Wet Scavenging Research Articles

Changes in aerosol size distributions over the Indian Ocean during different meteorological conditions

Aerosol emissions in South Asia are large. The emitted aerosols can travel significant distances and, during the Asian southwest monsoon especially, are prone to modification through cloud processing and wet scavenging while being transported. The scale of emissions and transport means that the global climate impact of these aerosols are sensitive to modification en route, but the process-level understanding is still largely lacking. In this study, we analyse long-term aerosol data measured at an observatory established in Hanimaadhoo, Republic of Maldives, to investigate the long-term properties of aerosols over the Indian Ocean as well as to understand the effect of precipitation on the aerosol particle size distribution during long-range transport. The observatory location is ideal because it is a receptor site with little local influence, and, depending on the season, receives either polluted air masses coming from the Indian subcontinent or clean marine air masses from the Indian Ocean. We analysed the sub-micron particle number size distribution measured during the years 2004–2008, and 2014–2017, and this is the first inter-seasonal long-term study of the sub-micron aerosol features in the region. The aerosol origin and its relative exposure to wet scavenging during long-range transport were analysed using back-trajectory analysis from HYSPLIT. By comparing aerosol measurements to precipitation along its transport, this study shows that there is a substantial change in particle number size distributions and concentrations depending on the amount of rainfall during transport. During the southwest monsoon season, the aerosol size distribution was notably bi-modal and total particle concentrations clearly reduced in comparison with the prevailing aerosol size distribution during the northeast monsoon season. Precipitation during transport usually corresponded with a greater reduction in accumulation mode concentrations than for smaller sizes, and the shape of the median size distribution showed a clear dependence on the trajectory origin and route taken.

Aerosols in the E3SM Version 1: New Developments and Their Impacts on Radiative Forcing

AbstractThe new Energy Exascale Earth System Model Version 1 (E3SMv1) developed for the U.S. Department of Energy has significant new treatments of aerosols and light‐absorbing snow impurities as well as their interactions with clouds and radiation. This study describes seven sets of new aerosol‐related treatments (involving emissions, new particle formation, aerosol transport, wet scavenging and resuspension, and snow radiative transfer) and examines how they affect global aerosols and radiative forcing in E3SMv1. Altogether, they give a reduced total aerosol radiative forcing (−1.6 W/m2) and sensitivity in cloud liquid water to aerosols, but an increased sensitivity in cloud droplet size to aerosols. A new approach for H2SO4 production and loss largely reduces a low bias in small particles concentrations and leads to substantial increases in cloud condensation nuclei concentrations and cloud radiative cooling. Emitting secondary organic aerosol precursor gases from elevated sources increases the column burden of secondary organic aerosol, contributing substantially to global clear‐sky aerosol radiative cooling (−0.15 out of −0.5 W/m2). A new treatment of aerosol resuspension from evaporating precipitation, developed to remedy two shortcomings of the original treatment, produces a modest reduction in aerosols and cloud droplets; its impact depends strongly on the model physics and is much stronger in E3SM Version 0. New treatments of the mixing state and optical properties of snow impurities and snow grains introduce a positive present‐day shortwave radiative forcing (0.26 W/m2), but changes in aerosol transport and wet removal processes also affect the concentration and radiative forcing of light‐absorbing impurities in snow/ice.

Effects of Precipitation on Air Pollution in Spring and Summer in Lanzhou

Using hourly data to study the impact of precipitation on air pollutants and AQI in 2018 spring and summer in Lanzhou. The results show that precipitation has different scavenging capacity for air pollutants. The sorting capacity of precipitation for different pollutants is: SO2> PM10> NO2> O3> PM2.5> CO. Different levels of precipitation scavenging capacity is also different, heavy rain and micro rain had the best effect on PM10 removal, moderate rain and micro rain had better wet scavenging capacity for O3. Precipitation duration and precipitation are the key factors of pollutant removal capacity.

