Cooling radiative forcing effect enhancement of atmospheric amines and mineral particles caused by heterogeneous uptake and oxidation

Abstract

The warming radiative forcing effect (RFE) derived from atmospheric amines attracts a lot of attention because of their contribution to brown carbon. Herein, the enhanced influence of amines (methyl-, dimethyl-, and trimethylamine) on cooling RFE of mineral particles is first confirmed at visible wavelengths. Present results state heterogeneous uptake and oxidation reactions of atmospheric amines are feasible on mineral particles under clean and polluted conditions, which are proven by related thermodynamics and kinetics data obtained using combined classical molecular dynamics and density function theory methods. Based on mineral particles, simple forcing efficiency (SFE) results explain that amine uptake induces at least 11.8 %-29.5 % enhancement on cooling RFE of amine-mineral particles at visible wavelengths. After amine heterogeneous oxidation, oxidized amine-mineral particle cooling RFEs are furthermore enhanced due to increased oxygen contents. Moreover, oxidized amine-mineral particles under clean conditions show 27.1 %-47.1 % SFE increments at 400-600 nm, which is at least 11.3 % higher than that of itself under polluted conditions, due to high-oxygen-content product formation through amine autoxidation. Our results suggest cooling RFE derived from atmospheric amines can be equally important to their warming RFE on the atmosphere. It is necessary to update the heterogeneous oxidation mechanism and kinetics data of amines in atmospheric models in order to accurately evaluate the whole RFE caused by amines on the atmosphere.