The significant uncertainties of Black Carbon (BC) radiative forcing are becoming an obstacle to the evaluation of their impacts and mitigation measures. One of the crucial reasons for this uncertainty could be the poorly constrained BC vertical profile. The BC has a lifetime of a few days to weeks and there is a clear pointer that it can be vertically transported through convection besides the horizontal advection. The present study aims for the intercomparison between the BC mass concentrations obtained through the aircraft-based observations and that derived from the selected Copernicus Atmosphere Monitoring Service (CAMS) reanalysis data over the three different locations of India, which is one of the largest emitters of BC aerosols. The aircraft-based BC observations were conducted from 0.5 to 7 km altitudes using Aethalometer during CAIPEEX (Cloud Aerosol Interaction and Precipitation Enhancement Experiment) Phase I campaigns from June to September 2009. The output of the present study suggests the CAMS reanalysis data significantly underestimated BC mass throughout the vertical profile with an average mass normalized mean bias of greater than -70% at all three locations. Furthermore, the vertical radiative forcing and heating rates of BC were also calculated for both observation and reanalysis data. The output depicts the net forcing due to CAMS simulated BC in all the layers were 1-12 folds lower over all the study regions compared with observed BC aerosols. Likewise, the estimated mean biases in heating rate were in the range of -0.001 to -0.190 K day(-1) for all the vertical layers over the study locations. The possible reasons for these disparities could be poorly constrained emissions, especially aircraft emissions and/or their transformation schemes in aerosol modules. The present study emphasized that the validation of the vertical profile is also an essential factor for better constraints of the BC aerosols in climate models.

In this study, we investigated the aerosol radiative forcing (ARF) using ground-based measurements of PM2.5 and black carbon aerosols at a semi-arid, rain shadow location, Solapur in peninsular India. It is observed that aerosols caused a net cooling effect at top of the atmosphere (TOP) indicating that the aerosols reflect more solar radiation back to space than they absorb. At the surface, the aerosols caused a net cooling effect indicating more presence of scattering type aerosols. The resulting ARF of the aerosols was found to be ranging from +38 Wm-2 in monsoon to +53 Wm-2 in pre-monsoon indicating trapping of energy which resulted in a warming of the atmosphere. However, BC -only forcing indicated a significant warming effect at TOP as well as in the atmosphere which showed the potential of the absorbing carbonaceous aerosols. Overall, BC was responsible for 44% and 32% of the composite ARF, even though it formed only 7% and 2% of composite aerosol in the dry and wet periods, respectively. The warming impact of BC aerosols was also manifested in terms of their contribution to aerosol radiative forcing efficiency (ARFE) which was about four times more for BC-only than that for composite aerosols. More atmospheric heating rates were observed during dry periods for composite and BC-only aerosols than during wet period. These findings have important implications for aerosol-cloud-precipitation studies as well as the atmospheric thermodynamics and hydrological cycle over this semi-arid region where the total aerosol load is not significant and rainfall amount is scarce.

Light-absorbing aerosols (LAA) impact the atmosphere by heating it. Their effect in the Arctic was investigated during two summer Arctic oceanographic campaigns (2018 and 2019) around the Svalbard Archipelago in order to unravel the differences between the Arctic background and the local anthropic settlements. Therefore, the LAA heating rate (HR) was experimentally determined. Both the chemical composition and high-resolution measurements highlighted substantial differences between the Arctic Ocean background (average eBC concentration of 11.7 +/- 0.1 ng/m3) and the human settlements, among which the most impacting appeared to be Tromso and Isfjorden (mean eBC of 99.4 +/- 3.1 ng/m3). Consequently, the HR in Isfjorden (8.2 x 10-3 +/- 0.3 x 10-3 K/day) was one order of magnitude higher than in the pristine background conditions (0.8 x 10-3 +/- 0.9 x 10-5 K/day). Therefore, we conclude that the direct climate impact of local LAA sources on the Arctic atmosphere is not negligible and may rise in the future due to ice retreat and enhanced marine traffic.

