A quantum molecular dynamics study of aqueous solvation dynamics

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Ring polymer molecular dynamics experiments have been carried out to examine effects derived from nuclear quantum fluctuations at ambient conditions on equilibrium and non-equilibrium dynamical characteristics of charge solvation by a popular simple, rigid, water model, SPC/E, and for a more recent,...

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Autores principales:	Videla, P.E., Rossky, P.J., Laria, D.
Formato:	Artículo publishedVersion
Publicado:	2013
Materias:	Ambient conditions Dynamical characteristics Linear-response theory Polarization fluctuations Quantum fluctuation Quantum molecular dynamics Quantum solvation Solvation response Molecular dynamics Positive ions Quantum electronics Solvation
Acceso en línea:	http://hdl.handle.net/20.500.12110/paper_00219606_v139_n16_p_Videla https://repositoriouba.sisbi.uba.ar/gsdl/cgi-bin/library.cgi?a=d&c=artiaex&d=paper_00219606_v139_n16_p_Videla_oai
Aporte de:	Repositorio Digital de la Universidad de Buenos Aires (UBA) de Universidad de Buenos Aires

id	I28-R145-paper_00219606_v139_n16_p_Videla_oai
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spelling	I28-R145-paper_00219606_v139_n16_p_Videla_oai2024-08-16 Videla, P.E. Rossky, P.J. Laria, D. 2013 Ring polymer molecular dynamics experiments have been carried out to examine effects derived from nuclear quantum fluctuations at ambient conditions on equilibrium and non-equilibrium dynamical characteristics of charge solvation by a popular simple, rigid, water model, SPC/E, and for a more recent, and flexible, q-TIP4P/F model, to examine the generality of conclusions. In particular, we have recorded the relaxation of the solvent energy gap following instantaneous, ±e charge jumps in an initially uncharged Lennard-Jones-like solute. In both charge cases, quantum effects are reflected in sharper decays at the initial stages of the relaxation, which produce up to a ∼20% reduction in the characteristic timescales describing the solvation processes. For anionic solvation, the magnitude of polarization fluctuations controlling the extent of the water proton localization in the first solvation shell is somewhat more marked than for cations, bringing the quantum solvation process closer to the classical case. Effects on the solvation response from the explicit incorporation of flexibility in the water Hamiltonian are also examined. Predictions from linear response theories for the overall relaxation profile and for the corresponding characteristic timescales are reasonably accurate for the solvation of cations, whereas we find that they are much less satisfactory for the anionic case. © 2013 AIP Publishing LLC. Fil:Videla, P.E. Universidad de Buenos Aires. Facultad de Ciencias Exactas y Naturales; Argentina. application/pdf http://hdl.handle.net/20.500.12110/paper_00219606_v139_n16_p_Videla info:eu-repo/semantics/openAccess http://creativecommons.org/licenses/by/2.5/ar J Chem Phys 2013;139(16) Ambient conditions Dynamical characteristics Linear-response theory Polarization fluctuations Quantum fluctuation Quantum molecular dynamics Quantum solvation Solvation response Molecular dynamics Positive ions Quantum electronics Solvation A quantum molecular dynamics study of aqueous solvation dynamics info:eu-repo/semantics/article info:ar-repo/semantics/artículo info:eu-repo/semantics/publishedVersion https://repositoriouba.sisbi.uba.ar/gsdl/cgi-bin/library.cgi?a=d&c=artiaex&d=paper_00219606_v139_n16_p_Videla_oai
institution	Universidad de Buenos Aires
institution_str	I-28
repository_str	R-145
collection	Repositorio Digital de la Universidad de Buenos Aires (UBA)
topic	Ambient conditions Dynamical characteristics Linear-response theory Polarization fluctuations Quantum fluctuation Quantum molecular dynamics Quantum solvation Solvation response Molecular dynamics Positive ions Quantum electronics Solvation
spellingShingle	Ambient conditions Dynamical characteristics Linear-response theory Polarization fluctuations Quantum fluctuation Quantum molecular dynamics Quantum solvation Solvation response Molecular dynamics Positive ions Quantum electronics Solvation Videla, P.E. Rossky, P.J. Laria, D. A quantum molecular dynamics study of aqueous solvation dynamics
topic_facet	Ambient conditions Dynamical characteristics Linear-response theory Polarization fluctuations Quantum fluctuation Quantum molecular dynamics Quantum solvation Solvation response Molecular dynamics Positive ions Quantum electronics Solvation
description	Ring polymer molecular dynamics experiments have been carried out to examine effects derived from nuclear quantum fluctuations at ambient conditions on equilibrium and non-equilibrium dynamical characteristics of charge solvation by a popular simple, rigid, water model, SPC/E, and for a more recent, and flexible, q-TIP4P/F model, to examine the generality of conclusions. In particular, we have recorded the relaxation of the solvent energy gap following instantaneous, ±e charge jumps in an initially uncharged Lennard-Jones-like solute. In both charge cases, quantum effects are reflected in sharper decays at the initial stages of the relaxation, which produce up to a ∼20% reduction in the characteristic timescales describing the solvation processes. For anionic solvation, the magnitude of polarization fluctuations controlling the extent of the water proton localization in the first solvation shell is somewhat more marked than for cations, bringing the quantum solvation process closer to the classical case. Effects on the solvation response from the explicit incorporation of flexibility in the water Hamiltonian are also examined. Predictions from linear response theories for the overall relaxation profile and for the corresponding characteristic timescales are reasonably accurate for the solvation of cations, whereas we find that they are much less satisfactory for the anionic case. © 2013 AIP Publishing LLC.
format	Artículo Artículo publishedVersion
author	Videla, P.E. Rossky, P.J. Laria, D.
author_facet	Videla, P.E. Rossky, P.J. Laria, D.
author_sort	Videla, P.E.
title	A quantum molecular dynamics study of aqueous solvation dynamics
title_short	A quantum molecular dynamics study of aqueous solvation dynamics
title_full	A quantum molecular dynamics study of aqueous solvation dynamics
title_fullStr	A quantum molecular dynamics study of aqueous solvation dynamics
title_full_unstemmed	A quantum molecular dynamics study of aqueous solvation dynamics
title_sort	quantum molecular dynamics study of aqueous solvation dynamics
publishDate	2013
url	http://hdl.handle.net/20.500.12110/paper_00219606_v139_n16_p_Videla https://repositoriouba.sisbi.uba.ar/gsdl/cgi-bin/library.cgi?a=d&c=artiaex&d=paper_00219606_v139_n16_p_Videla_oai
work_keys_str_mv	AT videlape aquantummoleculardynamicsstudyofaqueoussolvationdynamics AT rosskypj aquantummoleculardynamicsstudyofaqueoussolvationdynamics AT lariad aquantummoleculardynamicsstudyofaqueoussolvationdynamics AT videlape quantummoleculardynamicsstudyofaqueoussolvationdynamics AT rosskypj quantummoleculardynamicsstudyofaqueoussolvationdynamics AT lariad quantummoleculardynamicsstudyofaqueoussolvationdynamics
_version_	1809357066452598784

A quantum molecular dynamics study of aqueous solvation dynamics

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