TY - JOUR
T1 - Characterization of Excited States in a Multiple-Resonance-Type Thermally Activated Delayed Fluorescence Molecule Using Time-Resolved Infrared Spectroscopy
AU - Saigo, Masaki
AU - Shimoda, Yuushi
AU - Ehara, Takumi
AU - Ryu, Tomohiro
AU - Miyata, Kiyoshi
AU - Onda, Ken
N1 - Funding Information:
This work was supported in part by JSPS KAKENHI with grant numbers JP17H06375, JP18H05170, JP19K15508, and JP20J21226 and the Iketani Science and Technology Foundation (ISTF). The computations were performed using the Research Centre for Computational Science (National Institute of Natural Sciences) and the Research Institute for Information Technology (Kyushu University).
Publisher Copyright:
© 2022 Chemical Society of Japan. All rights reserved.
PY - 2022
Y1 - 2022
N2 - We investigated the correlation between the photophysical properties and detailed excited-state characteristics of a multiple-resonance-type thermally activated delayed fluorescence (TADF) molecule, DABNA-1, using time-resolved infrared vibrational spectroscopy. By comparing the distinctive vibrational spectra in the fingerprint region (10001700 cm11) to the simulated spectra, we found the optimal calculation conditions for density functional theory calculations to retrieve the vibrational spectra. Based on the calculations, the excited-state geometries and molecular orbitals in the lowest excited singlet (S1) and triplet (T1) states, as well as the ground state (S0), were determined. Consequently, we revealed that the similarity between the potential surfaces of T1 and S0 suppressed non-radiative decay and improved the high fluorescence quantum yield via TADF. Furthermore, we calculated the spin-orbit coupling matrix elements (SOCMEs) considering the experimentally confirmed geometries, and revealed that twisting of the main skeleton increases the SOCMEs.
AB - We investigated the correlation between the photophysical properties and detailed excited-state characteristics of a multiple-resonance-type thermally activated delayed fluorescence (TADF) molecule, DABNA-1, using time-resolved infrared vibrational spectroscopy. By comparing the distinctive vibrational spectra in the fingerprint region (10001700 cm11) to the simulated spectra, we found the optimal calculation conditions for density functional theory calculations to retrieve the vibrational spectra. Based on the calculations, the excited-state geometries and molecular orbitals in the lowest excited singlet (S1) and triplet (T1) states, as well as the ground state (S0), were determined. Consequently, we revealed that the similarity between the potential surfaces of T1 and S0 suppressed non-radiative decay and improved the high fluorescence quantum yield via TADF. Furthermore, we calculated the spin-orbit coupling matrix elements (SOCMEs) considering the experimentally confirmed geometries, and revealed that twisting of the main skeleton increases the SOCMEs.
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U2 - 10.1246/bcsj.20210403
DO - 10.1246/bcsj.20210403
M3 - Article
AN - SCOPUS:85127597148
SN - 0009-2673
VL - 95
SP - 381
EP - 388
JO - Bulletin of the Chemical Society of Japan
JF - Bulletin of the Chemical Society of Japan
IS - 3
ER -