Quantitative Hole Mobility Simulation and Validation in Substituted Acenes

Daniel Vong; Tahereh Nematiaram; Makena A. Dettmann; Tucker L. Murrey; Lucas S.R. Cavalcante; Sadi M. Gurses; Dhanya Radhakrishnan; Luke L. Daemen; John E. Anthony; Kristie J. Koski; Coleman X. Kronawitter; Alessandro Troisi; Adam J. Moulé

doi:10.1021/acs.jpclett.2c00898

Quantitative Hole Mobility Simulation and Validation in Substituted Acenes

Daniel Vong, Tahereh Nematiaram, Makena A. Dettmann, Tucker L. Murrey, Lucas S.R. Cavalcante, Sadi M. Gurses, Dhanya Radhakrishnan, Luke L. Daemen, John E. Anthony, Kristie J. Koski, Coleman X. Kronawitter, Alessandro Troisi, Adam J. Moulé

Chemical Spectroscopy

Research output: Contribution to journal › Article › peer-review

10 Scopus citations

Abstract

Knowledge of the full phonon spectrum is essential to accurately calculate the dynamic disorder (σ) and hole mobility (μ_h) in organic semiconductors (OSCs). However, most vibrational spectroscopy techniques under-measure the phonons, thus limiting the phonon validation. Here, we measure and model the full phonon spectrum using multiple spectroscopic techniques and predict μ_husing σ from only the Γ-point and the full Brillouin zone (FBZ). We find that only inelastic neutron scattering (INS) provides validation of all phonon modes, and that σ in a set of small molecule semiconductors can be miscalculated by up to 28% when comparing Γ-point against FBZ calculations. A subsequent mode analysis shows that many modes contribute to σ and that no single mode dominates. Our results demonstrate the importance of a thoroughly validated phonon calculation, and a need to develop design rules considering the full spectrum of phonon modes.

Original language	English
Pages (from-to)	5530-5537
Number of pages	8
Journal	Journal of Physical Chemistry Letters
Volume	13
Issue number	24
DOIs	https://doi.org/10.1021/acs.jpclett.2c00898
State	Published - Jun 23 2022

Funding

This research was supported by the Department of Energy, Basic Energy Sciences, Award DE-SC0010419, including salary for D.V., M.D., L.S.R.C., and A.J.M. This research used resources of the National Energy Research Scientific Computing Center (NERSC), a DOE Office of Science User Facility supported by the Office of Science of the U.S. Department of Energy under Contract No. DE-AC02-05CH11231. The INS spectrum was measured at the Spallation Neutron Source, a DOE Office of Science User Facility operated by the Oak Ridge National Laboratory, partly supported by LLNL under Contract DE-AC52-07NA27344. J.E.A. was supported by the National Science Foundation, under cooperative agreement No. 1849213. T.N. and A.T. acknowledge the financial support from ERC (PoC grant No. 403098).

Funders	Funder number
National Science Foundation	1849213
U.S. Department of Energy	DE-AC02-05CH11231
Office of Science
Basic Energy Sciences	DE-SC0010419
Lawrence Livermore National Laboratory	DE-AC52-07NA27344
Oak Ridge National Laboratory
Engineering Research Centers	403098

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Vong, D., Nematiaram, T., Dettmann, M. A., Murrey, T. L., Cavalcante, L. S. R., Gurses, S. M., Radhakrishnan, D., Daemen, L. L., Anthony, J. E., Koski, K. J., Kronawitter, C. X., Troisi, A., & Moulé, A. J. (2022). Quantitative Hole Mobility Simulation and Validation in Substituted Acenes. Journal of Physical Chemistry Letters, 13(24), 5530-5537. https://doi.org/10.1021/acs.jpclett.2c00898

