Long-range quadrupole electron-phonon interaction from first principles

Abstract

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.

9 pages, 5 figures, submitted

References in corpus (24)

• Quantum ESPRESSO: a modular and open-source software project for quantum simulations of materials
• Phonons and related properties of extended systems from density-functional perturbation theory
• Spontaneous polarization and piezoelectric constants of III-V nitrides
• The PseudoDojo: Training and grading a 85 element optimized norm-conserving pseudopotential table
• Wannier90 as a community code: new features and applications
• Fröhlich electron-phonon vertex from first principles
• Ab initio Electron Mobility and Polar Phonon Scattering in GaAs
• Wannier interpolation of the electron-phonon matrix elements in polar semiconductors: Polar-optical coupling in GaAs
• First-principles mode-by-mode analysis for electron-phonon scattering channels and mean free path spectra in GaAs
• Electron-Phonon Scattering in the Presence of Soft Modes and Electron Mobility in SrTiO${}_3$ Perovskite from First Principles
• Adiabatic and non-adiabatic phonon dispersion in a Wannier function approach
• Flexoelectricity from density-functional perturbation theory
• Mobility of 2D materials from first principles in an accurate and automated framework
• Ultrafast Hot Carrier Dynamics in GaN and its Impact on the Efficiency Droop
• Electron-Phonon Beyond Fröhlich: Dynamical Quadrupoles in Polar and Covalent Solids
• First-principles dynamics of electrons and phonons
• Phonon-limited electron mobility in Si, GaAs and GaP with exact treatment of dynamical quadrupoles
• Piezoelectric Electron-Phonon Interaction from Ab Initio Dynamical Quadrupoles: Impact on Charge Transport in Wurtzite GaN
• Charge Transport in Organic Molecular Semiconductors from First Principles: The Band-Like Hole Mobility in Naphthalene Crystal
• Predicting charge transport in the presence of polarons: The beyond-quasiparticle regime in SrTiO${}_3$
• First-principles theory of spatial dispersion: Dynamical quadrupoles and flexoelectricity
• Current-density implementation for calculating flexoelectric coefficients
• Ab Initio Electron-Phonon Interactions Using Atomic Orbital Wavefunctions
• Elliott-Yafet Spin-Phonon Relaxation Times from First Principles

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