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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

Journal Article · · Journal of Physical Chemistry Letters
 [1];  [2];  [3];  [3]
  1. Kyoto Univ. (Japan)
  2. TOBB Univ. of Economics and Technology, Sogutozu, Ankara (Turkey)
  3. Harvard Univ., Cambridge, MA (United States)
+ Show Author Affiliations

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.

Research Organization:
Energy Frontier Research Centers (EFRC) (United States). Center for Excitonics (CE)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
Grant/Contract Number:
SC0001088
OSTI ID:
1371366
Journal Information:
Journal of Physical Chemistry Letters, Journal Name: Journal of Physical Chemistry Letters Journal Issue: 7 Vol. 7; ISSN 1948-7185
Publisher:
American Chemical SocietyCopyright Statement
Country of Publication:
United States
Language:
English

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Cited By (10)

Tuning the effective spin-orbit coupling in molecular semiconductors text January 2017
The hierarchical and perturbative forms of stochastic Schrödinger equations and their applications to carrier dynamics in organic materials journal July 2018
Rational design of the nonlinear optical materials dinaphtho[2,3-b:2′,3′-d]thiophene-5,7,12,13-tetraone (DNTTRA) and its phenyldiazenyl derivatives using first-principles calculations journal January 2019
Tuning the effective spin-orbit coupling in molecular semiconductors journal May 2017
Charge separation at an organic/inorganic nano-hybrid interface: atomistic simulations of a para -sexiphenyl ZnO system journal January 2018
Thousand-atom ab initio calculations of excited states at organic/organic interfaces: toward first-principles investigations of charge photogeneration journal January 2018
Modeling the effects of molecular disorder on the properties of Frenkel excitons in organic molecular semiconductors journal September 2018
Charge-transfer excited states in the donor/acceptor interface from large-scale GW calculations journal September 2019
Tuning the effective spin-orbit coupling in molecular semiconductors text January 2017
The hierarchical and perturbative forms of stochastic Schrödinger equations and their applications to carrier dynamics in organic materials text January 2018

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Related Subjects

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
75 CONDENSED MATTER PHYSICS
SUPERCONDUCTIVITY AND SUPERFLUIDITY
charge transport
optics
photosynthesis (natural and artificial)
solar (photovoltaic)
solid state lighting
synthesis (novel materials)
synthesis (scalable processing)
synthesis (self-assembly)