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

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

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.

• Time period of project: 2018-10-01 to 2021-07-20

• 2022

• Cruzeiro, Vinícius Wilian D.

• Cruzeiro, Vinícius Wilian D.
• Galib, Mirza
• Götz, Andreas. W.
• Limmer, David T.

• Götz, Andreas. W.

All molecular dynamics simulations were performed with the pmemd program of the Amber molecular dynamics software package version 20 interfaced to the MBX many-body potential energy and force calculator. Molecular dynamics trajectories were analyzed using the cpptraj program of AmberTools version 20.

• Accomodation coefficient
• Aerosol
• Benchmarks
• Chemical accuracy
• Coupled cluster calculations
• Dinitrogen pentoxide
• Hydrolysis
• Liquid-vapor interface
• Many-body potential
• MB-nrg
• MB-pol
• Molecular dynamics
• N2O5
• Reaction-diffusion model
• Reactive uptake
• Solubility
• Solvation free energy
• Umbrella sampling
• Water

• data

• English

Primary associated publication

• Cruzeiro, V.W.D., Galib, M., Limmer, D.T. et al. Uptake of N2O5 by aqueous aerosol unveiled using chemically accurate many-body potentials. Nat Commun 13, 1266 (2022). https://doi.org/10.1038/s41467-022-28697-8

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2023-11-09