Atmospheric Aerosol Concentrations Research Articles

The algorithm of microphysical-parameter profiles of aerosol and small cloud droplets based on the dual-wavelength lidar data

Abstract. This study proposed an inversion method for atmospheric-aerosol or cloud microphysical parameters based on dual-wavelength lidar data. The matching characteristics between aerosol and cloud particle size distributions and gamma distributions were studied using aircraft observation data. The feasibility of the retrieval of the particle effective radius from lidar ratios and backscatter ratios was simulated and studied. A method for inverting the effective radius and number concentration of atmospheric aerosols or small cloud droplets using the backscatter ratio was proposed, and the error sources and applicability of the algorithm were analyzed. This algorithm was suitable for the inversion of uniformly mixed and single-property aerosol layers or small cloud droplets. Compared with the previous study, this algorithm could quickly obtain the microphysical parameters of atmospheric particles and has good robustness. For aerosol particles, the inversion range that this algorithm can achieve is 0.3–1.7 µm. For cloud droplets, it is 1.0–10 µm. An atmospheric-observation experiment was conducted using the multi-wavelength lidar developed by Xi'an University of Technology, and a thin cloud layer was captured. The microphysical parameters of aerosol and clouds during this process were retrieved. The results clearly demonstrate the growth of the effective radius and number concentration.

Aerosol uncertainties in tropical precipitation changes for the mid-Pliocene warm period

Abstract. The mid-Pliocene Warm Period (mPWP, 3.3–3.0 Ma) was characterised by an atmospheric CO2 concentration exceeding 400 ppmv with minor changes in continental and orbital configurations. Simulations of this past climate state have improved with newer models but still show some substantial differences from proxy reconstructions. There is little information about atmospheric aerosol concentrations during the Pliocene, but previous work suggests that it could have been quite different from the modern period. Here we apply idealised aerosol scenario experiments to examine the importance of aerosol forcing on mPWP tropical precipitation and the possibility of aerosol uncertainty explaining the mismatch between reconstructions and simulations. The absence of industrial pollutants leads to further warming, especially in the Northern Hemisphere. The Intertropical Convergence Zone (ITCZ) becomes narrower and stronger and shifts northward after removal of anthropogenic aerosols. Though not affecting the location of monsoon domain boundary, removal of anthropogenic aerosol alters the amount of rainfall within the domain, increasing summer rain rate over eastern and southern Asia and western Africa. This work demonstrates that uncertainty in aerosol forcing could be the dominant driver in tropical precipitation changes during the mid-Pliocene: causing larger impacts than the changes in topography and greenhouse gases.

The Relation between Atmospheric Aerosol Concentration and SARS-CoV-2 Variants’ Infection and Mortality Rates in the United States: A Remote-Sensing Perspective

The Relation between Atmospheric Aerosol Concentration and SARS-CoV-2 Variants’ Infection and Mortality Rates in the United States: A Remote-Sensing Perspective

Contrail formation on ambient aerosol particles for aircraft with hydrogen combustion: a box model trajectory study

Abstract. Future air traffic using (green) hydrogen (H2) promises zero carbon emissions, but the effects of contrails from this new technology have hardly been investigated. We study contrail formation behind aircraft with H2 combustion by means of the particle-based Lagrangian Cloud Module (LCM) box model. Assuming the absence of soot and ultrafine volatile particle formation, contrail ice crystals form solely on atmospheric background particles mixed into the plume. While a recent study extended the original LCM with regard to the contrail formation on soot particles, we further advance the LCM to cover the contrail formation on ambient particles. For each simulation, we perform an ensemble of box model runs using the dilution along 1000 different plume trajectories. The formation threshold temperature of H2 contrails is around 10 K higher than for conventional contrails (which form behind aircraft with kerosene combustion). Then, contrail formation becomes primarily limited by the homogeneous freezing temperature of the water droplets such that contrails can form at temperatures down to around 234 K. The number of ice crystals formed varies strongly with ambient temperature even far away from the contrail formation threshold. The contrail ice crystal number clearly increases with ambient aerosol number concentration and decreases significantly for ambient particles with mean dry radii ⪅ 10 nm due to the Kelvin effect. Besides simulations with one aerosol particle ensemble, we analyze contrail formation scenarios with two co-existing aerosol particle ensembles with different mean dry sizes or hygroscopicity parameters. We compare them to scenarios with a single ensemble that is the average of the two aerosol ensembles. We find that the total ice crystal number can differ significantly between the two cases, in particular if nucleation-mode particles are involved. Due to the absence of soot particle emissions, the ice crystal number in H2 contrails is typically reduced by more than 80 %–90 % compared to conventional contrails. The contrail optical thickness is significantly reduced, and H2 contrails either become visible later than kerosene contrails or are not visible at all for low ambient particle number concentrations. On the other hand, H2 contrails can form at lower flight altitudes where conventional contrails would not form.

