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dc.contributor.authorde Silva, Piotr
dc.contributor.authorKim, Changhae Andrew
dc.contributor.authorZhu, Tianyu
dc.contributor.authorVan Voorhis, Troy
dc.date.accessioned2020-05-26T17:40:23Z
dc.date.available2020-05-26T17:40:23Z
dc.date.issued2019-06
dc.identifier.issn0897-4756
dc.identifier.urihttps://hdl.handle.net/1721.1/125454
dc.description.abstractWe introduce a simple quantum-mechanical model for thermally activated delayed fluorescence (TADF). The Hamiltonian is represented in the basis of four spin-mixed diabatic states representing pure charge transfer (CT) and local excitations (LE). The model predicts that it is possible to realize lowest-lying adiabatic singlet (S1) and triplet (T1) states with a small singlet-triplet gap, differing CT/LE contributions, and appreciable LE component in the S1 state. These characteristics can explain the coexistence of fast T1 → S1 reverse intersystem crossing and S1 → S0 radiative decay in some chromophores. Through the sampling of the parameter space and statistical analysis of the data, we show which parameter combinations contribute the most to the TADF efficiency. We also show that conformational fluctuations of a single model donor-acceptor system sample a significant region of the parameter space and can enhance the TADF rate by almost 3 orders of magnitude. This study provides new guidelines for optimization of TADF emitters by means of electronic structure and conformation engineering.en_US
dc.description.sponsorshipUnited States. Department of Energy. Office of Basic Energy Sciences (Grant BES ER46474)en_US
dc.language.isoen
dc.publisherAmerican Chemical Society (ACS)en_US
dc.relation.isversionofhttps://dx.doi.org/10.1021/ACS.CHEMMATER.9B01601en_US
dc.rightsArticle is made available in accordance with the publisher's policy and may be subject to US copyright law. Please refer to the publisher's site for terms of use.en_US
dc.sourceOther repositoryen_US
dc.titleExtracting Design Principles for Efficient Thermally Activated Delayed Fluorescence (TADF) from a Simple Four-State Modelen_US
dc.typeArticleen_US
dc.identifier.citationSilva, Piotr de et al. “Extracting Design Principles for Efficient Thermally Activated Delayed Fluorescence (TADF) from a Simple Four-State Model.” Chemistry of materials 31 (2019): 6995-7006.en_US
dc.contributor.departmentMassachusetts Institute of Technology. Department of Chemistryen_US
dc.relation.journalChemistry of materialsen_US
dc.eprint.versionOriginal manuscripten_US
dc.type.urihttp://purl.org/eprint/type/JournalArticleen_US
eprint.statushttp://purl.org/eprint/status/NonPeerRevieweden_US
dc.date.updated2020-01-14T14:36:17Z
dspace.date.submission2020-01-14T14:36:19Z
mit.journal.volume31en_US
mit.journal.issue17en_US
mit.licensePUBLISHER_POLICY
mit.metadata.statusComplete


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