Path integral-molecular dynamics study of electronic states in supercritical water

We have carried out path integral-molecular dynamics simulations to describe microscopic details of excess electrons in supercritical water over a wide range of solvent densities, ρw, along the T = 645 K isotherm. The well-tested simple-point charge model for water was used. The transition from loca...

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Autores principales: Laria, D., Skaf, M.S.
Formato: JOUR
Materias:
Density of liquids
Electronic structure
Ground state
Molecules
Radiolysis
Solvents
Supercritical fluids
Water
Supercritical water
Molecular dynamics
Acceso en línea:http://hdl.handle.net/20.500.12110/paper_10895639_v106_n35_p8066_Laria
Aporte de:
Biblioteca Digital - Facultad de Ciencias Exactas y Naturales (UBA) de Universidad de Buenos Aires
id todo:paper_10895639_v106_n35_p8066_Laria
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spelling todo:paper_10895639_v106_n35_p8066_Laria2023-10-03T16:04:29Z Path integral-molecular dynamics study of electronic states in supercritical water Laria, D. Skaf, M.S. Density of liquids Electronic structure Ground state Molecules Radiolysis Solvents Supercritical fluids Water Supercritical water Molecular dynamics We have carried out path integral-molecular dynamics simulations to describe microscopic details of excess electrons in supercritical water over a wide range of solvent densities, ρw, along the T = 645 K isotherm. The well-tested simple-point charge model for water was used. The transition from localized to quasifree states described in terms of the electron spatial extent is observed in the vicinity of ρw = 0.15 g cm-3. For smaller densities, the electron undergoes quantum tunneling through nearest neighboring water molecules. The groundstate absorption spectrum exhibits significant red shifts in the absorption maxima with decreasing density, showing reasonable agreement with recent pulse radiolysis measurements. JOUR info:eu-repo/semantics/openAccess http://creativecommons.org/licenses/by/2.5/ar http://hdl.handle.net/20.500.12110/paper_10895639_v106_n35_p8066_Laria
institution Universidad de Buenos Aires
institution_str I-28
repository_str R-134
collection Biblioteca Digital - Facultad de Ciencias Exactas y Naturales (UBA)
topic Density of liquids
Electronic structure
Ground state
Molecules
Radiolysis
Solvents
Supercritical fluids
Water
Supercritical water
Molecular dynamics
spellingShingle Density of liquids
Electronic structure
Ground state
Molecules
Radiolysis
Solvents
Supercritical fluids
Water
Supercritical water
Molecular dynamics
Laria, D.
Skaf, M.S.
Path integral-molecular dynamics study of electronic states in supercritical water
topic_facet Density of liquids
Electronic structure
Ground state
Molecules
Radiolysis
Solvents
Supercritical fluids
Water
Supercritical water
Molecular dynamics
description We have carried out path integral-molecular dynamics simulations to describe microscopic details of excess electrons in supercritical water over a wide range of solvent densities, ρw, along the T = 645 K isotherm. The well-tested simple-point charge model for water was used. The transition from localized to quasifree states described in terms of the electron spatial extent is observed in the vicinity of ρw = 0.15 g cm-3. For smaller densities, the electron undergoes quantum tunneling through nearest neighboring water molecules. The groundstate absorption spectrum exhibits significant red shifts in the absorption maxima with decreasing density, showing reasonable agreement with recent pulse radiolysis measurements.
format JOUR
author Laria, D.
Skaf, M.S.
author_facet Laria, D.
Skaf, M.S.
author_sort Laria, D.
title Path integral-molecular dynamics study of electronic states in supercritical water
title_short Path integral-molecular dynamics study of electronic states in supercritical water
title_full Path integral-molecular dynamics study of electronic states in supercritical water
title_fullStr Path integral-molecular dynamics study of electronic states in supercritical water
title_full_unstemmed Path integral-molecular dynamics study of electronic states in supercritical water
title_sort path integral-molecular dynamics study of electronic states in supercritical water
url http://hdl.handle.net/20.500.12110/paper_10895639_v106_n35_p8066_Laria
work_keys_str_mv AT lariad pathintegralmoleculardynamicsstudyofelectronicstatesinsupercriticalwater
AT skafms pathintegralmoleculardynamicsstudyofelectronicstatesinsupercriticalwater
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