Coarse Mode Research Articles

Methylene Blue Active Substances (MBAS) and Linear Alkylbenzene Sulphonates (LAS) in Urban and Suburban Atmospheric Aerosol

Surfactant is one of the pollutants derived from atmospheric aerosol that can adversely affect the human health and environment. This study aims to characterize the level of anionic surfactants as Methylene Blue Active Substances (MBAS) and Linear Alkylbenzene Sulphonates (LAS) extracted from atmospheric aerosol from urban (Kuala Lumpur) and suburban (Bangi) area of Malaysia. For aerosol sampling, a high volume sampler (HVAS) with a cascade impactor was used to collect atmospheric aerosol sample according to particle size (coarse mode (> 1.5 µm) and fine mode (< 1.5 µm)). The level of MBAS was determined using UV-Vis Spectrophotometer based on colorimetric method, while the concentration of LAS was determined using High-Performance Liquid Chromatography (HPLC). Results showed that the composition of MBAS and LAS for both sampling stations was dominated by fine mode particles compared to coarse mode with a significant difference (p < 0.05). Kuala Lumpur showed higher concentration of MBAS (81.69 ± 13.01 ng m^-3) compared to LAS (2.96 ± 1.22 ng m^-3), while Bangi recorded lower level of both MBAS and LAS (44.58 ± 10.05 ng m^-3, 2.48 ± 1.28 ng m^-3), respectively. In terms of monsoonal effect, the highest level of surfactants as MBAS and LAS in both stations was recorded during southwest monsoon. A positive correlation was detected between MBAS and LAS. However, it was not significantly correlated (p > 0.05). From this study, it can be concluded that MBAS concentrations in urban and suburban atmosphere are not fully affected by commercial LAS. Majority of MBAS may be presented from other natural activities and anthropogenic sources such as motor vehicle emission, combustion of biomass, and the earth's crust. The management of surfactants' use needs to be reconsidered to enhance a better atmosphere especially in urban and suburban area in the future.

Impacts of the Variations of Aerosols Components and Relative Humidity on the Visibility and Particles Size Distribution of the Desert Atmosphere

This paper investigates the Impact of relative humidity, varying the concentrations of water-soluble aerosol particle concentrations (WASO), Mineral Nuclei Mode Aerosols Particle Concentration (MINN), mineral accumulation mode, nonspherical (MIAN) aerosol particles concentrations and Mineral Coarse Mode Aerosols Particle Concentration (MICN) on the visibility and particles size distribution of desert aerosols based on microphysical properties of desert aerosols. The microphysical properties (the extinction coefficients, volume mix ratios, dry mode radii and wet mode radii) were extracted from Optical Properties of Aerosols and Clouds (OPAC 4.0) at eight relative humidities, RHs (00 to 99%) and at the spectral visible range of 0.4-0.8mm, the concentrations were varied to obtain five different models for each above-mentioned component. Regression analysis of some standard equations were used to determine the Angstrom exponent (α), the turbidity coefficient (β), the curvature (α2), humidification factor (), the mean exponent of aerosol growth curve (µ) and the mean exponent of aerosol size distributions (n). The values of angstrom exponent (α) were observed to be less than 1 throughout the five models at all RHs for the four studied components, and this signifies the dominance of coarse mode particles over fine mode particles. But the magnitude of the angstrom exponent (α) fluctuates all through the studied components except for WASO which increased with the increase in RH across the models and this also signifies the dominance of coarse mode particles with some traces of fine mode particles. The investigation also revealed that the curvature (α2) has both monomodal (negative signs) and bimodal (positive signs) types of distributions all through the five models and this also signifies the dominance of coarse mode particles with some traces of fine mode particles across the individual models for all the studied components. it was also found that the visibility decreased with the increase in RH and increased with the increase in wavelength. The investigation further revealed that the turbidity coefficient (β) fluctuates with the increase in RH and the particles concentrations, and this might be due to major coagulation and sedimentation. The analysis further found that there is a direct inverse power relation between the humidification factor and the mean exponent of aerosols size distribution with the mean exponent of aerosols growth curve. It was also found that as the magnitude of µ increased for MIAN, MINN and MICN, the effective hygroscopic growth decreased. For WASO, it was found that as the magnitude of µ decreased, the effective hygroscopic growth increased with the increase in particles concentrations and RH. The decreased in the magnitude of µ for WASO might be due to the fact that as we increase the non-hygroscopic particles, we decrease the deliquescence. The mean exponent of aerosol size distribution (n) being less than 3 shows foggy condition of the desert atmosphere the four investigated components and five studied models.

