Air mass physiochemical characteristics over New Delhi: impacts on aerosol hygroscopicity and cloud condensation nuclei (CCN) formation

Delhi is a megacity subject to high local anthropogenic emissions and long-range transport of pollutants. This work presents for the first time time-resolved estimates of hygroscopicity parameter (kappa) and cloud condensation nuclei (CCN), spanning for more than a year, derived from chemical composition and size distribution data. As a part of the Delhi Aerosol Supersite (DAS) campaign, the characterization of aerosol composition and size distribution was conducted from January 2017 to March 2018. Air masses originating from the Arabian Sea (AS), Bay of Bengal (BB), and southern Asia (SA) exhibited distinct characteristics of time-resolved sub-micron non-refractory PM1 (NRPM1) species, size distributions, and CCN number concentrations. The SA air mass had the highest NRPM1 loading with high chloride and organics, followed by the BB air mass, which was more contaminated than AS, with a higher organic fraction and nitrate. The primary sources were identified as biomass-burning, thermal power plant emissions, industrial emissions, and vehicular emissions. The average hygroscopicity parameter (kappa), calculated by the mixing rule, was approximately 0.3 (varying between 0.13 and 0.77) for all the air masses (0.32 +/- 0.06 for AS, 0.31 +/- 0.06 for BB, and 0.32 +/- 0.10 for SA). The diurnal variations in kappa were impacted by the chemical properties and thus source activities. The total, Aitken, and accumulation mode number concentrations were higher for SA, followed by BB and AS. The mean values of estimated CCN number concentration (N-CCN; 3669-28926 cm(-3)) and the activated fraction (a(f); 0.19-0.87), for supersaturations varying from 0.1 % to 0.8 %, also showed the same trend, implying that these were highest in SA, followed by those in BB and then those in AS. The size turned out to be more important than chemical composition directly, and the N-CCN was governed by either the Aitken or accumulation modes, depending upon the supersaturation (SS) and critical diameter (D-c). a(f) was governed mainly by the geometric mean diameter (GMD), and such a high a(f) (0.71 +/- 0.14 for the most dominant sub-branch of the SA air mass - R1 - at 0.4 % SS) has not been seen anywhere in the world for a continental site. The high a(f) was a consequence of very low D-c (25-130 nm, for SS ranging from 0.1 % to 0.8 %) observed for Delhi. Indirectly, the chemical properties also impacted CCN and a(f) by impacting the diurnal patterns of Aitken and accumulation modes, kappa and D-c. The high-hygroscopic nature of aerosols, high N-CCN, and high a(f) can severely impact the precipitation patterns of the Indian monsoon in Delhi, impact the radiation budget, and have indirect effects and need to be investigated to quantify this impact.