction of organic aerosol composition preserved in glacier ice cores. A solid-phase-extraction method, optimized toward oxidation products of biogenic VOCs, provides an enrichment factor of ∼200 and quantitative recovery for compounds of interest. We applied the preconcentration method on ice core samples from the high-alpine Fiescherhorn glacier (Swiss Alps), and used high-performance liquid chromatography coupled to high-resolution mass spectrometry as a sensitive detection method. We describe a nontarget analysis that screens for organic molecules in the ice core samples. We evaluate the atmospheric origin of the detected compounds in the ice by molecular-resolved comparison with airborne particulate matter samples from the nearby high-alpine research station Jungfraujoch. The presented method is able to shed light upon the history of the evolution of organic aerosol composition in the anthropocene, a research field in paleoclimatology with considerable potential.

Spatial distribution of aerosol microphysical and optical properties and direct radiative effect from the China Aerosol Remote Sensing Network

Abstract. Multi-year observations of aerosol microphysical and optical properties, obtained through ground-based remote sensing at 50 China Aerosol Remote Sensing Network (CARSNET) sites, were used to characterize the aerosol climatology for representative remote, rural, and urban areas over China to assess effects on climate. The annual mean effective radii for total particles (ReffT) decreased from north to south and from rural to urban sites, and high total particle volumes were found at the urban sites. The aerosol optical depth at 440 nm (AOD440 nm) increased from remote and rural sites (0.12) to urban sites (0.79), and the extinction Ångström exponent (EAE440–870 nm) increased from 0.71 at the arid and semi-arid sites to 1.15 at the urban sites, presumably due to anthropogenic emissions. Single-scattering albedo (SSA440 nm) ranged from 0.88 to 0.92, indicating slightly to strongly absorbing aerosols. Absorption AOD440 nm values were 0.01 at the remote sites versus 0.07 at the urban sites. The average direct aerosol radiative effect (DARE) at the bottom of atmosphere increased from the sites in the remote areas (−24.40 W m−2) to the urban areas (−103.28 W m−2), indicating increased cooling at the latter. The DARE for the top of the atmosphere increased from −4.79 W m−2 at the remote sites to −30.05 W m−2 at the urban sites, indicating overall cooling effects for the Earth–atmosphere system. A classification method based on SSA440 nm, fine-mode fraction (FMF), and EAE440–870 nm showed that coarse-mode particles (mainly dust) were dominant at the rural sites near the northwestern deserts, while light-absorbing, fine-mode particles were important at most urban sites. This study will be important for understanding aerosol climate effects and regional environmental pollution, and the results will provide useful information for satellite validation and the improvement of climate modelling.

Modeling the aerosol chemical composition of the tropopause over the Tibetan Plateau during the Asian summer monsoon

Abstract. Enhanced aerosol abundance in the upper troposphere and lower stratosphere (UTLS) associated with the Asian summer monsoon (ASM) is referred to as the Asian Tropopause Aerosol Layer (ATAL). The chemical composition, microphysical properties, and climate effects of aerosols in the ATAL have been the subject of discussion over the past decade. In this work, we use the ECHAM/MESSy Atmospheric Chemistry (EMAC) general circulation model at a relatively fine grid resolution (about 1.1×1.1∘) to numerically simulate the emissions, chemistry, and transport of aerosols and their precursors in the UTLS within the ASM anticyclone during the years 2010–2012. We find a pronounced maximum of aerosol extinction in the UTLS over the Tibetan Plateau, which to a large extent is caused by mineral dust emitted from the northern Tibetan Plateau and slope areas, lofted to an altitude of at least 10 km, and accumulating within the anticyclonic circulation. We also find that the emissions and convection of ammonia in the central main body of the Tibetan Plateau make a great contribution to the enhancement of gas-phase NH3 in the UTLS over the Tibetan Plateau and ASM anticyclone region. Our simulations show that mineral dust, water-soluble compounds, such as nitrate and sulfate, and associated liquid water dominate aerosol extinction in the UTLS within the ASM anticyclone. Due to shielding of high background sulfate concentrations outside the anticyclone from volcanoes, a relative minimum of aerosol extinction within the anticyclone in the lower stratosphere is simulated, being most pronounced in 2011, when the Nabro eruption occurred. In contrast to mineral dust and nitrate concentrations, sulfate increases with increasing altitude due to the larger volcano effects in the lower stratosphere compared to the upper troposphere. Our study indicates that the UTLS over the Tibetan Plateau can act as a well-defined conduit for natural and anthropogenic gases and aerosols into the stratosphere.

