Aerosol Wet Removal Research Articles

Light Precipitation rather than Total Precipitation Determines Aerosol Wet Removal.

Precipitation scavenging is an important sink for both organic and inorganic pollutants in the atmosphere. However, there has been controversy over the relative importance of different precipitation characteristics (i.e., the precipitation amount, intensity, frequency, and duration) in the removal of air pollutants. It is critical to reach a consensus on which precipitation characteristics are most significant for aerosol wet removal. In this study, the analysis of multisource in situ observations of aerosol wet deposition worldwide indicates that the precipitation frequency plays a first-order role in scavenging aerosols. This is because large amounts of air pollutants are efficiently removed at precipitation initiation. As the duration and amount of precipitation increase, the scavenging efficiency decreases sharply. Consequently, it is featured that light precipitation, due to its high frequency of occurrence, rather than total precipitation, determines climatological aerosol wet deposition. To further confirm this, a state-of-the-art global climate model with convection resolved is modified to reduce the light precipitation frequency in both stratiform and convective cloud regimes. Results show widespread increases in aerosol optical depth (AOD) due to the reduced wet deposition. The spatial distribution of aerosol wet deposition changes resembles that of changes in the light precipitation frequency rather than that of total precipitation changes. These findings are consistent with those from the Coupled Model Intercomparison Project Phase 6 multimodel simulations, which show that the intermodel uncertainty in simulated AOD correlates more strongly with the uncertainty in light precipitation frequency than with that in total precipitation.

Improving Aerosol Radiative Forcing and Climate in E3SM: Impacts of New Cloud Microphysics and Improved Wet Removal Treatments

AbstractNumerous Earth system models exhibit excessive aerosol effective forcing at the top of the atmosphere (TOA), including the Department of Energy's Energy Exascale Earth System Model (E3SM). Here, in the context of the E3SM version 3 effort, the predicted particle property (P3) stratiform cloud microphysics scheme and an enhanced deep convection parameterization suite (ZM_plus) are implemented into E3SM. The ZM_plus includes a convective cloud microphysics scheme, a multi‐scale coherent structure parameterization for mesoscale convective systems, and a revised cloud base mass flux formulation considering impacts of the large‐scale environment. The P3 scheme improved cloud and radiation particularly over the Northern Hemisphere and the frequency of heavy precipitation over the tropics, and the ZM_plus improved clouds in the tropics. P3 decreases aerosol effective forcing by 0.15 W m−2, while the ZM_plus increases it by 0.27 W m−2, resulting from excessive direct (0.31 W m−2) and indirect forcing (−1.79 W m−2). The excessive aerosol forcings are due to aerosol overestimation associated with insufficient aerosol wet removal. By improving the physical treatments in the aerosol wet removal, we effectively mitigate anthropogenic aerosol overestimation and thus attenuate direct (0.09 W m−2) and indirect aerosol forcing (−1.52 W m−2). Adjustment to primary organic matter hygroscopicity reduces direct and indirect forcing to more reasonable values: −0.13 W m−2 and −1.31 W m−2, respectively. On climatology, improved aerosol treatments mitigate overestimation of aerosol optical depth.

Chemical Data Assimilation With Aqueous Chemistry in WRF‐Chem Coupled With WRFDA (V4.4.1)

