Regional climatic implications of aerosol black carbon (BC), which has a wide variety of anthropogenic sources in large abundance, are well recognized over South Asia. Significant uncertainties remain in its quantification due to a lack of sufficient information on the microphysical properties (its concentration, size, and mixing state with other aerosol components) that determine the absorption potential of BC. In particular, the information on the mixing state of BC is extremely sparse over this region. In this study, the first observations of the size distribution and mixing state of individual refractory black carbon (rBC) particles in the South Asian outflow to the south-eastern Arabian Sea and the northern and equatorial Indian Ocean regions are presented based on measurements using a single particle soot photometer (SP2) aboard the Integrated Campaign for Aerosols, gases, and Radiation Budget (ICARB-2018) ship during winter 2018 (16 January to 13 February). The results revealed significant spatial heterogeneity of BC characteristics. The highest rBC mass concentrations ($\sim \mathrm{938}\pm \mathrm{293}$ ng m⁻³) with the highest relative coating thickness (RCT; the ratio of BC core to its coating diameters) of $\sim \mathrm{2.16}\pm \mathrm{0.19}$ are found over the south-east Arabian Sea (SEAS) region, which is in the proximity of the continental outflow. As we move to farther oceanic regions, though the mass concentrations decreased by nearly half ($\sim \mathrm{546}\pm \mathrm{80}$ ng m⁻³), BC still remained thickly coated ($\text{RCT}\sim \mathrm{2.05}\pm \mathrm{0.07}$ ). The air over the remote equatorial Indian Ocean, which received considerable marine air masses compared to the other regions, showed the lowest rBC mass concentrations ($\sim \mathrm{206}\pm \mathrm{114}$ ng m⁻³) with a moderately thick coating ($\text{RCT}\sim \mathrm{1.73}\pm \mathrm{0.16}$ ). Even over oceanic regions far from the landmass, regions that received the outflow from the more industrialized east coast/the Bay of Bengal had a thicker coating (∼104 nm) compared to regions that received outflow from the west coast and/or peninsular India (∼86 nm). Although different regions of the ocean depicted contrasting concentrations and mixing state parameters due to the varied extent and nature of the continental outflow as well as the atmospheric lifetime of air masses, the modal parameters of rBC mass–size distributions (mean mass median diameters ∼ 0.19–0.20 µm) were similar over all regions. The mean fraction of BC-containing particles (F_BC) varied in the range of 0.08–0.12 (suggesting significant amounts of non-BC particles), whereas the bulk mixing ratio of coating mass to rBC mass was highest (8.31±2.40) over the outflow regions compared to the remote ocean (4.24±1.45), highlighting the role of outflow in providing condensable material for coatings on rBC. These parameters, along with the information on the size-resolved mixing state of BC cores, throw light on the role of sources and secondary processing of their complex mixtures for coatings on BC under highly polluted conditions. Examination of the non-refractory sub-micrometre aerosol chemical composition obtained using the aerosol chemical speciation monitor (ACSM) suggested that the overall aerosol system was sulfate-dominated over the far-oceanic regions. In contrast, organics were equally prominent adjacent to the coastal landmass. An association between the BC mixing state and aerosol chemical composition suggested that sulfate was the probable dominant coating material on rBC cores.

Measurements of the vertical profiles of the optical properties (namely the extinction coefficient and scattering and absorption coefficients respectively σ_ext ∕ σ_scat ∕ σ_abs) of aerosols have been made across the Indo-Gangetic Plain (IGP) using an instrumented aircraft operated from three base stations – Jodhpur (JDR), representing the semi-arid western IGP; Varanasi (VNS), the central IGP characterized by significant anthropogenic activities; and the industrialized coastal location in the eastern end of the IGP (Bhubaneswar, BBR) – just prior to the onset of the Indian summer monsoon. The vertical profiles depicted region-specific absorption characteristics, while the scattering characteristics remained fairly uniform across the region, leading to a west–east gradient in the vertical structure of single-scattering albedo (SSA). Integrated from near the ground to 3 km, the highest absorption coefficient and hence the lowest SSA occurred in the central IGP (Varanasi). Size distribution, inferred from the spectral variation of the scattering coefficient, showed a gradual shift from coarse-particle dominance in the western IGP to strong accumulation dominance in the eastern coast with the central IGP coming in between, arising from a change in the aerosol type from a predominantly natural (dust and sea salt) type in the western IGP to a highly anthropogenic type (industrial emissions, fossil fuel and biomass combustion) in the eastern IGP, with the central IGP exhibiting a mixture of both. Aerosol-induced short-wave radiative forcing, estimated using altitude-resolved SSA information, revealed significant atmospheric warming in the central IGP, while a top-of-atmosphere cooling is seen, in general, in the IGP. Atmospheric heating rate profiles, estimated using altitude-resolved SSA and column-averaged SSA, revealed considerable underestimation in the latter case, emphasizing the importance and necessity of having altitude-resolved SSA information as against a single value for the entire column.

