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Light-absorbing carbonaceous aerosols, comprising black carbon (BC) and brown carbon (BrC), significantly influence air quality and radiative forcing. Unlike traditional approaches that use a fixed value of absorption & Aring;ngstrom exponent (AAE), this study investigated the absorption and optical properties of carbonaceous aerosols in Beijing for both local emission and regional transport events during a wintertime pollution event by using improved AAE results that employs wavelength-dependent AAE (WDA). By calculating the difference of BC AAE at different wavelengths using Mie theory and comparing the calculated results to actual measurements from an Aethalometer (AE31), a more accurate absorption coefficient of BrC can be derived. Through the analysis of air mass sources, local emission was found dominated the pollution events during this study, accounting for 81 % of all cases, while regional transport played a minor role. Carbonaceous aerosols exhibited a continuous increasing trend during midday, which may be attributed to the re-entrainment of nighttime-accumulated carbonaceous aerosols to the surface during the early planetary boundary layer (PBL) development phase, as the mixed layer rises, combined with the variation of PBL and anthropogenic activity. At night, variations in the PBL height, in addition to anthropogenic activities, effectively contributed to surface aerosol concentrations, leading to peak surface aerosol values during local pollution episodes. The diurnal variation of AAE470/880 exhibited a decreasing trend, with a total decrease of approximately 12 %. Furthermore, the BrC fraction showed a constant diurnal variation, suggesting that the declining AAE470/880 was primarily influenced by BC, possibly due to enhanced traffic contributions.

期刊论文 2026-01-01 DOI: 10.1016/j.atmosenv.2025.121616 ISSN: 1352-2310

The long-term trend for aerosol optical properties and climate impact sensitivity in terms of radiative forcing efficiency were analyzed at a suburban station in Athens, Southeast Mediterranean, using an extensive dataset from 2008 to 2022. The study examined scattering (nsc) and absorption (nap) coefficients, scattering & Aring;ngstrom exponent (SAE), absorption & Aring;ngstrom exponent (AAE), single scattering albedo (SSA), asymmetry parameter (g), and radiative forcing efficiency (RFE). Seasonal variability was linked to meteorological conditions and human activities. Single Scattering Albedo (SSA) was lowest (0.86), and Radiative Forcing Efficiency (RFE) was highest (-61 W/m2) in winter, confirming enhanced contributions from traffic and biomass burning. Lower SAE values (1.5) in spring indicate a greater presence of coarse particles due to frequent Saharan dust events (SDEs). Daily patterns of nap and SSA reflect local emissions, with pronounced traffic-related peaks. Aerosol classification revealed that Black Carbon (BC) dominates the suburban aerosol (51 %), with mixed BrC-BC (16 %) peaking in winter and dust-pollution mixtures (13 %) increasing in spring. The presence of large particles mixed with BC (11 %) was more frequent in spring, further highlighting seasonal variability. Trend analysis showed statistically significant (ss) decreases in nsc (-0.611) and SSA (-0.003), alongside increases in nap (+0.027) and RFE (+0.270) at a 95 % confidence level, suggesting a shift toward more absorbing aerosols. The findings provide new insights and reveal a new aerosol regime, where a reduction in anthropogenic emissions is affecting the scattering rather than the absorbing aerosol component, while the impact from forest fires as a climate feedback mechanism has a significant effect in the Eastern Mediterranean. It is important for future studies and climate modelling to account for the regionally observed changes of the state of mixing of ambient aerosol leading to a shift in radiative forcing efficiency through the reduction in SSA. This is evident in the long term for the east Mediterranean region and must be accounted for in radiative forcing estimates and future climate projections.

