Deposition of ambient black carbon (BC) aerosols over snow-covered areas reduces surface albedo and accelerates snowmelt. Based on in-situ atmospheric BC data and the WRF-Chem model, we estimated the dry and wet deposition of BC over the Yala glacier of the central Himalayan region in Nepal during 2016-2018. The maximum and minimum BC dry deposition was reported in pre- and post-monsoon respectively. Approximately 50% of annual dry deposition occurred in the pre-monsoon season (March to May) and 27% of the annual dry deposition occurred in April. The total dry BC deposition rate was estimated as -4.6 mu g m- 2 day- 1 providing a total deposition of 531 mu g m- 2 during the pre-monsoon season. The contribution of biomass burning and fossil fuel sources to BC deposition on an annual basis was 28% and 72% respectively. The annual accumulated wet deposition of BC was 196 times higher than the annual dry deposition. The ten months of observed dry deposition of BC (October 1, 2016 to August 31, 2017 - except December 2016) was -39% lower than that of WRFChem's estimated annual dry deposition from September 1, 2016 to August 31, 2017 partially due to model bias. The deposited content of BC over the snow surface has an important role in albedo reduction, therefore snow samples were collected from the surface of the Yala Glacier and the surrounding region in April 2016, 2017, and 2018. Samples were analyzed for BC mass concentration through the thermal optical analysis and single particle soot photometer method. The BC calculated via the thermal optical method was in the range of 352-854 ng g- 1, higher than the BC calculated through the particle soot photometer method and estimated BC in 2 cm surface snow (imperial equation). The maximum surface snow albedo reduction due to BC was 8.8%, estimated by a widely used snow radiative transfer model and a linear regression equation.

Current models estimate global aviation contributes approximately 5% to the total anthropogenic climate forcing, with aerosol-cloud interactions having the greatest effect. However, radiative forcing estimates from aviation aerosol-cloud interactions remain undetermined. There is an expected significant increase in aircraft emissions with aviation demand expected to rise by over 4% per year. Soot may play an important role in the ice nucleation of aircraft-induced cirrus formation due to a high emission rate, but the ice nucleating properties are poorly constrained. Understanding the microphysical processes leading to atmospheric ice crystal formation is crucial for the reliable parameterization of aerosol-cloud interactions in climate models due to their impact on precipitation and cloud radiative properties. Ice nucleation of aircraft-emitted soot is potentially affected by particle morphology with condensation of supercooled water occurring in pores followed by ice nucleation. However, soot has heterogeneous properties and undergoes atmospheric aging and oxidation that could change surface properties and contribute to complex ice nucleation processes. This review synthesizes current knowledge of ice nucleation catalyzed by aviation in the cirrus regime and its effects on global radiative forcing. Further research is required to determine the ice nucleation and microphysical processes of cirrus cloud formation from aviation emissions in both controlled laboratory and field investigations to inform models for more accurate climate predictions and to provide efficient mitigation strategies. Aerosol particles can facilitate ice crystal formation in clouds that affect Earth's precipitation and climate by altering the amount of sunlight that clouds reflect and is absorbed by Earth. Human-induced pollution may affect atmospheric ice nucleation, such as black carbon (soot) from aircraft emissions. It has been known for decades that carbon dioxide is a major greenhouse gas emitted from aircraft that significantly warms Earth's surface, but the climate effects of aerosol-cloud interactions are still largely unknown. An understanding of what aerosol particles in the atmosphere contribute to ice nucleation is needed to better predict how they will affect future climate. This review summarizes what we currently know about ice nucleation processes from aircraft soot emissions and identifies future research priorities to understand human-induced ice cloud formation to better predict how it may affect global climate. Ice nucleation is a current major uncertainty in predicting future climate from aerosol-cloud interactions This review synthesizes the current state of knowledge on ice nucleation from anthropogenic aircraft emissions Future research includes direct observations and laboratory measurements of ice nucleation microphysical processes from aircraft emissions

Char-EC and soot-EC in the atmosphere produced from different fuel combustion have distinct optical properties which lead to different radiative forcing. Pollutants transported into high-altitude environment could have a long-lasting radiative effect due to being free of deposition. In this study, the mass absorption cross- (MAC), the sources, transport pathways and the direct radiative effects (DREs) of soot-EC and char-EC were investigated at a peak of Mountain Hua (Mt. Hua) in China. The measurement results showed that soot-EC and char-EC account for 15.7 % and 84.3 % of EC, respectively. The mean MAC (lambda = 633 nm) of soot-EC (13.7 +/- 3.8 m(2)/g) was much higher than that of char-EC (5.4 +/- 2.5 m(2)/g), indicating a stronger light absorption ability for soot-EC. During the study period, 62.1 % char-EC was from anthracite chunk coal, 24.3 % of it from liquid fuel combustion. By contrast, 59.0 % soot-EC from liquid fuel combustion and 36.6 % of it from anthracite chunk coal. EC (both char-EC and soot-EC) produced from anthracite chunk coal reached the peak of the Mt. Hua primarily through the raising of the planetary boundary layer (PBL), while the EC produced from liquid fuel arrived the peak mainly by the regional transport above the PBL of the site. Although soot-EC has a stronger ability (2.8 times higher) to absorb the light compared with char-EC, its DRE (5.7 +/- 3.9 W m(-2)) was lower than that of char-EC (11.6 +/- 6.9 W m(-2)) due to the smaller mass quantity. Liquid fuel consumption contributed 3.5 +/- 2.9 W m(-2) DRE of soot-EC, while the combustion of anthracite chunk coal contributed 7.5 +/- 5.7 W m(-2) DRE of char-EC. This study highlights the differences in DREs of soot-EC and char-EC from fossil fuel combustion and the DRE mass efficiency of soot-EC and char-EC. The results emphasize the divergent climate warming effects caused by the combustion of different fossil fuels and imply that setting path to a green transition of energy use would benefit reducing the EC perturbation to the radiation balance of earth-atmosphere.