Comparison of Anthropogenic Aerosol Climate Effects among Three Climate Models with Reduced Complexity

The same prescribed anthropogenic aerosol forcing was implemented into three climate models. The atmosphere components of these participating climate models were the GAMIL, ECHAM, and CAM models. Ensemble simulations were carried out to obtain a reliable estimate of anthropogenic aerosol effective radiative forcing (ERF). The ensemble mean ERFs from these three participating models with this aerosol forcing were −0.27, −0.63, and −0.54 W∙m−2. The model diversity in ERF is clearly reduced as compared with those based on the models’ own default approaches (−1.98, −0.21, and −2.22 W∙m−2). This is consistent with the design of this aerosol forcing. The modeled ERF can be decomposed into two basic components, i.e., the instantaneous radiative forcing (RF) from aerosol–radiation interactions (RFari) and the aerosol-induced changes in cloud forcing (△Fcloud*). For the three participating models, the model diversity in RFari (−0.21, −0.33, and −0.29 W∙m−2) could be constrained by reducing the differences in natural aerosol radiative forcings. However, it was difficult to figure out the reason for the model diversity in △Fcloud* (−0.05, −0.28, and −0.24 W∙m−2), which was the dominant source of the model diversity in ERF. The variability of modeled ERF was also studied. Ensemble simulations showed that the modeled RFs were very stable. The rapid adjustments (ERF − RF) had an important role to play in the quantification of the perturbation of ERF. Fortunately, the contribution from the rapid adjustments to the mean ERF was very small. This study also showed that we should pay attention to the difference between the aerosol climate effects we want and the aerosol climate effects we calculate.

Climate Effects of Anthropogenic Aerosol Forcing on Tropical Precipitation and Circulations

ABSTRACT Aerosols are one of the key factors influencing the hydrological cycle and radiation balance of the climate system. Although most aerosols deposit near their sources, the induced cooling effect is on a global scale and can influence the tropical atmosphere through slow processes, such as air–sea interactions. This study analyzes several simulations of fully coupled atmosphere–ocean climate models under the influence of anthropogenic aerosols, with the concentrations of greenhouse gases kept constant. In the cooling simulations, precipitation is reduced in deep convective areas but increased around the edges of convective areas, which is opposite to the “rich-get-richer” phenomenon in global warming scenarios in the first-order approximation. Tropical convection is intensified with a shallower depth, and tropical circulations are enhanced. The anomalous gross moist stability (M′) mechanism and the upped-ante mechanism can be used to explain the dynamic and thermodynamic processes in the changes in tropical precipitation and convection. There is a northward cross-equatorial energy transport due to the cooler Northern Hemisphere in most of the simulations, together with the southward shift of the intertropical convergence zone (ITCZ) and the enhancement of the Hadley circulation. The enhancement of the Hadley circulation is more consistent between models than the changes of the Walker circulation. The change in the Hadley circulation is not as negligible as in the warming cases in previous studies, which supports the consistency of the ITCZ shift in cooling simulations.

Vertical distribution of the Asian tropopause aerosols detected by CALIPSO

Characterizing the vertical distribution of aerosol optical properties is crucial to reduce the uncertainty in quantifying the radiative forcing and climate effects of aerosols. The analysis of four-year (2007–2010) Cloud-Aerosol Lidar and Infrared Pathfinder Satellite Observation (CALIPSO) lidar measurements revealed the existence of tropospheric aerosol layers associated with the Asian summer monsoon. The measurements of five typical aerosol optical and microphysical parameters were used to explore the properties, spatial/vertical distributions, annual evolution of tropopause aerosols over the South Asia region. Results extracted from various latitude-height and longitude-height cross sections of aerosol extinction coefficient at 532 and 1064 nm, backscatter coefficient at 532 nm, and depolarization ratio at 532 nm demonstrated that a large amount of aerosols vertically extended up to the tropopause (12 km) during the monsoon season over the north Arabian Sea, India, north Bay of Bengal, and equatorial Indian Ocean, finally reaching the southeast of the Tibetan Plateau. Convective transport associated with Asian summer monsoon is an important factor controlling the vertical distribution of tropopause aerosols. The evolution of aerosol scattering ratio at 532 nm indicated that from equatorial Indian Ocean to South Asia, there exists an upward tilting and ascending structure of the aerosols layer during the monsoon season, which typically indicates enhanced aerosols over the Asian monsoon region. Information on aerosol size distribution and detailed composition are needed for better understanding the nature and origin of this aerosol layer. Enhancement of the tropopause aerosols should be considered in the future studies in evaluating the regional or global climate systems. Further satellite observations of aerosols and in-situ observations are also urgently needed to diagnose this aerosol layer, which likely originate from anthropogenic emissions.