AbstractThis study introduces a new chemistry option in the Weather Research and Forecasting model data assimilation (WRFDA) system, coupled with the WRF‐Chem model (Version 4.4.1), to incorporate aqueous chemistry (AQCHEM) in the assimilation of ground‐level chemical measurements. The new DA capability includes the integration of aqueous‐phase aerosols from the Regional Atmospheric Chemistry Mechanism (RACM) gas chemistry, the Modal Aerosol Dynamics Model for Europe (MADE) aerosol chemistry, and the Volatility Basis Set (VBS) for secondary organic aerosol production. The RACM‐MADE‐VBS‐AQCHEM scheme facilitates aerosol‐cloud‐precipitation interactions by activating aerosol particles in cloud water during the model simulation. With the goal of enhancing air quality forecasting in cloudy conditions, this new implementation is demonstrated in the weakly coupled three‐dimensional variational data assimilation (3D‐Var) system through regional air quality cycling over East Asia. Surface particulate matter (PM) concentrations and four gas species (SO2, NO2, O3, and CO) are assimilated every 6 hr for the month of March 2019. The results show that including aqueous‐phase aerosols in both the analysis and forecast can represent aerosol wet removal processes associated with cloud development and rainfall production. During a pollution event with high cloud cover, simulations without aerosols defined in cloud water exhibit significantly higher values for liquid water path, and surface PM10 (PM2.5) concentrations are overestimated by a factor of 10 (3) when wet scavenging processes dominate. On the contrary, AQCHEM proves to be helpful in simulating the wet deposition of aerosols, accurately predicting the evolution of surface PM concentrations without such overestimation.

The Role of In‐Cloud Wet Removal in Simulating Aerosol Vertical Profiles and Cloud Radiative Forcing

AbstractAmong the physical processes controlling aerosol vertical profiles, in‐cloud wet removal is of utmost importance while its representation in global climate models (GCMs) is crude. In this study, we implement into the Community Atmosphere Model version 6 (CAM6) a physically‐based aerosol wet removal parameterization scheme that explicitly treats aerosol activation, removal and resuspension. Evaluation against in‐situ observations shows that the default scheme substantially overestimates the upper tropospheric black carbon (BC) and sea salt mass. Our physically‐based scheme reduces BC and sea salt mass by a factor of 10 and 1,000, respectively, in better agreement with observations. Also, the new scheme slightly increases number of aerosol particles between 12 nm and 4.8 μm in diameter, thereby mitigating the aerosol number underestimation in the default scheme. Our new scheme reduces the overestimation of coarse‐mode aerosol (0.5–4.8 μm) number. Overall, the aerosol property changes (mass decrease and number increase) reduce the cloud condensation nuclei (CCN) concentration at low supersaturation (i.e., 0.02% and 0.1%), and increase CCN at high supersaturations (i.e., 0.5% and 1%). Consequently, the global annual mean cloud liquid water path increases by 1.89 g m−2 and the ice water path increases by 0.51 g m−2. The global annual mean shortwave, longwave, and net cloud radiative forcing change by −1.06, 0.57, and −0.48 W m−2, respectively. Further improvement is needed to reflect the real physics that the removal efficiencies for aerosol mass and number are disproportionate and to advect cloud‐borne (activated) aerosols for a complete aerosol lifecycle.

Factors influencing aerosol and precipitation ion chemistry in urban background of Moscow megacity

In-depth study of aerosol and precipitation ion chemistry was carried out in order to cover an existing data gap in the seasonal-dependent ionic data in Moscow urban background atmosphere. Literature about atmospheric pollution in this megacity is, indeed, still poor, despite its peculiar climatological characteristics that make it a very interesting site for atmospheric research. Particulate matter (PM) and precipitation were collected at Moscow urban background during spring of 2018, summer, and autumn of 2019. Aerosol inorganic ions are characterized for the whole period, carboxylic acids and sugars for summer. Inorganic ions constitute a major PM10 fraction of 27% in autumn, it drops down to 16.5% in summer. Dominance of secondary inorganic aerosol (SIA) over all the other inorganic ion species is determined. Na+ and Ca2+ shows the largest variability between seasons, with maximum in summer and spring, respectively. Excess of anions in autumn is indicated by ion balance while adding carbonates, spring and summer aerosol is found electroneutral. Chloride depletion phenomenon follows the snow melt and remobilization of salt applied to roads for deicing, demonstrating the biggest impact in summer. Degree of neutralization of ammonia as sulfate and nitrate is found by the correlation between the concentration of NH4+ and calculated from SO42− and NO3−. Inorganic fraction in PM10 is higher (16.5%) than total carboxylic acids (3.5%), and total sugars and anhydrosugars (0.8%). Concentration polar plots show ion variation jointly with wind speed and wind direction and the source origin. Highest SIA concentrations relate a cluster of the prevalent air mass transportation and indicate the source in the northwestern direction in spring and summer. K+ acts as a marker of fires in spring and summer as well as of the domestic biomass burning in the region around a megacity in autumn. Source apportionment of inorganic ion and BC by Varimax analysis reveals major sources namely SIA, soil resuspension, biomass burning, deicing salt, and fossil fuel combustion. In summer, organic ions, anhydrosugars, and sugars shows additional impact of photochemistry and biological activities. Rainfall is heavier in summer than in autumn, with pH of acid rain during spring and summer. The highest concentrations for almost all ions were observed in spring, except HCO3−. Precipitation composition is described with aerosol wet removal by seasonal variability of SIA scavenging factors, decreasing in summer and increasing in autumn and spring.