Long-term trend of wintertime precipitation chemistry at a remote islet site influenced by anthropogenic emissions from continental East Asia

In this study, the trends and factors influencing wintertime precipitation chemistry at a remote site downwind of continental East Asia were investigated. A total of 336 precipitation samples were collected from 2005 to 2019 at Pengjia Islet, a site ~56 km north of the main island of Taiwan. Overall, the samples had a volume-weighted mean pH of 4.81 (ranging from 3.03 to 7.00), with 74% of samples considered as acid rain (pH < 5). PMF analysis of the samples identified sea-salt, anthropogenic emissions, and dust as sources of major ions in precipitation. Anthropogenic emissions were mostly associated with polluted air from East Asia. Four major air mass transport pathways to Pengjia Islet were identified, in which 87% originated from northern China (i.e. polluted air masses) with a relatively low pH and high ionic concentrations compared to the remaining samples. Wintertime pH values associated with the most common trajectory from China significantly increased at a rate of +1.7% yr−1 (p < 0.01) from 2005 to 2019, similar to those observed at other sites in East Asia in the previous two decades. The increasing pH trend in this study was attributed to the decrease in nss-SO42- concentrations and an increase in Ca2+ concentrations, of which the former aligns with the decrease in nss-SO42- at sites in China caused by the decline of SO2 emissions. The increase of Ca2+ concentrations is supported by the increase of coarse mode aerosol mass concentrations transported to northern Taiwan in winter. By splitting the dataset into two periods (i.e. 2005-2011 and 2012–2019), we found a close relationship between the changes in air-quality control in China and trends in precipitation chemistry at Pengjia Islet, including a consistently decreasing nss-SO42-/NO3− ratio in rainwater. Such a finding has important implications for the effectiveness of air pollution control policies on the regional scale. Additionally, changes in regional transport patterns of air masses might also contribute to the changes in precipitation chemistry at Pengjia Islet.

Spatial distribution of the size-fractional PNC and Pedestrian exposure to PM at an urban signalized intersection

To evaluate the respiratory health risk of pedestrians at signalized intersections, it is crucial to accurately investigate their spatial distribution of particulate matter (PM) in the air and the respiratory exposure dose to the public. The particle number concentrations (PNCs) of different sizes (10–2500 nm) along the horizontal and vertical vibrations of the intersection were measured in Xi'an, China, and the respiratory deposition dose (RDD) rate of pedestrians was calculated to estimate the pedestrian exposure level. The mean PNC at the intersection's entrance (1.59 × 104 # cm−3) was larger than at its exit (1.34 × 104 # cm−3) irrespective of the particle mode. At the exit, moreover, the PNC values decreased exponentially with increasing distance from the parking baseline of the intersection, while no such damping characterized the entrance to it. Concerning the vertical vibration of the intersection, both nucleation and Aitken modes of PNC peaked at a 0.4-m height and the maximum PNC in the accumulation mode and coarse mode appeared at a height of 3.4–4.5 m. Average RDD rate at the signalized intersection's entrance and exit was respectively 8.103 μg h−1 and 7.523 μg h−1. For this same intersection, the highest PM exposure dose was 8.444 μg h−1 for the elderly, followed by 8.061 μg h−1 for adults, and 3.221 μg h−1 for children.

Retrieval of aerosol microphysical properties from atmospheric lidar sounding: an investigation using synthetic measurements and data from the ACEPOL campaign

Abstract. This study presents an investigation of aerosol microphysical retrievals from high spectral resolution lidar (HSRL) measurements. Firstly, retrievals are presented for synthetically generated lidar measurements, followed by an application of the retrieval algorithm to real lidar measurements. Here, we perform the investigation for an aerosol state vector that is typically used in multi-angle polarimeter (MAP) retrievals, so that the results can be interpreted in relation to a potential combination of lidar and MAP measurements. These state vectors correspond to a bimodal size distribution, where column number, effective radius, and effective variance of both modes are treated as fit parameters, alongside the complex refractive index and particle shape. The focus is primarily on a lidar configuration based on that of the High Spectral Resolution Lidar-2 (HSRL-2), which participated in the ACEPOL (Aerosol Characterization from Polarimeter and Lidar) campaign, a combined project between NASA and SRON (Netherlands Institute for Space Research). The measurement campaign took place between October and November 2017, over the western region of the USA. Six different instruments were mounted on the aeroplane: four MAPs and two lidar instruments, HSRL-2 and the Cloud Physics Lidar (CPL). Most of the flights were carried out over land, passing over scenes with a low aerosol load. One of the flights passed over a prescribed forest fire in Arizona on 9 November, with a relatively higher aerosol optical depth (AOD), and it is the data from this flight that are focussed on in this study. A retrieval of the aerosol microphysical properties of the smoke plume mixture was attempted with the data from HSRL-2 and compared with a retrieval from the MAPs carried out in previous work pertaining to the ACEPOL data. The synthetic HSRL-2 retrievals resulted for the fine mode in a mean absolute error (MAE) of 0.038 (0.025) µm for the effective radius (with a mean truth value of 0.195 µm), 0.052 (0.037) for the real refractive index, 0.010 (7.20×10-3) for the imaginary part of the refractive index, 0.109 (0.071) for the spherical fraction, and 0.054 (0.039) for the AOD at 532 nm, where the retrievals inside brackets indicate the MAE for noise-free retrievals. For the coarse mode, we find the MAE is 0.459 (0.254) µm for the effective radius (with a mean truth value of 1.970 µm), 0.085 (0.075) for the real refractive index, 2.06×10-4 (1.90×10-4) for the imaginary component, 0.120 (0.090) for the spherical fraction, and 0.051 (0.039) for the AOD. A study of the sensitivity of retrievals to the choice of prior and first guess showed that, on average, the retrieval errors increase when the prior deviates too much from the truth value. These experiments revealed that the measurements primarily contain information on the size and shape of the aerosol, along with the column number. Some information on the real component of the refractive index is also present, with the measurements providing little on absorption or on the effective variance of the aerosol distribution, as both of these were shown to depend heavily on the choice of prior. Retrievals using the HSRL-2 smoke-plume data yielded, for the fine mode, an effective radius of 0.107 µm, a real refractive index of 1.561, an imaginary component of refractive index of 0.010, a spherical fraction of 0.719, and an AOD at 532 nm of 0.505. Additionally, the single-scattering albedo (SSA) from the HSRL-2 retrievals was 0.940. Overall, these results are in good agreement with those from the Spectropolarimeter for Planetary Exploration (SPEX) and Research Scanning Polarimeter (RSP) retrievals.

