Chasing the 'killer' phonon mode for the rational design of low disorder, high mobility molecular semiconductors

Guillaume Schweicher, Gabriele D'Avino, Michael T. Ruggiero, David J. Harkin, Katharina Broch, Deepak Venkateshvaran, Guoming Liu, Audrey Richard, Christian Ruzie, Jeff Armstrong, Alan R. Kennedy, Kenneth Shankland, Kazuo Takimiya, Yves H. Geerts, J. Axel Zeitler, Simone Fratini, Henning Sirringhaus

Research output: Contribution to journalArticle

Abstract

Molecular vibrations play a critical role in the charge transport properties of weakly van der Waals bonded organic semiconductors. To understand which specific phonon modes contribute most strongly to the electron – phonon coupling and ensuing thermal energetic disorder in some of the most widely studied high mobility molecular semiconductors, we have combined state-of-the-art quantum mechanical simulations of the vibrational modes and the ensuing electron phonon coupling constants with experimental measurements of the lowfrequency vibrations using inelastic neutron scattering and terahertz time-domain spectroscopy. In this way we have been able to identify the long-axis sliding motion as a 'killer' phonon mode, which in some molecules contributes more than 80% to the total thermal disorder. Based on this insight, we propose a way to rationalize mobility trends between different materials and derive important molecular design guidelines for new high mobility molecular semiconductors.
LanguageEnglish
Number of pages33
JournalAdvanced Materials
Publication statusAccepted/In press - 25 Jul 2019

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Molecular vibrations
Semiconductor materials
Inelastic neutron scattering
Semiconducting organic compounds
Electrons
Transport properties
Charge transfer
Spectroscopy
Molecules
Hot Temperature

Keywords

  • electron-photon coupling
  • molecular vibrations
  • organic semiconductors

Cite this

Schweicher, G., D'Avino, G., Ruggiero, M. T., Harkin, D. J., Broch, K., Venkateshvaran, D., ... Sirringhaus, H. (Accepted/In press). Chasing the 'killer' phonon mode for the rational design of low disorder, high mobility molecular semiconductors. Advanced Materials.
Schweicher, Guillaume ; D'Avino, Gabriele ; Ruggiero, Michael T. ; Harkin, David J. ; Broch, Katharina ; Venkateshvaran, Deepak ; Liu, Guoming ; Richard, Audrey ; Ruzie, Christian ; Armstrong, Jeff ; Kennedy, Alan R. ; Shankland, Kenneth ; Takimiya, Kazuo ; Geerts, Yves H. ; Zeitler, J. Axel ; Fratini, Simone ; Sirringhaus, Henning. / Chasing the 'killer' phonon mode for the rational design of low disorder, high mobility molecular semiconductors. In: Advanced Materials. 2019.
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abstract = "Molecular vibrations play a critical role in the charge transport properties of weakly van der Waals bonded organic semiconductors. To understand which specific phonon modes contribute most strongly to the electron – phonon coupling and ensuing thermal energetic disorder in some of the most widely studied high mobility molecular semiconductors, we have combined state-of-the-art quantum mechanical simulations of the vibrational modes and the ensuing electron phonon coupling constants with experimental measurements of the lowfrequency vibrations using inelastic neutron scattering and terahertz time-domain spectroscopy. In this way we have been able to identify the long-axis sliding motion as a 'killer' phonon mode, which in some molecules contributes more than 80{\%} to the total thermal disorder. Based on this insight, we propose a way to rationalize mobility trends between different materials and derive important molecular design guidelines for new high mobility molecular semiconductors.",
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author = "Guillaume Schweicher and Gabriele D'Avino and Ruggiero, {Michael T.} and Harkin, {David J.} and Katharina Broch and Deepak Venkateshvaran and Guoming Liu and Audrey Richard and Christian Ruzie and Jeff Armstrong and Kennedy, {Alan R.} and Kenneth Shankland and Kazuo Takimiya and Geerts, {Yves H.} and Zeitler, {J. Axel} and Simone Fratini and Henning Sirringhaus",
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Schweicher, G, D'Avino, G, Ruggiero, MT, Harkin, DJ, Broch, K, Venkateshvaran, D, Liu, G, Richard, A, Ruzie, C, Armstrong, J, Kennedy, AR, Shankland, K, Takimiya, K, Geerts, YH, Zeitler, JA, Fratini, S & Sirringhaus, H 2019, 'Chasing the 'killer' phonon mode for the rational design of low disorder, high mobility molecular semiconductors' Advanced Materials.

