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

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

14 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

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© 2022 American Chemical Society. All rights reserved.

ASJC Scopus subject areas

General Materials Science
Physical and Theoretical Chemistry

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10.1021/acs.jpclett.2c00898

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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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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.",

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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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