Efficient Nitrate Formation in Fog Events Implicates Fog Interstitial Aerosols as Significant Drivers of Atmospheric Chemistry

Abstract

Clouds and fogs, consisting of tiny water droplets formed by the condensation of water in supersaturated air, are vital in atmospheric chemistry, as they facilitate multiphase reactions. While measuring high-altitude cloud is challenging, fog as ground-level clouds offer a unique opportunity for direct observation. In this study, we explored radiation fogs in the North China Plain using an advanced aerosol-fog sampling system to measure the chemical and physical properties of both inactivated interstitial aerosols and activated fog droplet residues. Our findings revealed that efficient nitrate formation primarily occurred on fog interstitial aerosols rather than within fog droplets, with observed fog interstitial aerosol nitrate net production rates reaching up to 3.6 μg m^–3 h^–1. Box model simulations identified the hydrolysis of NO₂ and N₂O₅ as key pathways for nitrate formation. NO₂ hydrolysis was often overlooked in previous studies, contributing 40–79 and 57–76% to total nitrate production during nighttime and daytime fog periods. This oversight suggests that substantial nitrate formation through hydrolysis reactions involving interstitial aerosols may have been neglected. Our results highlight the need for further research into the chemistry of cloud and fog interstitial aerosols and their inclusion in atmospheric chemistry models.