Characterizing the Impact of Atmospheric Rivers on Aerosols in the Western U.S.

AbstractTwo 5‐year (2010–2014) quasi‐global simulations using the Weather Research and Forecasting model coupled with Chemistry have been analyzed to quantify the impacts of atmospheric rivers (ARs) on aerosols in the western United States (U.S.). We find that AR days have reduced trans‐Pacific as well as U.S. aerosol mass because of enhanced rainfall and hence, wet removal of aerosols, compared to non‐AR days. ARs reduce trans‐Pacific aerosol mass through the cyclonic circulation that shifts the aerosol transport pathway southward and brings cleaner air from the north. However, ARs have larger impact on aerosols that originate over the U.S., which are concentrated closer to the surface compared to trans‐Pacific aerosols that are distributed more uniformly with altitude. While dust and sulfates dominate the mass for both trans‐Pacific and U.S. aerosols, ARs reduce dust composition fractions of trans‐Pacific aerosols but the AR impacts on composition fractions of U.S. aerosols are more variable.

Improving Wet and Dry Deposition of Aerosols in WRF‐Chem: Updates to Below‐Cloud Scavenging and Coarse‐Particle Dry Deposition

AbstractWet and dry depositions of aerosols in WRF‐Chem are revisited and updated based on recent observational findings. Traditionally, in‐cloud scavenging was thought to play a more dominant role in aerosol wet removal than below‐cloud scavenging. However, recent field measurements indicated a considerable contribution of below‐cloud scavenging of 50%–60% to total wet deposition. In contrast, the simulated contribution of in‐cloud scavenging in the previous version of WRF‐Chem was too large, exhibiting 88%–95%, likely due to the binary representation of cloud fraction. To reduce the model bias, this study adopts a continuous‐type cloud fraction and implements a semi‐empirical below‐cloud scavenging parameterization. Simulation results with the new scheme show that the contribution of below‐cloud (in‐cloud) scavenging is increased to 63%–66% (decreased to 34%–37%), well capturing the observational estimates. The magnitude of total wet deposition is increased by 18.2% for SO4, 7.16% for NO3, and 14.8% for NH4, showing better agreements with observations particularly for SO4 and NH4 deposition. The increased wet removal with the new scheme reduces and so better reproduces surface PM2.5 and PM10 concentrations, which is also partly attributed to the increased contribution of below‐cloud scavenging. It is found that dry deposition velocity in the previous version was too high for coarse mode particles when friction velocity is large, which underestimates surface PM10 concentration. The updated dry deposition scheme that is constrained by observations effectively improves PM10 performance by reducing the dry deposition velocity for coarse mode particles.

