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Title: Modeling the Influence of Correlated Molecular Disorder on the Dynamics of Excitons in Organic Molecular Semiconductors

Journal Article · · Journal of Physical Chemistry. C
 [1]; ORCiD logo [2]; ORCiD logo [1]
  1. Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States). Dept. of Chemistry
  2. Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States). Dept. Chemistry and Chemical Biology
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In this paper, we investigate the role of correlated molecular disorder on the dynamics of excitons in oligothiophene-based organic semiconductors. We simulate exciton dynamics using the Frenkel exciton model and derive parameters for this model so that they reflect the specific characteristics of all-atom molecular systems. By systematically modifying the parameters of the Frenkel exciton model, we isolate the influence of spatial and temporal molecular correlations on the dynamics of excitons in these systems. For the oligothiophene systems considered here, we find that the molecular fluctuations exhibit long-lived memory effects, but these effects do not significantly influence the dynamic properties of excitons. We also find that excitons can be sensitive to the molecular-scale spatial correlations, and that this sensitivity grows with the amount of energetic disorder within the material. We conclude that control over spatial correlations can mitigate the negative influence of disorder on exciton transport.

Research Organization:
Energy Frontier Research Centers (EFRC) (United States). Center for Excitonics (CE); Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). National Energy Research Scientific Computing Center (NERSC); Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States); Univ. of California, Oakland, CA (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
Grant/Contract Number:
AC02-05CH11231; SC0001088
OSTI ID:
1543663
Journal Information:
Journal of Physical Chemistry. C, Journal Name: Journal of Physical Chemistry. C Journal Issue: 1 Vol. 123; ISSN 1932-7447
Publisher:
American Chemical SocietyCopyright Statement
Country of Publication:
United States
Language:
English

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