Dynamics of the charge transfer to solvent process in aqueous iodide.
Journal
Nature communications
ISSN: 2041-1723
Titre abrégé: Nat Commun
Pays: England
ID NLM: 101528555
Informations de publication
Date de publication:
21 Mar 2024
21 Mar 2024
Historique:
received:
21
09
2023
accepted:
05
03
2024
medline:
22
3
2024
pubmed:
22
3
2024
entrez:
22
3
2024
Statut:
epublish
Résumé
Charge-transfer-to-solvent states in aqueous halides are ideal systems for studying the electron-transfer dynamics to the solvent involving a complex interplay between electronic excitation and solvent polarization. Despite extensive experimental investigations, a full picture of the charge-transfer-to-solvent dynamics has remained elusive. Here, we visualise the intricate interplay between the dynamics of the electron and the solvent polarization occurring in this process. Through the combined use of ab initio molecular dynamics and machine learning methods, we investigate the structure, dynamics and free energy as the excited electron evolves through the charge-transfer-to-solvent process, which we characterize as a sequence of states denoted charge-transfer-to-solvent, contact-pair, solvent-separated, and hydrated electron states, depending on the distance between the iodine and the excited electron. Our assignment of the charge-transfer-to-solvent states is supported by the good agreement between calculated and measured vertical binding energies. Our results reveal the charge transfer process in terms of the underlying atomic processes and mechanisms.
Identifiants
pubmed: 38514610
doi: 10.1038/s41467-024-46772-0
pii: 10.1038/s41467-024-46772-0
doi:
Types de publication
Journal Article
Langues
eng
Sous-ensembles de citation
IM
Pagination
2544Subventions
Organisme : Simons Foundation
ID : 839534, MET
Informations de copyright
© 2024. The Author(s).
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