Role of Upwind Precipitation in Transboundary Pollution and Secondary Aerosol Formation: A Case Study during the KORUS-AQ Field Campaign

Abstract Clouds and precipitation play critical roles in wet removal of aerosols and soluble gases in the atmosphere, and hence their accurate prediction largely influences accurate prediction of air pollutants. In this study, the impacts of clouds and precipitation on wet scavenging and long-range transboundary transport of pollutants are examined during the 2016 Korea–United States Air Quality (KORUS-AQ) field campaign using the Weather Research and Forecasting Model coupled with chemistry. Two simulations—one in which atmospheric moisture is constrained and one in which it is not—are performed and evaluated against surface and airborne observations. The simulation with moisture constraints is found to better reproduce precipitation as well as surface PM2.5, whereas the areal extent and amount of precipitation are overpredicted in the simulation without moisture constraints. As a results of overpredicted clouds and precipitation and consequently overpredicted wet scavenging, PM2.5 concentration is generally underpredicted across the model domain in the simulation without moisture constraints. The effects are significant not only in the precipitating region (upwind region, southern China in this study) but also in the downwind region (South Korea) where no precipitation is observed. The difference in upwind precipitation by 77% on average between the two simulations leads to the difference in PM2.5 by ∼39% both in the upwind and downwind regions. The transboundary transport of aerosol precursors, especially nitric acid, has a considerable impact on ammonium-nitrate aerosol formation in the ammonia-rich downwind region. This study highlights that skillful prediction of atmospheric moisture can have ultimate potential to skillful prediction of aerosols across regions.

What rainfall rates are most important to wet removal of different aerosol types?

Abstract. Both frequency and intensity of rainfall affect aerosol wet deposition. With a stochastic deep convection scheme implemented into two state-of-the-art global climate models (GCMs), a recent study found that aerosol burdens are increased globally by reduced climatological mean wet removal of aerosols due to suppressed light rain. Motivated by their work, a novel approach is developed in this study to detect what rainfall rates are most efficient for wet removal (scavenging amount mode) of different aerosol species of different sizes in GCMs and applied to the National Center for Atmospheric Research Community Atmosphere Model version 5 (CAM5) with and without the stochastic convection cases. Results show that in the standard CAM5, no obvious differences in the scavenging amount mode are found among different aerosol types. However, the scavenging amount modes differ in the Aitken, accumulation and coarse modes, showing around 10–12, 8–9 and 7–8 mm d−1, respectively, over the tropics. As latitude increases poleward, the scavenging amount mode in each aerosol mode is decreased substantially. The scavenging amount mode is generally smaller over land than over ocean. With stochastic convection, the scavenging amount mode for all aerosol species in each mode is systematically increased, which is the most prominent along the Intertropical Convergence Zone, exceeding 20 mm d−1 for small particles. The scavenging amount modes in the two cases are both smaller than individual rainfall rates associated with the most accumulated rain (rainfall amount mode), further implying precipitation frequency is more important than precipitation intensity for aerosol wet removal. The notion of the scavenging amount mode can be applied to other GCMs to better understand the relation between rainfall and aerosol wet scavenging, which is important to better simulate aerosols.

An Improved Representation of Aerosol Wet Removal by Deep Convection and Impacts on Simulated Aerosol Vertical Profiles

AbstractWe introduce a physics‐based aerosol wet removal scheme with unified treatments of aerosol transport and removal by convective clouds into the Community Atmosphere Model version 6. Since several important physical processes are still neglected or poorly represented in this new physics‐based scheme, we develop secondary improvements to the parameterizations of aerosol activation, resuspension, and cloud‐borne aerosol detrainment in this new scheme. Changes in the aerosol wet removal scheme cause tropospheric aerosol concentrations to decrease to different extents: compared to the control run, the physics‐based scheme significantly decreases aerosol burdens by up to 60% over the southern Pacific Ocean, whereas the secondary improvements mitigate the decreasing tendency. The burden changes also depend on aerosol chemical components: the sulfate mass decrease is compensated by secondary production, black carbon (BC) is effectively removed via increasing the hygroscopicity of particulate organic matter from 0 to 0.2, and dust shows the most spatially heterogeneous changes. Simulated aerosol profiles are evaluated against aircraft‐based observations over the Pacific and Atlantic Oceans. The secondary‐improved scheme reduces the overestimations of upper tropospheric BC and sea salt concentrations by a factor of 10 and 1,000, respectively, and reproduces the dependence of BC mass decrease rates on cloud types. Consideration of convective cloud‐borne aerosol detrainment plays the most important role in enhancing the aerosol wet removal and decreasing the positive biases of tropospheric BC and sea salt concentrations. We also summarize unresolved issues related to convective cloud genesis and microphysics, cloud‐borne aerosol evolution, and BC and dust emissions.