Investigating air pollutant concentrations, impact factors, and emission control strategies in western China by using a regional climate-chemistry model

In this study, in situ observations were conducted for six criteria air pollutants (PM2.5, PM10, SO2, NO2, CO, and O3) at 23 sites in western China for 1 year. Subsequently, the detailed Weather Research and Forecasting model coupled with Chemistry (WRF-Chem) results for the pollutants were determined. The WRF-Chem model provided a clear perspective on the spatiotemporal distribution of air pollutants. High pollutant concentrations were mainly observed over highly populated mega-city regions, such as Sichuan and Guanzhong basins, whereas low concentration levels were observed over the Tibetan Plateau (TP). The TP also showed an increased concentration of O3. Seasonally, all six pollutants except O3 exhibited high concentration values during winter and low values during summer. O3 concentrations exhibited an opposite seasonal variation in low-altitude regions. Unlike other pollutants that exhibited gradually decreasing concentrations with an increase in altitude, O3 concentrations revealed an increasing trend. Furthermore, NO2 concentrations gradually increased in the upper atmosphere possibly due to lighting and stratospheric transmission. Atmospheric pollution is closely related to emissions and meteorological variations in western China. Meteorological conditions in the summer are conducive to pollutant dispersion and wet scavenging; however, unfavourable weather conditions (high pressure as well as a low planetary boundary layer height and precipitation level) in the winter can further worsen air pollution. Atmospheric pollutants from various emission sectors generally exhibited varying monthly profiles. In six typical cities, pollutants were positively correlated with multiple emission sources except for industrial emissions. Further sensitivity simulations indicated that eliminating residential emissions resulted in the largest decrease (up to 70%) in PM2.5 and PM10 concentrations. The most significant reductions in the concentrations of SO2 and NO2 were achieved by eliminating industrial and transportation emissions, respectively. The outcomes of this study could be helpful for future studies on pollution formation mechanisms as well as environmental and health risk assessments in western China.

Multi-method determination of the below-cloud wet scavenging coefficients of aerosols in Beijing, China

Abstract. Wet scavenging is one of the most efficient processes for removing aerosols from the atmosphere. This process is not well constrained in chemical transport models (CTMs) due to a paucity of localized parameterization regarding the below-cloud wet scavenging coefficient (BWSC). Here we conducted field measurements of the BWSC during the Atmospheric Pollution and Human Health Beijing (APHH-Beijing) campaign of 2016. Notably, the observed BWSC values based on the updated aerosol mass balance agree well with another estimation technique, and they fall in a range of 10−5 s−1. The measurement in this winter campaign, combined with that in summer of 2014, supported an exponential power distribution of BWSCs with rainfall intensity. The observed parameters were also compared with both the theoretical calculations and modeling results. We found that the theoretical estimations can effectively characterize the observed BWSCs of aerosols with sizes smaller than 0.2 µm and larger than 2.5 µm. However, the theoretical estimations were an order of magnitude lower than observed BWSCs within 0.2–2.5 µm, a domain size range of urban aerosols. Such an underestimation of BWSC through a theoretical method has been confirmed not only in APHH-Beijing campaign but also in all the rainfall events in summer of 2014. Since the model calculations usually originated from the theoretical estimations with simplified scheme, the significantly lower BWSC could well explain the underprediction of wet depositions in polluted regions as reported by the Model Inter-Comparison Study for Asia (MICS-Asia) and the global assessment of the Task Force on Hemispheric Transport of Atmospheric Pollutants (TF-HTAP). The findings highlighted that the wet deposition module in the CTMs requires improvement based on field measurement estimation to construct a more reasonable simulation scheme for BWSC, especially in polluted regions.

Design of a rain-shower based cleaning system for simultaneous PM2.5 removal and CO2 capture of ambient air

The first solar assisted large scale cleaning system (SALSCS, 1st generation), consisting of a large flat-plate solar collector, a tower (chimney) and filter banks, was built in Xi’an, China for urban PM2.5 mitigation. Experimental results showed that the Xi’an SALSCS maintained a strong nature convective flow created by thermal buoyancy, drawing a large volume of PM2.5-laden ambient air towards the filter banks and the center of the tower. The polluted air was filtered before discharging from the top of the tower. While filtration method works well, it requires changing and disposing these filter wastes on a maintenance schedule. A modified 2nd generation SALSCS with 18 m × 18 m × 16 m was designed, in which the PM2.5 removal applies an analogous method to the natural rain scavenging. With this concept, a rain-shower based cleaning system utilizing falling water drops to remove the ambient PM2.5 was built at Yancheng Environmental Science Park, Jiangsu, China. In this system, there were a large array of spraying nozzles used to provide a sufficient residence time and high rainfall intensity to increase the collision frequency between incoming particles and falling droplets. Theoretical calculations showed that under flow speed of 0.2 m s−1 and using only 752 nozzles, the created sprays can remove PM2.5 by 35% in mass. Applying two layers of mesh screens to form water films to enhance the particle capture, experimental data showed an improved efficiency of 50%. Further increasing the number of nozzles and deployment area, the wet scavenging method is feasible to remove fine particles with much higher efficiency. In addition to the removal of PM2.5, an additional benefit of using the rain-shower technology is that if appropriate alkaline is dissolved in the water, the rain shower can also remove the precursor gases, e.g., adding NaOH for capturing CO2 to reduce the greenhouse gas in the atmosphere.