Anthropogenic Aerosols Weaken Land–Atmosphere Coupling Over North China

AbstractNorth China, characterized by its strong land–atmosphere coupling, also has a high concentration of atmospheric aerosols from anthropogenic emissions. However, the impact of aerosols on land–atmosphere coupling in this region remains partially unclear. Here, we use Weather Research and Forecasting model coupled with Chemistry (WRF‐Chem) experiments to show that the aerosol radiative effect weakens land–atmosphere coupling in North China. This weakening occurs across all five indexes used to measure different aspects of land–atmosphere coupling. Notably, the weakening is more pronounced for indexes that describe surface coupling compared to the index that characterizes the coupling between the planetary boundary layer (PBL) and clouds. The mechanisms underlying the aerosol influence can be primarily attributed to the reduction of land surface fluxes and their sensitivities to soil moisture, while the weakened entrainment of moisture at the upper boundary of the PBL may also contribute to the effects.

Modeling of secondary organic aerosols (SOA) based on two commonly used air quality models in China: Consistent S/IVOCs contribution but large differences in SOA aging

Secondary organic aerosol (SOA) is an important component of atmospheric fine particulate matter (PM2.5), with contributions from anthropogenic and biogenic volatile organic compounds (AVOC and BVOC) and semi- (SVOC) and intermediate volatility organic compounds (IVOC). Policymakers need to know which SOA precursors are important but accurate simulation of SOA magnitude and contributions remain uncertain. Findings from existing SOA modeling studies have many inconsistencies due to differing emission inventory methodologies/assumptions, air quality model (AQM) algorithms, and other aspects of study methodologies. To address some of the inconsistencies, we investigated the role of different AQM SOA algorithms by applying two commonly used models, CAMx and CMAQ, with consistent emission inventories to simulate SOA concentrations and contributions for July and November 2018 in China. Both models have a volatility basis set (VBS) SOA algorithm but with different parameters and treatments of SOA photochemical aging. SOA generated from BVOC (i.e., BSOA) is found to be more important in southern China. In contrast, SOA generated from anthropogenic precursors is more prevalent in the North China Plain (NCP), Yangtze River Delta (YRD), Sichuan Basin and Central China. Both models indicate negligible SOA formation from SVOC emissions compared to other precursors. In July, when BVOC emissions are abundant, SOA is predominantly contributed by BSOA (except for NCP), followed by IVOC-SOA (i.e., SOA produced from IVOC) and ASOA (i.e., SOA produced from anthropogenic VOC). In contrast, in November, IVOC became the leading SOA contributor for all selected regions except PRD, illustrating the important contribution of IVOC emissions to SOA formation.While both models generally agree in terms of the spatial distributions and seasonal variations of different SOA components, CMAQ tends to predict higher BSOA, while CAMx generates higher ASOA concentrations. As a result, CMAQ results suggest that BSOA concentration is always higher than ASOA in November, while CAMx emphasizes the importance of ASOA. Utilizing a conceptual model, we found that different treatment of SOA aging between the two models is a major cause of differences in simulated ASOA concentrations. The step-wise SOA aging scheme implemented in the CAMx VBS (based on gas-phase reactions with OH radical and similar to other models) exhibits a strong enhancement effect on simulated ASOA concentrations, and this effect increases with the ambient organic aerosol (OA) concentrations. The CMAQ aerosol module implements a different SOA aging scheme that represents particle-phase oligomerization and has smaller impacts on total OA. Different structures and/or parameters of the SOA aging schemes are being used in current models, which could greatly affect model simulations of OA in ways that are difficult to anticipate. Our results indicate that future control policies should aim at reducing IVOC emissions as well as traditional VOC emissions. In addition, aging schemes are the major driver in CMAQ vs. CAMx treatments of ASOA and their resulting predicted mass. More sophisticated measurement data (e.g., with resolved OA components) and/or chamber experiments (e.g., investigating how aging influences SOA yields) are needed to better characterize SOA aging and constrain model parameterizations.

