An Ab Initio Journey toward the Molecular-LevelUnderstanding and Predictability of SubnanometricMetal Clusters

25 pags., 15 figs., 1 tab. -- Perspective

Detalles Bibliográficos
Autor: Lara Castells, María Pilar de
Tipo de recurso: artículo
Estado:Versión publicada
Fecha de publicación:2024
País:España
Institución:Consejo Superior de Investigaciones Científicas (CSIC)
Repositorio:DIGITAL.CSIC. Repositorio Institucional del CSIC
OAI Identifier:oai:digital.csic.es:10261/364023
Acceso en línea:http://hdl.handle.net/10261/364023
Access Level:acceso abierto
Palabra clave:Density functional theory and ab initio modeling
Fluxional Jahn–Teller molecules
Photocatalysis
Reversible oxidation
Subnanometric metal clusters
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spelling An Ab Initio Journey toward the Molecular-LevelUnderstanding and Predictability of SubnanometricMetal ClustersLara Castells, María Pilar deDensity functional theory and ab initio modelingFluxional Jahn–Teller moleculesPhotocatalysisReversible oxidationSubnanometric metal clusters25 pags., 15 figs., 1 tab. -- PerspectiveCurrent advances in synthesizing and characterizing atomically precise monodisperse metal clusters (AMCs) at the subnanometer scale have opened up new possibilities in quantum materials research. Their quantizied “molecule-like” electronic structure showcases unique stability, and physical and chemical properties differentiate them from larger nanoparticles. When integrated into inorganic materials that interact with the environment and sunlight, AMCs serve to enhance their (photo)catalytic activity and optoelectronic properties. Their tiny size makes AMCs isolated in the gas phase amenable to atom-scale modeling using either density functional theory (DFT) or methods at a high level of ab initio theory, even addressing nonadiabatic (e.g., Jahn–Teller) effects. Surface-sup ported AMCs can be routinely modeled using DFT, enabling long real-time molecular dynamics simulations. Their optical properties can also be addressed using time-dependent DFT or reduced density matrix (RDM) theory. These theoretical–computational efforts aim to achieve predictability and molecular level understanding of the stability and properties of AMCs as function of their composition, size, and structural fluxionality in different thermodynamical conditions (temperature and pressure). In this perspective, the potential of ab initio and DFT-based modeling is illustrated through recent studies of unsupported and surface-supported AMCs. Future directions of research are also discussed, including applications and methodological enhancements beyond the state-of-the-art.This work has been partially supported by the Spanish Agencia Estatal de Investigación (AEI) under Grant No. PID2020-117605GB-I00/AEI/10.13039/501100011033 and the EU Doctoral Network PHYMOL 101073474 (project call reference HORIZON-MSCA-2021-DN-01). This publication is also based on the work of COST Action CA21101 ”Confined molecular systems: from a new generation of materials to the stars” (COSY) supported by COST (European Cooperation in Science and Technology). The support of the CESGA supercomputer center (Spain) is also acknowledged. I also acknowledge support of the publication fee by the CSIC Open Access Support Initiative through its Unit of Information for Research (URICI).Peer reviewedWiley-VCHMinisterio de Ciencia e Innovación (España)European CommissionCentro de Supercomputación de GaliciaCSIC - Unidad de Recursos de Información Científica para la Investigación (URICI)Lara Castells, María Pilar de [0000-0001-8697-5770]Consejo Superior de Investigaciones Científicas [https://ror.org/02gfc7t72]202420242024info:eu-repo/semantics/articlehttp://purl.org/coar/resource_type/c_6501Publisher's versioninfo:eu-repo/semantics/publishedVersionhttp://hdl.handle.net/10261/364023reponame:DIGITAL.CSIC. Repositorio Institucional del CSICinstname:Consejo Superior de Investigaciones Científicas (CSIC)Inglés#PLACEHOLDER_PARENT_METADATA_VALUE##PLACEHOLDER_PARENT_METADATA_VALUE#info:eu-repo/grantAgreement/AEI/Plan Estatal de Investigación Científica y Técnica y de Innovación 2017-2020/PID2020-117605GB-I00info:eu-repo/grantAgreement/EC/HE/101073474https://doi.org/10.1002/sstr.202400147Síinfo:eu-repo/semantics/openAccessoai:digital.csic.es:10261/3640232026-05-22T06:33:51Z