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title = "Quantitative Hole Mobility Simulation and Validation in Substituted Acenes",

abstract = "Knowledge of the full phonon spectrum is essential to accurately calculate the dynamic disorder (σ) and hole mobility (μh) in organic semiconductors (OSCs). However, most vibrational spectroscopy techniques under-measure the phonons, thus limiting the phonon validation. Here, we measure and model the full phonon spectrum using multiple spectroscopic techniques and predict μhusing σ from only the Γ-point and the full Brillouin zone (FBZ). We find that only inelastic neutron scattering (INS) provides validation of all phonon modes, and that σ in a set of small molecule semiconductors can be miscalculated by up to 28% when comparing Γ-point against FBZ calculations. A subsequent mode analysis shows that many modes contribute to σ and that no single mode dominates. Our results demonstrate the importance of a thoroughly validated phonon calculation, and a need to develop design rules considering the full spectrum of phonon modes.",

author = "Daniel Vong and Tahereh Nematiaram and Dettmann, {Makena A.} and Murrey, {Tucker L.} and Cavalcante, {Lucas S.R.} and Gurses, {Sadi M.} and Dhanya Radhakrishnan and Daemen, {Luke L.} and Anthony, {John E.} and Koski, {Kristie J.} and Kronawitter, {Coleman X.} and Alessandro Troisi and Moul{\'e}, {Adam J.}",

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Vong, D, Nematiaram, T, Dettmann, MA, Murrey, TL, Cavalcante, LSR, Gurses, SM, Radhakrishnan, D, Daemen, LL, Anthony, JE, Koski, KJ, Kronawitter, CX, Troisi, A & Moulé, AJ 2022, 'Quantitative Hole Mobility Simulation and Validation in Substituted Acenes', Journal of Physical Chemistry Letters, vol. 13, no. 24, pp. 5530-5537. https://doi.org/10.1021/acs.jpclett.2c00898

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T1 - Quantitative Hole Mobility Simulation and Validation in Substituted Acenes

AU - Vong, Daniel

AU - Nematiaram, Tahereh

AU - Dettmann, Makena A.

AU - Murrey, Tucker L.

AU - Cavalcante, Lucas S.R.

AU - Gurses, Sadi M.

AU - Radhakrishnan, Dhanya

AU - Daemen, Luke L.

AU - Anthony, John E.

AU - Koski, Kristie J.

AU - Kronawitter, Coleman X.

AU - Troisi, Alessandro

AU - Moulé, Adam J.

PY - 2022/6/23

Y1 - 2022/6/23

N2 - Knowledge of the full phonon spectrum is essential to accurately calculate the dynamic disorder (σ) and hole mobility (μh) in organic semiconductors (OSCs). However, most vibrational spectroscopy techniques under-measure the phonons, thus limiting the phonon validation. Here, we measure and model the full phonon spectrum using multiple spectroscopic techniques and predict μhusing σ from only the Γ-point and the full Brillouin zone (FBZ). We find that only inelastic neutron scattering (INS) provides validation of all phonon modes, and that σ in a set of small molecule semiconductors can be miscalculated by up to 28% when comparing Γ-point against FBZ calculations. A subsequent mode analysis shows that many modes contribute to σ and that no single mode dominates. Our results demonstrate the importance of a thoroughly validated phonon calculation, and a need to develop design rules considering the full spectrum of phonon modes.

AB - Knowledge of the full phonon spectrum is essential to accurately calculate the dynamic disorder (σ) and hole mobility (μh) in organic semiconductors (OSCs). However, most vibrational spectroscopy techniques under-measure the phonons, thus limiting the phonon validation. Here, we measure and model the full phonon spectrum using multiple spectroscopic techniques and predict μhusing σ from only the Γ-point and the full Brillouin zone (FBZ). We find that only inelastic neutron scattering (INS) provides validation of all phonon modes, and that σ in a set of small molecule semiconductors can be miscalculated by up to 28% when comparing Γ-point against FBZ calculations. A subsequent mode analysis shows that many modes contribute to σ and that no single mode dominates. Our results demonstrate the importance of a thoroughly validated phonon calculation, and a need to develop design rules considering the full spectrum of phonon modes.

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Quantitative Hole Mobility Simulation and Validation in Substituted Acenes

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