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:	JOUR
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
Aporte de:	Biblioteca Digital - Facultad de Ciencias Exactas y Naturales (UBA) de Universidad de Buenos Aires

id	todo:paper_00219606_v139_n16_p_Videla
record_format	dspace
spelling	todo:paper_00219606_v139_n16_p_Videla2023-10-03T14:24:30Z A quantum molecular dynamics study of aqueous solvation dynamics Videla, P.E. Rossky, P.J. Laria, D. 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 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. JOUR info:eu-repo/semantics/openAccess http://creativecommons.org/licenses/by/2.5/ar http://hdl.handle.net/20.500.12110/paper_00219606_v139_n16_p_Videla
institution	Universidad de Buenos Aires
institution_str	I-28
repository_str	R-134
collection	Biblioteca Digital - Facultad de Ciencias Exactas y Naturales (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	JOUR
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
url	http://hdl.handle.net/20.500.12110/paper_00219606_v139_n16_p_Videla
work_keys_str_mv	AT videlape aquantummoleculardynamicsstudyofaqueoussolvationdynamics AT rosskypj aquantummoleculardynamicsstudyofaqueoussolvationdynamics AT lariad aquantummoleculardynamicsstudyofaqueoussolvationdynamics AT videlape quantummoleculardynamicsstudyofaqueoussolvationdynamics AT rosskypj quantummoleculardynamicsstudyofaqueoussolvationdynamics AT lariad quantummoleculardynamicsstudyofaqueoussolvationdynamics
_version_	1782026784005423104

A quantum molecular dynamics study of aqueous solvation dynamics

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