Energy Transfer Dynamics in Triplet–Triplet Annihilation Upconversion Using a Bichromophoric Heavy-Atom-Free Sensitizer

Chen, Qi; Liu, Yiming; Guo, Xinyan; Peng, Jiang; Garakyaraghi, Sofia; Papa, Christopher M.; Castellano, Felix N.; Zhao, Dahui; Ma, Yuguo

doi:10.1021/acs.jpca.8b05901

Title: Energy Transfer Dynamics in Triplet–Triplet Annihilation Upconversion Using a Bichromophoric Heavy-Atom-Free Sensitizer

Journal Article · Fri Jul 27 00:00:00 EDT 2018 · Journal of Physical Chemistry. A, Molecules, Spectroscopy, Kinetics, Environment, and General Theory

DOI:https://doi.org/10.1021/acs.jpca.8b05901· OSTI ID:1633631

Chen, Qi ^[1]; Liu, Yiming ^[1]; Guo, Xinyan ^[1]; Peng, Jiang ^[1];

^[2]; Papa, Christopher M. ^[2];

^[2];

^[1];

^[1]

Peking Univ., Beijing (China)
North Carolina State Univ., Raleigh, NC (United States)

A heavy-atom-free triplet sensitizer suitable for triplet-triplet annihilation-based photon upconversion was developed from the thermally activated delayed fluorescence (TADF) molecule 4CzPN by covalently tethering a pyrene derivative (DBP) as a triplet acceptor. The triplet exciton produced by 4CzPN is captured by the intramolecular pyrenyl acceptor and subsequently transferred via intermolecular triplet–triplet energy transfer (TTET) to freely diffusing pyrenyl acceptors in toluene. Transient absorption and time-resolved photoluminescence spectroscopy were employed to examine the dynamics of both the intra- and intermolecular TTET processes, and the results show that the intramolecular energy transfer from 4CzPN to DBP is swift, quantitative, and nearly irreversible. The reverse intersystem crossing is suppressed while intersystem crossing remains efficient, attaining high triplet yield and long triplet lifetime at the same time. The ultra-long excited state lifetime characteristic of the DBP triplet was shown to be crucial for enhancing the intermolecular TTET efficiency and the subsequent triplet–triplet annihilation photochemistry. It was further demonstrated that with the long triplet lifetime of the tethered DBP, TTET was enabled under low free acceptor concentrations and/or with sluggish molecular diffusion in polymer matrices.

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Research Organization:: North Carolina State University, Raleigh, NC (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences, and Biosciences Division; National Natural Science Foundation (NSFC)

Grant/Contract Number:: SC0011979

OSTI ID:: 1633631

Journal Information:: Journal of Physical Chemistry. A, Molecules, Spectroscopy, Kinetics, Environment, and General Theory, Vol. 122, Issue 33; ISSN 1089-5639

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 30 works

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