This study reports black carbon (BC) characteristics and climate effects for a 22-month period during 2018-2020 at a receptor location in the eastern Indo-Gangetic Plains (IGP). The overall averaged BC mass concentration was 7.8 & PLUSMN; 4.7 & mu;g m- 3, and the nighttime average (9.1 & PLUSMN; 6.1 & mu;g m- 3) was nearly double that of the daytime (5.8 & PLUSMN; 3.5 & mu;g m- 3). BC was most enhanced during winter, with mean concentration (14.3 & PLUSMN; 3.8 & mu;g m- 3) higher by 4 times as compared to summer. A two-component mixing model, frequency distribution of the Angstrom exponent, and a simultaneous increase in brown carbon (BrC) absorption coefficient suggested that this enhancement was mostly due to the biomass burning (BB) fraction of BC. CALIPSO-derived products showed that the extinction coefficient was highest at 0.62 & PLUSMN; 0.31 km-1 in winter and lowest at 0.12 & PLUSMN; 0.05 km-1 in summer. Backscatter plots and particle depolarization ratios indicated presence of spherical dust particles during summer and smoke plumes during post-monsoon and winter. Concentration-weighted trajectories (CWTs) helped in quantifying significant contributions of the IGP outflow to BC, BC-BB and BrC absorption. Finally, a large direct radiative forcing of the atmosphere by BC (37 & PLUSMN; 22 W m- 2) was estimated via the radiative transfer model SBDART, with an associated atmospheric heating rate of 1.02 K d-1.

This paper presents the results of the study on columnar aerosol optical and physical properties and radiative effects directly observed over Dushanbe, the capital city of Tajikistan, a NASA AERONET site (equipped with a CIMEL sunphotometer) in Central Asia. The average aerosol optical depth (AOD) and Angstrom exponent (AE) during the observation period from July 2010 to April 2018 were found to be 0.28 +/- 0.20 and 0.82 +/- 0.40, respectively. The highest seasonal AOD (0.32 +/- 0.24), accompanied by the lowest average AE (0.61 +/- 0.25) and fine-mode fraction in AOD (0.39), was observed during summer due to the influence of coarse particles like dust from arid regions. Fine particles were found in significant amounts during winter. The 'mixed aerosol' was identified as the dominant aerosol type with presence of 'dust aerosol' during summer and autumn seasons. Aerosol properties like volume size distribution, single scattering albedo, asymmetry parameter and refractive index suggested the influence of coarse particles (during summer and autumn). Most of the air masses reaching this site transported local and regional emissions, including from beyond Central Asia, explaining the presence of various aerosol types in Dushanbe's atmosphere. The seasonal aerosol radiative forcing efficiency (ARFE) in the atmosphere was found high (>100 Wm(-2)) and consistent throughout the year. Consequently, this resulted in similar seasonally coherent high atmospheric solar heating rate (HR) of 1.5 K day(-1) during summer-autumn-winter, and ca. 0.9 K day(-1) during spring season. High ARFE and HR values indicate that atmospheric aerosols could exert significant implications to regional air quality, climate and cryosphere over the central Asian region and downwind Tianshan and Himalaya-Tibetan Plateau mountain regions with sensitive ecosystems. (C) 2020 Elsevier Ltd. All rights reserved.