Characteristics and Variability of Carbonaceous Aerosols over a Semi Urban Location in Garhwal Himalayas

Extraction of organic carbon (OC) and elemental carbon (EC) were carried out over Srinagar, India, an ecologically sensitive semi-urban site in Garhwal Himalays. The PM2.5 sampling was carried out during January to December, 2017 over the site. The OC and EC were extracted from PM2.5 samples using a thermo optical OC/EC analyzer. Highest OC and EC concncentrations were found during postmonsoon (17.67 ± 1.1 μg/m3 OC and 6.34 ± 0.75 EC) and Winter (17.31 ± 3.045 μg/m3 OC and 6.32 ± 0.585 μg/m3 EC) seasons are attributed to boundary layer dynamics and anthropogenic activities. The lower concentration of OC/EC was observed during monsoon season (11.64 ± 1.75 μgm−3 OC and 3.46 ± 0.19μgm−3 EC) owing to wet scavenging of aerosols and minimum count of forest fire/biomass buring incidences. Both pre-monsoon and post-monsoon season concentrations are also influenced by biomass burning in the IGP (Indo-Gangetic Plain) region and forest fires in the adjecent areas. The OC/EC ratio sounds that vehicular exhaust and biomass burning are the major source of OC/EC over the site. Generation of secondary organic carbon (SOC) at the region causes variability in OC/EC ratio in different seasons. It is found that 24–32% of PM2.5 is contributed by carbonaceous aerosols (OC and EC) over Srinagar. The pivotal role of meteorology in modulating OC/EC concentrations has been illustared in detail.

Role of Cyclone “Ockhi” in the re-distribution of aerosols and its impact on the precipitation over the Arabian Sea

Abstract Tropical cyclone Ockhi, which matured into a very severe cyclonic storm (VSCS) in the southeast Arabian Sea, took atypical track over the Arabian Sea. Concurrently, an abrupt reduction in the precipitation rate, accompanied by weak updraft in the eye, was observed. The simultaneous presence of the capped inversion associated with the decreasing (increasing) convective available potential energy (convective inhibition) was observed after it matured into VSCS at 14:30 h local time on 1 December 2017. As cyclone Ockhi matured into VSCS, the major fraction of aerosols was pulled towards the cyclone from highly polluted Indo-Gangetic Plain. As a result, aerosol loading off the west coast and over Gujarat state during the intensifying and dissipating stages of cyclone Ockhi was found to be higher than during the mature stages, possibly due to lower wet scavenging arising from the capped inversion. Analysis of cloud microphysical properties revealed the presence of thicker convective tower clouds during the intensifying stages, associated with lower outgoing longwave radiation, while occurrence of towering high clouds reduced during mature and dissipating stages of the Cyclone Ockhi. This finding is substantiated by a narrow distribution of hydrometeors and the decreasing ice cloud effective radius with increasing altitude, which might have played a role in the reduced precipitation efficiency of cloud systems. These results have an important implication for re-distribution of aerosols and their impact on precipitation pattern under prevalent atmospheric circulation.

Characterization of Size-Resolved Hygroscopicity of Black Carbon-Containing Particle in Urban Environment.

