First-principles molecular dynamics simulations at solid-liquid interfaces with a continuum solvent

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Continuum solvent models have become a standard technique in the context of electronic structure calculations, yet no implementations have been reported capable to perform molecular dynamics at solid-liquid interfaces. We propose here such a continuum approach in a density functional theory framewor...

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Autores principales:	Sánchez, V.M., Sued, M., Scherlis, D.A.
Formato:	Artículo publishedVersion
Publicado:	2009
Materias:	A-density Acid-base equilibria Atomic coordinate Car-Parrinello molecular dynamics simulations Car-Parrinello simulation Computational costs Constant of motion Continuum model Continuum solvents Dielectric functions Dielectric medium Electronic density Electronic structure calculations Experimental research First-principles Interfacial region Kohn-Sham potential Molecular dynamics simulations Molecular mechanism Multigrid methods Periodic boundary conditions Plane-wave basis set Poisson problem Self-consistent calculation Solid-liquid interfaces TiO Two-dimension Water interface Continuum mechanics Density functional theory Dynamics Electronic structure Liquids Molecular dynamics Poisson equation Simulators Solvents Titanium dioxide Titanium oxides Phase interfaces
Acceso en línea:	http://hdl.handle.net/20.500.12110/paper_00219606_v131_n17_p_Sanchez http://repositoriouba.sisbi.uba.ar/gsdl/cgi-bin/library.cgi?a=d&c=artiaex&d=paper_00219606_v131_n17_p_Sanchez_oai
Aporte de:	Repositorio Digital de la Universidad de Buenos Aires (UBA) de Universidad de Buenos Aires

