Margaret Berrens^1*, Zekun Chen^1*, Kam-Tung Chan^1*, Cort Anastasio^2*, Davide Donadio^1*

1 Department of Chemistry, University of California Davis

2 Department of Land, Air, and Water Resources, University of California Davis

* Corresponding authors emails: mlberrens@ucdavis.edu, zkuchen@ucdavis.edu, tbchan@ucdavis.edu, canastasio@ucdavis.edu, ddonadio@ucdavis.edu

DOI10.24435/materialscloud:4d-p4 [version v1]

Publication date: Jul 26, 2023

How to cite this record

Margaret Berrens, Zekun Chen, Kam-Tung Chan, Cort Anastasio, Davide Donadio, Solvation Structure and UV-Visible Absorption Spectra of the Nitrate Anion at the Air-Ice Interface by First Principles Molecular Simulations, Materials Cloud Archive 2023.115 (2023), https://doi.org/10.24435/materialscloud:4d-p4

Description

Nitrate is a significant contaminant in Polar snow. Its photolysis in environmental sunlight generates reactive nitrogen, which impacts the oxidative capacity of the atmosphere, influencing the fate and lifetimes of pollutants. The photolysis of nitrate can produce either NO2 or NO2- , with recent experiments suggesting that the process is accelerated at the air-ice interface compared to the bulk solution. In this study, we employed multiscale modeling approaches to investigate the enhanced photoreactivity of nitrate at the ice surface in the presence of two different cations. We characterized the solvation shell of NO3- and explored its pairing with cations in water and ice using ab initio molecular dynamics and enhanced sampling. Molecular trajectories were used to calculate light absorption spectra at different solvation conditions and finite temperature. Our analysis revealed that the pairing of nitrate with cations may alter the molar absorption coefficient of nitrate at the air-ice interface affecting the rate of photolysis observed in experiments of ammonium nitrate deposited on snow.

Materials Cloud sections using this data

Files

File name	Size	Description
README.txt MD5md5:2d47d2f23b5904fdb84941eb5ae7d10b	1.2 KiB	Overview of the materials provided
Nitrate_Repository.zip MD5md5:d5e0061463e27e63dc56d4ffd0b027cc	49.1 MiB	This folder contains the input and starting files for the paper 'Solvation Structure and UV-Visible Absorption Spectra of the Nitrate Anion at the Air-Ice Interface by First Principles Molecular Simulations' including files for the AIMD Simulations using PBE-D3 with CP2K, input and output files for the well-tempered metadynamics runs using Plumed, and the input files for the TDDFT calculations using ORCA.

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Keywords

Nitrate Solvation Ice Surface DFT molecular dynamics TDDFT UV-Vis. Absorption