A numerical simulation of CCN impacts on weather modification efficiency

Aerosols affect development of clouds and precipitation by serving as cloud condensation nuclei (CCN) and ice nuclei (IN). Considering the dramatically changing ambient aerosol concentration, it is important to examine the potential “side effect” of aerosol pollution on precipitation enhancement by weather modification. In this study, the cloud seeding was performed on a precipitation event in Beijing in the summer of 2008, which is simulated by the NSSL two-moment cloud scheme of the Weather Research and Forecasting (WRF) model. Sensitivity tests were conducted by modifying the ambient aerosol concentration and the ice crystal seeding amount to investigate the cloud seeding efficacy in different CCN concentration scenarios. There was a slight difference in the precipitation distribution between the simulations with two ambient CCN concentrations: the northern precipitation center in polluted scenario was weaker and the southern center was stronger. Compared with normal CCN scenario, the cloud liquid water mass and ice crystal mass in the severe pollution scenario is larger, and the total contents of snow and graupel were not sensitive to the CCN concentration. With the same amount of man-made ice crystals seeding, the precipitation enhancement was quite different under different CCN conditions. The higher the CCN concentration usually leads to stronger precipitation suppression. As CCN concentration increase, the deposition growth of snow, auto-conversion and accretion of ice crystals to snow were weakened, as well as the conversion of melting snow and graupel into rainwater.

Stratospheric ozone, UV radiation, and climate interactions

This assessment provides a comprehensive update of the effects of changes in stratospheric ozone and other factors (aerosols, surface reflectivity, solar activity, and climate) on the intensity of ultraviolet (UV) radiation at the Earth’s surface. The assessment is performed in the context of the Montreal Protocol on Substances that Deplete the Ozone Layer and its Amendments and Adjustments. Changes in UV radiation at low- and mid-latitudes (0–60°) during the last 25 years have generally been small (e.g., typically less than 4% per decade, increasing at some sites and decreasing at others) and were mostly driven by changes in cloud cover and atmospheric aerosol content, caused partly by climate change and partly by measures to control tropospheric pollution. Without the Montreal Protocol, erythemal (sunburning) UV irradiance at northern and southern latitudes of less than 50° would have increased by 10–20% between 1996 and 2020. For southern latitudes exceeding 50°, the UV Index (UVI) would have surged by between 25% (year-round at the southern tip of South America) and more than 100% (South Pole in spring). Variability of erythemal irradiance in Antarctica was very large during the last four years. In spring 2019, erythemal UV radiation was at the minimum of the historical (1991–2018) range at the South Pole, while near record-high values were observed in spring 2020, which were up to 80% above the historical mean. In the Arctic, some of the highest erythemal irradiances on record were measured in March and April 2020. For example in March 2020, the monthly average UVI over a site in the Canadian Arctic was up to 70% higher than the historical (2005–2019) average, often exceeding this mean by three standard deviations. Under the presumption that all countries will adhere to the Montreal Protocol in the future and that atmospheric aerosol concentrations remain constant, erythemal irradiance at mid-latitudes (30–60°) is projected to decrease between 2015 and 2090 by 2–5% in the north and by 4–6% in the south due to recovering ozone. Changes projected for the tropics are ≤ 3%. However, in industrial regions that are currently affected by air pollution, UV radiation will increase as measures to reduce air pollutants will gradually restore UV radiation intensities to those of a cleaner atmosphere. Since most substances controlled by the Montreal Protocol are also greenhouse gases, the phase-out of these substances may have avoided warming by 0.5–1.0 °C over mid-latitude regions of the continents, and by more than 1.0 °C in the Arctic; however, the uncertainty of these calculations is large. We also assess the effects of changes in stratospheric ozone on climate, focusing on the poleward shift of climate zones, and discuss the role of the small Antarctic ozone hole in 2019 on the devastating “Black Summer” fires in Australia. Additional topics include the assessment of advances in measuring and modeling of UV radiation; methods for determining personal UV exposure; the effect of solar radiation management (stratospheric aerosol injections) on UV radiation relevant for plants; and possible revisions to the vitamin D action spectrum, which describes the wavelength dependence of the synthesis of previtamin D3 in human skin upon exposure to UV radiation.Graphical abstract

