Electronic transport computation in thermoelectric materials: From ab initio scattering rates to nanostructures

Abstract

Over the last two decades a plethora of new thermoelectric materials, their alloys, and their nanostructures were synthesized. The ZT figure of merit, which quantifies the thermoelectric efficiency of these materials increased from values of unity to values consistently beyond two across material families. At the same time, the ability to identify and optimize such materials, has stressed the need for advanced numerical tools for computing electronic transport in materials with arbitrary bandstructure complexity, multiple scattering mechanisms, and a large degree of nanostructuring. Many computational methods have been developed, the majority of which utilize the Boltzmann transport equation (BTE) formalism, spanning from fully ab initio to empirical treatment, with varying degree of computational expense and accuracy. In this paper we describe a suitable computational process that we have recently developed specifically for thermoelectric materials. The method consists of three independent software packages that we have developed and: 1) begins from ab initio calculation of the electron-phonon scattering rates, 2) to then be used within a Boltzmann transport simulator, and 3) calculated quantities from BTE are then passed on to a Monte Carlo simulator to examine electronic transport in highly nanostructured material configurations. The method we describe is computationally significantly advantageous compared to current fully ab initio and existing Monte Carlo methods, but with a similar degree of accuracy, thus making it truly enabling in understanding and assessing thermoelectric transport in complex band, nanostructured materials.

arXiv comment39 pages, 9 figures

References in corpus (21)

• BoltzTraP. A code for calculating band-structure dependent quantities
• Quantum ESPRESSO toward the exascale
• Wannier90 as a community code: new features and applications
• EPW: Electron-phonon coupling, transport and superconducting properties using maximally localized Wannier functions
• Efficient calculation of carrier scattering rates from first principles
• Prediction and accelerated laboratory discovery of previously unknown 18-electron ABX compounds
• Towards predictive many-body calculations of phonon-limited carrier mobilities in semiconductors
• Mobility of 2D materials from first principles in an accurate and automated framework
• Accelerated screening of thermoelectric materials by first-principles computations of electron-phonon scattering
• Beyond Marcus theory and the Landauer-Büttiker approach in molecular junctions: A unified framework
• Linear-Response Calculation of Electron-Phonon Coupling Parameters
• Band alignment and scattering considerations for enhancing the thermoelectric power factor of complex materials: The case of Co-based half-Heuslers
• Electron-phonon scattering and thermoelectric transport in $p$-type PbTe from first principles
• Deformation potential extraction and computationally efficient mobility calculations in silicon from first principles
• Impact of the scattering physics on the power factor of complex thermoelectric materials
• ElecTra Code: Full-Band Electronic Transport Properties of Materials
• Monte Carlo phonon transport simulations in hierarchically disordered silicon nanostructures
• Electron and Hole Mobility of SnO2 from Full-Band Electron-Phonon and Ionized Impurity Scattering Computations
• Monte Carlo Simulation of Electron Transport in Degenerate Semiconductors
• Thermoelectric transport trends in group 4 half-Heusler alloys
• Computationally efficient Monte Carlo electron transport algorithm for nanostructured thermoelectric material configurations