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Aerosol single-scattering albedo (SSA) is the most critical factor for the accurately calculating of aerosol radiative effects, however, the observation of vertical profiles of SSA is difficult to realize. Current assessments of aerosol radiative effects remain uncertain because of the lack of long-term, high-resolution vertical profiles of SSA observations. High-resolution SSA vertical profiles were observed in a semi-arid region of Northwest China during winter using a tethered balloon. The observed SSA vertical profiles were used to calculate the aerosol direct radiative forcing and radiative heating rates. Significant differences in the calculated radiative forcing were found (e.g., a 48.3% relative difference for the heating effect in the atmosphere at 14:00) between the observed SSA profiles and the constant assumption with SSA = 0.90. Diurnal variations in the vertical distribution of SSA decisively influenced direct radiative forcing of aerosols. Furthermore, high-resolution vertical profiles of absorbing aerosols and meteorological parameters provide robust observational evidence of the heating effect of an elevated absorbing aerosol layer. This study provides a more accurate calculation of aerosol radiative forcing using observed aerosol SSA profiles. The scarcity of single-scattering albedo (SSA) observations is the most critical factor limiting the accurate calculations of aerosol radiative effects. A tethered balloon platform was used to obtain long-term, high-resolution observations of the SSA and estimate aerosols' radiative effects. The relative differences in the heating rate and direct radiative forcing calculations using the observed SSA and a constant assumed SSA (i.e., ignoring the vertical distribution of absorbing aerosols) were quantified. The effects of diurnal variations in the vertical distribution of SSA on aerosol direct radiative forcing are summarized. This study has important scientific implications for assessing the radiative effects of aerosols in semi-arid regions, that are highly sensitive to climate change. Tethered balloon observations acquired high-resolution vertical aerosol single-scattering albedo (SSA) profiles The assumed SSA profiles caused a 48.3% relative error in radiative forcing in the atmosphere compared to the observed profiles at 14:00 A robust observational evidence of atmospheric heating by absorbing aerosols above the boundary layer was provided

期刊论文 2024-07-28 DOI: 10.1029/2023JD040605 ISSN: 2169-897X

Absorbing aerosols and their impact on the Indian monsoon system is highly complex and demands more scientific understanding. Our study using a chemistry-coupled regional climate model (RegCM 4.5) with idealized experiments observed that natural and anthropogenic absorbing aerosols (i.e., dust and carbonaceous aerosols) reduce monsoon precipitation in a seasonal time scale. More than 1 mm day(-1) decline in mean summertime rainfall was observed over parts of the central Indian region and Indo-Gangetic plane for dust aerosol. A substantial reduction in the land-sea pressure gradient and lower tropospheric moisture distribution were found to control the observed modulation in rainfall. Near-surface wind circulation responded distinctly to natural (dust) and anthropogenic (carbonaceous) aerosols. The dust forcing weakened the monsoon trough by creating an anomalous anticyclonic circulation. The Northern Arabian Sea acted as a moisture source for the carbonaceous aerosol forcing. Intraseasonal rainfall over central India appeared to have a sharp reduction for dust forcing during early June, with a moderate increase for carbonaceous aerosols. Such quantification is essential for understanding the impact of aerosol forcing on regional climate change and the water cycle and has implications for emissions management and mitigation policies.

期刊论文 2024-02-01 DOI: 10.1016/j.scitotenv.2023.168663 ISSN: 0048-9697

Duringthe summer and winter periods of 2019-2020, we conductedsampling of fine mode ambient aerosols in the western Himalayan glacialregion (WHR; Thajiwas glacier, 2799 m asl), central Himalayan glacialregion (CHR; Gomukh glacier, 3415 m asl), and eastern Himalayan glacialregion (EHR; Zemu glacier, 2700 m asl). We evaluated the aerosol opticalproperties, which included the mass absorption coefficient, mass absorptionefficiency, mass scattering efficiency, absorption angstrom exponent,single scattering albedo, as well as their simple radiative forcingefficiencies. We observed the highest absorption in the near ultraviolet-visiblewavelength range (200-400 nm), with CHR showing the highestabsorption compared to the other two sites, WHR and EHR, respectively.Across the wavelength range of 200-1100 nm, the overall contributionof black carbon to light attenuation was greater than that of browncarbon. However, brown carbon dominated the absorption in the nearUV-visible wavelengths, providing evidence of its non-trivialpresence over the Himalayan region. Additionally, we observed a positiveradiative forcing (W/g), which leads to net warming at these sites.The findings of this ground-based study contribute to our understandingof the light-absorbing nature of carbonaceous aerosols and their impacton the Himalayan glacier regions.