The hygroscopic properties of BC-containing particles (BCc) are important to determine their wet scavenging, atmospheric lifetime, and interactions with clouds. Such information is still lacking in the real world because of the challenges in isolating BCc from other aerosols to be directly characterized. In this study, the size-resolved chemical components of BCc including the refractory BC core and associated coatings were measured by a soot particle-aerosol mass spectrometer in suburban Nanjing. The size-resolved hygroscopicity parameter of BCc (κBCc) was obtained based on this full chemical characterization of BCc. We found increased inorganic fraction and more oxidized organic coatings with thicker coatings, which modified κBCc besides the determinant of particle size. The bulk κBCc was observed to range from 0.11 to 0.34. The size-resolved κBCc consistently showed minima at coated diameter (Dcoated) of 100 nm, parametrized as κ(x) = 0.28-0.35 × exp(-0.004 × x), x = Dcoated. Under critical supersaturations (SS) of 0.1% and 0.2%, the D50 values of BCc were 200 ± 20 and 135 ± 18 nm, respectively. On average 33 ± 16% and 59 ± 20% of BCc in number could be activated at SS = 0.1% and 0.2%, respectively. These results provide constraints on surface CCN sources for the light-absorbing BC-containing particles.

The Observed Influence of Tropical Convection on the Saharan Dust Layer

AbstractInteractions between convection and the Saharan Air Layer in the tropical Atlantic Ocean are quantified using a novel compositing technique that leverages geostationary cloud observations to add temporal context to the polar orbiting CloudSat and the Cloud Aerosol Lidar and Infrared Pathfinder Satellite Observations (CALIPSO) satellites allowing aerosol optical depth (AOD) changes to be tracked throughout a typical convective storm life cycle. Four years of CALIPSO observations suggests that approximately 20% of the dust mass in every 10° longitude band between 10°W and 80°W is deposited into the ocean. Combining a new convective identification algorithm based on hourly geostationary cloud products with AODdust profiles along the CALIPSO track reveals that wet scavenging by convection is responsible for a significant fraction of this deposition across the Atlantic. Composites of 4 years of convective systems reveal that, on average, convection accounts for 15% ± 7% of the dust deposition in each longitude band relative to preconvective amounts, implying that dry deposition and scavenging by nonconvective events are responsible for the remaining 85% of dust removal. In addition, dust layers are detrained at upper levels of the atmosphere between 8 and 12 km by convective storms across the Atlantic. The dust budget analysis presented here indicates that convection lofts 1.5% ± 0.6% of dust aerosol mass to altitudes greater than 6 km. This may have significant implications for cloud formation downstream of convection since lofted dust particles can act as effective ice nucleating particles, altering cloud microphysical and radiative properties, latent heating, and precipitation rates.

Satellite inference of water vapour and above-cloud aerosol combined effect on radiative budget and cloud-top processes in the southeastern Atlantic Ocean

Abstract. Aerosols have a direct effect on the Earth's radiative budget and can also affect cloud development and lifetime, and the aerosols above clouds (AAC) are particularly associated with high uncertainties in global climate models. Therefore, it is a prerequisite to improve the description and understanding of these situations. During the austral winter, large loadings of biomass burning aerosols originating from fires in the southern African subcontinent are lifted and transported westwards, across the southeastern Atlantic Ocean. The negligible wet scavenging of these absorbing aerosols leads to a near-persistent smoke layer above one of the largest stratocumulus cloud decks on the planet. Therefore, the southeastern Atlantic region is a very important area for studying the impact of above-cloud absorbing aerosols, their radiative forcing and their possible effects on clouds. In this study we aim to analyse and quantify the effect of smoke loadings on cloud properties using a synergy of different remote sensing techniques from A-Train retrievals (methods based on the passive instruments POLDER and MODIS and the operational method of the spaceborne lidar CALIOP), collocated with ERA-Interim re-analysis meteorological profiles. To analyse the possible mechanisms of AAC effects on cloud properties, we developed a high and low aerosol loading approach, which consists in evaluating the change in radiative quantities (i.e. cloud-top cooling, heating rate vertical profiles) and cloud properties with the smoke loading. During this analysis, we account for the variation in the meteorological conditions over our sample area by selecting the months associated with one meteorological regime (June–August). The results show that the region we focus on is primarily under the energetic influence of absorbing aerosols, leading to a significant positive shortwave direct effect at the top of the atmosphere. For larger loads of AACs, clouds are optically thicker, with an increase in liquid water path of 20 g m−2 and lower cloud-top altitudes by 100 m. These results do not contradict the semi-direct effect of above-cloud aerosols, explored in previous studies. Furthermore, we observe a strong covariance between the aerosol and the water vapour loadings, which has to be accounted for. A detailed analysis of the heating rate profiles shows that within the smoke layer, the absorbing aerosols are 90 % responsible for warming the ambient air by approximately 5.7 K d−1. The accompanying water vapour, however, has a longwave effect at distance on the cloud top, reducing its cooling by approximately 4.7 K d−1 (equivalent to 7 %). We infer that this decreased cloud-top cooling in particular, in addition with the higher humidity above the clouds, might modify the cloud-top entrainment rate and its effect, leading to thicker clouds. Therefore, smoke (the combination of aerosol and water vapour) events would have the potential to modify and probably reinforce the underlaying cloud cover.

