Electron-Phonon beyond Fröhlich: Dynamical Quadrupoles in Polar and Covalent Solids

Brunin, Guillaume; Miranda, Henrique; Giantomassi, Matteo; Royo, Miquel; Stengel, Massimiliano; Verstraete, Matthieu J.; Gonze, Xavier; Rignanese, Gian‐Marco; Hautier, Geoffroy

doi:10.1103/physrevlett.125.136601

Cited by 87 publications

(113 citation statements)

References 30 publications

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“…Note added.-Recently, we became aware of a related work by another group that reaches similar conclusions about the importance of the dynamical quadrupole term to obtain an accurate physical description of e-ph interactions [25,26].…”

mentioning

confidence: 84%

“…If the quadrupole correction is not included, in principle the interpolation could be improved at small q by using a denser q-point grid when computing the DFPT matrix elements. However, due to the nonanalyticity of the quadrupole term, prohibitively dense DFPT grids are required to approach the accuracy of the quadrupole term [25].…”

Section: -2mentioning

confidence: 99%

“…Yet, DFPT is too costly to use directly on the ultrafine Brillouin zone grids needed to compute e-ph relaxation times and charge transport using the BTE. The current approach relies on Fourier interpolation techniques to capture the short-range e-ph interactions [23][24][25][26] while adding the dipole Fröhlich term in reciprocal space for polar materials. Deriving and computing the Fröhlich interaction [27,28] has been a first step toward implementing Vogl's modern e-ph theory in firstprinciples calculations and correctly capturing the longrange e-ph contributions.…”

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confidence: 99%

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Piezoelectric Electron-Phonon Interaction from Ab Initio Dynamical Quadrupoles: Impact on Charge Transport in Wurtzite GaN

et al. 2020

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First-principles calculations of e-ph interactions are becoming a pillar of electronic structure theory. However, the current approach is incomplete. The piezoelectric (PE) e-ph interaction, a long-range scattering mechanism due to acoustic phonons in noncentrosymmetric polar materials, is not accurately described at present. Current calculations include short-range e-ph interactions (obtained by interpolation) and the dipolelike Frölich long-range coupling in polar materials, but lack important quadrupole effects for acoustic modes and PE materials. Here we derive and compute the long-range e-ph interaction due to dynamical quadrupoles, and apply this framework to investigate e-ph interactions and the carrier mobility in the PE material wurtzite GaN. We show that the quadrupole contribution is essential to obtain accurate e-ph matrix elements for acoustic modes and to compute PE scattering. Our work resolves the outstanding problem of correctly computing e-ph interactions for acoustic modes from first principles, and enables studies of e-ph coupling and charge transport in PE materials.

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confidence: 84%

Section: -2mentioning

confidence: 99%

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confidence: 99%

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Piezoelectric Electron-Phonon Interaction from Ab Initio Dynamical Quadrupoles: Impact on Charge Transport in Wurtzite GaN

et al. 2020

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“…Note added. Recently, we became aware of a related work by another group that reaches similar conclusions about the importance of the dynamical quadrupole term to obtain an accurate physical description of e-ph interactions [40,41].…”

Section: Discussionmentioning

confidence: 78%

“…This strategy improves the interpolation near q = 0 in nonpolar materials, at once capturing the correct physics and smoothing the coarse-grid matrix element to be interpolated. Due to the nonanalytic behavior, denser DFPT grids cannot fully remove the interpolation error if the quadrupole term is not subtracted on the coarse grid [40]. For polar materials such as PbTiO 3 , the nonanalytic behavior is due to both the dipole (Fröhlich) and quadrupole long-range e-ph interactions.…”

Section: Discussionmentioning

confidence: 99%

Long-range quadrupole electron-phonon interaction from first principles

et al. 2020

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Lattice vibrations in materials induce perturbations on the electron dynamics in the form of long-range (dipole and quadrupole) and short-range (octopole and higher) potentials. The dipole Fröhlich term can be included in current first-principles electron-phonon (e-ph) calculations and is present only in polar materials. The quadrupole e-ph interaction is present in both polar and nonpolar materials, but currently it cannot be computed from first principles. Here we show an approach to compute the quadrupole e-ph interaction and include it in ab initio calculations of e-ph matrix elements. The accuracy of the approach is demonstrated by comparing with direct density functional perturbation theory calculations. We apply our method to silicon as a case of a nonpolar semiconductor and tetragonal PbTiO 3 as a case of a polar piezoelectric material. In both materials we find that the quadrupole term strongly impacts the e-ph matrix elements. Analysis of e-ph interactions for different phonon modes reveals that the quadrupole term mainly affects optical modes in silicon and acoustic modes in PbTiO 3 , although the quadrupole term is needed for all modes to achieve quantitative accuracy. The effect of the quadrupole e-ph interaction on electron scattering processes and transport is shown to be important. Our approach enables accurate studies of e-ph interactions in broad classes of nonpolar, polar, and piezoelectric materials.

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Semiclassical electron and phonon transport from first principles: application to layered thermoelectrics

et al. 2023

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Electron-Phonon beyond Fröhlich: Dynamical Quadrupoles in Polar and Covalent Solids

Cited by 87 publications

References 30 publications

Piezoelectric Electron-Phonon Interaction from Ab Initio Dynamical Quadrupoles: Impact on Charge Transport in Wurtzite GaN

Piezoelectric Electron-Phonon Interaction from Ab Initio Dynamical Quadrupoles: Impact on Charge Transport in Wurtzite GaN

Long-range quadrupole electron-phonon interaction from first principles

Semiclassical electron and phonon transport from first principles: application to layered thermoelectrics

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