Free-energy derivatives and structure optimization within quasiharmonic lattice dynamics

A method is presented for the calculation of the gradient of the free energy with respect to all the internal and external degrees of freedom of a periodic crystal. This gradient can be used in conjunction with a static-energy Hessian for efficient geometrical optimization of systems with large unit...

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Autores principales: Taylor, M.B., Barrera, G.D., Allan, N.L., Barron, T.H.K.
Formato: JOUR
Lenguaje:English
Acceso en línea:http://hdl.handle.net/20.500.12110/paper_01631829_v56_n22_p14380_Taylor
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Biblioteca Digital - Facultad de Ciencias Exactas y Naturales (UBA) de Universidad de Buenos Aires
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spelling todo:paper_01631829_v56_n22_p14380_Taylor2023-10-03T15:01:47Z Free-energy derivatives and structure optimization within quasiharmonic lattice dynamics Taylor, M.B. Barrera, G.D. Allan, N.L. Barron, T.H.K. A method is presented for the calculation of the gradient of the free energy with respect to all the internal and external degrees of freedom of a periodic crystal. This gradient can be used in conjunction with a static-energy Hessian for efficient geometrical optimization of systems with large unit cells. The free energy is calculated using lattice statics and lattice dynamics in the quasiharmonic approximation, and its derivatives by means of first-order perturbation theory. In the present application of the method, particles are assumed to interact via arbitrary short-ranged spherically-symmetric pair potentials and long-ranged Coulomb forces, and polarizability effects are accounted for by use of the shell model. The method can be used directly as the basis for a computer program which makes efficient use of both storage and CPU time, especially for large unit cells. Detailed expressions for all the lattice sums are presented. Fil:Barrera, G.D. Universidad de Buenos Aires. Facultad de Ciencias Exactas y Naturales; Argentina. JOUR English info:eu-repo/semantics/openAccess http://creativecommons.org/licenses/by/2.5/ar http://hdl.handle.net/20.500.12110/paper_01631829_v56_n22_p14380_Taylor
institution Universidad de Buenos Aires
institution_str I-28
repository_str R-134
collection Biblioteca Digital - Facultad de Ciencias Exactas y Naturales (UBA)
language English
orig_language_str_mv English
description A method is presented for the calculation of the gradient of the free energy with respect to all the internal and external degrees of freedom of a periodic crystal. This gradient can be used in conjunction with a static-energy Hessian for efficient geometrical optimization of systems with large unit cells. The free energy is calculated using lattice statics and lattice dynamics in the quasiharmonic approximation, and its derivatives by means of first-order perturbation theory. In the present application of the method, particles are assumed to interact via arbitrary short-ranged spherically-symmetric pair potentials and long-ranged Coulomb forces, and polarizability effects are accounted for by use of the shell model. The method can be used directly as the basis for a computer program which makes efficient use of both storage and CPU time, especially for large unit cells. Detailed expressions for all the lattice sums are presented.
format JOUR
author Taylor, M.B.
Barrera, G.D.
Allan, N.L.
Barron, T.H.K.
spellingShingle Taylor, M.B.
Barrera, G.D.
Allan, N.L.
Barron, T.H.K.
Free-energy derivatives and structure optimization within quasiharmonic lattice dynamics
author_facet Taylor, M.B.
Barrera, G.D.
Allan, N.L.
Barron, T.H.K.
author_sort Taylor, M.B.
title Free-energy derivatives and structure optimization within quasiharmonic lattice dynamics
title_short Free-energy derivatives and structure optimization within quasiharmonic lattice dynamics
title_full Free-energy derivatives and structure optimization within quasiharmonic lattice dynamics
title_fullStr Free-energy derivatives and structure optimization within quasiharmonic lattice dynamics
title_full_unstemmed Free-energy derivatives and structure optimization within quasiharmonic lattice dynamics
title_sort free-energy derivatives and structure optimization within quasiharmonic lattice dynamics
url http://hdl.handle.net/20.500.12110/paper_01631829_v56_n22_p14380_Taylor
work_keys_str_mv AT taylormb freeenergyderivativesandstructureoptimizationwithinquasiharmoniclatticedynamics
AT barreragd freeenergyderivativesandstructureoptimizationwithinquasiharmoniclatticedynamics
AT allannl freeenergyderivativesandstructureoptimizationwithinquasiharmoniclatticedynamics
AT barronthk freeenergyderivativesandstructureoptimizationwithinquasiharmoniclatticedynamics
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