An improved representation of aerosol wet removal by deep convection and impacts on simulated aerosol vertical profiles

An improved representation of aerosol wet removal by deep convection and impacts on simulated aerosol vertical profiles

FLEXPART v10.1 simulation of source contributions to Arctic black carbon

Abstract. The Arctic environment is undergoing rapid changes such as faster warming than the global average and exceptional melting of glaciers in Greenland. Black carbon (BC) particles, which are a short-lived climate pollutant, are one cause of Arctic warming and glacier melting. However, the sources of BC particles are still uncertain. We simulated the potential emission sensitivity of atmospheric BC present over the Arctic (north of 66∘ N) using the FLEXPART (FLEXible PARTicle) Lagrangian transport model (version 10.1). This version includes a new aerosol wet removal scheme, which better represents particle-scavenging processes than older versions did. Arctic BC at the surface (0–500 m) and high altitudes (4750–5250 m) is sensitive to emissions in high latitude (north of 60∘ N) and mid-latitude (30–60∘ N) regions, respectively. Geospatial sources of Arctic BC were quantified, with a focus on emissions from anthropogenic activities (including domestic biofuel burning) and open biomass burning (including agricultural burning in the open field) in 2010. We found that anthropogenic sources contributed 82 % and 83 % of annual Arctic BC at the surface and high altitudes, respectively. Arctic surface BC comes predominantly from anthropogenic emissions in Russia (56 %), with gas flaring from the Yamalo-Nenets Autonomous Okrug and Komi Republic being the main source (31 % of Arctic surface BC). These results highlight the need for regulations to control BC emissions from gas flaring to mitigate the rapid changes in the Arctic environment. In summer, combined open biomass burning in Siberia, Alaska, and Canada contributes 56 %–85 % (75 % on average) and 40 %–72 % (57 %) of Arctic BC at the surface and high altitudes, respectively. A large fraction (40 %) of BC in the Arctic at high altitudes comes from anthropogenic emissions in East Asia, which suggests that the rapidly growing economies of developing countries could have a non-negligible effect on the Arctic. To our knowledge, this is the first year-round evaluation of Arctic BC sources that has been performed using the new wet deposition scheme in FLEXPART. The study provides a scientific basis for actions to mitigate the rapidly changing Arctic environment.

Carbonaceous Aerosols Collected at the Observatory of Monte Curcio in the Southern Mediterranean Basin

This work provides the first continuous measurements of carbonaceous aerosol at the Global Atmosphere Watch (GAW) Monte Curcio regional station, within the southern Mediterranean basin. We specifically analyzed elemental carbon (EC) and organic carbon (OC) concentrations in particulate matter (PM) samples, collected from April to December during the two years of 2016 and 2017. The purpose of the study is to understand the behavior of both PM and carbonaceous species, in their fine and coarse size fraction, along with their seasonal variability. Based on 18 months of observations, we obtained a dataset that resulted in a vast range of variability. We found the maximum values in summer, mainly related to the enhanced formation of secondary pollutants owing to intense solar radiation, also due to the high frequency of wildfires in the surrounding areas, as well as to the reduced precipitation and aerosol-wet removal. We otherwise observed the lowest levels during fall, coinciding with well-ventilated conditions, low photochemical activity, higher precipitation amounts, and less frequency of Saharan dust episodes. We employed the HYSPLIT model to identify long-range transport from Saharan desert. We found that the Saharan dust events caused higher concentrations of PM and OC in the coarser size fraction whereas the wildfire events likely influenced the highest PM, OC, and EC concentrations we recorded for the finer fraction.

