Subha S Raj

and 21 more

The Indo-Gangetic Plain (IGP) is one of the dominant sources of air pollution worldwide. During winter, the variations in planetary boundary layer (PBL) height, driven by a strong radiative thermal inversion, affect the regional air pollution dispersion. To date, measurements of aerosol-water vapour interactions, especially cloud condensation nuclei (CCN) activity, are limited in the Indian sub-continent, causing large uncertainties in the radiative forcing estimates of aerosol-cloud interactions. We present the results of a one-month field campaign (February-March 2018) in the megacity, Delhi, a significant polluter in the IGP. We measured the composition of fine particulate matter (PM1) and size-resolved CCN properties over a wide range of water vapour supersaturations. The analysis includes PBL modelling, backward trajectories, and fire spots to elucidate the influence of PBL and air mass origins on the aerosols. The aerosol properties depended strongly on the PBL height, and a simple power-law fit could parameterize the observed correlations of PM1 mass, aerosol particle number, and CCN number with PBL height, indicating PBL induced changes in aerosol accumulation. The low inorganic mass fractions, low aerosol hygroscopicity and high externally mixed weakly CCN-active particles under low PBL height (<100 m) indicated the influence of the PBL on aerosol aging processes. In contrast, aerosol properties did not depend strongly on air mass origins or wind direction, implying that the observed aerosol and CCN are from local emissions. An error function could parameterize the relationship between CCN number and supersaturation throughout the campaign.
Aerosol Liquid Water Content (ALWC), a ubiquitous component of atmospheric aerosols, contributes to total aerosol mass burden, modulating atmospheric chemistry through aerosol surface reactions and reducing atmospheric visibility. However, the complex dependency of ALWC on aerosol chemistry and relative humidity (RH) in the Indian region remains poorly characterized. Here, we combine available measurements of aerosol chemical composition with thermodynamic model ISORROPIA2.1 to reveal a comprehensive picture of ALWC in fine mode aerosols during the winter season in the Indian region. The fac-tors modulating ALWC are primarily dependent on the RH, such that the effect of aerosol dry mass and hygroscopicity are significant at high RH while the effect of hygroscopicity loses its significance as RH is lowered. ALWC, depending upon the particle hygroscopicity, displays a sharp non-linear rise beyond a critical value of ambient RH. Further analysis coupling WRF-Chem simulation with ISORROPIA2.1 revealed significant spatial heterogeneity in ALWC over India, strongly associating with regions of high aerosol loading and RH. The Indo-Gangetic Plain is consequently observed to be a hotspot of higher ALWC, which explains the prevalent conditions of haze and smog during winter in the region. Our findings re-emphasize that high aerosol mass resulting from intense pollution is vital in modulating aerosol–climate interaction under favorable meteorological conditions. They suggest the need for pollution control strategies to be directed at the reduction in emissions of specific species like NH3 and NOx, which were observed to contribute to the enhancement of PM and ALWC during wintertime in the region.