Potential Impacts on Ozone and Climate From a Proposed Fleet of Supersonic Aircraft

AbstractThere has been renewed interest in developing commercial supersonic transport aircraft due to the increased overall demands by the public for air travel, the aspiration for more intercontinental travel, and the desire for shorter flight times. Various companies and academic institutions have been actively considering the designs of such supersonic aircraft. As these new designs are developed, the environmental impact on ozone and climate of these fleets need to be explored. This study examines one such proposed commercial supersonic fleet of 55‐seater that is projected to fly at Mach 2.2, corresponding to cruise altitudes of 17–20 km, and which would burn 122.32 Tg of fuel and emit 1.78 Tg of NOx each year. Our analyses indicate this proposed fleet would cause a 0.74% reduction in global column ozone (∼2 Dobson Units), which is mainly attributed to the large amounts of nitrogen oxides released in the atmosphere from the supersonic aircraft. The maximum ozone loss occurs at the tropics in the fall season, with a reduction of −1.4% in the total column ozone regionally. The stratospheric‐adjusted radiative forcing on climate from this fleet was derived based on changes in atmospheric concentrations of ozone (59.5 mW/m2), water vapor (10.1 mW/m2), black carbon (−3.9 mW/m2) and sulfate aerosols (−20.3 mW/m2), resulting in a net non‐CO2, non‐contrail forcing of 45.4 mW/m2, indicating an overall warming effect.

How Do Dust Devil-Like Vortices Depend on Model Resolution? A Grid Convergence Study Using Large-Eddy Simulation

Dust devils are organized convective vortices with pressure drops of hundreds of pascals that spirally lift surface material into the air. This material modifies the radiation budget by contributing to the atmospheric aerosol concentration. Quantification of this contribution requires good knowledge of the dust devil statistics and dynamics. The latter can also help to understand vortex genesis, evolution and decay, in general. Dust devil-like vortices are numerically investigated mainly by large-eddy simulation (LES). A critical parameter in these simulations is the grid spacing, which has a great influence on the dust devil statistics. So far, it is unknown which grid size is sufficient to capture dust devils accurately. We investigate the convergence of simulated convective vertical vortices that resemble dust devils by using the LES model PALM. We use the nesting capabilities of PALM to explore grid spacings from 10 to 0.625 m. Grid spacings of 1 m or less have never been used for the analysis of dust devil-like vortices that develop in a horizontal domain of more than 10 km^2. Our results demonstrate that a minimum resolution of 1.25 m is necessary to achieve a convergence for sample-averaged quantities like the core pressure drop. This grid spacing or smaller should be used for future quantifications of dust devil sediment fluxes. However, sample maxima of the investigated dust devil population and peak velocity values of the general flow show no convergence. If a qualitative description of the dust devil flow pattern is sufficient, we recommend a grid spacing of 2.5 m or smaller.