Concentrations and size-distributions of water-soluble inorganic and organic species on aerosols over the Arctic Ocean observed during the US GEOTRACES Western Arctic Cruise GN01

Marine aerosols affect the climate directly and indirectly as well as serving as tracers of biogenic processes. Here we present the results from size-segregated and bulk aerosol samples collected from 2nd August to 10th October 2015 during the US GEOTRACES Arctic Ocean (GN01) expedition. Samples were analyzed for concentrations of major water-soluble organic and inorganic species, including acetate, formate, methanesulfonate (MSA), oxalate, propionate, chloride, nitrate, sulfate and major cations (Na+, K+, Mg2+, Ca2+, NH4+). Back-trajectory analysis was performed to categorize the wind patterns into three types; type 1, originating from the North Pacific and the Bering Sea, type–2, consisting entirely of marine Arctic air, and type 3, consisting of marine Arctic air mixed with air masses from the surrounding continents. Sea-salt was the major aerosol component, dominating in the coarse mode, 1.8–5.6 μm. Non-sea-salt sulfate and MSA were predominantly present in the fine mode, 0.18–0.32 μm, and MSA was associated with type 1 and type 2 air masses. The results from this study provide useful information on the origins and chemical processes involving these aerosol species over the Arctic in summer and help elucidate the significance of natural sources as contributors for the formation of cloud condensation nuclei.

Overview of the SLOPE I and II campaigns: aerosol properties retrieved with lidar and sun–sky photometer measurements

Abstract. The Sierra Nevada Lidar aerOsol Profiling Experiment I and II (SLOPE I and II) campaigns were intended to determine the vertical structure of aerosols by remote sensing instruments and test the various retrieval schemes for obtaining aerosol microphysical and optical properties with in situ measurements. The SLOPE I and II campaigns were developed during the summers of 2016 and 2017, respectively, combining active and passive remote sensing with in situ measurements at stations belonging to the AGORA observatory (Andalusian Global ObseRvatory of the Atmosphere) in the Granada area (Spain). In this work, we use the in situ measurements of these campaigns to evaluate aerosol properties retrieved by the GRASP code (Generalized Retrieval of Atmosphere and Surface Properties) combining lidar and sun–sky photometer measurements. We show an overview of aerosol properties retrieved by GRASP during the SLOPE I and II campaigns. In addition, we evaluate the GRASP retrievals of total aerosol volume concentration (discerning between fine and coarse modes), extinction and scattering coefficients, and for the first time we present an evaluation of the absorption coefficient. The statistical analysis of aerosol optical and microphysical properties, both column-integrated and vertically resolved, from May to July 2016 and 2017 shows a large variability in aerosol load and types. The results show a strong predominance of desert dust particles due to North African intrusions. The vertically resolved analysis denotes a decay of the atmospheric aerosols with an altitude up to 5 km a.s.l. Finally, desert dust and biomass burning events were chosen to show the high potential of GRASP to retrieve vertical profiles of aerosol properties (e.g. absorption coefficient and single scattering albedo) for different aerosol types. The aerosol properties retrieved by GRASP show good agreement with simultaneous in situ measurements (nephelometer, aethalometer, scanning mobility particle sizer, and aerodynamic particle sizer) performed at the Sierra Nevada Station (SNS) in Granada. In general, GRASP overestimates the in situ data at the SNS with a mean difference lower than 6 µm3 cm−3 for volume concentration, and 11 and 2 Mm−1 for the scattering and absorption coefficients. On the other hand, the comparison of GRASP with airborne measurements also shows an overestimation with mean absolute differences of 14 ± 10 and 1.2 ± 1.2 Mm−1 for the scattering and absorption coefficients, showing a better agreement for the absorption (scattering) coefficient with higher (lower) aerosol optical depth. The potential of GRASP shown in this study will contribute to enhancing the representativeness of the aerosol vertical distribution and provide information for satellite and global model evaluation.

