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

Abstract

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.

Authors:
 [1];  [1];  [1];  [1]; ORCiD logo [2];  [2]; ORCiD logo [2]; ORCiD logo [1]; ORCiD logo [1]
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  1. Peking Univ., Beijing (China)
  2. North Carolina State Univ., Raleigh, NC (United States)
Publication Date:
Research Org.:
North Carolina State University, Raleigh, NC (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences, and Biosciences Division; National Natural Science Foundation (NSFC)
OSTI Identifier:
1633631
Grant/Contract Number:  
SC0011979
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Physical Chemistry. A, Molecules, Spectroscopy, Kinetics, Environment, and General Theory
Additional Journal Information:
Journal Volume: 122; Journal Issue: 33; Journal ID: ISSN 1089-5639
Publisher:
American Chemical Society
Country of Publication:
United States
Language:
English
Subject:
14 SOLAR ENERGY

Citation Formats

Chen, Qi, Liu, Yiming, Guo, Xinyan, Peng, Jiang, Garakyaraghi, Sofia, Papa, Christopher M., Castellano, Felix N., Zhao, Dahui, and Ma, Yuguo. Energy Transfer Dynamics in Triplet–Triplet Annihilation Upconversion Using a Bichromophoric Heavy-Atom-Free Sensitizer. United States: N. p., 2018. Web. doi:10.1021/acs.jpca.8b05901.
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Chen, Qi, Liu, Yiming, Guo, Xinyan, Peng, Jiang, Garakyaraghi, Sofia, Papa, Christopher M., Castellano, Felix N., Zhao, Dahui, & Ma, Yuguo. Energy Transfer Dynamics in Triplet–Triplet Annihilation Upconversion Using a Bichromophoric Heavy-Atom-Free Sensitizer. United States. https://doi.org/10.1021/acs.jpca.8b05901
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Chen, Qi, Liu, Yiming, Guo, Xinyan, Peng, Jiang, Garakyaraghi, Sofia, Papa, Christopher M., Castellano, Felix N., Zhao, Dahui, and Ma, Yuguo. Fri . "Energy Transfer Dynamics in Triplet–Triplet Annihilation Upconversion Using a Bichromophoric Heavy-Atom-Free Sensitizer". United States. https://doi.org/10.1021/acs.jpca.8b05901. https://www.osti.gov/servlets/purl/1633631.
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@article{osti_1633631,
title = {Energy Transfer Dynamics in Triplet–Triplet Annihilation Upconversion Using a Bichromophoric Heavy-Atom-Free Sensitizer},
author = {Chen, Qi and Liu, Yiming and Guo, Xinyan and Peng, Jiang and Garakyaraghi, Sofia and Papa, Christopher M. and Castellano, Felix N. and Zhao, Dahui and Ma, Yuguo},
abstractNote = {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.},
doi = {10.1021/acs.jpca.8b05901},
journal = {Journal of Physical Chemistry. A, Molecules, Spectroscopy, Kinetics, Environment, and General Theory},
number = 33,
volume = 122,
place = {United States},
year = {Fri Jul 27 00:00:00 EDT 2018},
month = {Fri Jul 27 00:00:00 EDT 2018}
}
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