期刊论文 2026-01-01 DOI: 10.1016/j.atmosenv.2025.121633 ISSN: 1352-2310

The aerosol scattering phase function (ASPF), a crucial element of aerosol optical properties, is pivotal for radiative forcing calculations and aerosol remote sensing detection. Current detection methods for the ASPF include multi-sensor detection, single-sensor rotational detection and imaging detection. However, these methods face challenges in achieving high-resolution full-angle measurement, particularly for small forward (i.e., less than 10 degrees) or backward (i.e., more than 170 degrees) scattering angles in open path. In this work, a full-angle ASPF detection system based on the multi-field-of-view Scheimpflug lidar technique has been proposed and demonstrated. A 450 nm continuous-wave semiconductor laser was utilized as the light source and four CMOS image sensors were employed as detectors. To detect the full-angle ASPF, four receiving units capture angular scattering signals across different angle ranges, namely 0 degrees-20 degrees, 10 degrees-96 degrees, 84 degrees-170 degrees, 160 degrees-180 degrees, respectively. The influence of the relative illumination and angular response of the used image sensors have been corrected, and a signal stitching algorithm was developed to obtain a complete 0-180 degrees angular scattering signal. Atmospheric measurements have been conducted by employing the full-angle ASPF detection system in open path. The experimental results of the ASPF have been compared with the AERONET data from the Socheongcho station and simulated ASPF based on the typical aerosol models in mainland China, showing excellent agreement. The promising results demonstrated in this work have shown a great potential for detecting the full-angle ASPF in open path.

期刊论文 2025-12-01 DOI: 10.1016/j.optlastec.2025.113386 ISSN: 0030-3992

The present study performed classification global aerosols based on particle linear depolarization ratio (PLDR) and single scattering albedo (SSA) provided from AErosol RObotic NETwork (AERONET) Version 3.0 and Level 2.0 inversion products of 171 AERONET sites located in six continents. Current methodology could distinguish effectively between dust and non-dust aerosols using PLDR and SSA. These selected sites include dominant aerosol types such as, pure dust (PD), dust dominated mixture (DDM), pollution dominated mixture (PDM), very weakly absorbing (VWA), strongly absorbing (SA), moderately absorbing(MA), and weakly absorbing (WA). Biomass-burning aerosols which are associated with black carbon are assigned as combinations of WA, MA and SA. The key important findings show the sites in the Northern African region are predominantly influenced by PD, while south Asian sites are characterized by DDM as well as mixture of dust and pollution aerosols. Urban and industrialized regions located in Europe and North American sites are characterized by VWA, WA, and MA aerosols. Tropical regions, including South America, South-east-Asia and southern African sites which prone to forest and biomass-burning, are dominated by SA aerosols. The study further examined the impacts by radiative forcing for different aerosol types. Among the aerosol types, SA and VWA contribute with the highest (30.14 +/- 8.04 Wm-2) and lowest (7.83 +/- 4.12 Wm-2) atmospheric forcing, respectively. Consequently, atmospheric heating rates are found to be highest by SA (0.85 K day-1) and lowest by VWA aerosols (0.22 Kday-1). The current study provides a comprehensive report on aerosol optical, micro-physical and radiative properties for different aerosol types across six continents.

期刊论文 2025-12-01 DOI: 10.1016/j.atmosenv.2025.121530 ISSN: 1352-2310

The recent large reduction in anthropogenic aerosol emissions across China has improved China's air quality but has potential consequences for climate forcing. This sharp reduction in anthropogenic emissions has occurred against a background influenced by changing regional biomass burning emissions over a similar period of time. Here, we use the UK Earth System Model (UKESM) to estimate aerosol instantaneous radiative forcing (IRF) due to changes in emissions of aerosols and precursors from biomass burning and anthropogenic sources (separately and in combination) over 2008-2016, with a focus on China and regions downwind. We also separately quantify the IRF due to changes in anthropogenic aerosol emissions inside China (CHN) and the Rest Of the World (ROW). Reductions in Chinese anthropogenic emissions of BC, SO2 and OC contributed -0.30 +/- 0.01, +1.00 +/- 0.04, and +0.05 +/- 0.01 W m-2, respectively to IRF over China, accounting for similar to 97% of the total local anthropogenic aerosol IRF. These emission changes contributed a remote regional IRF of 0.22 +/- 0.04 W m-2 over the North Pacific Ocean. The reduction in SO2 emissions from China contributed a global IRF of equal magnitude to that from SO2 emissions from ROW (similar to 0.08 W m-2). Changes in global biomass burning emissions contributed 0.03 W m-2 (equivalent to over 20% of the magnitude of anthropogenic aerosol IRF), enhancing the global anthropogenic aerosol IRF, whereas they partly offset the anthropogenic IRF over China. Meanwhile, biomass burning emissions dominated the total IRF (around 98%) over the Arctic.