Investigating Day and Nighttime Variability of Major Water-Soluble Inorganic Species and Role of Reactive Nitrogen Species in PM2.5 and PM10 - A Two Year Study

The study reports day and nighttime temporal variation of prominent water-soluble inorganic species (WSIS) of fine and coarse mode particulate matter at a site in central Delhi for 2012 and 2013. The two years’ concentrations of major ionic species (NH4+, K+, Ca2+ and Mg2+ and NO3-, SO42-) showed that mean levels of both ∑cations and ∑anions were higher in nighttime than daytime in both PM2.5 and PM10. Moreover, the difference of mean levels in daytime and nighttime was noticed higher in PM2.5 compared to PM10. Among anions, more variation was observed for NO3-, i.e., ~49% higher level in nighttime compared to daytime, while~9% higher values in the nighttime for SO42-. Higher variation of NO3- level might be due to active participation of NOx in daytime photo-oxidation process. Among cations,Ca2+ and Mg2+ showed higher concentration in daytime compared to nighttime. Higher day and nighttime variation of Ca2+ and Mg2+ in coarse particulate matter suggested their dominance in PM10 compared to PM2.5. In PM10, the highest Ca2+ concentration was observed in daytime summer and least in nighttime monsoon, indicating the role of loose soil and meteorological conditions. The higher daytime SO42- concentration in monsoon compared to summer show edits significant formation as secondary aerosols in fine mode. The reactive nitrogen species NO3- and NH4+ were correlated during the day and nighttime in PM2.5 and PM10.Moreover, NH4+ was highly correlated to SO42- and NO3-, mainly in the form of (NH4)2SO4 and NH4NO3.

Urban aerosol size distributions: a global perspective

Abstract. Urban aerosol measurements are necessary to establish associations between air pollution and human health outcomes and to evaluate the efficacy of air quality legislation and emissions standards. The measurement of urban aerosol particle size distributions (PSDs) is of particular importance as they enable characterization of size-dependent processes that govern a particle's transport, transformation, and fate in the urban atmosphere. PSDs also improve our ability to link air pollution to health effects through evaluation of particle deposition in the respiratory system and inhalation toxicity. To inform future measurements of urban aerosol observations, this paper reviews and critically analyzes the current state of knowledge on urban aerosol PSD measurements by synthesizing 737 PSD observations made between 1998 to 2017 in 114 cities in 43 countries around the globe. Significant variations in the shape and magnitude of urban aerosol number and mass PSDs were identified among different geographical regions. In general, number PSDs in Europe (EU) and North America, Australia, and New Zealand (NAAN) are dominated by nucleation- and Aitken-mode particles. PSDs in Central, South, and Southeast Asia (CSSA) and East Asia (EA) are shifted to larger sizes, with a meaningful contribution from the accumulation mode. Urban mass PSDs are typically bimodal, presenting a dominant mode in the accumulation mode and a secondary mode in the coarse mode. Most PSD observations published in the literature are short-term, with only 14 % providing data for longer than 6 months. There is a paucity of PSDs measured in Africa (AF), CSSA, Latin America (LA), and West Asia (WA), demonstrating the need for long-term aerosol measurements across wide size ranges in many cities around the globe. Geographical variations in urban aerosol effective densities were also reviewed. Size-resolved urban aerosol effective density functions from 3 to 10 000 nm were established for different geographical regions and intra-city sampling locations in order to accurately translate number PSDs to mass PSDs, with significant variations observed between near-road and urban background sites. The results of this study demonstrate that global initiatives are urgently needed to develop infrastructure for routine and long-term monitoring of urban aerosol PSDs spanning the nucleation to coarse mode. Doing so will advance our understanding of spatiotemporal trends in urban PSDs throughout the world and provide a foundation to more reliably elucidate the impact of urban aerosols on atmospheric processes, human health, and climate.

