Characteristics of carbonaceous aerosols derived from long-term high-resolution measurements at a high-altitude site in the central Himalayas: radiative forcing estimates and role of meteorology and biomass burning.

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Simultaneous observations (2014-2017) of organic carbon (OC) and elemental carbon (EC) are made over a high-altitude site (Nainital, 29.4°N, 79.5°E, 1958m a.m.s.l) in the central Himalayas, and the role of long-range transport, meteorology and biomass burning is studied. There are only a few online and simultaneous observations of OC and EC over South Asia and none in the high-altitude Himalayan region. This work presents the first diurnal variations with a unimodal pattern in both OC and EC at the Himalayan site. Such a diurnal pattern is in contrast with the bimodal pattern observed at any continental polluted site. Clear seasonal variations in OC and EC were seen with a primary maximum during spring and a secondary maximum in autumn/winter. OC and EC concentrations are observed to be as high as 65.8μg/m3 and 12μg/m3, in May, respectively. Concentration weighted trajectory (CWT)-assisted analysis shows that the biomass burning in northern India is one of the major sources for the springtime maximum even at this high-altitude site. The coinciding rise in OC/EC ratio from 4.6 to 7.9, along with fire events, further convinces that the enhancement in the concentrations is due to the biomass burning at distant regions and long-range transport of air masses influencing this high-altitude site. A poor covariation between OC-EC and the boundary-layer height during autumn and winter suggests that secondary maxima in OC and EC are most likely due to local sources, e.g. household burning for heating during this cold period when the temperature drops sharply after October and remains low until February. The higher temporal resolution of online measurements reveals that swiftly varying meteorological parameters change the OC-EC concentrations at diurnal scales. Back-air trajectory-assisted analysis of residence time and its relationship with OC and EC confirms the increase in their concentration in slow-moving air masses. The observed diurnal variations of EC are utilized to estimate the radiative forcing and shown that the atmospheric radiative forcing during the afternoon is about 70% higher than the forenoon one. It is envisaged that this dataset with diurnal observations of OC and EC would be an important input for studying the radiation budget and source apportionment over this high-altitude region.