期刊论文 2023-08-08 DOI: 10.1021/acsearthspacechem.3c00088 ISSN: 2472-3452

This study employs a fully coupled meteorology-chemistry-snow model to investigate the impacts of light-absorbing particles (LAPs) on snow darkening in the Sierra Nevada. After comprehensive evaluation with spatially and temporally complete satellite retrievals, the model shows that LAPs in snow reduce snow albedo by 0.013 (0-0.045) in the Sierra Nevada during the ablation season (April-July), producing a midday mean radiative forcing of 4.5 W m(-2) which increases to 15-22 W m(-2) in July. LAPs in snow accelerate snow aging processes and reduce snow cover fraction, which doubles the albedo change and radiative forcing caused by LAPs. The impurity-induced snow darkening effects decrease snow water equivalent and snow depth by 20 and 70 mm in June in the Sierra Nevada bighorn sheep habitat. The earlier snowmelt reduces root-zone soil water content by 20%, deteriorating the forage productivity and playing a negative role in the survival of bighorn sheep.

期刊论文 2022-06-16 DOI: 10.1029/2022GL098102 ISSN: 0094-8276

Recent increases in surface temperature and snow melt acceleration in the Himalayan region are influenced by many factors. Here we investigate the influence of absorbing aerosols, including black carbon and dust, on surface temperature and snow melt in western, central, and eastern parts of the India-Nepal Himalayan region (INHR). We compare 40-y simulations (1971-2010) one with all evolving forcing agents representative of a present-day aerosol scenario, compared to a low aerosol forcing scenario. The difference between these scenarios shows a significant increase in surface air temperature, with higher warming in parts of Western and Central Himalaya (-0.2-2 degrees C) in the months of April and May. Higher absorbing aerosol (BC and dust abundance) both at the surface and in the atmospheric column, in the present-day aerosol simulations, led to increases in atmospheric radiative forcing and surface shortwave heating rate forcing (SWHRF), compared to the low aerosol forcing case. Therefore, the absorbing aerosols cause anomalous atmospheric heat energy transfer to land due to high surface SWHRF and changes in surface energy flux, leading to snow melt. The present model version did not parameterize snow albedo feedback, which would increase the magnitudes of the changes simulated here. (C) 2021 Elsevier B.V. All rights reserved.

期刊论文 2022-03-01 DOI: 10.1016/j.scitotenv.2021.151299 ISSN: 0048-9697

Aerosol absorption constitutes a significant component of the total radiative effect of aerosols, and hence its representation in general circulation models is crucial to radiative forcing estimates. We use here multiple observations to evaluate the performance of CAM5.3-Oslo with respect to its aerosol representation. CAM5.3-Oslo is the atmospheric component of the earth system model NorESM1.2 and shows on average an underestimation of aerosol absorption in the focus region over East and South Asia and a strong aerosol absorption overestimation in desert and arid regions compared to observations and other AeroCom phase III models. We explore the reasons of the model spread and find that it is related to the column burden and residence time of absorbing aerosols, in particular black carbon and dust. We conduct further sensitivity simulations with CAM5.3-Oslo to identify processes which are most important for modelled aerosol absorption. The sensitivity experiments target aerosol optical properties, and contrast their impact with effects from changes in emissions and deposition processes, and the driving meteorology. An improved agreement with observations was found with the use of a refined emission data set, transient emissions and assimilation of meteorological observations. Changes in optical properties of absorbing aerosols can also reduce the under- and overestimation of aerosol absorption in the model. However, changes in aerosol absorption strength between the sensitivity experiments are small compared to the inter-model spread among the AeroCom phase III models.

期刊论文 2021-05-10 DOI: 10.1080/16000889.2021.1909815 ISSN: 1600-0889

Heat waves in India during the pre-monsoon months have significant impacts on human health, productivity and mortality. While greenhouse gas-induced global warming is believed to accentuate high temperature extremes, anthropogenic aerosols predominantly constituted by radiation-scattering sulfate are believed to cause an overall cooling in most world regions. However, the Indian region is marked by an abundance of absorbing aerosols, such as black carbon (BC) and dust. The goal of this work was to understand the association between aerosols, particularly those that are absorbing in nature, and high-temperature extremes in north-central India during the pre-monsoon season. We use 30-year simulations from a chemistry-coupled atmosphere-only general circulation model (GCM), ECHAM6-HAM2, forced with evolving aerosol emissions in an interactive aerosol module, along with observed evolving SSTs. A composite of high-temperature extremes in the model simulations, compared to climatology, shows large-scale conditions conducive to heat waves. Importantly, it reveals concurrent positive anomalies of BC and dust aerosol optical depths. Changes in near-surface properties include a reduction in single scattering albedo (implying greater absorption) and enhancement in short-wave heating rate, compared to climatological conditions. Alterations in surface energy balance include reduced latent heat flux, but increased sensible heat flux, consistent with enhanced temperatures. Thus, chemistry-coupled GCM simulations capture an association of absorbing aerosols with high-temperature extremes in north India, arising from radiative heating in the surface layer.