Significant Climate Impact of Highly Hygroscopic Atmospheric Aerosols in Delhi, India

AbstractHygroscopicity of aerosol (κchem) is a key factor affecting its direct and indirect climate effects, however, long‐term observation in Delhi is absent. Here we demonstrate an approach to derive κchem from publicly available data sets and validate it (bias of 5%–30%) with long‐term observations in Beijing. Using this approach, we report the first estimation of κchem in Delhi and discuss its climate implications. The bulk‐averaged κchem of aerosols in Delhi is estimated to be 0.42 ± 0.07 during 2016–2018, implying a higher activation ability as cloud condensation nuclei in Delhi compared with Beijing and continental averages worldwide. To activate a 0.1‐μm particle, it averagely requires just a supersaturation of ~0.18% ± 0.015% in Delhi but ~0.3% (Beijing), 0.28%–0.31% (Asia, Africa, and South America) and ~0.22% (Europe and North America). Our results imply that representing κchem of Delhi using Asian/Beijing average may result in a significant underestimation of aerosol climate effects.

Impact of Anthropogenic Emission Injection Height Uncertainty on Global Sulfur Dioxide and Aerosol Distribution

AbstractAnthropogenic sulfur compounds play an important role in acid deposition, aerosol particle formation, and subsequent radiative forcing and human fine particulate exposure. There are substantial uncertainties in processes influencing sulfate and precursor distributions, however, that have not yet been resolved through comparisons with observations. We find here an underappreciated factor that has a large impact on model results: uncertain emission height. Global aerosol‐climate model simulations indicate that the assumed effective anthropogenic emission height is very important to SO2 near‐surface concentrations and vertical profile. The global range of near‐surface SO2 concentration over land (ocean) due to uncertainty in industrial (international shipping) emission injection height is 81% (76%), relative to the average concentration. This sensitivity is much larger than the uncertainty of SO2 emission rates. Black carbon and primary organic matter concentration and profiles are also sensitive to emission heights (53% over land and 28% over oceans). The impact of emission height uncertainty is larger in winter for land‐based emissions, but larger in summer over the Northern Hemisphere ocean for shipping emissions. The variation in aerosol optical depth related to shipping emission injection heights is 11% over oceans, revealing the potential importance of injection height on aerosol forcing and climatic effects. The large impact on SO2 concentrations can confound attempts to use surface, aircraft, and satellite observations to constrain the importance of other processes that govern sulfur compound distributions in the atmosphere. The influence of emission height on vertical SO2 column also will impact the accuracy of satellite retrievals.

Studying the impact of biomass burning aerosol radiative and climate effects on the Amazon rainforest productivity with an Earth system model

Abstract. Diffuse light conditions can increase the efficiency of photosynthesis and carbon uptake by vegetation canopies. The diffuse fraction of photosynthetically active radiation (PAR) can be affected by either a change in the atmospheric aerosol burden and/or a change in cloudiness. During the dry season, a hotspot of biomass burning on the edges of the Amazon rainforest emits a complex mixture of aerosols and their precursors and climate-active trace gases (e.g. CO2, CH4, NOx). This creates potential for significant interactions between chemistry, aerosol, cloud, radiation and the biosphere across the Amazon region. The combined effects of biomass burning on the terrestrial carbon cycle for the present day are potentially large, yet poorly quantified. Here, we quantify such effects using the Met Office Hadley Centre Earth system model HadGEM2-ES, which provides a fully coupled framework with interactive aerosol, radiative transfer, dynamic vegetation, atmospheric chemistry and biogenic volatile organic compound emission components. Results show that for present day, defined as year 2000 climate, the overall net impact of biomass burning aerosols is to increase net primary productivity (NPP) by +80 to +105 TgC yr−1, or 1.9 % to 2.7 %, over the central Amazon Basin on annual mean. For the first time we show that this enhancement is the net result of multiple competing effects: an increase in diffuse light which stimulates photosynthetic activity in the shaded part of the canopy (+65 to +110 TgC yr−1), a reduction in the total amount of radiation (−52 to −105 TgC yr−1) which reduces photosynthesis and feedback from climate adjustments in response to the aerosol forcing which increases the efficiency of biochemical processes (+67 to +100 TgC yr−1). These results illustrate that despite a modest direct aerosol effect (the sum of the first two counteracting mechanisms), the overall net impact of biomass burning aerosols on vegetation is sizeable when indirect climate feedbacks are considered. We demonstrate that capturing the net impact of aerosols on vegetation should be assessed considering the system-wide behaviour.

