Abstract
Significant progress on parameter-free calculations of carrier mobilities in real materials has been made during the past decade; however, the role of various approximations remains unclear and a unified methodology is lacking. Here, we present and analyse a comprehensive and efficient approach to compute the intrinsic, phonon-limited drift and Hall carrier mobilities of semiconductors, within the framework of the first-principles Boltzmann transport equation. The methodology exploits a novel approach for estimating quadrupole tensors and including them in the electron-phonon interactions, and capitalises on a rigorous and efficient procedure for numerical convergence. The accuracy reached in this work allows to assess common approximations, including the role of exchange and correlation functionals, spin-orbit coupling, pseudopotentials, Wannier interpolation, Brillouin-zone sampling, dipole and quadrupole corrections, and the relaxation-time approximation. A detailed analysis is showcased on ten prototypical semiconductors, namely diamond, silicon, GaAs, 3C-SiC, AlP, GaP, c-BN, AlAs, AlSb, and SrO. By comparing this extensive dataset with available experimental data, we explore the intrinsic nature of phonon-limited carrier transport and magnetotransport phenomena in these compounds. We find that the most accurate calculations predict Hall mobilities up to a factor of two larger than experimental data; this could point to promising experimental improvements in the samples quality, or to the limitations of density-function theory in predicting the carrier effective masses and overscreening the electron-phonon matrix elements. By setting tight standards for reliability and reproducibility, the present work aims to facilitate validation and verification of data and software towards predictive calculations of transport phenomena in semiconductors.
Highlights
The ability of metals and semiconductors to transport electrical charges is a fundamental property in manifold applications, ranging from solar cells, light-emitting devices, thermoelectric, transparent conductors, photodetectors, photocatalysts, and transistors [1,2,3,4,5]
We find that Wannier-function interpolations converge more slowly than previously estimated with respect to the sampling of the coarse grid employed in the Wannier representation
This work answers crucial methodological and physical questions. It establishes welldefined criteria for high-accuracy calculations of transport coefficients, clarifying the role and the level of (i) the approximations in the underlying first-principles calculation to extract materials parameters, (ii) the interpolation procedures for quasiparticle dispersions and interactions, and (iii) the numerical techniques that ensure the efficient convergence of transport coefficients
Summary
The ability of metals and semiconductors to transport electrical charges is a fundamental property in manifold applications, ranging from solar cells, light-emitting devices, thermoelectric, transparent conductors, photodetectors, photocatalysts, and transistors [1,2,3,4,5]. Predicting transport properties from first principles [6] offers a powerful tool for the design of new materials and devices. Already in 1966, in a seminal work Cohen and Bergstresser [7] computed the band structure of 14 semiconductors with the diamond and zinc-blende structure. In 2013, Malone and Cohen [8] repeated this task computing the quasiparticle band structure in the many-body GW approximation, including spin-orbit coupling (SOC) effects. Miglio et al [9] studied the zero-point renormalization of the electronic band gap of 30 semiconductors, mostly of the zinc-blende, wurtzite, and rocksalt crystal structure. We deliver an accurate and efficient calculation method for carrier mobilities, including spin-orbit coupling, dynamical quadrupoles and, magnetic Hall effects, focusing on prototypical semiconductors. For the last five of these, no first-principles calculations of carrier mobility have been reported to date
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