The role of coarse aerosol particles as a sink of HNO&amp;lt;sub&amp;gt;3&amp;lt;/sub&amp;gt; in wintertime pollution events in the Salt Lake Valley

Abstract. Wintertime ammonium nitrate (NH4NO3) pollution events burden urban mountain basins around the globe. In the Salt Lake Valley of Utah in the United States, such pollution events are often driven by the formation of persistent cold-air pools (PCAPs) that trap emissions near the surface for several consecutive days. As a result, secondary pollutants including fine particulate matter less than 2.5 µm in diameter (PM2.5), largely in the form of NH4NO3, build up during these events and lead to severe haze. As part of an extensive measurement campaign to understand the chemical processes underlying PM2.5 formation, the 2017 Utah Winter Fine Particulate Study, water-soluble trace gases and PM2.5 constituents were continuously monitored using the ambient ion monitoring ion chromatograph (AIM-IC) system at the University of Utah campus. Gas-phase NH3, HNO3, HCl, and SO2 along with particulate NH4+, Na+, K+, Mg2+, Ca2+, NO3-, Cl−, and SO42- were measured from 21 January to 21 February 2017. During the two PCAP events captured, the fine particulate matter was dominated by secondary NH4NO3. The comparison of total nitrate (HNO3 + PM2.5 NO3-) and total NHx (NH3 + PM2.5 NH4+) showed NHx was in excess during both pollution events. However, chemical composition analysis of the snowpack during the first PCAP event revealed that the total concentration of deposited NO3- was nearly 3 times greater than that of deposited NH4+. Daily snow composition measurements showed a strong correlation between NO3- and Ca2+ in the snowpack. The presence of non-volatile salts (Na+, Ca2+, and Mg2+), which are frequently associated with coarse-mode dust, was also detected in PM2.5 by the AIM-IC during the two PCAP events, accounting for roughly 5 % of total mass loading. The presence of a significant particle mass and surface area in the coarse mode during the first PCAP event was indicated by size-resolved particle measurements from an aerodynamic particle sizer. Taken together, these observations imply that atmospheric measurements of the gas-phase and fine-mode particle nitrate may not represent the total burden of nitrate in the atmosphere, implying a potentially significant role for uptake by coarse-mode dust. Using the NO3- : NH4+ ratio observed in the snowpack to estimate the proportion of atmospheric nitrate present in the coarse mode, we estimate that the amount of secondary NH4NO3 could double in the absence of the coarse-mode sink. The underestimation of total nitrate indicates an incomplete account of the total oxidant production during PCAP events. The ability of coarse particles to permanently remove HNO3 and influence PM2.5 formation is discussed using information about particle composition and size distribution.

Hybrid controller of a linear piezoelectric walking stage relying on stack/shear piezoelectric actuators

This paper proposes a hybrid control strategy of a novel linear piezoelectric walking stage based on two sorts of piezoelectric actuators, which takes the load variation into account. The proposed stage consists of two parallel 4-bar lever amplification mechanisms with flexure hinges actuated by piezoelectric stacks to heighten the vertical distance (that is more tolerable to the assembly discrepancy), two compression springs (that is able to maintain a fixed linear position without powering), and two shear piezoelectric actuators (that can achieve longer and equivalent to walking motion) in a small form factor. The proposed stage has two operating modes, namely a coarse positioning mode with a more extensive travel range and a fine positioning mode with a nanometer-level resolution, to possess excellent performance for the linear piezoelectric walking stage of load variations. One multimodal switching controller and one feedforward-feedback controller conduct the coarse mode and fine mode, respectively. The optimal frequency for a specific load is obtained through a backpropagation neural network in the multimodal switching control. In the feedforward-feedback control, the inverse mathematical model based on the Bouc-Wen hysteresis model is used to mitigate the hysteresis effect in the feedforward part while the proportional–integral–derivative controller in the feedback part handles the external system disturbances. Experimental results show the proposed hybrid coarse/fine mode control strategy's effectiveness to satisfy an efficient and accurate positioning task.

Aerosol Optical Properties around the East China Seas Based on AERONET Measurements

Understanding aerosols optical properties over the oceans is vital for enhancing our knowledge of aerosol effects on climate and pollutant transport between continents. In this study, the characteristics of aerosol optical thickness (AOT) at 500 nm (τ500nm), Ångström exponent for the wavelength pair 440–870 nm (α) and volume size distribution (VSD), are presented and analyzed over the East China seas based on the observations at four AERONET sites during 1999–2019. The main results are: (1) the mean τ500nm (α) value ranged from 0.31 to 0.36 (1.17–1.31); (2) the distribution of τ500nm (α) is similar to a log-normal distribution with a right-skewed long tail larger than 0.5 (closer to the normal distribution); (3) large AOT (τ500nm&gt;0.6) was frequently observed in summer (June and July) and spring (March to May), followed by autumn and winter; (4) all aerosol types were observed, and urban/industrial aerosols and mixed types were dominant throughout the period. The atmospheric column aerosol was characterized by a bimodal lognormal size distribution with a fine mode at effective radius, Reff = 0.16 ± 0.01 μm, and coarse mode at Reff = 2.05 ± 0.1 μm.