dc.title.none.fl_str_mv An Ab Initio Journey toward the Molecular-LevelUnderstanding and Predictability of SubnanometricMetal Clusters
title An Ab Initio Journey toward the Molecular-LevelUnderstanding and Predictability of SubnanometricMetal Clusters
spellingShingle An Ab Initio Journey toward the Molecular-LevelUnderstanding and Predictability of SubnanometricMetal Clusters
Lara Castells, María Pilar de
Density functional theory and ab initio modeling
Fluxional Jahn–Teller molecules
Photocatalysis
Reversible oxidation
Subnanometric metal clusters
title_short An Ab Initio Journey toward the Molecular-LevelUnderstanding and Predictability of SubnanometricMetal Clusters
title_full An Ab Initio Journey toward the Molecular-LevelUnderstanding and Predictability of SubnanometricMetal Clusters
title_fullStr An Ab Initio Journey toward the Molecular-LevelUnderstanding and Predictability of SubnanometricMetal Clusters
title_full_unstemmed An Ab Initio Journey toward the Molecular-LevelUnderstanding and Predictability of SubnanometricMetal Clusters
title_sort An Ab Initio Journey toward the Molecular-LevelUnderstanding and Predictability of SubnanometricMetal Clusters
dc.creator.none.fl_str_mv Lara Castells, María Pilar de
author Lara Castells, María Pilar de
author_facet Lara Castells, María Pilar de
author_role author
dc.contributor.none.fl_str_mv Ministerio de Ciencia e Innovación (España)
European Commission
Centro de Supercomputación de Galicia
CSIC - Unidad de Recursos de Información Científica para la Investigación (URICI)
Lara Castells, María Pilar de [0000-0001-8697-5770]
Consejo Superior de Investigaciones Científicas [https://ror.org/02gfc7t72]
dc.subject.none.fl_str_mv Density functional theory and ab initio modeling
Fluxional Jahn–Teller molecules
Photocatalysis
Reversible oxidation
Subnanometric metal clusters
topic Density functional theory and ab initio modeling
Fluxional Jahn–Teller molecules
Photocatalysis
Reversible oxidation
Subnanometric metal clusters
description 25 pags., 15 figs., 1 tab. -- Perspective
publishDate 2024
dc.date.none.fl_str_mv 2024
2024
2024
dc.type.none.fl_str_mv info:eu-repo/semantics/article
http://purl.org/coar/resource_type/c_6501
Publisher's version
info:eu-repo/semantics/publishedVersion
format article
status_str publishedVersion
dc.identifier.none.fl_str_mv http://hdl.handle.net/10261/364023
url http://hdl.handle.net/10261/364023
dc.language.none.fl_str_mv Inglés
language_invalid_str_mv Inglés
dc.relation.none.fl_str_mv #PLACEHOLDER_PARENT_METADATA_VALUE#
#PLACEHOLDER_PARENT_METADATA_VALUE#
info:eu-repo/grantAgreement/AEI/Plan Estatal de Investigación Científica y Técnica y de Innovación 2017-2020/PID2020-117605GB-I00
info:eu-repo/grantAgreement/EC/HE/101073474
https://doi.org/10.1002/sstr.202400147
Sí
dc.rights.none.fl_str_mv info:eu-repo/semantics/openAccess
eu_rights_str_mv openAccess
dc.publisher.none.fl_str_mv Wiley-VCH
publisher.none.fl_str_mv Wiley-VCH
dc.source.none.fl_str_mv reponame:DIGITAL.CSIC. Repositorio Institucional del CSIC
instname:Consejo Superior de Investigaciones Científicas (CSIC)
instname_str Consejo Superior de Investigaciones Científicas (CSIC)
reponame_str DIGITAL.CSIC. Repositorio Institucional del CSIC
collection DIGITAL.CSIC. Repositorio Institucional del CSIC
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