Enhanced land–sea warming contrast elevates aerosol pollution in a warmer world

Many climate models simulate an increase in anthropogenic aerosol species in response to warming1, particularly over the Northern Hemisphere mid-latitudes during June, July and August. Recently, it has been argued that this increase in anthropogenic aerosols can be linked to a decrease in wet removal associated with reduced precipitation2, but the mechanisms remain uncertain. Here, using a state-of-the-art climate model (the Community Atmosphere Model version 5), we expand on this notion to demonstrate that the enhanced aerosol burden and hydrological changes are related to a robust climate change phenomenon—the land–sea warming contrast3,4. Enhanced land warming is associated with continental reductions in lower-tropospheric humidity that drive decreases in low clouds—particularly large scale (stratus) clouds—which, in turn, lead to reduced large-scale precipitation and aerosol wet removal. Idealized model simulations further show that muting the land–sea warming contrast weakens these hydrological changes, thereby suppressing the aerosol increase. Moreover, idealized simulations that only feature land warming yield enhanced continental aridity and an increase in aerosol burden. Thus, unless anthropogenic emission reductions occur, our results add confidence that a warmer world will be associated with enhanced aerosol pollution. Greater land–sea temperature contrast under anthropogenic warming will enhance aerosol concentrations, reveal model simulations, linked to reductions in large-scale cloud cover and corresponding decreases in precipitation and aerosol wet removal.

A new aerosol wet removal scheme for the Lagrangian particle model FLEXPART v10

Abstract. A new, more physically based wet removal scheme for aerosols has been implemented in the Lagrangian particle dispersion model FLEXPART. It uses three-dimensional cloud water fields from the European Centre for Medium-Range Weather Forecasts (ECMWF) to determine cloud extent and distinguishes between in-cloud and below-cloud scavenging. The new in-cloud nucleation scavenging depends on cloud water phase (liquid, ice or mixed-phase), based on the aerosol's prescribed efficiency to serve as ice crystal nuclei and liquid water nuclei, respectively. The impaction scavenging scheme now parameterizes below-cloud removal as a function of aerosol particle size and precipitation type (snow or rain) and intensity.Sensitivity tests with the new scavenging scheme and comparisons with observational data were conducted for three distinct types of primary aerosols, which pose different challenges for modeling wet scavenging due to their differences in solubility, volatility and size distribution: (1) 137Cs released during the Fukushima nuclear accident attached mainly to highly soluble sulphate aerosol particles, (2) black carbon (BC) aerosol particles, and (3) mineral dust. Calculated e-folding lifetimes of accumulation mode aerosols for these three aerosol types were 11.7, 16.0, and 31.6 days respectively, when well mixed in the atmosphere. These are longer lifetimes than those obtained by the previous removal schem, and, for mineral dust in particular, primarily result from very slow in-cloud removal, which globally is the primary removal mechanism for these accumulation mode particles.Calculated e-folding lifetimes in FLEXPART also have a strong size dependence, with the longest lifetimes found for the accumulation-mode aerosols. For example, for dust particles emitted at the surface the lifetimes were 13.8 days for particles with 1 µm diameter and a few hours for 10 µm particles. A strong size dependence in below-cloud scavenging, combined with increased dry removal, is the primary reason for the shorter lifetimes of the larger particles. The most frequent removal is in-cloud scavenging (85 % of all scavenging events) but it occurs primarily in the free troposphere, while below-cloud removal is more frequent below 1000 m (52 % of all events) and can be important for the initial fate of species emitted at the surface, such as those examined here.For assumed realistic in-cloud removal efficiencies, both BC and sulphate have a slight overestimation of observed atmospheric concentrations (a factor of 1.6 and 1.2 respectively). However, this overestimation is largest close to the sources and thus appears more related to overestimated emissions rather than underestimated removal. The new aerosol wet removal scheme of FLEXPART incorporates more realistic information about clouds and aerosol properties and it compares better with both observed lifetimes and concentration than the old scheme.

