Simulation and Theory of Ions at Atmospherically Relevant Aqueous Liquid-Air Interfaces

TL;DR

This paper reviews simulation studies of ions at atmospheric aqueous interfaces, highlighting advances, challenges, and the development of a dielectric continuum theory to better understand ion behavior relevant to climate and air quality.

Contribution

It provides a comprehensive overview of simulation results, discusses methodological challenges, and introduces a dielectric continuum theory for ion adsorption at aqueous interfaces.

Findings

Simulation studies reveal ion adsorption mechanisms at water surfaces.

Recent dielectric theory reproduces experimental ion behavior.

Challenges include refining simulation accuracy and experimental validation.

Abstract

Chemistry occurring at or near the surfaces of aqueous droplets and thin films in the atmosphere influences air quality and climate. Molecular dynamics simulations are becoming increasingly useful for gaining atomic-scale insight into the structure and reactivity of aqueous interfaces in the atmosphere. Here we review simulation studies of atmospherically relevant aqueous liquid-air interfaces, with an emphasis on ions that play important roles in the chemistry of atmospheric aerosols. In addition to surveying results from simulation studies, we discuss challenges to the refinement and experimental validation of the methodology for simulating ion adsorption to the air-water interface, and recent advances in elucidating the driving forces for adsorption. We also review the recent development of a dielectric continuum theory that is capable of reproducing simulation and experimental data on ion behavior at aqueous interfaces.