Multiyear Ground‐Based Measurements of Aerosol Optical Properties and Direct Radiative Effect Over Different Surface Types in Northeastern China

AbstractAerosol microphysical and optical properties as well as aerosol direct radiative effect (ADRE) were measured at a few ground sites to investigate aerosol optical‐radiative characteristics in northeastern China. Bimodal size distributions showed a dominance of fine mode particles at Shenyang, a megacity, and more impacts from larger particles at Fushun and Dalian, industrial and coastal sites, respectively. High aerosol optical depths at 440 nm in July (0.67–1.25) were ascribed to hygroscopic effects or cloud processing. Single scattering albedos at 440 nm show strong to moderate absorption at the urban and industrial sites (0.84–0.86) and weaker absorption at the coastal and rural sites (0.92–0.94). The single scattering albedo wavelength dependence implied influences of dust at the urban, industrial, and coastal regions (shorter wavelengths) and biomass emissions at the rural site (longer wavelengths). Absorptive aerosol optical depths at the urban and industrial sites were ~2.5 and 3.7 times higher than at the coastal and rural sites. Large negative ADREs at the bottom of the atmosphere at the urban and industrial sites implied strong surface cooling and the larger ADREs at the top of the atmosphere at the coastal site indicated more cooling of the Earth‐atmosphere system. The main aerosol types at the urban and industrial sites were mixed absorbing particles, while weakly‐absorbing fine mode particles dominated the coastal and rural sites. This study provides new information on the aerosol distributions and potential regional climate effects of aerosols in northeastern China.

Source apportionment of the organic aerosol over the Atlantic Ocean from 53° N to 53° S: significant contributions from marine emissions and long-range transport

Abstract. Marine aerosol particles are an important part of the natural aerosol systems and might have a significant impact on the global climate and biological cycle. It is widely accepted that truly pristine marine conditions are difficult to find over the ocean. However, the influence of continental and anthropogenic emissions on the marine boundary layer (MBL) aerosol is still less understood and non-quantitative, causing uncertainties in the estimation of the climate effect of marine aerosols. This study presents a detailed chemical characterization of the MBL aerosol as well as the source apportionment of the organic aerosol (OA) composition. The data set covers the Atlantic Ocean from 53∘ N to 53∘ S, based on four open-ocean cruises in 2011 and 2012. The aerosol particle composition was measured with a high-resolution time-of-flight aerosol mass spectrometer (HR-ToF-AMS), which indicated that sub-micrometer aerosol particles over the Atlantic Ocean are mainly composed of sulfates (50 % of the particle mass concentration), organics (21 %) and sea salt (12 %). OA has been apportioned into five factors, including three factors linked to marine sources and two with continental and/or anthropogenic origins. The marine oxygenated OA (MOOA, 16 % of the total OA mass) and marine nitrogen-containing OA (MNOA, 16 %) are identified as marine secondary products with gaseous biogenic precursors dimethyl sulfide (DMS) or amines. Marine hydrocarbon-like OA (MHOA, 19 %) was attributed to the primary emissions from the Atlantic Ocean. The factor for the anthropogenic oxygenated OA (Anth-OOA, 19 %) is related to continental long-range transport. Represented by the combustion oxygenated OA (Comb-OOA), aged combustion emissions from maritime traffic and wild fires in Africa contributed, on average, a large fraction to the total OA mass (30 %). This study provides the important finding that long-range transport was found to contribute averagely 49 % of the submicron OA mass over the Atlantic Ocean. This is almost equal to that from marine sources (51 %). Furthermore, a detailed latitudinal distribution of OA source contributions showed that DMS oxidation contributed markedly to the OA over the South Atlantic during spring, while continental-related long-range transport largely influenced the marine atmosphere near Europe and western and central Africa (15∘ N to 15∘ S). In addition, supported by a solid correlation between marine tracer methanesulfonic acid (MSA) and the DMS-oxidation OA (MOOA, R2>0.85), this study suggests that the DMS-related secondary organic aerosol (SOA) over the Atlantic Ocean could be estimated by MSA and a scaling factor of 1.79, especially in spring.

Three-wavelength cavity-enhanced albedometer for measuring wavelength-dependent optical properties and single-scattering albedo of aerosols.