Study of elemental concentration, surface morphology and chemical characterization of atmospheric aerosols and trace gases in an urban environment (India)

The severe harmful impact of atmospheric aerosols over the environment leads to create the diverse human interests and concerns. The increase in population growth, anthropogenic activities, land use pattern, and urbanisation have led to change in the environmental conditions. This study represents the different aspect of elemental concentration, morphology, and chemical composition of particulate matter and trace gases during different time periods of an Indian festival (Diwali) in the Greater Noida region of Uttar Pradesh (India). The average elemental concentration during night period (Diwali days) for PM10, PM2.5, SO2, NO2 and O3 were 540 ± 162 μg m−3, 343 ± 193 μg m−3, 25 ± 12 μg m−3, 44 ± 13 μg m−3 and 8 ± 5 μg m−3 respectively. The SEM-EDS studies revealed the different pattern and shapes of fine (≤ 2.5 μm), coarse (≤ 10 μm) and total suspended particles (≥ 10 μm) as spherical and uneven shapes, bunches, clusters, biogenic elements in the form of honeycomb structure (Brochosomes) and pollen were observed from different sources. The mineralogical studies showed the presence of quartz, feldspar, kaolinite, calcium aluminium silicate, and organic carbon in the studied region.

Using the Sentinel-3B Satellite in Geospatial Analysis of Suspended Aerosols in the Kiev, Ukraine Region

The use of images from the Sentinel-3B SYN satellite (surface reflectance and aerosol parameters over land) is currently one of the most advanced technologies utilized to identify atmospheric aerosol concentrations on a global scale. The general aim of this study is to analyze the evolution of aerosols in the atmosphere of the Kiev region in northern Ukraine during 2019, 2020, 2021 and 2022. Due to this study’s timing, both prior to and during the current military incursion into Ukraine, this study also evaluates the consequences of the invasion of the Russian army on the territory of Ukraine, in relation to the quantitative levels of aerosols present in the atmosphere. Satellite image data were modelled in SNAP software (Sentinel Application Platform). Using the JASP software (version 0.14.1.0), clusters with variations of T550 (Aerosol Optical Thickness) were generated. The Sentinel-3B SYN satellite images were made available by the European Space Agency (ESA), with moderate spatial resolution (>300 m), calibrated and normalized to an average standard of 0.83 µg/mg, with a maximum error of 6.62% in the 30 sampled points. Satellite image data were modelled in SNAP software. Using the JASP software (version 0.14.1.0), clusters with variations of T550 (Aerosol Optical Thickness) were generated. The results show variations in the concentration of T550 in different periods, revealing that the military conflict between Russia and Ukraine directly influenced the dynamics of aerosol concentration, attributed to factors incompatible with environmental sustainability.

Characterization of Timau National Observatory using limited in situ measurements

ABSTRACT A new astronomical observatory in south-eastern Indonesia is currently under construction. This Timau National Observatory will host a 3.8-m telescope for optical and near-infrared observations. To support the operation and planning, the characterization of the site needs to be appropriately performed. However, limited resources and access to the site hindered the deployment of instruments for comprehensive site testing. Fortunately, in situ sky brightness data from the Sky Quality Meter (SQM) have been available for almost 2 yr. Based on the data acquired in 470 nights, we obtain a background sky brightness of μ0 = 21.86 ± 0.38 mag arcsec−2. Additionally, we evaluate the moonlit sky brightness to estimate the atmospheric extinction coefficient (k) and level of scattering on site. We find an elevated value of k = 0.48 ± 0.04, associated with a high atmospheric aerosol content. It is considered regular for an equatorial area situated at a low altitude (∼1300 masl). By analysing the fluctuation of the sky brightness and infrared images from Himawari-8 satellite, we estimate the available observing time (AOT) of at least 5.3 h/night and the yearly average percentage of usable nights of $66{{\ \rm per\ cent}}$. The monthly average AOT from SQM and satellite data analysis correlate with R = 0.82. In terms of the monthly percentage of usable nights, the correlation coefficient is R = 0.78. During the wet season (November–April), the results from SQM and satellite data analysis deviate more significantly, mainly due to the limited capability of Himawari-8 in detecting fragmented low-altitude clouds. According to these results, we expect Timau to complement other observatories greatly.

