Please use this identifier to cite or link to this item: https://hdl.handle.net/10356/147043
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dc.contributor.authorWong, Walter P. D.en_US
dc.contributor.authorYin, Junen_US
dc.contributor.authorChaudary, Bhumikaen_US
dc.contributor.authorChin, Xin Yuen_US
dc.contributor.authorCortecchia, Danieleen_US
dc.contributor.authorLo, Shu-Zee A.en_US
dc.contributor.authorGrimsdale, Andrew C.en_US
dc.contributor.authorMohammed, Omar F.en_US
dc.contributor.authorLanzani, Guglielmoen_US
dc.contributor.authorSoci, Cesareen_US
dc.date.accessioned2021-03-22T02:14:05Z-
dc.date.available2021-03-22T02:14:05Z-
dc.date.issued2020-
dc.identifier.citationWong, W. P. D., Yin, J., Chaudary, B., Chin, X. Y., Cortecchia, D., Lo, S. A., Grimsdale, A. C., Mohammed, O. F., Lanzani, G. & Soci, C. (2020). Large polaron self-trapped states in three-dimensional metal-halide perovskites. ACS Materials Letters, 2(1), 20-27. https://dx.doi.org/10.1021/acsmaterialslett.9b00276en_US
dc.identifier.issn2639-4979en_US
dc.identifier.urihttps://hdl.handle.net/10356/147043-
dc.description.abstractIn recent years, metal halide perovskites have generated tremendous interest for optoelectronic applications and their underlying fundamental properties. Due to the large electron-phonon coupling characteristic of soft lattices, self-trapping phenomena are expected to dominate hybrid perovskite photoexcitation dynamics. Yet, while the photogeneration of small polarons was proven in low dimensional perovskites, the nature of polaron excitations in technologically relevant 3D perovskites, and their influence on charge carrier transport, remain elusive. In this study, we used a combination of first principle calculations and advanced spectroscopy techniques spanning the entire optical frequency range to pin down polaron features in 3D metal halide perovskites. Mid-infrared photoinduced absorption shows the photogeneration of states associated to low energy intragap electronic transitions with lifetime up to the ms time scale, and vibrational mode renormalization in both frequency and amplitude. Density functional theory supports the assignment of the spectroscopic features to large polarons leading to new intra gap transitions, hardening of phonon mode frequency, and renormalization of the oscillator strength. Theory provides quantitative estimation for the charge carrier masses and mobilities increase upon polaron formation, confirming experimental results. Overall, this work contributes to complete the scenario of elementary photoexcitations in metal halide perovskites and highlights the importance of polaronic transport in perovskite-based optoelectronic devices.en_US
dc.description.sponsorshipMinistry of Education (MOE)en_US
dc.description.sponsorshipNational Research Foundation (NRF)en_US
dc.language.isoenen_US
dc.relationNRF-CRP14-2014-03en_US
dc.relationMOE2016-T1-1-164en_US
dc.relation.ispartofACS Materials Lettersen_US
dc.rightsThis document is the Accepted Manuscript version of a Published Work that appeared in final form in ACS Materials Letters, copyright © American Chemical Society after peer review and technical editing by the publisher. To access the final edited and published work see https://doi.org/10.1021/acsmaterialslett.9b00276en_US
dc.subjectEngineering::Materials::Energy materialsen_US
dc.subjectScience::Physics::Optics and lighten_US
dc.titleLarge polaron self-trapped states in three-dimensional metal-halide perovskitesen_US
dc.typeJournal Articleen
dc.contributor.schoolSchool of Physical and Mathematical Sciencesen_US
dc.contributor.schoolSchool of Materials Science and Engineeringen_US
dc.contributor.schoolInterdisciplinary Graduate School (IGS)en_US
dc.contributor.researchEnergy Research Institute @ NTU (ERI@N)en_US
dc.identifier.doi10.1021/acsmaterialslett.9b00276-
dc.description.versionAccepted versionen_US
dc.identifier.issue1en_US
dc.identifier.volume2en_US
dc.identifier.spage20en_US
dc.identifier.epage27en_US
dc.subject.keywordsPerovskiteen_US
dc.subject.keywordsPolaronen_US
dc.description.acknowledgementResearch was supported by the National Research Foundation (NRF-CRP14-2014-03) and by the Ministry of Education (MOE2016-T1-1-164) of Singapore.en_US
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