Coherent Dynamics of Mixed Frenkel and Charge-Transfer Excitons in Dinaphtho[2,3- b :2'3'- f ]thieno[3,2- b ]-thiophene Thin Films: The Importance of Hole Delocalization
Abstract
Charge-transfer states in organic semiconductors play crucial roles in processes such as singlet fission and exciton dissociation at donor/acceptor interfaces. Recently, a time-resolved spectroscopy study of dinaphtho[2,3-b:2'3'-f]thieno[3,2-b]-thiophene (DNTT) thin films provided evidence for the formation of mixed Frenkel and charge-transfer excitons after the photoexcitation. In this study, we investigate optical properties and excitation dynamics of the DNTT thin films by combining ab initio calculations and a stochastic Schrödinger equation. Our theory predicts that the low-energy Frenkel exciton band consists of 8–47% CT character. The quantum dynamics simulations show coherent dynamics of Frenkel and CT states in 50 fs after the optical excitation. Lastly, we demonstrate the role of charge delocalization and localization in the mixing of CT states with Frenkel excitons as well as the role of their decoherence.
- Authors:
-
- Kyoto Univ. (Japan)
- TOBB Univ. of Economics and Technology, Sogutozu, Ankara (Turkey)
- Harvard Univ., Cambridge, MA (United States)
- Publication Date:
- Research Org.:
- Energy Frontier Research Centers (EFRC) (United States). Center for Excitonics (CE)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES)
- OSTI Identifier:
- 1371366
- Grant/Contract Number:
- SC0001088
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Journal of Physical Chemistry Letters
- Additional Journal Information:
- Journal Volume: 7; Journal Issue: 7; Related Information: CE partners with Massachusetts Institute of Technology (lead); Brookhaven National Laboratory; Harvard University; Journal ID: ISSN 1948-7185
- Publisher:
- American Chemical Society
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITY; 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; solar (photovoltaic); solid state lighting; photosynthesis (natural and artificial); charge transport; optics; synthesis (novel materials); synthesis (self-assembly); synthesis (scalable processing)
Citation Formats
Fujita, Takatoshi, Atahan-Evrenk, Sule, Sawaya, Nicolas P. D., and Aspuru-Guzik, Alán. Coherent Dynamics of Mixed Frenkel and Charge-Transfer Excitons in Dinaphtho[2,3- b :2'3'- f ]thieno[3,2- b ]-thiophene Thin Films: The Importance of Hole Delocalization. United States: N. p., 2016.
Web. doi:10.1021/acs.jpclett.6b00364.
Fujita, Takatoshi, Atahan-Evrenk, Sule, Sawaya, Nicolas P. D., & Aspuru-Guzik, Alán. Coherent Dynamics of Mixed Frenkel and Charge-Transfer Excitons in Dinaphtho[2,3- b :2'3'- f ]thieno[3,2- b ]-thiophene Thin Films: The Importance of Hole Delocalization. United States. https://doi.org/10.1021/acs.jpclett.6b00364
Fujita, Takatoshi, Atahan-Evrenk, Sule, Sawaya, Nicolas P. D., and Aspuru-Guzik, Alán. Thu .
"Coherent Dynamics of Mixed Frenkel and Charge-Transfer Excitons in Dinaphtho[2,3- b :2'3'- f ]thieno[3,2- b ]-thiophene Thin Films: The Importance of Hole Delocalization". United States. https://doi.org/10.1021/acs.jpclett.6b00364. https://www.osti.gov/servlets/purl/1371366.
@article{osti_1371366,
title = {Coherent Dynamics of Mixed Frenkel and Charge-Transfer Excitons in Dinaphtho[2,3- b :2'3'- f ]thieno[3,2- b ]-thiophene Thin Films: The Importance of Hole Delocalization},
author = {Fujita, Takatoshi and Atahan-Evrenk, Sule and Sawaya, Nicolas P. D. and Aspuru-Guzik, Alán},
abstractNote = {Charge-transfer states in organic semiconductors play crucial roles in processes such as singlet fission and exciton dissociation at donor/acceptor interfaces. Recently, a time-resolved spectroscopy study of dinaphtho[2,3-b:2'3'-f]thieno[3,2-b]-thiophene (DNTT) thin films provided evidence for the formation of mixed Frenkel and charge-transfer excitons after the photoexcitation. In this study, we investigate optical properties and excitation dynamics of the DNTT thin films by combining ab initio calculations and a stochastic Schrödinger equation. Our theory predicts that the low-energy Frenkel exciton band consists of 8–47% CT character. The quantum dynamics simulations show coherent dynamics of Frenkel and CT states in 50 fs after the optical excitation. Lastly, we demonstrate the role of charge delocalization and localization in the mixing of CT states with Frenkel excitons as well as the role of their decoherence.},
doi = {10.1021/acs.jpclett.6b00364},
journal = {Journal of Physical Chemistry Letters},
number = 7,
volume = 7,
place = {United States},
year = {Thu Mar 24 00:00:00 EDT 2016},
month = {Thu Mar 24 00:00:00 EDT 2016}
}
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