Abstract

Abstract. Over the Indian region, aerosol absorption is considered to have a potential impact on the regional climate, monsoon and hydrological cycle. Black carbon (BC) is the dominant absorbing aerosol, whose absorption potential is determined mainly by its microphysical properties, including its concentration, size and mixing state with other aerosol components. The Indo-Gangetic Plain (IGP) is one of the regional aerosol hot spots with diverse sources, both natural and anthropogenic, but still the information on the mixing state of the IGP aerosols, especially BC, is limited and a significant source of uncertainty in understanding their climatic implications. In this context, we present the results from intensive measurements of refractory BC (rBC) carried out over Bhubaneswar, an urban site in the eastern coast of India, which experiences contrasting air masses (the IGP outflow or coastal/marine air masses) in different seasons. This study helps to elucidate the microphysical characteristics of BC over this region and delineates the IGP outflow from the other air masses. The observations were carried out as part of South West Asian Aerosol Monsoon Interactions (SWAAMI) collaborative field experiment during July 2016–May 2017, using a single-particle soot photometer (SP2) that uses a laser-induced incandescence technique to measure the mass and mixing state of individual BC particles and an aerosol chemical speciation monitor (ACSM) to infer the possible coating material. Results highlighted the distinctiveness in aerosol microphysical properties in the IGP air masses. BC mass concentration was highest during winter (December–February) (∼1.94±1.58 µg m−3), when the prevailing air masses were mostly of IGP origin, followed by post-monsoon (October–November) (mean ∼1.34±1.40 µg m−3). The mass median diameter (MMD) of the BC mass size distributions was in the range 0.190–0.195 µm, suggesting mixed sources of BC, and, further, higher values (∼ 1.3–1.8) of bulk relative coating thickness (RCT) (ratio of optical and core diameters) were seen, indicating a significant fraction of highly coated BC aerosols in the IGP outflow. During the pre-monsoon (March–May), when marine/coastal air masses prevailed, BC mass concentration was lowest (∼0.82±0.84 µg m−3), and larger BC cores (MMD > 0.210 µm) were seen, suggesting distinct source processes, while RCT was ∼ 1.2–1.3, which may translate into higher extent of absolute coating on BC cores, which may have crucial regional climate implications. During the summer monsoon (July–September), BC size distributions were dominated by smaller cores (MMD ≤ 0.185 µm), with the lowest coating indicating fresher BC, likely from fossil fuel sources. A clear diurnal variation pattern of BC and RCT was noticed in all the seasons, and daytime peak in RCT suggested enhanced coating on BC due to the condensable coating material originating from photochemistry. Examination of submicrometre aerosol chemical composition highlighted that the IGP outflow was dominated by organics (47 %–49 %), and marine/coastal air masses contained higher amounts of sulfate (41 %–47 %), while ammonium and nitrate were seen in minor amounts, with significant concentrations only during the IGP air mass periods. The diurnal pattern of sulfate resembled that of the RCT of rBC particles, whereas organic mass showed a pattern similar to that of the rBC mass concentration. Seasonally, the coating on BC showed a negative association with the mass concentration of sulfate during the pre-monsoon season and with organics during the post-monsoon season. These are the first experimental data on the mixing state of BC from a long time series over the Indian region and include new information on black carbon in the IGP outflow region. These data help in improving the understanding of regional BC microphysical characteristics and their climate implications.

Highlights

  • The state of mixing of aerosols, especially that of absorbing aerosols, remains poorly quantified, despite its important role in determining the regional and global radiative impacts of aerosols and aerosol–cloud interactions (Bond et al, 2013; Liu et al, 2013; IPCC, 2013)

  • Number concentrations of black carbon (BC) and scattering particles peak in winter, while they are the lowest in the pre-monsoon season (PMS) with moderate values through the post-monsoon season (PoMS)

  • The particle size distribution shows the increased presence of larger particles and higher median diameters indicating a change in the nature of sources. All these resulted in an increase in the overall coating during the PoMS with seasonal mean values of 1.32 ± 0.14 for relative coating thickness (RCT) and 28.74 ± 12.31 nm for absolute coating thickness (ACT) highlighting an enhancement of ∼ 32 % of the particle sizes due to thick coating of condensable vapours on BC cores during this season

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Summary

Introduction

The state of mixing of aerosols, especially that of absorbing aerosols, remains poorly quantified, despite its important role in determining the regional and global radiative impacts of aerosols and aerosol–cloud interactions (Bond et al, 2013; Liu et al, 2013; IPCC, 2013). Large heterogeneity in the nature of aerosol sources over the IGP (industrial and vehicular emissions, crop residue, and residential fuel burning) results in BC particles with varying microphysical properties (size, concentrations and mixing state) which determine BC’s absorption potential and radiative effects (Jacobson, 2001; Cappa et al, 2012; Petzold et al, 2013; Bond et al, 2013). The key objectives have been (a) the assessment of the impact of BC and co-emitted organic/inorganic species on the radiation budget via the direct, semi-direct and indirect effects, and (b) the evaluation of the effects of the aerosol radiative forcing on the local energy budget, atmospheric dynamics and hydrological cycle over India To meet these objectives, state-of-the-art instruments were installed at Bhubaneswar, which included a single-particle soot photometer for characterization of refractory BC (rBC) aerosols and an aerosol chemical speciation monitor (ACSM) for the measurements of non-refractory submicrometre aerosol chemical composition for long-term measurements. The contributions from distinct sources to BC concentrations and the association of coating on BC with possible condensable coating material are examined, and the implications are discussed

Experimental details
Instrumentation
BC mass and number concentrations
Seasonal distinctiveness of BC size distribution and modal parameters
10. Cranfield Airport in Aircraft emissions near source UK
Seasonal changes in mixing state of BC
Diurnal variations of rBC mass concentration and RCT
Summary and conclusions
Full Text
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