A comprehensive study on classifying the aerosol types and absorbing aerosol types, and quantifying the effect of absorbing aerosols on aerosol optical and radiative properties using four years (2015-2016, 2018-2019) of high-quality Aerosol Robotic Network (AERONET) datasets over Kanpur (urban) and Gandhi College (rural) in the Indo-Gangetic Plain (IGP) region is conducted on a seasonal scale, for the first time. Biomass burning (BB), urban-industrial, and mixed aerosol types are always present, whereas dust aerosol and mostly dust absorbing aerosol types are only present in pre-monsoon and monsoon seasons. During winter and post-monsoon seasons, BB aerosols andmostly black carbon (MBC) absorbing aerosols dominate, and the contribution of aerosol optical depth (AOD) and single scattering albedo (SSA) corresponding to MBC to total AOD and SSA are higher. SSA for MBC varies over a broader range due to mixing of BC with water-soluble aerosols. During pre-monsoon and monsoon seasons, mixing of dust with anthropogenic aerosols increases the amount of mixed aerosol type. Surface cooling and atmospheric heating efficiency for mixed aerosols are higher than MBC and dust aerosols due to enhancement in aerosol absorption over both locations. Seasonal analysis of aerosol radiative properties showed that during winter and post-monsoon, MBC absorbing aerosols are the major contributor in controlling/influencing the total aerosol radiative forcing (ARF) and heating rate (HR). During the other seasons, each absorbing aerosol type significantly influences ARF depending on their AOD and SSA values. In addition to Kanpur and Gandhi College, data from seven other AERONET sites located at Karachi, Lahore, Jaipur, Lumbini, Pokhara, Bhola, and Dhaka in South Asia are analysed to conduct a regional-scale examination of aerosol optical parameters and radiative effects due to different absorbing aerosol types. As the aerosol characteristics and trends are similar over these sites, the findings from such a regional-scale analysis can be an appropriate representative for the South Asian region. The regional analysis revealed that the annual mean atmospheric ARF (ARF(ATM)) and ARF efficiency (ARFE(ATM)), and HR are higher for MBC, followed by mixed and MD aerosols over South Asia due to higher AOD, and higher absorbing efficiency of MBC aerosols. In comparison, mixed aerosols exhibit higher ARF(ATM) over East Asia. This quantification of absorbing aerosol types over a global aerosol hotspot will be useful for an accurate quantification of climate impacts of aerosols.

The study examines the thermodynamic structure of the marine atmospheric boundary layer (MABL) and its effect on the aerosol dynamics in the Indian Ocean sector of Southern Ocean (ISSO) between 30 degrees S-67 degrees S and 57 degrees E-77 degrees E. It includes observations of aerosols and meteorology collected during the Xth Southern Ocean Expedition conducted in December 2017. The results revealed the effect of frontal-region-specific air-sea coupling on the thermodynamic structure of MABL and its role in regulating aerosols in ISSO. The MABL over the subtropical front was unstable and formed a well-evolved mixed layer ( 2400 m) capped by low-level inversions ( 660 m). Convective activities in the Sub-Antarctic Frontal region were associated with the Agulhas Retroflection Current, which supported the forma-tion of a well-developed mixed layer ( 1860 m). The mean estimates of aerosol optical depth (AOD) and black carbon (BC) mass concentrations were 0.095 +/- 0.006 and 50 +/- 14 ng m-3, respectively, and the resultant clear sky direct shortwave radiative forcing (DARF) and atmospheric heating rate (HR) were 1.32 +/- 0.11 W m-2 and 0.022 +/- 0.002 K day-1, respectively. In the polar front (PF) region, frequent mid-latitude cyclones led to highly stabilized MABL, supported low-level multi-layered clouds (>3-layers) and multiple high-level inversions (strength > 0.5 K m-1 > 3000 m). The clouds were mixed-phased with temperatures less than -12 degrees C at 3000 m altitude. Interestingly, there was higher loading of dust and BC aerosols (276 +/- 24 ng m-3), maximum AOD (0.109 +/- 0.009), clear sky DARF (1.73 +/- 0.02 W m-2), and HR (0.029 +/- 0.005 K day-1). This showed an accumulation of long-range advected anthro-pogenic aerosols within baroclinic-boundaries formed over the PF region. Specifically, in the region south of PF, weak convection caused weakly-unstable MABL with a single low-level inversion followed by no clouds/single-layer clouds. Predominant clean maritime air holding a small fraction of dust and BC accounted for lower estimates of AOD (0.071 +/- 0.004), BC concentrations (90 +/- 55 ng m-3) and associated clear sky DARF and HR were 1.16 +/- 0.06 W m-2 and 0.019 +/- 0.001 K day-1, respectively.