Fossil fuel combustion and biomass burning sources of global black carbon from GEOS-Chem simulation and carbon isotope measurements

Abstract. We identify sources (fossil fuel combustion versus biomass burning) of black carbon (BC) in the atmosphere and in deposition using a global 3-D chemical transport model GEOS-Chem. We validate the simulated sources against carbon isotope measurements of BC around the globe and find that the model reproduces mean biomass burning contribution (fbb; %) in various regions within a factor of 2 (except in Europe, where fbb is underestimated by 63 %). GEOS-Chem shows that contribution from biomass burning in the Northern Hemisphere (fbb: 35±14 %) is much less than that in the Southern Hemisphere (50±11 %). The largest atmospheric fbb is in Africa (64±20 %). Comparable contributions from biomass burning and fossil fuel combustion are found in southern (S) Asia (53±10 %), southeastern (SE) Asia (53±11 %), S America (47±14 %), the S Pacific (47±7 %), Australia (53±14 %) and the Antarctic (51±2 %). fbb is relatively small in eastern Asia (40±13 %), Siberia (35±8 %), the Arctic (33±6 %), Canada (31±7 %), the US (25±4 %) and Europe (19±7 %). Both observations and model results suggest that atmospheric fbb is higher in summer (59 %–78 %, varying with sub-regions) than in winter (28 %–32 %) in the Arctic, while it is higher in winter (42 %–58 %) and lower in summer (16 %–42 %) over the Himalayan–Tibetan Plateau. The seasonal variations of Atmosphericfbb are relatively flat in North America, Europe and Asia. We conducted four experiments to investigate the uncertainties associated with biofuel emissions, hygroscopicity of BC in fresh emissions, the aging rate and size-resolved wet scavenging. We find that doubling biofuel emissions for domestic heating north of 45∘ N increases fbb values in Europe in winter by ∼30 %, reducing the discrepancy between observed and modeled atmospheric fbb from −63 % to −54 %. The remaining large negative discrepancy between model and observations suggests that the biofuel emissions are probably still underestimated at high latitudes. Increasing the fraction of thickly coated hydrophilic BC from 20 % to 70 % in fresh biomass burning plumes increases the fraction of hydrophilic BC in biomass burning plumes by 0 %–20 % (varying with seasons and regions) and thereby reduces atmospheric fbb by up to 11 %. Faster aging (4 h e-folding time versus 1.15 d e-folding time) of BC in biomass burning plumes reduces atmospheric fbb by 7 % (1 %–14 %, varying with seasons and regions), with the largest reduction in remote regions, such as the Arctic, the Antarctic and the S Pacific. Using size-resolved scavenging accelerates scavenging of BC particles in both fossil fuel and biomass burning plumes, with a faster scavenging of BC in fossil fuel plumes. Thus, atmospheric fbb increases in most regions by 1 %–14 %. Overall, atmospheric fbb is determined mainly by fbb in emissions and, to a lesser extent, by atmospheric processes, such as aging and scavenging. This confirms the assumption that fbb in local emissions determines atmospheric fbb in previous studies, which compared measured atmospheric fbb directly with local fbb in bottom-up emission inventories.

