Simplified Models for Accelerated Structural Prediction of Conjugated Semiconducting Polymers

Henry, Michael M.; Jones, Matthew L.; Oosterhout, Stefan D.; Braunecker, Wade A.; Kemper, Travis W.; Larsen, Ross E.; Kopidakis, Nikos; Toney, Michael F.; Olson, Dana C.; Jankowski, Eric

doi:10.1021/acs.jpcc.7b09701

Simplified Models for Accelerated Structural Prediction of Conjugated Semiconducting Polymers

Journal Article · Wed Nov 08 00:00:00 EST 2017 · Journal of Physical Chemistry. C

DOI:https://doi.org/10.1021/acs.jpcc.7b09701· OSTI ID:1412100

^[1]; ^[1]; ^[2]; ^[2]; Kemper, Travis W. ^[2]; Larsen, Ross E. ^[2]; Kopidakis, Nikos ^[3]; ^[4]; Olson, Dana C. ^[2]; ^[5]

Boise State Univ., ID (United States)
National Renewable Energy Lab. (NREL), Golden, CO (United States)
National Renewable Energy Lab. (NREL), Golden, CO (United States); Macquarie Univ., NSW (Australia)
SLAC National Accelerator Lab., Menlo Park, CA (United States)
National Renewable Energy Lab. (NREL), Golden, CO (United States); Boise State Univ., ID (United States)

We perform molecular dynamics simulations of poly(benzodithiophene-thienopyrrolodione) (BDT-TPD) oligomers in order to evaluate the accuracy with which unoptimized molecular models can predict experimentally characterized morphologies. The predicted morphologies are characterized using simulated grazing-incidence X-ray scattering (GIXS) and compared to the experimental scattering patterns. We find that approximating the aromatic rings in BDT-TPD with rigid bodies, rather than combinations of bond, angle, and dihedral constraints, results in 14% lower computational cost and provides nearly equivalent structural predictions compared to the flexible model case. The predicted glass transition temperature of BDT-TPD (410 +/- 32 K) is found to be in agreement with experiments. Predicted morphologies demonstrate short-range structural order due to stacking of the chain backbones (p-p stacking around 3.9 A), and long-range spatial correlations due to the self-organization of backbone stacks into 'ribbons' (lamellar ordering around 20.9 A), representing the best-to-date computational predictions of structure of complex conjugated oligomers. We find that expensive simulated annealing schedules are not needed to predict experimental structures here, with instantaneous quenches providing nearly equivalent predictions at a fraction of the computational cost of annealing. We therefore suggest utilizing rigid bodies and fast cooling schedules for high-throughput screening studies of semiflexible polymers and oligomers to utilize their significant computational benefits where appropriate.

View Accepted Manuscript (DOE)

Research Organization:: National Renewable Energy Lab. (NREL), Golden, CO (United States)

Sponsoring Organization:: USDOE Office of Energy Efficiency and Renewable Energy (EERE), Solar Energy Technologies Office (EE-4S), SunShot National Laboratory Multiyear Partnership (SuNLaMP)

Grant/Contract Number:: AC36-08GO28308

OSTI ID:: 1412100

Report Number(s):: NREL/JA--5900-70618

Journal Information:: Journal of Physical Chemistry. C, Journal Name: Journal of Physical Chemistry. C Journal Issue: 47 Vol. 121; ISSN 1932-7447

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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