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

17 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).

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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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doi = "10.1021/acs.jpclett.2c00898",

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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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