Seasonal variation and sources of carbonaceous species and elements in PM2.5 and PM10 over the eastern Himalaya.

The study represents the seasonal characteristics (carbonaceous aerosols and elements) and the contribution of prominent sources of PM2.5 and PM10 in the high altitude of the eastern Himalaya (Darjeeling) during August 2018-July 2019. Carbonaceous aerosols [organic carbon (OC), elemental carbon (EC), and water soluble organic carbon (WSOC)] and elements (Al, Fe, Ti, Cu, Zn, Mn, Cr, Ni, Mo, Cl, P, S, K, Zr, Pb, Na, Mg, Ca, and B) in PM2.5 and PM10 were analyzed to estimate their possible sources. The annual concentrations of PM2.5 and PM10 were computed as 37±12 μg m-3 and 58±18 μg m-3, respectively. In the present case, total carbonaceous species in PM2.5 and PM10 were accounted for 20.6% of PM2.5 and 18.6% of PM10, respectively, whereas trace elements in PM2.5 and PM10 were estimated to be 15% of PM2.5 and 12% of PM10, respectively. Monthly and seasonal variations in mass concentrations of carbonaceous aerosols and elements in PM2.5 and PM10 were also observed during the observational period. In PM2.5, the annual concentrations of POC and SOC were 2.35 ± 1.06 μg m-3 (66% of OC) and 1.19±0.57 μg m-3 (34% of OC), respectively, whereas annual average POC and SOC concentrations in PM10 were 3.18 ± 1.13 μg m-3 (63% of OC) and 2.05±0.98 μg m-3 (37% of OC), respectively. The seasonal contribution of POC and SOC were ranging from 55 to 77% and 33 to 45% of OC in PM2.5, respectively, whereas in PM10, the seasonal contributions of POC and SOC were ranging from 51 to 73% and 37 to 49% of OC, respectively. The positive relationship between OC & EC and OC & WSOC of PM2.5 and PM10 during all the seasons (except monsoon in case of PM10) indicates their common sources. The enrichment factors (EFs) and significant positive correlation of Al with othe crustal elements (Fe, Ca, Mg, and Ti) of fine and coarse mode aerosols indicate the influence of mineral dust at Darjeeling. Principal component analysis (PCA) resolved the four common sources (biomass burning + fossil fuel combustion (BB + FFC), crustal/soil dust, vehicular emissions (VE), and industrial emissions (IE)) of PM2.5 and PM10 in Darjeeling.

Temporal and Spatial Distribution Characteristics of Aerosol Optical Properties in Urban Agglomerations on the North Slope of the Tianshan Mountains

In order to explore the temporal and spatial distribution characteristics of atmospheric aerosol optical depth (AOD) in the urban agglomeration on the northern slope of the Tianshan Mountains, the temporal and spatial distribution characteristics and trends of changes in the AOD in the study area from 2000 to 2019 were analyzed by MODIS aerosol products(MCD19-A2). For 2016-2019, when the AOD was relatively stable, the parameters such as the AOD and Ångström wavelength index (α) were analyzed using multi-band sun photometer ground-based remote sensing technology. The results showed that ① the spatial distribution of AOD in the study area was consistent with the topography, and high values were mainly distributed in the low altitude area. The spatial distribution of AOD in the four seasons showed a strong seasonal change from spring (0.15±0.03) > autumn (0.14±0.03) > summer (0.14±0.02). ② In terms of time, the annual average AOD value of the study area was 0.12 from 2000 to 2019 with an annual growth rate of 1.03%, thereby showing an overall increasing trend. The annual variation in the monthly mean value of AOD was bimodal; the first and second peaks were in May and November. The main reason for the increase in AOD was the release and transmission of dust from natural sources and heating. ③ Under the influence of dust weather, the AOD changed sharply in spring, and the size and change range of aerosol particles were larger than those in summer. The high value of AOD in the study area was mainly affected by coarse mode particles. The moisture absorption growth of fine mode particles caused a fluctuation in the AOD, but it was not the cause of the high value of AOD.

An Aerosol Climatology and Implications for Clouds at a Remote Marine Site: Case Study Over Bermuda.

