Surfaces are ubiquitous in indoor and atmospheric environments. In the atmosphere, surfaces are present in the form of aerosols, which can impact climate by scattering or absorbing solar radiation and influencing cloud formation and precipitation processes. Sea spray aerosols are a major biogenic aerosol, whose physiochemical properties and composition are reflective of the marine environment. In indoor environments, surfaces are extremely diverse, ranging from walls to skin to window glass. Due to the higher prevalence of surfaces indoors, developing a molecular level understanding of surface processes is necessary for accurately understanding the role surfaces play in regulating indoor air quality and consequently the health of the occupants.

In this dissertation, the surface properties and composition of window glass and sea spray aerosols are investigated. These surfaces are probed upon their nascent production and subsequent physical and chemical transformations under environmentally relevant conditions. In both environments, indoors and outdoors, due to the messy nature of authentic surfaces, comparisons are made back to simple model systems to provide molecular mimetics that can be used for future studies. Due to the small size scales of surface processes, higher resolution chemical analyses and imaging techniques reveal the chemical and morphological heterogeneities across the sample surface. Overall, these studies provide insights into how high resolution spectromicroscopic techniques can be utilized to elucidate nanoscale heterogeneous evolution of atmospherically and indoor relevant surfaces, and their subsequent reactions with trace gases.