First-principles dynamics of electrons and phonons*

Bernardi, Marco

doi:10.1140/epjb/e2016-70399-4

Cited by 103 publications

(115 citation statements)

References 95 publications

(206 reference statements)

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“…However, note that intramolecular phonons are expected to dominate carrier dynamics at higher hole energy above the phonon emission threshold, where their combined scattering rate overwhelms that from the (much fewer) intermolecular modes. This analysis shows that intramolecular phonons play an essential role in the dynamics of excited carriers [32][33][34]60] in organic semiconductors.…”

Section: Resultsmentioning

confidence: 88%

“…Methods combining band theory and many-body perturbation theory have been recently employed to accurately compute electron-phonon (e-ph) scattering and charge transport, for now in simple inorganic materials with a handful of atoms in the unit cell [31][32][33][34]. Due to computational cost, these calculations have not yet been applied to organic crystals with tens of atoms in the unit cell.…”

Section: Introductionmentioning

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: 88%

Section: Introductionmentioning

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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“…The e-ph interactions are included in the cumulant C nk (t); an approximate expression derived in Ref. [35] computes C nk (t) using the off-shell lowest-order e-ph self-energy, Σ nk (ω) [23] as input:…”

Section: Electron Spectral Functionmentioning

confidence: 99%

Predicting charge transport in the presence of polarons: The beyond-quasiparticle regime inSrTiO3

Zhou

Bernardi

2019

Phys. Rev. Research

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In materials with strong electron-phonon (e-ph) interactions, the electrons carry a phonon cloud during their motion, forming quasiparticles known as polarons. Predicting charge transport and its temperature dependence in the polaron regime remains an open challenge. Here, we present first-principles calculations of charge transport in a prototypical material with large polarons, SrTiO3. Using a cumulant diagram-resummation technique that can capture the strong e-ph interactions, our calculations can accurately predict the experimental electron mobility in SrTiO3 between 150−300 K. They further reveal that for increasing temperature the charge transport mechanism transitions from band-like conduction, in which the scattering of renormalized quasiparticles is dominant, to a beyond-quasiparticle transport regime governed by incoherent contributions due to the interactions between the electrons and their phonon cloud. Our work reveals long-sought microscopic details of charge transport in SrTiO3, and provides a broadly applicable method for predicting charge transport in materials with strong e-ph interactions and polarons.

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“…Several properties have been computed with this approach, including the magnetoresistance due to impurity scattering [7], the residual resistivity of metals and alloys [8], and spin relaxation [9][10][11][12] and the spin Hall effect [13][14][15]. In contrast, ab initio e-d calculations using pseudopotentials or projector augmented waves [16][17][18] have seen slower progress, mainly due to the high computational cost of obtaining the e-d interaction matrix elements needed for perturbative calculations [19].…”

Section: Introductionmentioning

confidence: 99%

Ab initio electron-defect interactions using Wannier functions

Park

Zhou

et al. 2020

npj Comput Mater

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Computing electron-defect (e-d) interactions from first principles has remained impractical due to computational cost. Here we develop an interpolation scheme based on maximally localized Wannier functions (WFs) to efficiently compute e-d interaction matrix elements. The interpolated matrix elements can accurately reproduce those computed directly without interpolation, and the approach can significantly speed up calculations of e-d relaxation times and defect-limited charge transport. We show example calculations of vacancy defects in silicon and copper, for which we compute the e-d relaxation times on fine uniform and random Brillouin zone grids (and for copper, directly on the Fermi surface) as well as the defect-limited resistivity at low temperature. Our interpolation approach opens doors for atomistic calculations of charge carrier dynamics in the presence of defects.

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First-principles dynamics of electrons and phonons*

Cited by 103 publications

References 95 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

Predicting charge transport in the presence of polarons: The beyond-quasiparticle regime inSrTiO3

Ab initio electron-defect interactions using Wannier functions

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