Source apportionment resolved by time of day for improved deconvolution of primary source contributions to air pollution

Abstract

Abstract. Present methodologies for source apportionment assume fixed source profiles. Since meteorology and human activity patterns change seasonally and diurnally, application of source apportionment techniques to shorter rather than longer time periods generates more representative mass spectra. Here, we present 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. We report on source apportionment conducted on four example time periods in two seasons (winter and monsoon seasons of 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. Compared to the traditional seasonal PMF approach, we extract a larger number of factors as well as PMF factors that represent the expected sources of primary organic aerosol using time-of-day PMF. By capturing diurnal time series patterns of sources at a low computational cost, time-of-day PMF can utilize large datasets collected using long-term monitoring and improve the characterization of sources of organic aerosol compared to traditional PMF approaches that do not resolve by time of day.