Source analyses of ambient VOCs considering reactive losses: methods of reducing loss effects, impacts of losses, and sources

Abstract. Chemical losses of ambient reactive volatile organic compounds (VOCs) is a long-term issue yet to be resolved in VOC source apportionments. These losses substantially reduce the concentrations of highly reactive species in the apportioned factor profiles and result in the underestimation of source contributions. This review assesses the common methods and existing issues in ways to reduce losses and loss impacts in source analyses and suggest research directions for improved VOC source apportionments. Positive Matrix Factorization (PMF) is now the main VOC source analysis method compared to other mathematical models. The issue in using any apportionment tool is the processing of the data to be analyzed to reduce the impacts of reactive losses. Estimating the initial concentrations of ambient VOCs based on photochemical age has become the primary approach to reduce reactive loss effects in PMF except for selecting low reactivity species or nighttime data into the analysis. Currently, the initial concentration method only considers daytime reactions with hydroxyl (•OH) radicals. However, the •OH rate constants vary with temperature and that has not been considered. Losses from reactions with O₃ and NO₃ radicals especially for alkene species remain to be included. Thus, the accuracy of the photochemical-age estimation is uncertain. Beyond developing accurate quantitative approaches for reactive losses, source analyses methods for the consumed VOCs and the accurate quantification of different source contributions to O₃ and secondary organic aerosols are important additional directions for future research.