The spectral dependence of aerosol light absorption (αabs) and single-scattering albedo-[ω, defined as the ratio of the scattering (αscat) and extinction coefficients (αext = αabs + αscat)]-has proven effective in classifying dominant aerosol types. It is also helpful in understanding aerosol sources, transformation, climate and environmental effects, testing aerosol models, and improving the retrieval accuracy of satellite and remote sensing data. Despite the significant progress that has been made with measurement of light absorption and ω, many of the reported instruments either operate at a fixed wavelength or can only measure a single optical parameter. Quantitative multi-parameter wavelength-dependent measurement remains a challenge. In this work, a three-wavelength cavity-enhanced albedometer was developed. The albedometer can measure multiple optical parameters, αext, αscat, αabs, and ω, at λ = 365, 532, and 660 nm, in real time. The instrument's performance was evaluated using four different type laboratory generated aerosols, including polystyrene latex spheres (PSL, non-absorbing); ammonium sulfate (AS, non-absorbing); suwannee river fulvic acid (SRFA, slightly absorbing; a proxy for light absorbing organic aerosol); and nigrosin (strongly absorbing).

Studies on the Climate Effects of Black Carbon Aerosols in China and Their Sensitivity to Particle Size and Optical Parameters

In this paper, based on the principle of Mie scattering, we calculated the optical parameters of BC aerosols at different scales and then applied the new optical parameters to simulate the BC aerosols concentration distribution, radiative forcing, and their climate effects. We also compared the results of optical parameters of BC aerosols with homogeneous scales and analyzed the effect on climate. Compared with the conventional uniform-scheme optical parameterization, the concentrations of the first mode of BC aerosols simulated with the optical parameters that were recalculated based on the particle size are significantly higher, while the concentrations of the other modes and the total of BC aerosols are lower. In the respective of statistics, the changes of column burdens of BC in four modes are 0.085, −0.095, −0.089, −0.054 mg/m2. The clear-sky TRF of BC are weakened in the value of 0.03 W/m2 averaged over the domain, while the all-sky TRF of BC are enhanced of 0.06 W/m2 in general. The warming effect of BC becomes weaker when using the new scheme by −0.04 K to −0.24 K. When using the new optical parameters scheme, the regional average surface concentrations of BC in four modes are 0.372, 0.264, 0.055 and 0.004 μg/m3, respectively. Especially, the first and the second mode account for as large as 53% and 38%. The surface concentration and column burden of total BC are 0.69 μg/m3 and 0.28 mg/m2 can be dropped. The regional average direct RFs of BC at the top of the atmosphere are 0.49 W/m2 under clear-sky and 0.36 W/m2 under all-sky averaged over the domain. Over most areas of central China, North China, and East China, BC may increase the temperature in a range of 0.05∼0.15 K, while over South China, BC shows cooling effect. In average, the precipitation variations caused by BC over East China, North China, South China, and Northeast China are −0.83, −0.05, −0.11, and −0.13 mm/d, respectively. As a whole, the variations of circulation, pressure, and temperature show a good correspondence.

Analysis of water vapor effects on aerosol properties and direct radiative forcing in China

The effects of column water vapor (CWV) on aerosol optical properties, radiative effects and classification are studied by using aerosol and CWV data from eight Aerosol Robotic Network (AERONET) sites in China: Beijing, XiangHe, Shouxian, Taihu, Hong_Kong, Zhongshan_Univ, SACOL, and Mt_WLG, which represents 5 distinct aerosol climatologies in China. Contrast in correlations between aerosol optical depth (AOD) and CWV is found. High correlation coefficient (R) ranging from 0.63–0.94 is observed at Beijing and XiangHe (North China Plain), SACOL (Northwest China) and Mt_WLG (the Tibetan Plateau). R values at stations in the Middle-East China (Shouxian and Taihu) are within 0.32–0.45. AOD shows poor correlation to CWV in Southeast China (R at Hong_Kong and Zhongshan_Univ of 0.15 and 0.27). At most sites, the asymmetry (ASYM) of fine-mode aerosol increases with CWV with R larger than ~0.4. Aerosol direct radiative forcing efficiency (ADRFE) at the bottom of the atmosphere (BOA) is affected by CWV, with R >~0.5 over the north and Middle-East China sites. The statistic results show that an increase of CWV by 0.1 cm could result in enhancements of ADREF at the BOA by about 1.1–2.8 W m−2 at all the sites except Mt_WLG. The aerosol classification shows that the mix-small aerosol type is always dominated under the high CWV air. The clusters of back-trajectories with relative humidity (RH) from Hybrid Single-Particle Lagrangian Integrated Trajectory (HYSPLIT) model indicate that the air mass with high RH is often from south and east directions. The influence of CWV on aerosol properties is mainly shown in the properties of fine mode aerosol, which needs to be considered in the study of aerosol radiative forcing and climate effects.