Invisible ship tracks show large cloud sensitivity to aerosol

Cloud reflectivity is sensitive to atmospheric aerosol concentrations because aerosols provide the condensation nuclei on which water condenses1. Increased aerosol concentrations due to human activity affect droplet number concentration, liquid water and cloud fraction2, but these changes are subject to large uncertainties3. Ship tracks, long lines of polluted clouds that are visible in satellite images, are one of the main tools for quantifying aerosol–cloud interactions4. However, only a small fraction of the clouds polluted by shipping show ship tracks5,6. Here we show that even when no ship tracks are visible in satellite images, aerosol emissions change cloud properties substantially. We develop a new method to quantify the effect of shipping on all clouds, showing a cloud droplet number increase and a more positive liquid water response when there are no visible tracks. We directly detect shipping-induced cloud property changes in the trade cumulus regions of the Atlantic, which are known to display almost no visible tracks. Our results indicate that previous studies of ship tracks were suffering from selection biases by focusing only on visible tracks from satellite imagery. The strong liquid water path response we find translates to a larger aerosol cooling effect on the climate, potentially masking a higher climate sensitivity than observed temperature trends would otherwise suggest.

Improving the particle dry deposition scheme in the CMAQ photochemical modeling system

Dry deposition of atmospheric aerosols in large-scale models is a critical, but highly uncertain, sink process with a strong dependence on particle size, meteorological conditions, and land surface properties. This study investigates the particle dry deposition scheme implemented in the standard Community Multiscale Air Quality (CMAQ) model v5.2.1, characterizes its underlying parameterized components with comparison to a similar scheme in a contemporary regional-scale model, and proposes two updated schemes that are then evaluated with available ambient particle deposition velocity (Vd) measurements. Both updated schemes reduce the surprisingly strong dependence of deposition velocity on the aerosol mode width, with one scheme further introducing a dependence on vegetation coverage that is broadly consistent with variability in observations between vegetated and non-vegetated surfaces. Compared to the base scheme, the updated scheme with vegetation dependence increases Vd for submicron particles and decreases it for larger particles by an average of 37% and −66%, respectively. This scheme performs statistically better than the base scheme, reducing fractional biases by 56%–97% for vegetated land-use types and has roughly equivalent performance over water. The base and updated schemes are tested with three annual CMAQ (v5.2.1) simulations for the year 2011; predicted ambient aerosol concentrations are evaluated with routine monitoring network observations and predicted dry deposition fluxes are evaluated with data from the Clean Air Status and Trends Network (CASTNET). The updated scheme with vegetation dependence reduces negative fractional biases for PM10 by 41% and positive fractional biases for PM2.5 organic carbon by 15%. This scheme has been incorporated into the most recent publicly accessible versions of CMAQ (v5.3 and beyond) to replace the scheme used in previous versions of CMAQ (v4.5 through v5.2.1).

Black carbon and particulate matter mass concentrations in the Metropolitan District of Caracas, Venezuela: An assessment of temporal variation and contributing sources

Atmospheric aerosols play an important role in atmospheric processes and human health. Characterizing atmospheric aerosols and identifying their sources in large cities is relevant to propose site-specific air pollution mitigation strategies. In this study, we measured the mass concentration of atmospheric aerosols with an aerodynamic diameter smaller than 2.5 µm (PM2.5) in the city of Caracas (urban) and in a tropical montane cloud forest (suburban site, located in a mountainous area 11 km far from Caracas) between June 2018 and October 2019. We also measured equivalent black carbon (eBC) mass concentration in PM2.5 in Caracas during the same period. Our goal is to assess PM2.5 and eBC temporal variation and identify their major sources in the area. eBC showed a pronounced diurnal cycle in the urban site, mainly modulated by traffic circulation and the diurnal changes of the mixing layer height. In contrast, PM2.5 showed stable median values during the day with slight variations like that of eBC. In the forest site, PM2.5 values were higher in the afternoons due to the convective transport of aerosols from Caracas and other surrounding urban areas located in adjacent valleys. The annual median for eBC and PM2.5 was 1.6 and 9.2 µg m–3, respectively, in the urban site, while PM2.5 in the forest site was 6.6 µg m–3. To our knowledge, these are the first measurements of this type in the northernmost area of South America. eBC and PM2.5 sources identification during wet and dry seasons was obtained by percentiles of the conditional bivariate probability function (CBPF). CBPF showed seasonal variations of eBC and PM2.5 sources and that their contributions are higher during the dry season. Biomass burning events are a relevant contributing source of aerosols for both sites of measurements inferred by fire pixels from satellite data, the national fire department’s statistics data, and backward trajectories. Our results indicate that biomass burning might affect the atmosphere on a regional scale, contribute to regional warming, and have implications for local and regional air quality and, therefore, human health.