Aerosol transport and wet scavenging in deep convective clouds: A case study and model evaluation using a multiple passive tracer analysis approach

AbstractWet scavenging of aerosols by continental deep convective clouds is studied for a supercell storm complex observed over Oklahoma during the Deep Convective Clouds and Chemistry campaign. A new passive‐tracer‐based transport analysis framework is developed to characterize convective transport using vertical profiles of several passive trace gases. For this case, the analysis estimates that observed passive gas mixing ratios in the upper troposphere convective outflow consist of 47% low level (<3 km) inflow air, 32% entrained midtroposphere air, and 21% upper troposphere air. The new analysis framework is used to estimate aerosol wet scavenging efficiencies. Observations yield high overall scavenging efficiencies of 81% for submicron aerosol mass. Organic, sulfate, and ammonium aerosols have similar wet scavenging efficiencies (80%–84%). The apparent scavenging efficiency for nitrate aerosol is much lower (57%), but the scavenging efficiency for nitrate aerosol plus nitric acid combined (84%) is close to the other species. Scavenging efficiencies for aerosol number are high for larger particles (84% for 0.15–2.5 µm diameter) but are lower for smaller particles (64% for 0.03–0.15 µm). The storm is simulated using the chemistry version of the Weather Research and Forecasting model. Compared to the observation‐based analysis, the standard model strongly underestimates aerosol scavenging efficiencies by 32% and 41% in absolute differences for submicron mass and number. Adding a new treatment of secondary activation significantly improves simulated aerosol scavenging, producing wet scavenging efficiencies that are only 7% and 8% lower than observed efficiencies. This finding emphasizes the importance of secondary activation for aerosol wet removal in deep convective storms.

Trends in aerosol optical depth over Indian region: Potential causes and impact indicators

AbstractThe first regional synthesis of long‐term (back to ~ 25 years at some stations) primary data (from direct measurement) on aerosol optical depth from the ARFINET (network of aerosol observatories established under the Aerosol Radiative Forcing over India (ARFI) project of Indian Space Research Organization over Indian subcontinent) have revealed a statistically significant increasing trend with a significant seasonal variability. Examining the current values of turbidity coefficients with those reported ~ 50 years ago reveals the phenomenal nature of the increase in aerosol loading. Seasonally, the rate of increase is consistently high during the dry months (December to March) over the entire region whereas the trends are rather inconsistent and weak during the premonsoon (April to May) and summer monsoon period (June to September). The trends in the spectral variation of aerosol optical depth (AOD) reveal the significance of anthropogenic activities on the increasing trend in AOD. Examining these with climate variables such as seasonal and regional rainfall, it is seen that the dry season depicts a decreasing trend in the total number of rainy days over the Indian region. The insignificant trend in AOD observed over the Indo‐Gangetic Plain, a regional hot spot of aerosols, during the premonsoon and summer monsoon season is mainly attributed to the competing effects of dust transport and wet removal of aerosols by the monsoon rain. Contributions of different aerosol chemical species to the total dust, simulated using Goddard Chemistry Aerosol Radiation and Transport model over the ARFINET stations, showed an increasing trend for all the anthropogenic components and a decreasing trend for dust, consistent with the inference deduced from trend in Angstrom exponent.