On the nature of sea salt aerosol at a coastal megacity: Insights from Manila, Philippines in Southeast Asia

This study utilizes multiple aerosol datasets collected in Metro Manila, Philippines to investigate sea salt aerosol characteristics. This coastal megacity allows for an examination of the impacts of precipitation and mixing of different air masses on sea salt properties, including overall concentration and size-resolved composition, hygroscopicity, and morphology. Intensive size-resolved measurements with a Micro-Orifice Uniform Deposit Impactor (MOUDI) between July–December 2018 revealed the following major results: (i) sea salt levels exhibit wide variability during the wet season, driven primarily by precipitation scavenging; (ii) ssNa+ and Cl− peaked in concentration between 1.8 and 5.6 μm, with Cl− depletion varying between 21.3 and 90.7%; (iii) mixing of marine and anthropogenic air masses yielded complex non-spherical shapes with species attached to the outer edges and Na+ uniformly distributed across particles unlike Cl−; (iv) there was significant contamination of sea salt aerosol by a variety of crustal and anthropogenic pollutants (Fe, Al, Ba, Mn, Pb, NO3−, V, Zn, NH4+); (v) categorization of samples in five different pollutant type categories (Background, Clean, Fire, Continental Pollution, Highest Rain) revealed significant differences in overall Cl− depletion with enhanced depletion in the submicrometer range versus the supermicrometer range; (vi) κ values ranged from 0.02 to 0.31 with a bimodal profile across all stages, with the highest value coincident with the highest sea salt volume fraction in the 3.2–5.6 μm stage, which is far lower than pure sea salt due to the significant influence of organics and black carbon. Analysis of longer term PM2.5 (particulate matter with aerodynamic diameter less than 2.5 μm) and PMcoarse (= PM10 – PM2.5) data between August 2005 and October 2007 confirmed findings from the MOUDI data that more Cl− depletion occurred both in the wet season versus the dry season and on weekdays versus weekend days. This study demonstrates the importance of accounting for two factors in future studies on sea salt: (i) non-sea salt (nss) sources of Na+ impact calculations such as for Cl− depletion that typically assume that total Na+ concentration is derived from salt; and (ii) considering precipitation data over a larger spatial domain rather than a point measurement at the study site to investigate wet scavenging.

Size-resolved composition and morphology of particulate matter during the southwest monsoon in Metro Manila, Philippines

Abstract. This paper presents novel results from size-resolved particulate matter (PM) mass, composition, and morphology measurements conducted during the 2018 southwest monsoon (SWM) season in Metro Manila, Philippines. Micro-orifice uniform deposit impactors (MOUDIs) were used to collect PM sample sets composed of size-resolved measurements at the following aerodynamic cut-point diameters (Dp): 18, 10, 5.6, 3.2, 1.8, 1.0, 0.56, 0.32, 0.18, 0.10, and 0.056 µm. Each sample set was analyzed for composition of the water-soluble fraction. Analysis for mass was carried out on two sample sets, whereas black carbon (BC) and morphology analysis were analyzed on a single sample set. The bulk of the PM mass was between 0.18 and 1.0 µm with a dominant mode between 0.32 and 0.56 µm. Similarly, most of the black carbon (BC) mass was found between 0.10 and 1.0 µm, peaking between 0.18 and 0.32 µm. These peaks are located in the Greenfield gap, or the size range between 0.10 and 1.0 µm, where wet scavenging by rain is relatively inefficient. In the range between 0.10 and 0.18 µm, BC constituted 78.1 % of the measured mass. Comparable contributions of BC (26.9 %) and the water-soluble fraction (33.4 %) to total PM were observed and most of the unresolved mass, which amounted to 39.6 % in total, was for diameters exceeding 0.32 µm. The water-soluble ions and elements exhibited an average combined concentration of 8.53 µg m−3, with SO42-, NH4+, NO3-, Na+, and Cl− as the major contributors. Positive matrix factorization (PMF) was applied to identify the possible aerosol sources and estimate their contribution to the water-soluble fraction of collected PM. The factor with the highest contribution was attributed to “aged aerosol” (48.0 %), while “sea salt” (22.5 %) and “combustion” emissions (18.7 %) had comparable contributions. “Vehicular/resuspended dust” (5.6 %) and “waste processing” emissions (5.1 %) were also identified. Microscopy analysis highlighted the ubiquity of nonspherical particles regardless of size, which is significant when considering calculations of parameters such as single scattering albedo, the asymmetry parameter, and the extinction efficiency. The significant influence from aged aerosol to Metro Manila during the SWM season indicates that local sources in this megacity do not fully govern this coastal area's aerosol properties. The fact that the majority of the regional aerosol mass burden is accounted for by BC and other insoluble components has important downstream effects on the aerosol hygroscopic properties, which depend on composition. The results are relevant for understanding the impacts of monsoonal features on size-resolved aerosol properties, notably aqueous processing and wet scavenging. Finally, the results of this work provide contextual data for future sampling campaigns in Southeast Asia such as the airborne component of the Cloud, Aerosol, and Monsoon Processes Philippines Experiment (CAMP2Ex) planned for the SWM season in 2019.

