journal article·2023-09Open access

Untangling the Fundamental Electronic Origins of Non‐Local Electron–Phonon Coupling in Organic Semiconductors

Peter A. Banks, Gabriele D'Avino, Guillaume Schweicher, Jeff Armstrong, Christian Ruzié, Jong Won Chung, Jeong‐Il Park, Chizuru Sawabe, Toshihiro Okamoto, Jun Takeya, Henning Sirringhaus, Michael T. Ruggiero

Advanced Functional Materials· Volume 33· Issue 38

Abstract

Abstract Organic semiconductors with distinct molecular properties and large carrier mobilities are constantly developed in attempt to produce highly‐efficient electronic materials. Recently, designer molecules with unique structural modifications have been expressly developed to suppress molecular motions in the solid state that arise from low‐energy phonon modes, which uniquely limit carrier mobilities through electron–phonon coupling. However, such low‐frequency vibrational dynamics often involve complex molecular dynamics, making comprehension of the underlying electronic origins of electron–phonon coupling difficult. In this study, first a mode‐resolved picture of electron–phonon coupling in a series of materials that are specifically designed to suppress detrimental vibrational effects, is generated. From this foundation, a method is developed based on the crystalline orbital Hamiltonian population (COHP) analyses to resolve the origins—down to the single atomic‐orbital scale—of surprisingly large electron–phonon coupling constants of particular vibrations, explicitly detailing the manner in which the intermolecular wavefunction overlap is perturbed. Overall, this approach provides a comprehensive explanation into the unexpected effects of less‐commonly studied molecular vibrations, revealing new aspects of molecular design that should be considered for creating improved organic semiconducting materials.
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Research context

OpenAlex topics: Organic and Molecular Conductors Research · Organic Electronics and Photovoltaics · Perovskite Materials and Applications

SciVX discovery tags are terminology-based. OpenAlex topics are source-provided classifications.

Affiliations

Department of Chemistry, University of Vermont 82 University Place Burlington Vermont 05405 USA

Grenoble Alpes University, CNRS, Grenoble INP, Institut Néel 38042 Grenoble France

Laboratoire de Chimie des Polymres, Facult des Sciences Universit Libre de Bruxelles (ULB) Boulevard du Triomphe, CP 206/01 Bruxelles 1050 Belgium

ISIS Facility, Rutherford Appleton Laboratory Harwell Oxford, Didcot Oxfordshire OX11 0QX UK

Organic Material Lab. Samsung Advanced Institute of Technology (SAIT), Samsung Electronics Suwon 16678 South Korea

Material Innovation Research Center (MIRC) and Department of Advanced Materials Science, School of Frontier Sciences The University of Tokyo, 5‐1‐5 Kashiwanoha Kashiwa Chiba 277‐8561 Japan

National Institute of Advanced Industrial Science and Technology (AIST)‐University of Tokyo Advanced Operando‐Measurement Technology Open Innovation Laboratory (OPERANDO‐OIL) AIST, 5‐1‐5 Kashiwanoha Kashiwa Chiba 277‐8561 Japan

Optoelectronics Group, Cavendish Laboratory University of Cambridge JJ Thomson Avenue Cambridge CB3 0HE UK

Funding

National Science Foundation · Fonds De La Recherche Scientifique - FNRS · Agence Nationale de la Recherche · Engineering and Physical Sciences Research Council · H2020 European Research Council · Royal Society

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