Sensitivity of remote aerosol distributions to representation of cloud–aerosol interactions in a global climate model

Abstract. Many global aerosol and climate models, including the widely used Community Atmosphere Model version 5 (CAM5), have large biases in predicting aerosols in remote regions such as the upper troposphere and high latitudes. In this study, we conduct CAM5 sensitivity simulations to understand the role of key processes associated with aerosol transformation and wet removal affecting the vertical and horizontal long-range transport of aerosols to the remote regions. Improvements are made to processes that are currently not well represented in CAM5, which are guided by surface and aircraft measurements together with results from a multi-scale aerosol–climate model that explicitly represents convection and aerosol–cloud interactions at cloud-resolving scales. We pay particular attention to black carbon (BC) due to its importance in the Earth system and the availability of measurements. We introduce into CAM5 a new unified scheme for convective transport and aerosol wet removal with explicit aerosol activation above convective cloud base. This new implementation reduces the excessive BC aloft to better simulate observed BC profiles that show decreasing mixing ratios in the mid- to upper-troposphere. After implementing this new unified convective scheme, we examine wet removal of submicron aerosols that occurs primarily through cloud processes. The wet removal depends strongly on the subgrid-scale liquid cloud fraction and the rate of conversion of liquid water to precipitation. These processes lead to very strong wet removal of BC and other aerosols over mid- to high latitudes during winter months. With our improvements, the Arctic BC burden has a 10-fold (5-fold) increase in the winter (summer) months, resulting in a much-better simulation of the BC seasonal cycle as well. Arctic sulphate and other aerosol species also increase but to a lesser extent. An explicit treatment of BC aging with slower aging assumptions produces an additional 30-fold (5-fold) increase in the Arctic winter (summer) BC burden. This BC aging treatment, however, has minimal effect on other underpredicted species. Interestingly, our modifications to CAM5 that aim at improving prediction of high-latitude and upper-tropospheric aerosols also produce much-better aerosol optical depth (AOD) over various other regions globally when compared to multi-year AERONET retrievals. The improved aerosol distributions have impacts on other aspects of CAM5, improving the simulation of global mean liquid water path and cloud forcing.

Size dependence of wet removal of black carbon aerosols during transport from the boundary layer to the free troposphere

Size distributions of black carbon (BC) measured by aircraft over East Asia in spring 2009 were highly correlated with BC transport efficiency in air parcels uplifted from the planetary boundary layer to the free troposphere. The average single‐particle BC mass decreased with decreasing transport efficiency, which suggests that aerosols containing larger BC mass were removed more efficiently. This is the first successful observation of the size‐dependent wet removal of aerosols, qualitatively consistent with the Köhler theory. The size distribution of BC uplifted to the free troposphere with high efficiency was similar to the size distribution of BC in the planetary boundary layer. Conversely, the size distribution of BC uplifted with low efficiency was similar to that of background air in the free troposphere. We conclude that wet removal during upward transport is important in controlling the size distribution of BC in the free troposphere.

Implications of droplet nucleation to mineral dust aerosol deposition and transport

Calculations from a microphysics model are shown which indicate the factors that control droplet nucleation scavenging of hydrophilic mineral dust particles over a large range of conditions including the size, chemical composition, and number density of particles in both cumulus and stratus clouds. We focus specifically on the activation threshold radius (ATR) for droplet nucleation which determines the particles that are activated and those available for further transport and subsequent iron deposition to the remote ocean. Results suggest: the ATR is typically found in the range of clay‐sized particles (radius = .1 to 1. μm), a spectrum over which the amount of dust removed declines ∼60% both in surface area and particle number; nucleation of silt‐sized particles (1.–10. μm) occurs under most conditions; larger fractions of mineral aerosols are removed in cumulus clouds than in stratus; and while acid coating of dust particles in polluted environments acts to decrease the ATR, the effect is reduced by competition with soluble aerosols. Regional mineral dust environments exhibit potentially diverse aerosol wet removal impacts. The ATR representative of the tropical Atlantic ocean basin (<.2 μm) indicates ∼80% removal of the total dust surface area, while in the pristine southern hemisphere mid latitudes an ATR ∼.5 μm implies ∼60%. In contrast, varying conditions in the polluted region of East Asia suggest a large ATR spectrum (.2 to 3. μm) with dust surface area removal ranging from >80% to <10%.