Band gap renormalization, carrier mobility, and transport in Mg${}_2$Si and Ca${}_2$Si: \textit{Ab initio} scattering and Boltzmann transport equation study

Abstract

We perform first-principles electron-phonon interaction (EPI) calculations based on many-body perturbation theory to study the temperature-dependent band-gap and charge-carrier transport properties for Mg${}_2$Si and Ca${}_2$Si using the Boltzmann transport equation (BTE) under different relaxation-time approximations (RTAs). For a PBE band gap of 0.21 (0.56) eV in Mg${}_2$Si (Ca${}_2$Si), a zero-point renormalization correction of 29-33 (37-51) meV is obtained using various approaches, while the gap at 300 K is 0.15-0.154 (0.46-0.5) eV. The electron mobility (${\mu }_e$), with a detailed convergence study at 300 K, is evaluated using linearized (self-energy and momentum RTA, or SERTA and MRTA) and iterative BTE (IBTE) solutions. At 300 K, the ${\mu }_e$ values are 351 (100), 573 (197), and 524 (163) cm${}^2{V}^{-1}{s}^{-1}$ from SERTA, MRTA, and IBTE, respectively, for Mg${}_2$Si (Ca${}_2$Si). SERTA (MRTA) provides results in better agreement with IBTE at higher (lower) temperatures, while SERTA-derived ${\mu }_e$ closely matches experimental ${\mu }_e$ values for Mg${}_2$Si. Thermoelectric (TE) transport coefficients significantly influenced by the choice of RTA, with SERTA and MRTA yielding improved agreement with experimental results compared to constant RTA (CRTA) for Mg${}_2$Si over an electron concentration range of $10^{17}$ to $10^{20}$ cm${}^{-3}$. The lattice thermal conductivity (${\kappa }_{ph}$) at 300 K due to phonon-phonon interactions is estimated to be 22.7 (7.2) W m${}^{-1}{K}^{-1}$ for Mg${}_2$Si (Ca${}_2$Si). The highest calculated figure of merit (zT) under CRTA is 0.35 (0.38), which decreases to 0.08 (0.085) when EPI is included using MRTA. This study clearly identifies the critical role of EPI in accurate transport predictions of TE silicides. Finally, we explore strategies to enhance zT by reducing ${\kappa }_{ph}$ through nanostructuring and mass-difference scattering.

arXiv commentAccepted manuscript in Phys. Rev. B

References in corpus (30)

• Phonons and related properties of extended systems from density-functional perturbation theory
• BoltzTraP. A code for calculating band-structure dependent quantities
• Optimized norm-conserving Vanderbilt pseudopotentials
• BoltzTraP2, a program for interpolating band structures and calculating semi-classical transport coefficients
• Electron-phonon interactions from first principles
• Distribution of phonon lifetime in Brillouin zone
• First-principles calculations of charge carrier mobility and conductivity in bulk semiconductors and two-dimensional materials
• Significant reduction of lattice thermal conductivity by electron-phonon interaction in silicon with high carrier concentrations: a first-principles study
• Towards predictive many-body calculations of phonon-limited carrier mobilities in semiconductors
• Calculated thermoelectric properties of La-filled skutterudites
• {\it Ab--initio} finite temperature excitons
• First-Principles Simulation of Electron Mean-Free-Path Spectra and Thermoelectric Properties in Silicon
• Hole mobility of strained GaN from first principles
• Temperature Dependence of the Band Gap of Semiconducting Carbon Nanotubes
• Dynamical and anharmonic effects on the electron-phonon coupling and the zero-point renormalization of the electronic structure
• Effect of the quantistic zero-point atomic motion on the opto-electronic properties of diamond and trans-polyacetylene
• The temperature dependence of electronic eigenenergies in the adiabatic harmonic approximation
• First-principles dynamics of electrons and phonons
• Importance of relativistic effects in electronic structure and thermopower calculations for Mg2Si, Mg2Ge and Mg2Sn
• Phonon-limited electron mobility in Si, GaAs and GaP with exact treatment of dynamical quadrupoles
• Deep-learning density functional perturbation theory
• Ab Initio Electron-Phonon Interactions Using Atomic Orbital Wavefunctions
• Band gap renormalization, carrier mobilities, and the electron-phonon self-energy in crystalline naphthalene
• Investigation of the Thermoelectric Properties of ZnV${}_2$O${}_4$ Compound in High Temperature Region
• Temperature effects on the electronic band structure of PbTe from first principles
• Assessing the quality of relaxation-time approximations with fully-automated computations of phonon-limited mobilities
• Thermoelectric properties, efficiency and thermal expansion of ZrNiSn half-Heusler by first-principles calculations
• First-principles study of optoelectronic and thermoelectronic properties of the ScAgC half-Heusler compound
• Mg${}_2$Si and Ca${}_2$Si semiconductors for photovoltaic applications: Calculations based on density-functional theory and the Bethe-Salpeter equation
• Ab-initio study of phononic thermal conduction in ScAgC half-Heusler

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