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Description
Publication abstract: The reactive uptake of N2O5 to aqueous aerosol is a major loss channel for nitrogen oxides in the troposphere. Despite its importance, a quantitative picture of the uptake mechanism is missing. Here we use molecular dynamics simulations with a data-driven many-body model of coupled-cluster accuracy to quantify thermodynamics and kinetics of solvation and adsorption of N2O5 in water. The free energy profile highlights that N2O5 is selectively adsorbed to the liquid-vapor interface and weakly solvated. Accommodation into bulk water occurs slowly, competing with evaporation upon adsorption from gas phase. Leveraging the quantitative accuracy of the model, we parameterize and solve a reaction-diffusion equation to determine hydrolysis rates consistent with experimental observations. We find a short reaction-diffusion length, indicating that the uptake is dominated by interfacial features. The parameters deduced here, including solubility, accommodation coefficient, and hydrolysis rate, afford a foundation for which to consider the reactive loss of N2O5 in more complex solutions Research Data Curation Program, UC San Diego, La Jolla, 92093-0175 (https://lib.ucsd.edu/rdcp) Cruzeiro, V. W. D.; Galib, M.; Limmer, D. T.; Götz, A. W. (2022). Data from: Uptake of N2O5 by Aqueous Aerosol Unveiled Using Chemically Accurate Many-Body Potentials. In Center for Aerosol Impacts on Chemistry of the Environment (CAICE) Collection. UC San Diego Library Digital Collections. https://doi.org/10.6075/J0FF3SHB This package contains a README file (.txt), input data samples for molecular dynamics simulations of N2O5 at the water/vapor interface and in bulk water using the MB-nrg many-body potential, all data extracted from the molecular dynamics simulations, the scripts used to generate plots from the data, and the Python code that was used to solve the reaction-diffusion model.
Type
Dataset
Language
English
Subject
N2O5 Chemical accuracy MB-pol Many-body potential Reaction-diffusion model Liquid-vapor interface Reactive uptake Umbrella sampling Solvation free energy MB-nrg Benchmarks Accomodation coefficient Dinitrogen pentoxide Water Coupled cluster calculations Aerosol Molecular dynamics Hydrolysis Solubility
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