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Charge transport in organic molecular semiconductors from first principles: The bandlike hole mobility in a naphthalene crystal

Lee, Nien-En and Zhou, Jin-Jian and Agapito, Luis A. and Bernardi, Marco (2018) Charge transport in organic molecular semiconductors from first principles: The bandlike hole mobility in a naphthalene crystal. Physical Review B, 97 (11). Art. No. 115203. ISSN 2469-9950. doi:10.1103/PhysRevB.97.115203.

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Predicting charge transport in organic molecular crystals is notoriously challenging. Carrier mobility calculations in organic semiconductors are dominated by quantum chemistry methods based on charge hopping, which are laborious and only moderately accurate. We compute from first principles the electron-phonon scattering and the phonon-limited hole mobility of naphthalene crystal in the framework of ab initio band theory. Our calculations combine GW electronic bandstructures, ab initio electron-phonon scattering, and the Boltzmann transport equation. The calculated hole mobility is in very good agreement with experiment between 100 – 300 K, and we can predict its temperature dependence with high accuracy. We show that scattering between intermolecular phonons and holes regulates the mobility, though intramolecular phonons possess the strongest coupling with holes. We revisit the common belief that only rigid molecular motions affect carrier dynamics in organic molecular crystals. Our paper provides a quantitative and rigorous framework to compute charge transport in organic crystals and is a first step toward reconciling band theory and carrier hopping computational methods.

Item Type:Article
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URLURL TypeDescription Paper
Lee, Nien-En0000-0002-3172-7750
Zhou, Jin-Jian0000-0002-1182-9186
Bernardi, Marco0000-0001-7289-9666
Additional Information:© 2018 American Physical Society. Received 1 December 2017; revised manuscript received 9 February 2018; published 16 March 2018. The authors thank M. Palummo for discussions. N.-E.L. acknowledges the Physics department at Caltech for the TA Relief Fellowship. M.B. and L.A. acknowledge support by the National Science Foundation under Grant No. ACI-1642443, which provided for basic theory and electron-phonon code development. This work was partially supported by the Young Investigator Program of the Air Force Office of Scientific Research (AFOSR), under Grant FA9550-18-1-0280. J.-J. Zhou was supported by the Joint Center for Artificial Photosynthesis, a DOE Energy Innovation Hub, as follows: The development of the scattering rate and mobility calculations was supported through the Office of Science of the U.S. Department of Energy under Award No. DE-SC0004993. This research used resources of the National Energy Research Scientific Computing Center, 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.
Funding AgencyGrant Number
Air Force Office of Scientific Research (AFOSR)FA9550-18-1-0280
Department of Energy (DOE)DE-SC0004993
Department of Energy (DOE)DE-AC02-05CH11231
Issue or Number:11
Record Number:CaltechAUTHORS:20180321-075518336
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Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:85387
Deposited By: Tony Diaz
Deposited On:26 Mar 2018 17:12
Last Modified:11 Apr 2022 22:17

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