Chasing the 'killer' phonon mode for the rational design of low disorder, high mobility molecular semiconductors. / Schweicher, Guillaume; D'Avino, Gabriele; Ruggiero, Michael T.; Harkin, David J.; Broch, Katharina; Venkateshvaran, Deepak; Liu, Guoming; Richard, Audrey; Ruzie, Christian ; Armstrong, Jeff; Kennedy, Alan R.; Shankland, Kenneth; Takimiya, Kazuo; Geerts, Yves H.; Zeitler, J. Axel; Fratini, Simone; Sirringhaus, Henning.

In: Advanced Materials, 25.07.2019.

Research output: Contribution to journalArticle

TY - JOUR

T1 - Chasing the 'killer' phonon mode for the rational design of low disorder, high mobility molecular semiconductors

AU - Schweicher, Guillaume

AU - D'Avino, Gabriele

AU - Ruggiero, Michael T.

AU - Harkin, David J.

AU - Broch, Katharina

AU - Venkateshvaran, Deepak

AU - Liu, Guoming

AU - Richard, Audrey

AU - Ruzie, Christian

AU - Armstrong, Jeff

AU - Kennedy, Alan R.

AU - Shankland, Kenneth

AU - Takimiya, Kazuo

AU - Geerts, Yves H.

AU - Zeitler, J. Axel

AU - Fratini, Simone

AU - Sirringhaus, Henning

PY - 2019/7/25

Y1 - 2019/7/25

N2 - Molecular vibrations play a critical role in the charge transport properties of weakly van der Waals bonded organic semiconductors. To understand which specific phonon modes contribute most strongly to the electron – phonon coupling and ensuing thermal energetic disorder in some of the most widely studied high mobility molecular semiconductors, we have combined state-of-the-art quantum mechanical simulations of the vibrational modes and the ensuing electron phonon coupling constants with experimental measurements of the lowfrequency vibrations using inelastic neutron scattering and terahertz time-domain spectroscopy. In this way we have been able to identify the long-axis sliding motion as a 'killer' phonon mode, which in some molecules contributes more than 80% to the total thermal disorder. Based on this insight, we propose a way to rationalize mobility trends between different materials and derive important molecular design guidelines for new high mobility molecular semiconductors.

AB - Molecular vibrations play a critical role in the charge transport properties of weakly van der Waals bonded organic semiconductors. To understand which specific phonon modes contribute most strongly to the electron – phonon coupling and ensuing thermal energetic disorder in some of the most widely studied high mobility molecular semiconductors, we have combined state-of-the-art quantum mechanical simulations of the vibrational modes and the ensuing electron phonon coupling constants with experimental measurements of the lowfrequency vibrations using inelastic neutron scattering and terahertz time-domain spectroscopy. In this way we have been able to identify the long-axis sliding motion as a 'killer' phonon mode, which in some molecules contributes more than 80% to the total thermal disorder. Based on this insight, we propose a way to rationalize mobility trends between different materials and derive important molecular design guidelines for new high mobility molecular semiconductors.

KW - electron-photon coupling

KW - molecular vibrations

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JF - Advanced Materials

SN - 1521-4095

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Schweicher G, D'Avino G, Ruggiero MT, Harkin DJ, Broch K, Venkateshvaran D et al. Chasing the 'killer' phonon mode for the rational design of low disorder, high mobility molecular semiconductors. Advanced Materials. 2019 Jul 25.