Source Apportionment of Brown Carbon Absorption by Coupling Ultraviolet-Visible Spectroscopy with Aerosol Mass Spectrometry

Abstract

The impact of brown carbon (BrC) on climate has been widely acknowledged but remains uncertain, because either its contribution to absorption is being ignored in most climate models or the associated mixed emission sources and atmospheric lifetime are not accounted for. In this work, we propose positive matrix factorization as a framework to apportion the contributions of individual primary and secondary organic aerosol (OA) source components of BrC absorption, by combining long-term aerosol mass spectrometry (AMS) data with concurrent ultraviolet-visible (UV-vis) spectroscopy measurements. The former feature time-depend ent factor contributions to OA mass, and the latter consist of wavelength-dependent absorption coefficients. Using this approach for a full-year case study, we estimate for the first time the mass absorption efficiency (MAE) of major light-absorbing water soluble OA components in the atmosphere. We show that secondary biogenic OA contributes negligibly to absorption despite dominating the mass concentration in the summer. In contrast, primary and secondary wood burning emissions are highly absorbing up to 500 nm. The approach allowed us to constrain their MAE within a confined range consistent with previous laboratory work, which can be used in climate models to estimate the impact of BrC from these emissions on the overall absorption.

The impact of brown carbon (BrC) on climate has been widely acknowledged but remains uncertain, because either its contribution to absorption is being ignored in most climate models or the associated mixed emission sources and atmospheric lifetime are not accounted for. In this work, we propose positive matrix factorization as a framework to apportion the contributions of individual primary and secondary organic aerosol (OA) source components of BrC absorption, by combining long-term aerosol mass spectrometry (AMS) data with concurrent ultraviolet-visible (UV-vis) spectroscopy measurements. The former feature time-depend ent factor contributions to OA mass, and the latter consist of wavelength-dependent absorption coefficients. Using this approach for a full-year case study, we estimate for the first time the mass absorption efficiency (MAE) of major light-absorbing water soluble OA components in the atmosphere. We show that secondary biogenic OA contributes negligibly to absorption despite dominating the mass concentration in the summer. In contrast, primary and secondary wood burning emissions are highly absorbing up to 500 nm. The approach allowed us to constrain their MAE within a confined range consistent with previous laboratory work, which can be used in climate models to estimate the impact of BrC from these emissions on the overall absorption.