期刊论文 2025-11-18 DOI: 10.1029/2025JD044548 ISSN: 2169-897X

This study investigates the inter-annual variability of carbonaceous aerosols (CA) over Kolkata, a megacity in eastern India, using dual carbon isotopes (C-14 and C-13) alongside measurements of the optical properties of brown carbon (BrC). Sampling was conducted during the post-monsoon, winter, and spring seasons over two consecutive years (2020-21 and 2021-22). The analysis reveals that PM2.5 and CA concentrations were higher in 2020-21 (194 +/- 40 and 54 +/- 15 mu g m(-3), respectively) compared to 2021-22 (141 +/- 31 and 44 +/- 21 mu g m(-3)), likely due to higher precipitation in 2021-22. The contribution of biomass burning and biogenic sources to CA (f(bio_TC)) was slightly higher in 2020-21 (70 +/- 3 %) than in 2021-22 (68 +/- 3 %), with both years exhibiting a consistent decreasing trend from post-monsoon to spring. Observed lower values for oxidised CA proxies, such as the WSOC/OC ratio (0.41 +/- 0.08) and AMS-derived f(44) (0.13 +/- 0.02), throughout the study period suggest that surface CA over Kolkata primarily originates from local sources rather than long-range transport. The relative radiative forcing (RRF) also showed a clear reduction in the subsequent year; however, on average, the RRF of methanol-soluble BrC (16 +/- 6 %) was approximately three times higher than that of the water-soluble fraction (5.5 +/- 2.2 %), highlighting the substantial role of BrC in influencing regional radiative forcing. These findings underscore the substantial impact of local emissions over transported pollutants on Kolkata's ground-level air quality.

期刊论文 2025-11-15 DOI: 10.1016/j.atmosenv.2025.121458 ISSN: 1352-2310

Black carbon (BC) is a major pollutant entering the human body through PM2.5 and posing major health effects. India lying in the Asia region is a major contributor to BC emissions from the combustion of biofuels. BC present in the atmosphere is a pollutant deteriorating air quality and is a light-absorbing aerosol (LAA), thus playing a dual role. In India, several studies have been published quantifying BC concentration. The optical measurement of BC has been carried out at multiple locations in India, and its radiative effect has been studied using the Santa Barbara DISORT Atmospheric Radiative Transfer (SBDART) model. This review is an attempt to collate those studies that have measured BC and estimated its radiative effect. The BC levels, spectral Aerosol Optical Depth (AOD), single scattering albedo (SSA) and direct radiative forcing (DRF) at the top of the atmosphere (TOA), at the surface (SUR) and heat within the atmosphere (ATM) for 20 years (2002 to 2023) have been analysed. It was found that many studies for performing DRF calculations have not used BC measurements and have used AOD analysis to characterise the sources of aerosols as direct BC measurements are not required to estimate the DRF. The selection of AOD wavelength 500 nm or 550 nm is not clear in the literature for BC-RF calculations and needs to be standardised for DRF. IPCC AR6 has estimated Effective Radiative Forcing (ERF) due to BC with temperature and surface feedbacks, and future studies for ERF need to use climate models with tools like WRF-Chem. The source of BC is mostly from fossil fuel or biomass burning during the winter season, while it is dust aerosols during the summer. Biomass burning, use of traditional cook stoves and aerosol episodes contribute to the warming of the ambient environment. Beijing, China, has reduced ATM forcing in the summer when compared to Delhi, India, and has reduced the fraction of heat exerted in the atmosphere. The interactions of BC-UHI are not studied yet in India, and with the ARFINET network, an attempt can be made in this direction. The Urban Pollution Island (UPI)-Urban Heat Island (UHI) review identified PM2.5 contributing to UHI intensity during the summer and winter in metro cities, while BC-UHI interactions are not dealt with in detail.

