Charge transport in organic crystals: Critical role of correlated fluctuations unveiled by analysis of Feynman diagrams

Packwood, Daniel M.; Oniwa, Kazuaki; Jin, Tienan; Asao, Naoki

doi:10.1063/1.4916385

Cited by 9 publications

(6 citation statements)

References 34 publications

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“…[106] The effects of short-time correlations in the dynamics of disorder have been recently studied in Ref. [107] using a stochastic model similar to Ref. [19].…”

Section: Relaxation Time Approximationmentioning

confidence: 99%

The Transient Localization Scenario for Charge Transport in Crystalline Organic Materials

Fratini

Mayou

Ciuchi

2016

Adv Funct Materials

338

452

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Charge transport in crystalline organic semiconductors is intrinsically limited by the presence of large thermal molecular motions, which are a direct consequence of the weak van der Waals inter-molecular interactions. These lead to an original regime of transport called transient localization, sharing features of both localized and itinerant electron systems. After a brief review of experimental observations that pose a challenge to the theory, we concentrate on a commonly studied model which describes the interaction of the charge carriers with inter-molecular vibrations. We present different theoretical approaches that have been applied to the problem in the past, and then turn to more modern approaches that are able to capture the key microscopic phenomenon at the origin of the puzzling experimental observations, i.e. the quantum localization of the electronic wavefuntion at timescales shorter than the typical molecular motions. We describe in particular a relaxation time approximation which clarifies how the transient localization due to dynamical molecular motions relates to the Anderson localization realized for static disorder, and allows us to devise strategies to improve the mobility of actual compounds. The relevance of the transient localization scenario to other classes of systems is briefly discussed.

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“…[106] The effects of short-time correlations in the dynamics of disorder have been recently studied in Ref. [107] using a stochastic model similar to Ref. [19].…”

Section: Relaxation Time Approximationmentioning

confidence: 99%

The Transient Localization Scenario for Charge Transport in Crystalline Organic Materials

Fratini

Mayou

Ciuchi

2016

Adv Funct Materials

338

452

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“…Symmetric and antisymmetric coupling modes give opposite temperature dependence of mobility. Packwood et al have put forward the critical role of correlated fluctuations on charge transport dynamics . In a nutshell, this short overview of theoretical developments shows that the actual mechanism of charge transport is still debated, nowadays.…”

Section: Charge Transportmentioning

confidence: 99%

Molecular Semiconductors for Logic Operations: Dead‐End or Bright Future?

et al. 2020

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The field of organic electronics has been prolific in the last couple of years, leading to the design and synthesis of several molecular semiconductors presenting a mobility in excess of 10 cm2 V−1 s−1. However, it is also started to recently falter, as a result of doubtful mobility extractions and reduced industrial interest. This critical review addresses the community of chemists and materials scientists to share with it a critical analysis of the best performing molecular semiconductors and of the inherent charge transport physics that takes place in them. The goal is to inspire chemists and materials scientists and to give them hope that the field of molecular semiconductors for logic operations is not engaged into a dead end. To the contrary, it offers plenty of research opportunities in materials chemistry.

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“…Many theoretical works have attempted a description of this highly coupled charge-phonon dynamics involving methods developed in chemical physics and solid state physics and including Erhenfest dynamics and modified surface hopping , on model Hamiltonian − or realistic chemical models. , All these models suggest that the effect of dynamic disorder is to cause dynamic localization, i.e. the instantaneous eigenstates of the system are localized, but the dynamic nature of the disorder itself promotes propagation of the charge.…”

Section: Introductionmentioning

confidence: 99%

Nonlocal Electron–Phonon Coupling in Prototypical Molecular Semiconductors from First Principles

Xie

Santana‐Bonilla

Troisi

2018

J. Chem. Theory Comput.

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A substantial amount of evidence indicates a relevant role played by the nonlocal electron-phonon couplings in the mechanism of charge transport in organic semiconductors. In this work, we compute the nonlocal electron-phonon coupling for the prototypical molecular semiconductors rubrene and tetracene using the phonon modes obtained from ab initio methods. We do not make the rigid molecular approximation allowing a mixing of intra- and intermolecular modes, and we use a supercell approach to sample the momentum space. Indeed, we find that some low-frequency intramolecular modes are mixed with the rigid-molecule translations and rotations in the modes with the strongest electron-phonon coupling. To rationalize the results we propose a convenient decomposition of the delocalized lattice modes into molecular-based modes.

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Charge transport in organic crystals: Critical role of correlated fluctuations unveiled by analysis of Feynman diagrams

Cited by 9 publications

References 34 publications

The Transient Localization Scenario for Charge Transport in Crystalline Organic Materials

The Transient Localization Scenario for Charge Transport in Crystalline Organic Materials

Molecular Semiconductors for Logic Operations: Dead‐End or Bright Future?

Nonlocal Electron–Phonon Coupling in Prototypical Molecular Semiconductors from First Principles

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