PM10 carbonaceous aerosols and their real-time wet scavenging during monsoon and non-monsoon seasons at Delhi, India

Real-time simultaneous measurements of rainwater and PM10 chemistry were carried out at Delhi during the year 2016–17 in order to assess the levels of carbonaceous species and their wet scavenging during monsoon and non-monsoon seasons at Delhi. The PM10 samples were collected Before Rain (BR), During Rain (DR) and After Rain (AR) events, while rainwater samples collected on an event basis. The ambient OC levels were always higher than the levels of EC during both monsoon and non-monsoon seasons in ambient aerosol as well as in rainwater. On an average, during rain (DR) 30% of OC aerosols and 28.2% of EC aerosols removed via wet scavenging process. In after rain (AR), 26.2% OC and 1.8% EC aerosols further decreased in comparison to DR samples due to the presence of OC and EC free air parcel. Overall it observed that the OC concentration significantly lowered from BR to DR and AR. However, EC concentrations in AR were found to be higher than DR samples indicating their build-up after the rains. The Scavenging Ratios (SRs) of OC and rain intensity had a significant positive correlation, whereas the SRs of EC showed a weak correlation with rain intensity. The SRs of EC were significantly higher during non-monsoon as compared to monsoon season. Such characteristics can be explained based on the particles size, source and the hygroscopicity of both types of carbonaceous aerosol.

Deposition of Organic and Black Carbon: Direct Measurements at Three Remote Stations in the Himalayas and Tibetan Plateau

AbstractCarbonaceous matter in the atmosphere has an important influence on climate change. Currently, the deposition of carbonaceous matter is one of the largest uncertainties in the climate system. This phenomenon is common in remote regions, such as the Himalayas and Tibetan Plateau. In this study, for the first time, we reported in situ measurements of wet and dry deposition rates of carbonaceous matter at three remote stations: Nam Co, Lulang, and Everest. The results showed that the annual wet deposition rates of water‐insoluble organic carbon (WIOC) and black carbon (BC) were 60.2 and 5.8 mg·m−2·year−1, 330 and 34.6 mg·m−2·year−1, and 47.0 and 2.6 mg·m−2·year−1 at the Nam Co, Lulang, and Everest stations, respectively. Seasonal variations in the wet deposition rates of WIOC and BC were controlled by precipitation amount and their atmospheric concentrations. In addition, the wet scavenging ratios of WIOC and BC at Nam Co Station were close to those observed in other remote areas. The total BC deposition at Nam Co Station (15.3 mg·m−2·year−1) was higher than that from chemical transport models, implying a dominant role of dry deposition of BC in the total deposition at this station and an urgent need to improve the aerosol deposition in models for the Himalayas and Tibetan Plateau. It was found that the deposition rates of carbonaceous matter in the Himalayas and Tibetan Plateau had large spatial variation; thus, high‐resolution models need to be applied in the future.

Revised treatment of wet scavenging processes dramatically improves GEOS-Chem 12.0.0 simulations of surface nitric acid, nitrate, and ammonium over the United States

