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

Lee, Chee Kong; Shi, Liang; Willard, Adam P.

doi:10.1021/acs.jpcc.8b11504

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

Journal Article · Wed Dec 05 00:00:00 EST 2018 · Journal of Physical Chemistry. C

DOI:https://doi.org/10.1021/acs.jpcc.8b11504· OSTI ID:1543663

Lee, Chee Kong ^[1];

^[2];

^[1]

Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States). Dept. of Chemistry
Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States). Dept. Chemistry and Chemical Biology

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.

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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); Univ. of California, Oakland, CA (United States); Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: AC02-05CH11231; SC0001088

OSTI ID:: 1543663

Journal Information:: Journal of Physical Chemistry. C, Vol. 123, Issue 1; ISSN 1932-7447

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 9 works

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