Influence of Ammonia and Relative Humidity on the Formation and Composition of Secondary Brown Carbon from Oxidation of 1-Methylnaphthalene and Longifolene

Abstract

Improved understanding of the optical properties of secondary organic aerosol (SOA) particles is needed to better predict their climate impacts. Here, SOA was produced by reacting 1-methylnaphthalene or longifolene with hydroxyl radicals (OH) under variable ammonia (NH3), nitrogen oxide (NOx), and relative humidity (RH) conditions. In the presence of NH3 and NOx, longifolene-derived aerosols had relatively high single scattering albedo (SSA) values and low absorption coefficients at 375 nm independent of RH, suggesting that the longifolene SOA is mostly scattering. In 1-methylnaphthalene experiments, the resulting SSA and SOA mass absorption coefficient (MACorg) values suggest the formation of light-absorbing SOA, and the addition of high NOx and high NH3 enhanced the SOA absorption. Under intermediate-NOx dry conditions, the MACorg values increased from 0.13 m2 g–1 in NH3-free conditions to 0.28 m2 g–1 in high-NH3 conditions. Under high-NH3 conditions, the MACorg value further increased to 0.36 m2 g–1 with an increase in RH. Under dry high-NOx conditions, the MACorg value increased from 0.42 to 0.67 m2 g–1 with the addition of NH3, while with elevated RH, the MACorg value reached 0.70 m2 g–1. The time series of MACorg showed increasing trends only in the presence of NH3. Composition analysis of SOA suggests that organonitrates, nitroorganics, and other nitrogen-containing organic compounds (NOCs) are potential chromophores in the 1-methylnaphthalene SOA. Significant formation of NOCs was observed in the presence of high-NOx and NH3 and was enhanced under elevated RH.