id	I28-R145-paper_00219606_v131_n17_p_Sanchez_oai
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spelling	I28-R145-paper_00219606_v131_n17_p_Sanchez_oai2020-10-19 Sánchez, V.M. Sued, M. Scherlis, D.A. 2009 Continuum solvent models have become a standard technique in the context of electronic structure calculations, yet no implementations have been reported capable to perform molecular dynamics at solid-liquid interfaces. We propose here such a continuum approach in a density functional theory framework using plane-wave basis sets and periodic boundary conditions. Our work stems from a recent model designed for Car-Parrinello simulations of quantum solutes in a dielectric medium [D. A. Scherlis, J. Chem. Phys. 124, 074103 (2006)], for which the permittivity of the solvent is defined as a function of the electronic density of the solute. This strategy turns out to be inadequate for systems extended in two dimensions: the dependence of the dielectric function on the electronic density introduces a new term in the Kohn-Sham potential, which becomes unphysically large at the interfacial region, seriously affecting the convergence of the self-consistent calculations. If the dielectric medium is properly redefined as a function of the atomic coordinates, a good convergence is obtained and the constant of motion is conserved during the molecular dynamics simulations. The Poisson problem is solved using a multigrid method, and in this way Car-Parrinello molecular dynamics simulations of solid-liquid interfaces can be performed at a very moderate computational cost. This scheme is employed to investigate the acid-base equilibrium at the TiO2 -water interface. The aqueous behavior of titania surfaces has stimulated a large amount of experimental research, but many open questions remain concerning the molecular mechanisms determining the chemistry of the interface. Here we make an attempt to answer some of them, putting to the test our continuum model. © 2009 American Institute of Physics. Fil:Sánchez, V.M. Universidad de Buenos Aires. Facultad de Ciencias Exactas y Naturales; Argentina. Fil:Sued, M. Universidad de Buenos Aires. Facultad de Ciencias Exactas y Naturales; Argentina. application/pdf http://hdl.handle.net/20.500.12110/paper_00219606_v131_n17_p_Sanchez info:eu-repo/semantics/openAccess http://creativecommons.org/licenses/by/2.5/ar J Chem Phys 2009;131(17) A-density Acid-base equilibria Atomic coordinate Car-Parrinello molecular dynamics simulations Car-Parrinello simulation Computational costs Constant of motion Continuum model Continuum solvents Dielectric functions Dielectric medium Electronic density Electronic structure calculations Experimental research First-principles Interfacial region Kohn-Sham potential Molecular dynamics simulations Molecular mechanism Multigrid methods Periodic boundary conditions Plane-wave basis set Poisson problem Self-consistent calculation Solid-liquid interfaces TiO Two-dimension Water interface Continuum mechanics Density functional theory Dynamics Electronic structure Liquids Molecular dynamics Poisson equation Simulators Solvents Titanium dioxide Titanium oxides Phase interfaces First-principles molecular dynamics simulations at solid-liquid interfaces with a continuum solvent info:eu-repo/semantics/article info:ar-repo/semantics/artículo info:eu-repo/semantics/publishedVersion http://repositoriouba.sisbi.uba.ar/gsdl/cgi-bin/library.cgi?a=d&c=artiaex&d=paper_00219606_v131_n17_p_Sanchez_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	A-density Acid-base equilibria Atomic coordinate Car-Parrinello molecular dynamics simulations Car-Parrinello simulation Computational costs Constant of motion Continuum model Continuum solvents Dielectric functions Dielectric medium Electronic density Electronic structure calculations Experimental research First-principles Interfacial region Kohn-Sham potential Molecular dynamics simulations Molecular mechanism Multigrid methods Periodic boundary conditions Plane-wave basis set Poisson problem Self-consistent calculation Solid-liquid interfaces TiO Two-dimension Water interface Continuum mechanics Density functional theory Dynamics Electronic structure Liquids Molecular dynamics Poisson equation Simulators Solvents Titanium dioxide Titanium oxides Phase interfaces
spellingShingle	A-density Acid-base equilibria Atomic coordinate Car-Parrinello molecular dynamics simulations Car-Parrinello simulation Computational costs Constant of motion Continuum model Continuum solvents Dielectric functions Dielectric medium Electronic density Electronic structure calculations Experimental research First-principles Interfacial region Kohn-Sham potential Molecular dynamics simulations Molecular mechanism Multigrid methods Periodic boundary conditions Plane-wave basis set Poisson problem Self-consistent calculation Solid-liquid interfaces TiO Two-dimension Water interface Continuum mechanics Density functional theory Dynamics Electronic structure Liquids Molecular dynamics Poisson equation Simulators Solvents Titanium dioxide Titanium oxides Phase interfaces Sánchez, V.M. Sued, M. Scherlis, D.A. First-principles molecular dynamics simulations at solid-liquid interfaces with a continuum solvent
topic_facet	A-density Acid-base equilibria Atomic coordinate Car-Parrinello molecular dynamics simulations Car-Parrinello simulation Computational costs Constant of motion Continuum model Continuum solvents Dielectric functions Dielectric medium Electronic density Electronic structure calculations Experimental research First-principles Interfacial region Kohn-Sham potential Molecular dynamics simulations Molecular mechanism Multigrid methods Periodic boundary conditions Plane-wave basis set Poisson problem Self-consistent calculation Solid-liquid interfaces TiO Two-dimension Water interface Continuum mechanics Density functional theory Dynamics Electronic structure Liquids Molecular dynamics Poisson equation Simulators Solvents Titanium dioxide Titanium oxides Phase interfaces
description	Continuum solvent models have become a standard technique in the context of electronic structure calculations, yet no implementations have been reported capable to perform molecular dynamics at solid-liquid interfaces. We propose here such a continuum approach in a density functional theory framework using plane-wave basis sets and periodic boundary conditions. Our work stems from a recent model designed for Car-Parrinello simulations of quantum solutes in a dielectric medium [D. A. Scherlis, J. Chem. Phys. 124, 074103 (2006)], for which the permittivity of the solvent is defined as a function of the electronic density of the solute. This strategy turns out to be inadequate for systems extended in two dimensions: the dependence of the dielectric function on the electronic density introduces a new term in the Kohn-Sham potential, which becomes unphysically large at the interfacial region, seriously affecting the convergence of the self-consistent calculations. If the dielectric medium is properly redefined as a function of the atomic coordinates, a good convergence is obtained and the constant of motion is conserved during the molecular dynamics simulations. The Poisson problem is solved using a multigrid method, and in this way Car-Parrinello molecular dynamics simulations of solid-liquid interfaces can be performed at a very moderate computational cost. This scheme is employed to investigate the acid-base equilibrium at the TiO2 -water interface. The aqueous behavior of titania surfaces has stimulated a large amount of experimental research, but many open questions remain concerning the molecular mechanisms determining the chemistry of the interface. Here we make an attempt to answer some of them, putting to the test our continuum model. © 2009 American Institute of Physics.
format	Artículo Artículo publishedVersion
author	Sánchez, V.M. Sued, M. Scherlis, D.A.
author_facet	Sánchez, V.M. Sued, M. Scherlis, D.A.
author_sort	Sánchez, V.M.
title	First-principles molecular dynamics simulations at solid-liquid interfaces with a continuum solvent
title_short	First-principles molecular dynamics simulations at solid-liquid interfaces with a continuum solvent
title_full	First-principles molecular dynamics simulations at solid-liquid interfaces with a continuum solvent
title_fullStr	First-principles molecular dynamics simulations at solid-liquid interfaces with a continuum solvent
title_full_unstemmed	First-principles molecular dynamics simulations at solid-liquid interfaces with a continuum solvent
title_sort	first-principles molecular dynamics simulations at solid-liquid interfaces with a continuum solvent
publishDate	2009
url	http://hdl.handle.net/20.500.12110/paper_00219606_v131_n17_p_Sanchez http://repositoriouba.sisbi.uba.ar/gsdl/cgi-bin/library.cgi?a=d&c=artiaex&d=paper_00219606_v131_n17_p_Sanchez_oai
work_keys_str_mv	AT sanchezvm firstprinciplesmoleculardynamicssimulationsatsolidliquidinterfaceswithacontinuumsolvent AT suedm firstprinciplesmoleculardynamicssimulationsatsolidliquidinterfaceswithacontinuumsolvent AT scherlisda firstprinciplesmoleculardynamicssimulationsatsolidliquidinterfaceswithacontinuumsolvent
_version_	1766026570212835328

First-principles molecular dynamics simulations at solid-liquid interfaces with a continuum solvent

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