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Dual Fluorescence of Octatetraene Hints at a Novel Type of Singlet-to-Singlet Thermally Activated Delayed Fluorescence Process

Park, Woojin and Shen, Jun and Lee, Seunghoon and Piecuch, Piotr and Joo, Taiha and Filatov (Gulak), Michael and Choi, Cheol Ho (2022) Dual Fluorescence of Octatetraene Hints at a Novel Type of Singlet-to-Singlet Thermally Activated Delayed Fluorescence Process. Journal of Physical Chemistry C, 126 (35). pp. 14976-14985. ISSN 1932-7447. doi:10.1021/acs.jpcc.2c04105.

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A novel type of singlet-to-singlet thermally activated delayed fluorescence (STS-TADF) from the optically bright 1⁺Bᵤ⁺ and dark 2¹A_(g)⁻ states of octatetraene is proposed based on state-of-the-art ab initio simulations. The new phenomenon bears similarity with TADF, the key difference being that in the normal TADF the emissive state is repopulated from a nearby triplet, whereas in STS-TADF it occurs from a nearby dark singlet state (2¹A_(g)⁻). The nonadiabatic populations of the bright and dark singlet excited states are dynamically redistributed through a conical intersection mediated by an ultrafast skeleton C–C stretching vibration, establishing a steady state for a sufficiently long time to undergo radiative decay. The steady state manifests itself in the experimentally observed dual fluorescence. It is expected that the STS-TADF can be observed in other π-conjugated chromophores as well.

Item Type:Article
Related URLs:
URLURL TypeDescription
Shen, Jun0000-0003-1838-3719
Lee, Seunghoon0000-0003-3665-587X
Piecuch, Piotr0000-0002-7207-1815
Joo, Taiha0000-0003-2690-7789
Filatov (Gulak), Michael0000-0002-1541-739X
Choi, Cheol Ho0000-0002-8757-1396
Additional Information:C.H.C. thanks the Samsung Science and Technology Foundations (SSTF-BA1701-12) and the National Research Foundation of Korea (2020R1A2C2008246 and 2020R1A5A1019141). This work was also supported by the Korea Polar Research Institute (KOPRI, PE22120) funded by the Ministry of Oceans and Fisheries. P.P. thanks the Chemical Sciences, Geosciences and Biosciences Division, Office of Basic Energy Sciences, Office of Science, U.S. Department of Energy (DE-FG02-01ER15228).
Funding AgencyGrant Number
Samsung Science and Technology FoundationSSTF-BA1701-12
National Research Foundation of Korea2020R1A2C2008246
National Research Foundation of Korea2020R1A5A1019141
Ministry of Oceans and Fisheries (Korea)PE22120
Department of Energy (DOE)DE-FG02-01ER15228
Issue or Number:35
Record Number:CaltechAUTHORS:20221010-454096500.19
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Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:117303
Deposited By: Research Services Depository
Deposited On:14 Oct 2022 17:52
Last Modified:14 Oct 2022 17:52

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