Up-Conversion Intersystem Crossing Rates in Organic Emitters for Thermally Activated Delayed Fluorescence: Impact of the Nature of Singlet vs Triplet Excited States

Samanta, Pralok K.; Kim, Dongwook; Coropceanu, Veaceslav; Brédas, Jean-Luc

doi:10.1021/jacs.6b12124

Cited by 1,025Organic Light-Emitting Diodes ResearchLuminescence and Fluorescent MaterialsPhotochemistry and Electron Transfer Studies

Up-Conversion Intersystem Crossing Rates in Organic Emitters for Thermally Activated Delayed Fluorescence: Impact of the Nature of Singlet vs Triplet Excited States

Samanta, Pralok K., Kim, Dongwook, Coropceanu, Veaceslav, Brédas, Jean-Luc·2017·Journal of the American Chemical Society

DOI 10.1021/jacs.6b12124

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Abstract

The rates for up-conversion intersystem crossing (UISC) from the T 1 state to the S 1 state are calculated for a series of organic emitters with an emphasis on thermally activated delayed fluorescence (TADF) materials. Both the spin–orbit coupling and the energy difference between the S 1 and T 1 states (Δ E ST ) are evaluated, at the density functional theory (DFT) and time-dependent DFT levels. The calculated UISC rates and Δ E ST values are found to be in good agreement with available experimental data. Our results underline that small Δ E ST values and sizable spin–orbit coupling matrix elements have to be simultaneously realized in order to facilitate UISC and ultimately TADF. Importantly, the spatial separation of the highest occupied and lowest unoccupied molecular orbitals of the emitter, a widely accepted strategy for the design of TADF molecules, does not necessarily lead to a sufficient reduction in Δ E ST; in fact, either a significant charge-transfer (CT) contribution to the T 1 state or a minimal energy difference between the local-excitation and charge-transfer triplet states is required to achieve a small Δ E ST . Also, having S 1 and T 1 states of a different nature is found to strongly enhance spin–orbit coupling, which is consistent with the El-Sayed rule for ISC rates. Overall, our results indicate that having either similar energies for the local-excitation and charge-transfer triplet states or the right balance between a substantial CT contribution to T 1 and somewhat different natures of the S 1 and T 1 states, paves the way toward UISC enhancement and thus TADF efficiency improvement.

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Authors: Samanta, P. K., Kim, D., Coropceanu, V., & Brédas, J.-L.
Affiliations: King Abdullah University of Science and Technology (SA)
Kyonggi University (KR)
Georgia Institute of Technology (US)
Corresponding author: Kim, Dongwook
Brédas, Jean-Luc
ORCID: Samanta, Pralok K.
Kim, Dongwook
Coropceanu, Veaceslav
Brédas, Jean-Luc
Venue: Journal of the American Chemical Society
Publisher: American Chemical Society (ACS)
Published: 2017-03-13
Volume: 139
Issue: 11
Pages: 4042-4051
ISSN: 0002-7863 (ISSN-L)
1520-5126
DOI: 10.1021/jacs.6b12124
OpenAlex: W2592066197
Cited by: 1,025
References: 60
Citations by year: 2026: 91 · 2025: 125 · 2024: 142 · 2023: 150 · 2022: 143 · 2021: 120 · 2020: 98 · 2019: 79 · 2018: 62 · 2017: 15
FWCI: 28.88
Type: journal article
Language: en
Open access: closed
Locations: Journal of the American Chemical Society (publishedVersion)
PubMed (publishedVersion)
King Abdullah University of Science and Technology Repository (King Abdullah University of Science and Technology) (submittedVersion)
Funders: National Research Foundation of Korea (2015R1D1A1A01061487)
King Abdullah University of Science and Technology
Topics: Physical Sciences › Engineering › Electrical and Electronic Engineering › Organic Light-Emitting Diodes Research
Physical Sciences › Materials Science › Materials Chemistry › Luminescence and Fluorescent Materials
Physical Sciences › Chemistry › Physical and Theoretical Chemistry › Photochemistry and Electron Transfer Studies
Keywords: thermally activated delayed fluorescence, spin-orbit coupling, singlet-triplet energy difference, organic emitters, charge-transfer states

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Up-Conversion Intersystem Crossing Rates in Organic Emitters for Thermally Activated Delayed Fluorescence: Impact of the Nature of Singlet vs Triplet Excited States

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