Aerosol characteristics and aerosol-cloud interactions remain uncertain in remote marine regions. We use over a decade of data (2000-2012) from the NASA AErosol RObotic NETwork, aerosol and wet deposition samples, satellite remote sensors, and models to examine aerosol and cloud droplet number characteristics at a representative open ocean site (Bermuda) over the Western North Atlantic Ocean (WNAO). Annual mean values were as follows: aerosol optical depth (AOD) = 0.12, Ångström Exponent (440/870 nm) = 0.95, fine mode fraction = 0.51, asymmetry factor = 0.72 (440 nm) and 0.68 (1020 nm), and Aqua-MODIS cloud droplet number concentrations = 51.3 cm-3. The winter season (December-February) was characterized by high sea salt optical thickness and the highest aerosol extinction in the lowest 2 km. Extensive precipitation over the WNAO in winter helps contribute to the low FMFs in winter (~0.40-0.50) even though air trajectories often originate over North America. Spring and summer had more pronounced influence from sulfate, dust, organic carbon, and black carbon. Volume size distributions were bimodal with a dominant coarse mode (effective radii: 1.85-2.09 μm) and less pronounced fine mode (0.14-0.16 μm), with variability in the coarse mode likely due to different characteristic sizes for transported dust (smaller) versus regional sea salt (larger). Extreme pollution events highlight the sensitivity of this site to long-range transport of urban emissions, dust, and smoke. Differing annual cycles are identified between AOD and cloud droplet number concentrations, motivating a deeper look into aerosol-cloud interactions at this site.

Size-Segregated Atmospheric Humic-Like Substances (HULIS) in Shanghai: Abundance, Seasonal Variation, and Source Identification

Humic-like substances (HULIS) are of great interest due to their optical and chemical characteristics. In this study, a total of 180 samples of atmospheric particulate matter (PM) of different sizes were collected from summer 2018 to spring 2019, in order to analyze the size distribution, to investigate the seasonal variation and then to identify the key sources of HULIS. The annual mean concentration of HULIS in the total suspended particulates reached 5.12 ± 1.42 μg/m3. The HULIS concentration was extremely higher in winter (8.35 ± 2.06 μg/m3) than in autumn (4.88 ± 0.95 μg/m3), in summer (3.62 ± 1.68 μg/m3) and in spring (3.36 ± 0.99 μg/m3). The average annual ratio of water-soluble organic carbon (WSOC) to OC and the ratio of HULIS to WSOC reached 0.546 ± 0.092 and 0.56 ± 0.06, respectively. Throughout the whole year, the size distributions of WSOC and HULIS-C were relatively smooth. The peaks of WSOC appeared at 1.8~3.2 μm and 0.56~1.0 μm, while the peaks of HULIS-C were located at 3.2~5.6 μm, 1.0~1.8 μm and 0.18~0.32 μm. The distribution of the HULIS particle mode was similar in spring, summer and autumn, while there was a lower proportion of the coarse mode and a higher proportion of the condensation mode in winter. By using the comprehensive analysis of principal component analysis (PCA), air mass backward trajectories (AMBTs) and fire point maps, key sources of WSOC and HULIS in Shanghai were identified as biomass combustion (48.42%), coal combustion (17.49%), secondary formation (16.07%) and vehicle exhaust (5.37%). The remaining part might be contributed by crustal dust sources, marine sources and/or other possible sources. This study provides new insight into the characteristics and size distribution of HULIS in Shanghai, thereby providing a practical base for further modeling.

Aerosol optical properties over Delhi during a dust event in summer 2014: plausible implications

Delhi experiences frequent dust storms during the pre-monsoon season. We studied one such event that occurred on May 30th, 2014 at New Delhi to understand the changes in the optical properties of aerosols. The present study utilizes the aerosol optical depth (AOD) from the ground and satellite measurements along with reanalysis data. The aerosol characteristics were examined during the pre-week and post-week of the dust storm event. The results show that AOD values reach ~ 1.0 in all the modes of measurements (i.e., sun photometer, MODIS, and MERRA-2) on the dust event day. MODIS-derived Aerosol Angstrom Exponent (AAE), which gradually decreases from 1.7 ± 0.3 to 1.1 ± 0.3, shows the presence of coarse mode particles during the event. The aerosol layer at an elevation from 1 to 2 km was observed using indigenously developed dual-polarization micro-pulse lidar (MPL) system during the dust event. The source of the dust during the storm was identified by the air mass back-trajectories analysis. The dust column mass density averaged 24 hourly at 850 hPa is 780 mg m−2 with a prevailing wind direction of west to east with wind speed of 11–13 ms−1. Shortwave aerosol direct radiative forcing (SWADRF) diurnally averaged at the top of the atmosphere (TOA), the atmosphere (ATM), and surface (SUR) are found to be − 10 W m−2, 27 W m−2, and − 37 W m−2, respectively. The heating rate was enhanced by 56% (from 0.16 to 0.25 K day−1) during the event in the whole atmospheric column. Visibility decreased by 31% during the dust storm day compared with its average value of non-dust storm days.

