Identification of species and sources of atmospheric chromophores by fluorescence excitation-emission matrix with parallel factor analysis

Abstract

It is essential to fully understand the physicochemical properties and sources of atmospheric chromophores to evaluate their impacts on environmental quality and global climate. Three-dimensional excitation-emission matrix (EEM) fluorescence spectroscopy is an important method for directly characterizing the occurrences, origins, and chemical behaviors of atmospheric chromophores. However, there is still a lack of adequate information on the sources and chemical structures of EEM-defined chromophores. This situation limits the extensive application of the EEM method in the study of atmospheric chromophores. Under these adverse conditions, this work uses the analysis of EEM data by the parallel factor (PARAFAC) analysis model and a comprehensive comparison of the types and abundances of different chromophores in different aerosol samples (combustion source samples, secondary organic aerosols, and ambient aerosols) to demonstrate that the EEM method can distinguish among different chromophore types and aerosol sources. Indeed, approximately half of all fluorescent substances can be attributed to specific chemicals and sources. These findings provide an important basis for the study of the sources and chemical processes of atmospheric chromophores by the EEM approach.