Soot particles released in the atmosphere have long been investigated for their ability to affect the radiative forcing. Although freshly emitted soot particles are generally considered to yield only positive contributions to the radiative forcing, atmospheric aging can activate them into efficient cloud condensation or ice nuclei, which can trigger the formation of persistent clouds and ultimately provide a negative contribution to the radiative forcing. Depending on their residence time in the atmosphere, soot particles can undergo several physical and chemical aging processes that affect their chemical composition, particle size distribution and morphology, and ultimately their optical and hygroscopic properties. The impact of the physical-chemical aging on the properties of soot particles is still difficult to quantify, as well as their effect on the radiative forcing of the atmosphere.This work investigates the hygroscopic properties of chemically aged soot particles obtained from the combustion of aviation fuel, and in particular the interplay between aging mechanisms initiated by two widespread atmospheric oxidizers (O-3 and SO2). Activation is measured in water supersaturation conditions using a cloud condensation nuclei counter. Once particle morphology and size distribution are taken into account, the hygroscopicity parameter kappa is derived using kappa-K & ouml;hler theory and correlated to the change of the chemical composition of the particles aged in a simulation chamber. While fresh soot particles are poor cloud condensation nuclei (kappa < 10(-4)) and are not significantly affected by either O-3 or SO2 at the timescale of the experiments, rapid activation is observed when they are simultaneously exposed to both oxidizers. Activated particles become efficient cloud condensation nuclei, comparable to the highly hygroscopic particulate matter typically found in the atmosphere (kappa = 0.2-0.6 at RH = 20 %). Statistical analysis reveals a correlation between the activation and sulfur-containing ions detected on the chemically aged particles that are absent from the fresh particles.

Emissions from road traffic are one of the most important sources of soot aerosols and they can affect the surfaces in the area. In the case of snow surfaces, this effect may lead to changes in the radiative forcing and snow melt, also influenced by particle transport such as particle diffusion and advection. An experimental campaign in The Andes, Chile, was carried out measuring the radiance and irradiance of the snow perpendicularly to a road with high traffic load, together with the meteorological conditions (to identify the diffusion and advection phenomena), the aerosol size distribution, the concentration of particles (PM1, PM2.5 and PM10), and the concentration of black carbon (BC) in both, the atmosphere and the snowpack. The aim of the study was to quantify the contribution of four factors affecting the albedo (black carbon -BC- concentration in snow, grain size, cloudiness, and roughness) by comparing the measured albedo of the contaminated snow surface with that of the same surface prior to contamination, considered as a reference. Results showed a trade-off between diffusion and advection. Close to the road, diffusion was predominant, leading to an increase in BC concentration and a reduction in snow albedo. On the contrary, far from the road, where winds are channeled along the centre of the valley, advection of particles became dominant, leading to another increase in particle concentration and another reduction in snow albedo. Among the factors contributing to reduce the snow albedo, BC concentration dominates at all distances from the road, although the effect of the grain size becomes as significant as that of BC in the centre of the valley, with the effects of surface roughness and cloudiness remaining minor. This information can be used in snow models to get a better knowledge of the effect of particle deposition on albedo reductions.

The snow physical parameters are closely related to the sizes, shapes, and chemical composition of light-absorbing particles (LAPs). By utilizing a computer-controlled scanning electron microscope software called IntelliSEM-EPAS (TM), we first report the measured size-resolved concentration of soot, dust, and fly ash particles in fresh (wet) and aged (dry deposition) snow samples collected at an industrial city in China during and after a snowfall at intervals of 6-8 days. Due to wet scavenging by seasonal snow, soot and dust particles in snow are absorbed by 69.7% and 30.3% at wavelengths of 550 nm, lowering snow albedo by 0.0089 and 0.0039, respectively. Soot particle size increases slightly during dry deposition, whereas size-resolved mineral dust does not undergo a significant shift in particle size. These results indicate the essentiality to involve the effects of accurate size and composition of in-snow LAPs for a better assessment of snow light absorption and reflectance. Plain Language Summary A field survey was undertaken to collect freshly fallen (1) and aged surface (15) snow samples at 1-day intervals in the center of Changchun city, China, which is surrounded by heavy industrial emission sources. We used an advanced computer-controlled scanning electron microscope to determine particle size and number distributions of three major light-absorbing particle types with diameters of 0.2-10 mu m in seasonal snow, namely soot, dust, and fly ash. Soot and dust particles deposited in various ice-grain sizes via wet and dry deposition were also examined in terms of their contributions to light absorption and snow albedo reduction. We report here a first attempt to detect a combination of log-normal soot, dust, and fly ash in seasonal snow, as well as their potential effects on the reduction of snow albedo.