Size-segregated aerosols over a high altitude Himalayan and a tropical urban metropolis in Eastern India: Chemical characterization, light absorption, role of meteorology and long range transport

A study has been conducted focusing on the chemical and optical characterization of water soluble inorganic and organic components of aerosols at different sizes, over a high altitude Himalayan station, Darjeeling (27.1° N and 88.15° E, 2200 m amsl) and a tropical urban metropolis, Kolkata (22.5° N, 88.3° E, ~6 m amsl) for two-year long period (March 2016–February 2018). It was observed that local meteorology and long range transport of pollution plumes have played the pivotal role in governing the temporal variation of the mass distribution and concentration of aerosols and its various components over both the sites. The aerosol mass-size distributions were found to be bimodal in nature with the relative dominance of accumulation mode (0.1–1.0 μm) over coarse mode (1.8–10 μm) over both the stations, indicating dominance of the anthropogenic emissions. Among the size classes, accumulation mode aerosols alone contributed 55–75% over Darjeeling and 40–60% over Kolkata to PM10. The coarse mode aerosols were mainly consisted of primary inorganic species over Kolkata and water soluble organic carbons (WSOC) over Darjeeling whereas the fine mode aerosols (accumulation: 0.1–1.0 μm) were primarily composed of the secondary inorganic aerosols for both the stations. Irrespective of the seasons and stations, SO42− and NH4+ exhibited peaks in the mass-size distribution at 1.0–0.1 μm whereas that of NO3− varied with the seasons. The photochemical oxidation and the aqueous phase oxidation of SO2 (g) were the pathways for SO42− formation over Darjeeling whereas the later dominated over Kolkata. Concentration weighted trajectory (CWT) model has revealed that the secondary inorganic aerosols and WSOC were local/regional in origin over Kolkata megacity whereas Darjeeling was influenced by mixed sources. The accumulation mode aerosols were found to be the highest light absorbing over both the stations irrespective of the seasons. Over Darjeeling, the absorption coefficient (babs_365) and the mass absorption efficiency (MAE) of WSOC were maximum for local biomass burning aerosols than the transported plumes whereas those over Kolkata were maximum for transported biomass burning plumes from Eastern Ghats.

Development and Evaluation of Chemistry-Aerosol-Climate Model CAM5-Chem-MAM7-MOSAIC: Global Atmospheric Distribution and Radiative Effects of Nitrate Aerosol.

An advanced aerosol treatment, with a focus on semivolatile nitrate formation, is introduced into the Community Atmosphere Model version 5 with interactive chemistry (CAM5‐chem) by coupling the Model for Simulating Aerosol Interactions and Chemistry (MOSAIC) with the 7‐mode Modal Aerosol Module (MAM7). An important feature of MOSAIC is dynamic partitioning of all condensable gases to the different fine and coarse mode aerosols, as governed by mode‐resolved thermodynamics and heterogeneous chemical reactions. Applied in the free‐running mode from 1995 to 2005 with prescribed historical climatological conditions, the model simulates global distributions of sulfate, nitrate, and ammonium in good agreement with observations and previous studies. Inclusion of nitrate resulted in ∼10% higher global average accumulation mode number concentrations, indicating enhanced growth of Aitken mode aerosols from nitrate formation. While the simulated accumulation mode nitrate burdens are high over the anthropogenic source regions, the sea‐salt and dust modes respectively constitute about 74% and 17% of the annual global average nitrate burden. Regional clear‐sky shortwave radiative cooling of up to −5 W m−2 due to nitrate is seen, with a much smaller global average cooling of −0.05 W m−2. Significant enhancements in regional cloud condensation nuclei (at 0.1% supersaturation) and cloud droplet number concentrations are also attributed to nitrate, causing an additional global average shortwave cooling of −0.8 W m−2. Taking into consideration of changes in both longwave and shortwave radiation under all‐sky conditions, the net change in the top of the atmosphere radiative fluxes induced by including nitrate aerosol is −0.7 W m−2.

Unexpected High Absorption of Atmospheric Aerosols Over a Western Tibetan Plateau Site in Summer

AbstractThe assessment of atmospheric aerosol radiative effects in the Tibetan Plateau (TP) suffers from large uncertainties due to limited understanding of aerosol physicochemical properties. To quantify aerosol optical properties, size distributions, and chemical compositions in the western TP, an intensive field campaign was carried out at Shiquanhe National Reference Climatological Station from July 8 to August 2, 2019. Unexpected low single scattering albedo (SSA) at 870 nm was found for the fine aerosols with an average value of 0.73 ± 0.18. SSA was even lower than 0.60 in the morning when fine aerosols peaked, indicating high absorption of the fine aerosols induced by anthropogenic activities. Coarse mode aerosols accounted for 70.58% ± 14.98% of the total volume concentration and mineral dust was the most abundant species in total suspended particles with a mass fraction of 48.7%. Fine mode aerosol concentrations showed little dependence on wind speed while coarse mode aerosols and metallic element concentrations exhibited strong positive correlations with wind speed, indicating the importance of wind‐blown dust particles. The present study for the first time quantified key aerosol parameters in the western TP and unexpected high absorption of atmospheric aerosols were found over the site in summer. Our results suggest the need to carefully consider the radiative effects caused by aerosol absorption in the TP region.