Influence of urban heat islands on seasonal aerosol acidity and aerosol liquid water content in humid subtropical Hong Kong, South China

Aerosol acidity governs many important atmospheric processes that modulate the composition and mass concentrations of atmospheric aerosols. Temperature and RH are two key drivers of aerosol acidity. Increasing levels of urbanization in humid subtropical South China have led to the frequent occurrence of urban heat islands (UHIs) in the region. However, the effects that UHIs have on aerosol acidity in cities in South China are currently unknown. In this study, we investigated the effects of UHIs on aerosol acidity and aerosol liquid water concentrations at two urban sites with different land use characteristics in Hong Kong, South China, in winter and summer from 2011 to 2019. Our results showed that the UHI effect resulted in both urban sites having significantly higher temperatures and lower RH than the refence rural site. Higher UHI intensities were observed in winter, but RH differences between the urban and rural sites were the greatest in summer. Temperature and RH changes associated with the UHI effect resulted in urban aerosols having aerosol liquid water concentrations that were up to 6 to 7 times lower than rural aerosols, and urban aerosols being more acidic than rural aerosols by as much as 1.16 pH units. While the pH differences between urban and rural aerosols correlated with temperature and RH differences induced by the UHI effect, these correlations were season-dependent due to differences in the winter and summer aerosol compositions. In addition, although the UHI was most intense in winter, pH differences between urban and rural aerosols were the largest in summer. Changes in temperature, RH, and aerosol liquid water concentrations linked to the UHI effect were found to lead to substantial reductions (by as much as 38%) in the partitioning of semi-volatile basic and acidic species NH3 and HNO3 to the aerosol phase. Our results indicate that changes in the aerosol acidity, aerosol liquid water concentrations, and gas-aerosol partitioning associated with UHIs have significant implications for aqueous urban aerosol chemistry in Hong Kong. Since UHIs will intensify in many cities in South China in the future due to their increasing levels of urbanization and a warming climate, changes in urban aerosol acidity and liquid water concentrations induced by intensifying UHIs need to be considered when modeling urban aerosol composition and levels in the region.

Quantifying Mechanisms of Aeolian Dust Emission: Field Measurements at Etosha Pan, Namibia

AbstractDetermining the controls on aeolian dust emissions from major sources is necessary for reliable quantification of atmospheric aerosol concentrations and fluxes. However, ground‐based measurements of dust emissions at‐source are rare and of generally short duration, failing to capture the annual cycle. Here, we provide new insights into dust dynamics by measuring aerosol concentrations and meteorological conditions for a full year (July 2015–June 2016) at Etosha Pan, Namibia, a globally significant dust source. Surface deployed field instrumentation provided 10‐min averaged data on meteorological conditions, aerosol concentration (mg/m3), and horizontal dust flux (g/m2/min10). A Doppler lidar provided additional data for some of the period. 51 significant dust events were identified in response to strong E‐ENE winds. We demonstrate that these events occurred throughout the year and were not restricted to the austral winter, as previously indicated by satellite observations. Peak horizontal flux occurred in the spring (November) due to strengthening erosive winds and highly desiccating conditions increasing surface erodibility. We identify a strong seasonal differentiation in the meteorological mechanisms controlling dust uplift; low‐level jets on dry winter mornings (61% of all events), and cold pool outflows in humid summer evenings (39% of events). Significantly, we demonstrate a very strong bias toward the contribution of low frequency and high magnitude events, with nearly 31% of annual horizontal dust flux generated by only 6 individual events. Our study demonstrates how longer‐term (≈1 year), ground‐based, and at‐source field measurements can radically improve interpretations of dust event dynamics and controls at major source locations.

