Exploring the Atmosphere of Neoproterozoic Earth: The Effect of O$_{2}$ on Haze Formation and Composition

Abstract

Previous studies of haze formation in the atmosphere of the Early Earth have focused on N$_{2}$/CO$_{2}$/CH$_{4}$ atmospheres. Here, we experimentally investigate the effect of O$_{2}$ on the formation and composition of aerosols to improve our understanding of haze formation on the Neoproterozoic Earth. We obtained in situ size, particle density, and composition measurements of aerosol particles produced from N$_{2}$/CO$_{2}$/CH$_{4}$/O$_{2}$ gas mixtures subjected to FUV radiation (115-400 nm) for a range of initial CO$_{2}$/CH$_{4}$/O$_{2}$ mixing ratios (O$_{2}$ ranging from 2 ppm to 0.2\%). At the lowest O$_{2}$ concentration (2 ppm), the addition increased particle production for all but one gas mixture. At higher oxygen concentrations (20 ppm and greater) particles are still produced, but the addition of O$_{2}$ decreases the production rate. Both the particle size and number density decrease with increasing O$_{2}$, indicating that O$_{2}$ affects particle nucleation and growth. The particle density increases with increasing O$_{2}$. The addition of CO$_{2}$ and O$_{2}$ not only increases the amount of oxygen in the aerosol, but it also increases the degree of nitrogen incorporation. In particular, the addition of O$_{2}$ results in the formation of nitrate bearing molecules. The fact that the presence of oxygen bearing molecules increases the efficiency of nitrogen fixation has implications for the role of haze as a source of molecules required for the origin and evolution of life. The composition changes also likely affect the absorption and scattering behavior of these particles but optical properties measurements are required to fully understand the implications for the effect on the planetary radiative energy balance and climate.