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Dielectric control of reverse intersystem crossing in thermally activated delayed fluorescence emitters (Record no. 1666)

MARC details
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100 10 - MAIN ENTRY--PERSONAL NAME
Personal name Gillett, Alexander J.
Relator term author
9 (RLIN) 1393
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Title Dielectric control of reverse intersystem crossing in thermally activated delayed fluorescence emitters
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Date of publication, distribution, etc. 2022-10.
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General note /pmc/articles/PMC7613666/
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General note /pubmed/35927434
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Summary, etc. Thermally-activated delayed fluorescence (TADF) enables organic semiconductors with charge transfer (CT)-type excitons to convert dark triplet states into bright singlets via reverse intersystem crossing (rISC). However, thus far the contribution from the dielectric environment has received insufficient attention. Here, we study the role of the dielectric environment in a range of TADF materials with varying changes in dipole moment upon optical excitation. In dipolar emitters, we observe how environmental reorganisation after excitation triggers the full CT exciton formation, minimising the singlet-triplet energy gap, with the emergence of two (reactant-inactive) modes acting as a vibrational fingerprint of the CT product. In contrast, the dielectric environment plays a smaller role in less dipolar materials. The analysis of energy-time trajectories and their free-energy functions reveal that the dielectric environment significantly reduces the activation energy for rISC in dipolar TADF emitters, increasing the rISC rate by three orders of magnitude versus the isolated molecule.
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Terms governing use and reproduction
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Terms governing use and reproduction https://www.springernature.com/gp/open-research/policies/accepted-manuscript-termsUsers may view, print, copy, and download text and data-mine the content in such documents, for the purposes of academic research, subject always to the full Conditions of use: https://www.springernature.com/gp/open-research/policies/accepted-manuscript-terms
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Language note en
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Topical term or geographic name as entry element Article
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Genre/form data or focus term Text
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Personal name Pershin, Anton
Relator term author
9 (RLIN) 1394
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Personal name Pandya, Raj
Relator term author
9 (RLIN) 1395
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Personal name Feldmann, Sascha
Relator term author
9 (RLIN) 1396
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Personal name Sneyd, Alexander J.
Relator term author
9 (RLIN) 1397
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Personal name Alvertis, Antonios M.
Relator term author
9 (RLIN) 1398
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Personal name Evans, Emrys W.
Relator term author
9 (RLIN) 1399
700 10 - ADDED ENTRY--PERSONAL NAME
Personal name Thomas, Tudor H.
Relator term author
9 (RLIN) 1400
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Personal name Cui, Lin-Song
Relator term author
9 (RLIN) 1401
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Personal name Drummond, Bluebell H.
Relator term author
9 (RLIN) 1402
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Personal name Scholes, Gregory D.
Relator term author
9 (RLIN) 1403
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Personal name Olivier, Yoann
Relator term author
9 (RLIN) 1404
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Personal name Rao, Akshay
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9 (RLIN) 1405
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Personal name Friend, Richard H.
Relator term author
9 (RLIN) 1406
700 10 - ADDED ENTRY--PERSONAL NAME
Personal name Beljonne, David
Relator term author
9 (RLIN) 1407
786 0# - DATA SOURCE ENTRY
Note Nat Mater
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Uniform Resource Identifier <a href="http://dx.doi.org/10.1038/s41563-022-01321-2">http://dx.doi.org/10.1038/s41563-022-01321-2</a>
Public note Connect to this object online.

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