dc.creator | Menéndez-Proupin, Eduardo | es |
dc.creator | Grover, Shivani | es |
dc.creator | Montero-Alejo, Ana L. | es |
dc.creator | Midgley, Scott D. | es |
dc.creator | Butler, Keith T. | es |
dc.creator | Grau-Crespo, Ricardo | es |
dc.date.accessioned | 2024-04-23T11:14:34Z | |
dc.date.available | 2024-04-23T11:14:34Z | |
dc.date.issued | 2022-05 | |
dc.identifier.issn | 2050-7488 | es |
dc.identifier.issn | 2050-7496 | es |
dc.identifier.uri | https://hdl.handle.net/11441/157025 | |
dc.description.abstract | Mixed-anion mixed-cation perovskites with (FAPbI₃)₁-ₓ(MAPbBr₃)ₓ composition have allowed record
efficiencies in photovoltaic solar cells, but their atomic-scale behaviour is not well understood yet, in
part because their theoretical modelling requires consideration of complex and interrelated dynamic and
disordering effects. We present here an ab initio molecular dynamics investigation of the structural,
thermodynamic, and electronic properties of the (FAPbI₃)₀ꓸ₈₇₅ (MAPbBr₃)₀ꓸ₁₂₅ perovskite. A special quasirandom
structure is proposed to mimic the disorder of both the molecular cations and the halide anions,
in a stoichiometry that is close to that of one of today's most efficient perovskite solar cells. We show
that the rotation of the organic cations is more strongly hindered in the mixed structure in comparison
with the pure compounds. Our analysis suggests that this mixed perovskite is thermodynamically stable
against phase separation despite the endothermic mixing enthalpy, due to the large configurational
entropy. The electronic properties are investigated by hybrid density functional calculations including
spin–orbit coupling in carefully selected representative configurations extracted from the molecular
dynamics. Our model, that is validated here against experimental information, provides a more
sophisticated understanding of the interplay between dynamic and disordering effects in this important
family of photovoltaic materials. | es |
dc.format | application/pdf | es |
dc.format.extent | 13 p. | es |
dc.language.iso | eng | es |
dc.publisher | American Chemical Society | es |
dc.rights | Atribución 4.0 Internacional | * |
dc.rights.uri | http://creativecommons.org/licenses/by/4.0/ | * |
dc.title | Mixed-anion mixed-cation perovskite (FAPbI₃)₀ꓸ₈₇₅ (MAPbBr₃)₀ꓸ₁₂₅: an ab initio molecular dynamics study | es |
dc.type | info:eu-repo/semantics/article | es |
dc.type.version | info:eu-repo/semantics/acceptedVersion | es |
dc.rights.accessRights | info:eu-repo/semantics/openAccess | es |
dc.contributor.affiliation | Universidad de Sevilla. Departamento de Física Aplicada I | es |
dc.relation.projectID | NLHPC ECM-02 | es |
dc.relation.projectID | EP/R029431 | es |
dc.relation.projectID | EP/P020194/1 | es |
dc.relation.projectID | EP/T022213/1 | es |
dc.relation.projectID | ANID/CONICYT/FONDECYT Regular 1171807 | es |
dc.relation.publisherversion | https://pubs.rsc.org/en/content/articlelanding/2022/ta/d1ta10860c | es |
dc.identifier.doi | 10.1039/D1TA10860C | es |
dc.contributor.group | Universidad de Sevilla. FQM401: Simulación y Aplicación de Materiales | es |
dc.journaltitle | Journal of Materials Chemistry A | es |
dc.publication.volumen | 10 | es |
dc.publication.issue | 17 | es |
dc.publication.initialPage | 9592 | es |
dc.publication.endPage | 9603 | es |
dc.contributor.funder | Laboratorio Nacional de Computación de Alto Rendimiento (NLHPC). Chile | es |
dc.contributor.funder | Engineering and Physical Sciences Research Council (UK) | es |
dc.contributor.funder | La Agencia Nacional de Investigación y Desarrollo (ANID). Chile | es |
dc.contributor.funder | Comisión Nacional de Investigación Científica y Tecnológica (CONICYT). Chile | es |
dc.contributor.funder | Fondo Nacional de Desarrollo Científico y Tecnológico (FONDECYT). Chile | es |