Long‐term trends in aerosol optical properties and their relationship with cloud properties over southern India and Sri Lanka

AbstractAsia is one of the continents where aerosol levels are comparatively higher across the world. India and Sri Lanka are some of the regions in the South Asian continent where pollution is increasing rapidly due to the rise in industrialization. The present study investigated the interactions between atmospheric aerosol and cloud microphysical properties and their spatial, temporal, and seasonal variation at local and regional scales during 2000–2020 using remotely sensed data sets in south India and Sri Lanka. High values (>0.5) of annual mean aerosol optical depth (AOD) were detected over southern India. On the other hand, lower values (0.2) were detected over Sri Lanka. In terms of seasonality, a high level of AOD was registered in both southern India and Sri Lanka during the premonsoon and monsoon periods. The angstrom exponent (AE412‐470) revealed the dominance of fine‐mode particles during winter and the postmonsoon, generally from biomass burning and industrial activities. The long‐term analysis exhibited an increasing trend of atmospheric aerosol concentration over southern India and Sri Lanka. Interestingly, there was a decrease in AOD during the year 2020; the reduction in anthropogenic activities in the region was attributed to the COVID‐19 lockdown, hence less accumulation of pollutants in the atmosphere. AOD showed a positive correlation with cloud effective radius over the western areas along with the Indian Ocean, north, southeast, and southern end of India, while negatively correlated with high AOD areas such as northeast of the study domain. The AOD and cloud optical depth were positively correlated over continental areas, while negative correlations were notable over the Indian Ocean around Sri Lanka, implying heterogeneities of aerosol's effect on cloud microphysical properties over the study area. Finally, the results from wind circulation and backward air mass trajectories reveal higher concentrations of fine‐mode particles associated with the continent, whereas coarse‐mode particles originate from the oceans.

A local marine source of atmospheric particles in the High Arctic

The chemical composition of non-refractory submicron aerosol (NR-PM1) was characterized at the Villum Research Station (Villum) at Station Nord in North Greenland during spring-summer 2016 using a Time of Flight Aerosol Chemical Speciation Monitor (ToF-ACSM). The composition is dominated by sulfate (48%) and organic species (40%). Positive Matrix Factorization (PMF) identified three key factors corresponding to a primary hydrocarbon-like organic aerosol (HOA), and two types of secondary organic aerosol: oxygenated organic aerosol (OOA) and a marine organic aerosol (MOA). The HOA factor accounts for 5% of the organic aerosol mass, which is consistent with previous findings at Villum. The OOA factor accounts for 77% of the organic aerosol mass and correlates with accumulation mode particles, which supports previous findings indicating that oxidized organic aerosols are predominantly from long-range transport during winter and spring at Villum. The MOA factor was characterized by mass spectral fragments of methane sulfonic acid (MSA) from atmospheric oxidation of dimethyl sulfide, for which reason the MOA factor is considered to be of biogenic origin. MOA accounts for 18% of the organic aerosol mass and correlates with locally produced Aitken mode particles. This indicates that biogenic processes are not only a significant source of aerosols at Villum, but MOA also appears to be formed in the vicinity of the measurement site. This local geographical origin was confirmed through air mass back trajectory modelling and source-receptor analysis. During May, air masses frequently arrived from the east, with source regions for the MOA factor and therewith MSA located in the Barents Sea and Lincoln Sea with lesser contributions from the Greenland Sea. During June, air mass origin shifted to the west, with source regions for the MOA factor and MSA shifting correspondingly to Baffin Bay and the Canadian Arctic Archipelago. While shifting transport patterns between May and June lead to shifting source regions, sea ice likely played a role as well. During May, marginal ice zones were present in the Barents Sea between Svalbard and Franz Josef Land, while during June, sea ice in the northern part of Baffin Bay retreated and sea ice in the Canadian Arctic Archipelago decreased. Although May and June experienced different transport patterns and sea ice conditions, levels of the MOA factor and MSA were similar between the months. This is likely due to similarities between marine biological activities in the Barents Sea and Baffin Bay. This research highlights the complex relationship between transport patterns, sea ice conditions, and atmospheric particle concentrations. Multiyear aerosol chemical composition from several High Arctic sites is encouraged to determine the full effects of ocean-atmosphere interactions and transport patterns on atmospheric aerosol concentrations.