Extensive measurements of cloud condensation nuclei (CCN) and condensation nuclei (CN) concentrations in the South Asian outflow to the northern Indian Ocean were carried out on board an instrumented research vessel, as part of the Integrated Campaign for Aerosols, gases and Radiation Budget (ICARB) during the winter season (January–February 2018). Measurements include a north–south transect across the South Asian plume over the northern Indian Ocean and an east–west transect over the equatorial Indian Ocean (∼2 ^∘ S), which is far away from the continental sources. South Asian outflow over the northern Indian Ocean is characterized by the high values of CCN number concentration (∼5000 cm⁻³), low CCN activation efficiency (∼25 %) and a steep increase in CCN concentration with the increase in supersaturation. In contrast, low CCN concentration (∼1000 cm⁻³) with flat supersaturation spectra was found over the equatorial Indian Ocean. The CCN properties exhibited significant dependence on the geometric mean diameter (GMD) of the aerosol number size distribution, and CCN activation efficiency decreased to low values (<20 %) at the time of new-particle formation events over near-coastal and remote oceanic regions. The analysis of the activation efficiencies for the “similar” aerosol size distributions over the northern Indian Ocean indicated the primary role of aerosol number size distribution on CCN activation efficiency. The dependence of CCN properties and activation efficiency on size-segregated aerosol number concentration, especially during the ultrafine (<100 nm) particle events, is investigated in detail for the first time over the region.

The seasonality and mutual dependence of aerosol optical properties and cloud condensation nuclei (CCN) activity under varying meteorological conditions at the high‐altitude Nainital site (~2 km) in the Indo‐Gangetic Plains were examined using nearly year‐round measurements (June 2011 to March 2012) at the Atmospheric Radiation Measurement mobile facility as part of the Regional Aerosol Warming Experiment–Ganges Valley Aerosol Experiment of the Indian Space Research Organization and the U.S. Department of Energy. The results from collocated measurements provided enhanced aerosol scattering and absorption coefficients, CCN concentrations, and total condensation nuclei concentrations during the dry autumn and winter months. The CCN concentration (at a supersaturation of 0.46) was higher during the periods of high aerosol absorption (single scattering albedo (SSA) < 0.80) than during the periods of high aerosol scattering (SSA > 0.85), indicating that the aerosol composition seasonally changes and influences the CCN activity. The monthly mean CCN activation ratio (at a supersaturation of 0.46) was highest (>0.7) in late autumn (November); this finding is attributed to the contribution of biomass‐burning aerosols to CCN formation at high supersaturation conditions.

Concurrent measurements of the altitude profiles of the concentration of cloud condensation nuclei (CCN), as a function of supersaturation (ranging from 0.2 % to 1.0 %), and aerosol optical properties (scattering and absorption coefficients) were carried out aboard an instrumented aircraft across the Indo-Gangetic Plain (IGP) just prior to the onset of the Indian summer monsoon (ISM) of 2016. The experiment was conducted under the aegis of the combined South-West Asian Aerosol–Monsoon Interactions and Regional Aerosol Warming Experiment (SWAAMI–RAWEX) campaign. The measurements covered coastal, urban and arid environments. In general, the CCN concentration was highest in the central IGP, decreasing spatially from east to west above the planetary boundary layer (PBL), which is ∼1.5 km for the IGP during pre-monsoon period. Despite this, the CCN activation efficiency at 0.4 % supersaturation was, interestingly, the highest over the eastern IGP (∼72 %), followed by that in the west (∼61 %), and it was the least over the central IGP (∼24 %) within the PBL. In general, higher activation efficiency is noticed above the PBL than below it. The central IGP showed remarkably low CCN activation efficiency at all altitudes, which appears to be associated with high black carbon (BC) mass concentration there, indicating the role of anthropogenic sources in suppressing the CCN efficiency. These first-ever CCN measurements over the western IGP, encompassing “the Great Indian Desert” also known as “the Thar Desert”, showed high CCN efficiency, ∼61 % at 0.4 % supersaturation, indicating the hygroscopic nature of the dust. The vertical structure of CCN properties is found to be air mass dependent, with higher activation efficiency even over the central IGP during the prevalence of marine air mass. Wet scavenging associated with precipitation episodes seems to have reduced the CCN activation efficiency below cloud level. An empirical relation has emerged between the CCN concentration and the scattering aerosol index (AI), which would facilitate the prediction of CCN from aerosol optical properties.