期刊论文 2021-01-01 DOI: 10.1002/joc.6783 ISSN: 0899-8418

Light-absorbing aerosols (LAAs), mainly composed of black carbon (BC) and dust aerosols, are responsible for significant climate forcing through their strong absorption of solar radiation. A fully coupled meteorology-chemistry model (WRF-Chem) associated with satellite retrievals and in situ measurements is used to investigate the direct radiative forcing (DRF) induced by LAAs in different climate regions over East Asia. Results show that the annual all-sky dust and BC DRF are -0.84 and 1.06 W m(-2)at the top of atmosphere (TOA), -1.23 and -1.55 W m(-2)at the surface (SUR), and 0.39 and 2.61 W m(-2)within the atmosphere (ATM) over East Asia. Large LAAs DRF can be found in hyper-arid, subhumid, and humid regions at the SUR and ATM where dust DRF dominates the surface cooling effect, while BC DRF is predominant in the eminent warming effect on ATM in most climate regions. The meteorological conditions in hyper-arid region are associated with enhanced surface wind and weakened atmospheric wind, which is in favor of the emission and accumulation of dust supporting the positive LAAs DRF anomalies higher than 10 W m(-2)in hyper-arid region. The positive geopotential height anomalies over Northeast China weaken the westerly winds, which is beneficial to the accumulation of LAAs, and results in the positive LAAs DRF anomalies of 3 W m(-2)in semiarid regions. The large LAAs mass loading, strong aerosol absorptive ability, and decreased cloudiness caused by northerly anomalies are responsible for the high LAAs DRF in humid region.

期刊论文 2020-07-27 DOI: 10.1029/2019JD032228 ISSN: 2169-897X

Methods for determining aerosol types in cases where chemical composition measurements are not available are useful for improved aerosol radiative forcing estimates. In this study, two aerosol characterization methods by Cazorla et al. (2013, https://doi.org/10.5194/acp-13-9337-2013; CA13) and Costabile et al. (2013,10.5194/acp-13-2455-2013; CO13) using wavelength-dependent particle absorption and scattering are used, to assess their applicability and examine their limitations. Long-term ambient particle optical property and chemical composition (major inorganic ions and bulk carbon) measurements from the Maldives Climate Observatory Hanimaadhoo as well as concurrent air mass trajectories are utilized to test the classifications based on the determined absorption angstrom ngstrom exponent, scattering angstrom ngstrom exponent, and single scattering albedo. The resulting aerosol types from the CA13 method show a good qualitative agreement with the particle chemical composition and air mass origin. In general, the size differentiation using the scattering angstrom ngstrom exponent works very well for both methods, while the composition identification depending mainly on the absorption angstrom ngstrom exponent can result in aerosol misclassifications at Maldives Climate Observatory Hanimaadhoo. To broaden the applicability of the CA13 method, we suggest to include an underlying marine aerosol group in the classification scheme. The classification of the CO13 method is less clear, and its applicability is limited when it is extended to aerosols in this environment at ambient humidity.

期刊论文 2019-08-16 DOI: 10.1029/2018JD029685 ISSN: 2169-897X

Light-absorbing components of atmospheric aerosols have gained particular attention in recent years due to their climatic and environmental effects. Based on two-year measurements of aerosol absorption at seven wavelengths, aerosol absorption properties and black carbon (BC) were investigated in the North China Plain (NCP), one of the most densely populated and polluted regions in the world. Aerosol absorption was stronger in fall and the heating season (from November to March) than in spring and summer at all seven wavelengths. Similar spectral dependence of aerosol absorption was observed in non-heating seasons despite substantially strong absorption in fall. With an average absorption Angstrom exponent (alpha) of 1.36 in non-heating seasons, freshly emitted BC from local fossil fuel burning was thought to be the major component of light-absorbing aerosols. In the heating season, strong ultraviolet absorption led to an average alpha of 1.81, clearly indicating the importance of non-BC light-absorbing components, which were possibly from coal burning for domestic heating and aging processes on a regional scale. Diurnally, the variation of BC mass concentrations experienced a double-peak pattern with a higher level at night throughout the year. However, the diurnal cycle of alpha in the heating season was distinctly different from that in non-heating seasons. a peaked in the late afternoon in non-heating seasons with concomitantly observed low valley in BC mass concentrations. In contrast, alpha peaked around the midnight in the heating season and lowered down during the daytime. The relationship of aerosol absorption and winds in non-heating seasons also differed from that in the heating season. BC mass concentrations declined while alpha increased with increasing wind speed in non-heating seasons, which suggested elevated non-BC light absorbers in transported aged aerosols. No apparent dependence of alpha on wind speed was found in the heating season, probably due to well mixed regional pollution. Pollution episodes were mostly encountered under low winds and had a low level of alpha, implying aerosol absorption should be largely attributed to freshly emitted BC from local sources under such conditions. Extensive field campaigns and long-term chemical and optical measurements of light-absorbing aerosols are needed in the future to further advance our understanding on optical properties of light-absorbing aerosols and their radiative forcing in this region. (C) 2016 The Authors. Published by Elsevier Ltd.

期刊论文 2016-10-01 DOI: 10.1016/j.atmosenv.2016.07.014 ISSN: 1352-2310
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