dc.contributor.author Escribano, B. dc.contributor.author Lozano, A. dc.contributor.author Radivojevic, T. dc.contributor.author Fernández-Pendás, M. dc.contributor.author Carrasco, J. dc.contributor.author Akhmatskaya, E. dc.date.accessioned 2017-03-07T19:12:28Z dc.date.available 2017-03-07T19:12:28Z dc.date.issued 2017-03-07 dc.identifier.issn 1432-881X dc.identifier.uri http://hdl.handle.net/20.500.11824/649 dc.description.abstract The study of ion transport in electrochemically active materials for energy storage systems requires simulations on quantum-, atomistic- and meso-scales. The methods accessing these scales not only have to be effective but also well compatible to provide a full description of the underlying processes. We propose to adapt the Generalized Shadow Hybrid Monte Carlo (GSHMC) method to atomistic simulation of ion intercalation electrode materials for batteries. The method has never been applied to simulations in solid-state chemistry but it has been successfully used for simulation of biological macromolecules, demonstrating better performance and accuracy than can be achieved with the popular molecular dynamics (MD) method. It has been also extended to simulations on meso-scales, making it even more attractive for simulation of battery materials. We combine GSHMC with the dynamical core–shell model to incorporate polarizability into the simulation and apply the new Modified Adaptive Integration Approach, MAIA, which allows for a larger time step due to its excellent conservation properties. Also, we modify the GSHMC method, without losing its performance and accuracy, to reduce the negative effect of introducing a shell mass within a dynamical shell model. The proposed approach has been tested on olivine NaFePO$_4$, which is a promising cathode material for Na-ion batteries. The calculated Na-ion diffusion and structural properties have been compared with the available experimental data and with the results obtained using MD and the original GSHMC method. Based on these tests, we claim that the new technique is advantageous over MD and the conventional GSHMC and can be recommended for studies of other solid-state electrode and electrolyte materials whenever high accuracy and efficient sampling are critical for obtaining tractable simulation results. en_US dc.description.sponsorship MTM2013-46553-C3-1-P en_US Iberdrola Foundation “Grants for Research in Energy and Environment 2014” ELKARTEK Programme KK-2016/00026 BES-2014-068640 BERC 2014-2017 SEV-2013-0323 dc.format application/pdf en_US dc.language.iso eng en_US dc.rights Reconocimiento-NoComercial-CompartirIgual 3.0 España en_US dc.rights.uri http://creativecommons.org/licenses/by-nc-sa/3.0/es/ en_US dc.subject Enhanced sampling en_US dc.subject Molecular dynamics en_US dc.subject Hybrid Monte Carlo en_US dc.subject Shadow Hamiltonians en_US dc.subject Adaptive integrators en_US dc.subject Adiabatic Core-Shell model en_US dc.subject Na-ion batteries en_US dc.title Enhancing sampling in atomistic simulations of solid state materials for batteries: a focus on olivine NaFePO$_4$ en_US dc.type info:eu-repo/semantics/article en_US dc.identifier.doi 10.1007/s00214-017-2064-4 dc.relation.publisherversion http://link.springer.com/article/10.1007%2Fs00214-017-2064-4 en_US dc.relation.projectID ES/1PE/SEV-2013-0323 en_US dc.relation.projectID EUS/BERC/BERC.2014-2017 en_US dc.relation.projectID EUS/ELKARTEK en_US dc.rights.accessRights info:eu-repo/semantics/openAccess en_US dc.type.hasVersion info:eu-repo/semantics/acceptedVersion en_US dc.journal.title Theoretical Chemistry Accounts en_US
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