Comment on acp-2022-179

Abstract

Delhi, India experiences extremely high concentrations of primary organic aerosol (POA). Few prior source apportionment studies on Delhi have captured the influence of biomass burning (BBOA) and cooking (COA) on POA. In a companion paper, we develop a new method to conduct source apportionment resolved by time of day using the underlying approach of positive matrix factorization (PMF). We call this approach “time-of-day PMF” and statistically demonstrate the improvements in this approach over traditional PMF. Here, we quantify the contributions of BBOA, COA, and hydrocarbon-like organic aerosol (HOA) by applying positive matrix factorization (PMF) resolved by time-of-day on two seasons (winter and monsoon 2017) using organic aerosol measurements from an Aerosol Chemical Speciation Monitor (ACSM). We deploy the EPA PMF tool with the underlying Multilinear Engine (ME-2) as the PMF solver. We also conduct detailed uncertainty analysis for statistical validation of our results. HOA is a major constituent of POA in both winter and monsoon. In addition to HOA, COA is found to be a major constituent of POA in monsoon and BBOA is found to be a major constituent of POA in the winter. Neither COA nor BBOA was resolved in the seasonal (not time-resolved) analysis. The COA mass spectral profiles (MS) are consistent with mass spectral profiles from Delhi and around the world, particularly resembling MS of heated cooking oils with a high m/z 41. The BBOA MS have a very prominent m/z 29 in addition to the characteristic peak at m/z 60, consistent with previous MS observed in Delhi and from wood burning sources. In addition to separating the POA, our technique also captures changes in MS profiles with the time of day, a unique feature among source apportionment approaches available. In addition to the primary factors, we separate 2–3 OOA components. When all factors are recombined to total POA and OOA, our results are consistent with seasonal PMF analysis conducted using EPA PMF. Results from this work can be used to better design policies that target relevant primary sources of organic aerosols in Delhi.