Abstract. The widely used community model GEOS-Chem 12.0.0 and previous versions have been recognized to significantly overestimate the concentrations of gaseous nitric acid, aerosol nitrate, and aerosol ammonium over the United States. The concentrations of nitric acid are also significantly overpredicted in most global models participating in a recent model intercomparison study. In this study, we show that most or all of this overestimation issue appears to be associated with wet scavenging processes. The replacement of constant in-cloud condensation water (ICCW) assumed in GEOS-Chem standard versions with one varying with location and time from the assimilated meteorology significantly reduces mass loadings of nitrate and ammonium during the wintertime, while the employment of an empirical washout rate for nitric acid significantly decreases mass concentrations of nitric acid and ammonium during the summertime. Compared to the standard version, GEOS-Chem with updated ICCW and washout rate significantly reduces the simulated annual mean mass concentrations of nitric acid, nitrate, and ammonium at surface monitoring network sites in the US from 2.04 to 1.03, 1.89 to 0.88, and 1.09 to 0.68 µg m−3, respectively, in much better agreement with corresponding observed values of 0.83, 0.70, and 0.60 µg m−3, respectively. In addition, the agreement of model-simulated seasonal variations of corresponding species with measurements is also improved. The updated wet scavenging scheme improves the skill of the model in predicting nitric acid, nitrate, and ammonium concentrations, which are important species for air quality and climate.

Observed Interactions Between Black Carbon and Hydrometeor During Wet Scavenging in Mixed‐Phase Clouds

AbstractWet scavenging of black carbon (BC) has been subject to large uncertainty, which importantly determines its atmospheric lifetime and indirect forcing impact on cloud microphysics. This study reveals the complex BC‐hydrometeor interactions in mixed‐phase clouds via single particle measurements in the real‐world environment, by capturing precipitation processes throughout cloud formation, cold rain/graupel, and subsequent snow events at a mountain site influenced by anthropogenic sources in wintertime. We found highly efficient BC wet scavenging during cloud formation, with large and thickly coated BC preferentially incorporated into droplets. During snow processes, BC core sizes in the interstitial phase steadily increased. A mechanism was proposed whereby the BC mass within each droplet was accumulated through droplet collision, leading to larger BC cores, which were then released back to the interstitial air through the Wegener‐Bergeron‐Findeisen processes when ice dominated. These results provide fundamental basis for constraining BC wet scavenging.

Strengthened Indian Summer Monsoon Precipitation Susceptibility Linked to Dust‐Induced Ice Cloud Modification

AbstractA growing body of research has underscored the radiative impact of mineral dust in influencing Indian summer monsoon rainfall variability. However, the various aerosol‐cloud‐precipitation interaction mechanisms remain poorly understood. Here we analyze multisatellite observations to examine dust‐induced modification in ice clouds and precipitation susceptibility. We show contrasting dust‐induced changes in ice cloud regimes wherein despite a 25% reduction in ice particle radius in thin ice clouds, we find ~40% increase in ice particle radius and ice water path in thick ice clouds resulting in the cloud deepening and subsequently strengthened precipitation susceptibility, under strong updraft regimes. The observed dust‐ice cloud‐precipitation interactions are supported by a strong correlation between the interannual monsoon rainfall variability and dust frequency. This microphysical‐dynamical coupling appears to provide negative feedback to aerosol‐cloud interactions, which acts to buffer enhanced aerosol wet scavenging. Our results underscore the importance of incorporating meteorological regime‐dependent dust‐ice cloud‐precipitation interactions in climate simulations.

Wet Scavenging in WRF‐Chem Simulations of Parameterized Convection for a Severe Storm During the DC3 Field Campaign

AbstractDeep convection can transport surface moisture and pollution from the planetary boundary layer to the upper troposphere (UT) within a few minutes. The convective transport of precursors of both ozone and aerosols from the planetary boundary layer affects the concentrations of these constituents in the UT and can influence the Earth's radiation budget and climate. Some precursors of both ozone and aerosols are soluble and reactive in the aqueous phase. This study uses the Weather Research and Forecasting model coupled with Chemistry (WRF‐Chem) to simulate the wet scavenging of precursors of both ozone and aerosols including CH2O, CH3OOH, H2O2, and SO2 in a supercell system observed on 29 May 2012, during the 2012 Deep Convective Clouds and Chemistry (DC3) field campaign at cloud‐parameterized resolution. The default WRF‐Chem simulations underestimate the mixing ratios of soluble ozone precursors in the UT because the dissolved soluble trace gases are not released when the droplets freeze. In order to improve the model simulation of cloud‐parameterized wet scavenging, we added ice retention factors for various species to the cloud‐parameterized wet scavenging module and adjusted the conversion rate of cloud water to rainwater at temperatures below freezing in the cloud parameterization as well as in the subgrid‐scale wet‐scavenging calculation. The introduction of these model modifications greatly improved the model simulation of less soluble species.