期刊论文 2025-11-07 DOI: 10.1007/s44273-025-00062-3 ISSN: 1976-6912

This study analyzes the aerosol and precipitable water vapor (PWV) properties at six sites in the Indo-Gangetic Plains (IGP), a densely populated and highly polluted region. The main objective is to explore how the columnar PWV is related to the attenuation of shortwave solar radiation (SWR), as well as the combined role of aerosol properties and PWV on radiative forcing based on AERONET data and model (SBDART) simulations. The analysis revealed high aerosol optical depth (AOD) values (0.4-0.6) throughout the year in all the sites, associated with increased PWV (4-5 cm) during the summer monsoon. Comprehensive investigation shows that changes in PWV levels also affect aerosols' size distribution, optical properties and radiation balance in a similar way - but in different magnitudes - between the examined sites. The water vapor radiative effect (WVRE) is highly dependent on aerosol presence, with its magnitude for both surface (-130 to -140 Wm(-2)) and atmospheric forcing becoming higher under clean atmospheres (without aerosols). Aerosol presence is also considered in the computations of the WVRE. In that case, the WVRE becomes more pronounced at the top of the atmosphere (TOA) (30 to 35 Wm(-2)) but exhibits a lower forcing impact on the surface (about -45 Wm(-2)) and within the atmosphere (70-80 Wm(-2)), suggesting important aerosol-PWV interrelations. The atmospheric heating rate due to PWV is more than double (3.5-4.5 K Day(-1)) that of aerosols (1-1.9 K Day(-1)), highlighting its essential role in radiative effects and climate implications over the IGP region. The radiative impacts of PWV and aerosols are further examined as a function of the single scattering albedo, solar zenith angle, and absorbing AOD at the different sites, revealing dependence on both astronomical and atmospheric variables related to aerosol absorption, thus unravelling the combined role of aerosols and PWV in climate implications.

期刊论文 2025-11-01 DOI: 10.1016/j.atmosres.2025.108343 ISSN: 0169-8095

Characterizing vertical profiles of in-situ particle properties is relevant because being only based on the surface or column-integrated measurements cannot unambiguously conclude the radiative impact on aerosol. Vertical profiles of in-situ aerosol properties on-board an unmanned aerial vehicle (UAV) were measured above El Arenosillo (37.1 N,-6.7 W) in the southwest of Spain during four flight missions. Measured properties included particle number size distribution, total particle concentration and multiwavelength absorption coefficient up to 3100 m during cold season (February 4, 2022 and December 11, 2023) and warm season (September 20, 2023 and April 2, 2024). The heterogeneity of particle properties has been shown around two types of events: a mineral particle event of desert origin during cold season and a new particle formation event during warm season. During cold season, a comparison between the flight missions with and without desert dust episodes shows that mineral particles decrease the planetary boundary layer (PBL) height. This behavior is probably related to absorber particles aloft atmosphere, which traps solar radiation and heat up the upper layer of the atmosphere and deteriorates the vertical dispersion. In the literature, this effect is called as 'dome effect'. During warm season, new particle formation was observed above PBL. This event could be related to the presence of precursor gases in the residual layer, and enhanced by a low concentration of pre-existing particles. The characteristic parameter during the observed event was the fine-to-total particle volume concentration ratio close to zero. These observations highlight the necessity to establish a long-term multi-temporal monitoring of vertical profiles for atmospheric parameters onboard UAV systems and to integrate in Earth observations networks. For example, radiative forcing is usually estimated from surface data, but the heterogeneity in the vertical profiles of atmospheric particles properties, which are used to the forcing quantification, is a result of inaccuracies.

期刊论文 2025-11-01 DOI: 10.1016/j.atmosres.2025.108316 ISSN: 0169-8095

The direct radiative impact of atmospheric aerosols remains more uncertain than that of greenhouse gases, largely due to the complex transformations' aerosols undergo during atmospheric aging. Sulfate aerosols have been the subject of considerable research, with a robust body of literature characterising their cooling effect. In contrast, the light-absorbing properties and warming potential of black carbon and related products remain less well understood, with limited research available to date. The present study examines the iron-catalyzed reaction of catechol in levitated microdroplets, tracked in situ using elastic light scattering spectroscopy. The reaction forms water-insoluble polycatechol aggregates, which drive a transition from homogeneous spheres to heterogeneous droplets with internal inclusions. To interpret the evolving optical behaviour, the Multiple Sphere T-Matrix (MSTM) model is employed, a method which overcomes the limitations of Mie theory by accounting for internal morphological complexity. The model provides realistic complex refractive indices and fractal parameters, though it should be noted that its solutions are not unique due to sensitivity to input assumptions and droplet variability. This underscores the necessity for supplementary measurements and more comprehensive models incorporating evaporation, chemical dynamics, and phase transitions. These findings emphasise the potential of elastic scattering spectroscopy for real-time monitoring of multiphase chemistry and offer new constraints for improving aerosol aging schemes in climate models, thereby contributing to reduced uncertainties in aerosol radiative forcing.

期刊论文 2025-11-01 DOI: 10.1016/j.jaerosci.2025.106659 ISSN: 0021-8502
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