Observation of the Band-Hopping Transition for Electrons in Naphthalene

Schein, L. B.; Duke, C. B.; McGhie, A. R.

doi:10.1103/physrevlett.40.197

Cited by 132 publications

(66 citation statements)

References 25 publications

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“…Their scattering rate decreases monotonically with phonon energy (and thus with mode number, since the modes are numbered in order of increasing energy). Similar to simple metals and nonpolar inorganic semiconductors, the main source of scattering is acoustic modes, with smaller contributions from other molecular rigid vibrations and librations (modes [4][5][6][7][8][9][10][11][12]. This result is further illustrated in Fig.…”

Section: Resultsmentioning

confidence: 89%

“…3(b) for selected intramolecular phonons. Note that the intermolecular phonons have either zero or very small minimum frequency since they correspond to transverse acoustic (TA) and longitudinal acoustic (LA) vibrations (modes 1-3) or other rigid vibrations or librations of the molecules (modes [4][5][6][7][8][9][10][11][12]. By contrast, the intramolecular modes 20-90 in Fig.…”

Section: Resultsmentioning

confidence: 99%

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

et al. 2018

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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.

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Section: Resultsmentioning

confidence: 89%

Section: Resultsmentioning

confidence: 99%

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

et al. 2018

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“…Two decades later, the interplay between metallic (bandlike) conduction and activated (hopping) transport in organic crystals was seen for the electrons in naphthalene but not for the holes. [12][13][14] Later, Kenkre et al were able to fit the measured electron mobilities reasonably well to Holstein's model, assuming directionally dependent local-coupling constants. 15 Despite the success of such a fitting procedure, the lack of a first-principles description of charge-carrier mobilities in organic crystals has left several fundamental questions unanswered.…”

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confidence: 99%

Ab initio theory of charge-carrier conduction in ultrapure organic crystals

Hannewald

Bobbert

2004

Applied Physics Letters

181

159

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“…At high temperature, the charge transport occurs by phonon-assisted hopping between localized states, and the mobility increases with temperature. The transition between band and hopping mechanisms in organic crystals was first observed in naphthalene crystal through the crossover in temperature dependence of mobility [10]. Thus naphthalene is normally chosen as the model systems to investigate the charge transport mechanism in molecular crystals.…”

Section: Application: Naphthalenementioning

confidence: 99%

Polaron Mechanism

Shuai¹,

Wang²,

Song³

2012

SpringerBriefs in Molecular Science

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The intrinsic charge transport in organic semiconductors is an electronphonon interacting process. Due to the ''soft'' nature of organic materials, the existence of an electron can cause significant deformation of local nuclear vibrations, which moves together with the electron itself, and thus the effective diffusing quasiparticle is composed of the electron and its accompanying phonons. This is the basic idea of the polaron mechanism. In principle, it is a more general description for charge transport since it does not presume that the charge is localized within one molecule as in the hopping mechanism described in Chap. 2. In this chapter, we adopt the general Holstein-Peierls Hamiltonian coupled with first-principles calculations to investigate the fundamental aspects concerning charge transport. All kinds of electron-phonon couplings, including both local and nonlocal parts for inter-and intra-molecular vibrations, have been taken into considerations. Detailed studies are performed to study their contributions to the total electron-phonon coupling strength and the temperature dependence of mobility, especially the band-hopping crossover feature. We also investigate the pressure-and temperature-dependent crystal structure effects on the charge transport properties.Keywords Polaron mechanism Á Holstein-Peierls Hamiltonian Á Electron-phonon coupling Á Band-hopping crossover Á Pressure and temperature dependence of mobility Á Thermal expansion of lattice In Sect. 3.1, we discuss the derivation for the mobility expression from HolsteinPeierls Hamiltonian with polaron transformation and linear response theory. Application to naphthalene crystal is presented in Sect. 3.2 to investigate the role of inter-and intra-molecular vibrations on the temperature dependence of mobility. In Sect. 3.3, the temperature dependence is improved after including the thermal expansion of the lattice. Finally, the pressure dependence of mobility is studied in Sect. 3.4. Z. Shuai et al.,

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Observation of the Band-Hopping Transition for Electrons in Naphthalene

Cited by 132 publications

References 25 publications

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

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

Ab initio theory of charge-carrier conduction in ultrapure organic crystals

Polaron Mechanism

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