Multi year measurements of surface-reaching solar (shortwave) radiation fluxes across a network of aerosol observatories (ARFINET) are combined with concurrent satellite (CERES)-based top of the atmosphere (TOA) fluxes to estimate regional aerosol direct radiative forcing (ARF) over the Indian region. The synergistic approach improves the accuracy of ARF estimates, which otherwise results in an overestimation or underestimation of the atmospheric forcing. During summer, an overestimation of similar to 5 W m(-2) (corresponding heating rate similar to 0.15 K day(-1)) is noticed. The regional average ARF from the synergistic approach reveals the surface forcing reaching -49 W m(-2) over the Indo Gangetic Plains, -45 W m(-2) over northeast India, -34 W m(-2) over the southern Peninsula, and - 16 W m(-2) in the oceanic regions of the Bay of Bengal. The ARF over the northern half of the Indian subcontinent is influenced mainly by anthmpogenic sulfate and carbonaceous aerosols. Dust is dominant in the western region of India during MAM and JJAS. Overall, the clear sky surface reaching solar radiation fluxes is reduced by 3-22% due to the abundance of aerosols in the atmosphere, with the highest reduction over the IGP during autumn and winter.

The vertical distributions of BC mass concentration (m(BC)) during a winter pollution period in 2017 over Chengdu, a megacity in the Sichuan Basin, China, were measured by a micro-aethalometer equipped on a tethered balloon. This observation experienced severe air pollution with an averaged ground BC of 11.1 mu g.m(-3), which is higher than two times the annual mean in Chengdu for 2018. The available 68 BC vertical profiles are grouped in to five types: Type A (18%) is the uniform vertical distribution of BC with an unrecognizable mixing layer (ML) height; BC in Type B (26%) is also uniformly distributed in the ML while decreases rapidly above the ML; Type C (7%) is a unimodal distribution with BC peak within the ML when the suspended temperature inversion forms; BC in Type D (29%) is accumulated in the near-ground layer and quickly decreases with height; Type E (20%) is the bimodal or trimodal distribution with BC peaks around the top of ML. Types A and B dominate from noon to afternoon, and Types C-E play critical roles during the evening and night. The different vertical patterns of BC are mainly associated with the evolution of the ML and the local emissions. For all the five types, the calculated radiative forcing of BC (f(BC)) is negative at the surface but positive at the top of profile (TOP), indicating the net absorption of radiation by the atmosphere due to BC. The absolute values of f(BC) at the surface and the TOP are increased with the increase of columnar BC loading, and there is no significant difference in f(BC) at the TOP and the surface among different patterns when the same BC loading is considered. However, the vertical distribution of atmospheric heating rate contributed by BC (h(BC)) is highly related to BC's vertical profile. The uniform distributed BC can result in a positive gradient of h(BC) with altitude, and thus, enhance the stability of the atmosphere. The plateau terrain induced small-scale secondary circulation and relatively lower thermal inversion in the west of the Sichuan basin have an essential effect on the vertical distribution of aerosols and can contribute to an accumulation of aerosols at 0.8-1.4 km above ground level. This study would hopefully have a preliminary understanding of the vertical distribution of BC in the Sichuan Basin, and a vital implication for accurately estimating direct radiative forcing by BC in this region.

Simultaneous measurements of ambient atmospheric black carbon (BC) mass concentrations and radiative fluxes were carried out over Satopanth glacier in the central Himalayas from September 22 to October 2, 2016, as a part of a glacier campaign experiment. The daily mean atmospheric BC concentrations varied between 165 +/- 20-263 +/- 32 ng m(-3) with a mean of 199 +/- 54 ng m(-3) during the observational period. The measured average surface albedo was found to be 0.24 +/- 0.11 during the entire period of observation. Spectral albedo from Moderate Resolution Imaging Spectroradiometer - Bidirectional Reflectance Distribution Function (MODIS-BRDF) satellite observation and net radiometer derived glacier albedo was found to be in good agreement with a correlation of 0.64 over the region. Concentration weighted trajectory analysis (CWT) over the site indicates a 70% BC transport from the Indo-Gangetic plain, Pakistan, and the Middle East region. BC radiative forcing was estimated using an optical model along with a radiative transfer model. An average BC direct radiative forcing of -5.4 +/- 0.25 W m(-2) and 2.4 +/- 0.19 W m(-2) was found respectively in the surface and at the top of the atmosphere (TOA) during the experimental period. The estimated average BC induced heating rate was found to be 0.33 +/- 0.04 K day(-1) over the region.