Effective density (peff) is an important property describing particle transportation in the atmosphere and in the human respiratory tract. In this study, the particle size dependency of peff was determined for fresh and photochemically aged particles from residential combustion of wood logs and brown coal, as well as from an aerosol standard (CAST) burner. peff increased considerably due to photochemical aging, especially for soot agglomerates larger than 100 nm in mobility diameter. The increase depends on the presence of condensable vapors and agglomerate size and can be explained by collapsing of chain-like agglomerates and filling of their voids and formation of secondary coating. The measured and modeled particle optical properties suggest that while light absorption, scattering, and the single-scattering albedo of soot particle increase during photochemical processing, their radiative forcing remains positive until the amount of nonabsorbing coating exceeds approximately 90% of the particle mass.

This study inspects the concentrations of fine particulate matter (PM2.5) mass and carbonaceous species, including organic carbon (OC) and elemental carbon (EC), as well as their thermal fractions in the Indian Himalayan glacier region at the western Himalayan region (WHR; Thajiwas glacier, 2799 m asl), central Himalayan region (CHR; Gomukh glacier, 3415 m asl), and eastern Himalayan region (EHR; Zemu glacier, 2700 m asl) sites, throughout the summer and winter periods of 2019-2020. Ambient PM2.5 samples were collected on quartz fiber filters using a low-volume sampler, followed by carbon (OC and EC) quantification using the IMPROVE_A thermal/optical reflectance methodology. Different seasonal variations in PM2.5 and carbonaceous species levels were found at all three sites investigated. Averaged PM2.5 mass ranged 55-87 mu g m-3 with a mean of 55.45 +/- 16.30 mu g m-3 at WHR, 86.80 +/- 35.73 mu g m-3 at CHR, and 72.61 +/- 24.45 mu g m-3 at EHR. Among the eight carbon fractions, high-temperature OC4 (evolved at 580 degrees C in the helium atmosphere) was the most prevalent carbon fraction, followed by low-temperature OC2 (280 degrees C) and EC1 (580 degrees C at 2% oxygen and 98% helium). Char-EC representing incomplete combustion contributed to 56, 67, and 53% of total EC, whereas soot EC contributed to 38, 26, and 43% of total EC in WHR, CHR, and EHR, respectively. The measured OC/EC ratios imply the presence of secondary organic carbon, whereas char-EC/soot-EC ratios suggested that biomass burning could be the predominant source of carbon at CHR, whereas coal combustion and vehicular emission might be dominant sources at WHR and EHR sites.

The radiative forcing of soot is dependent on the morphology, mixing state and structure. Cloud processing has been predicted to affect their mixing properties but little is known about the resulting light absorption properties. We collected ambient particles in the pre-cloud period, the cloud residues and interstitials in the in-cloud period at Mt. Tianjing (southern China). The morphology parameters of soot aggregates with varying mixing materials [sulfate (S) and organics (OM)] and mixing structures were investigated by a transmission electron microscope, and their absorption cross were calculated based on discrete dipole approximation. We found that the number contribution of soot-S decreased from 45% in the pre-cloud period to 32% in the in-cloud period, and that of soot-OM increased from 44% to 60%. Moreover, the number proportion of soot-OM with fully embedded structure increased remarkably in the in-cloud period (29%), compared with that in the pre-cloud period (3%). In addition, the soot-S aggregates became denser after in-cloud aqueous process. However, for soot-OM aggregates, the morphology remained relatively constant. The distinctly different change of soot-S and soot-OM in morphology highlights the chemically resolved reconstruction of soot morphology. Theoretical calculation further shows that the changes of soot particles in the mixing state and morphological characteristics by the cloud process resulted in the light absorption enhancement increase from 1.57 to 2.01. This study highlights that the evolution of microphysical properties upon cloud processing should also be considered in climate models to more accurately evaluate the impacts of soot particles.

The radiative forcing of dust particles in Earth atmosphere is still poorly characterized. A better estimation of the absorption cross of dust particles in the UV-visible part of the spectrum is thus needed. Among the methods used for this purpose, the Atomic Point Dipole Interaction model has the distinctive advantage of being sensitive to the atomistic geometry of the particle and to the chemical functions it contains. However, this requires an adequate parameterization of the atomic polarizabilities for all the atomic species forming the particle, over the UV-visible spectrum. In this paper, we illustrate how new methodological improvements based on quantum chemistry, allow taking into account the curvature of the carbon network in the parametrization of the carbon atomic polarizabilities, using the C-60 molecule to fit the adequate set of parameters. We thus show how this leads to significant differences in the computed curves of the absorption cross of pure carbonaceous nanoparticles as a function of the frequency, with respect to calculations performed using parameters issued from graphite.