Towards theoretical framework for probing the accuracy limit of electronic transport properties of SnSe₂using many-body calculations

Abstract

A theoretical framework to investigate the accuracy limit of phonon-limited carrier mobility in intrinsic n-type SnSe2 has been developed by solving the Boltzmann transport equation based on ab initio calculated electron-phonon interactions. The electron-phonon coupling matrix elements have been computed using maximally localized Wannier functions and density functional perturbation theory. The intrinsic electron mobility of ∼8.75 cm 2 V −1 s −1 has been achieved at 300 K, incorporating spin-orbit coupling, many-body quasiparticle corrections, and iterative solution of the Boltzmann transport equation using dense sampling of the Brillouin zone. The calculated intrinsic mobility is in close agreement with the experimental values. Furthermore, the electron mean-free path, electrical conductivity, and Seebeck coefficient have been calculated for SnSe2 under varying temperatures. The maximum mean-free path of 20 nm has been achieved for electrons at 300 K. This contribution provides a comprehensive method to investigate the transport properties and presents a framework towards the accuracy limit of prototypical SnSe2.

Electronic and Thermoelectric Properties of Transition-Metal Dichalcogenides

“…The transport properties are calculated within the Boltzmann transport formalism and the constant relaxation time approximation using the BoltzTraP transport code . Other approaches have been used in the literature, within the Boltzmann approximation, but with an ab initio relaxation time based on phonon or impurity scattering, e.g., refs and − . These show interesting effects but are much heavier to calculate: our goal is to be systematic and compare the different TMDs on the same footing.…”

First-principles predictions of Hall and drift mobilities in semiconductors

“…The low-field phonon-limited charge carrier mobility is calculated as [10][11][12][13][14][15][15][16][17][18][19][20][21][22][23][24][25][27][28][29][30][31][32][33][34][35][36][37][38][39][40][41][42][43][44][45][46] :…”

“…Due to the complexity of computing carrier mobilities fully from first principles, the first calculation appeared only in 2009 10 . Since then, only 19 bulk semiconductors have been investigated: Si [10][11][12][13][14][15][16] , Diamond 17 , GaAs 13,[18][19][20][21][22] , GaN [23][24][25] , 3C-SiC 26,27 , GaP 22 , GeO 2 28 , SnSe 29 , SnSe 2 30 , BAs 31,32 , PbTe 33,34 , naphtalene 35,36 , Bi 2 Se 3 37 , Ga 2 O 3 [38][39][40][41] , TiO 2 42 , SrTiO 3 43,44 , PbTiO 3 15 , Rb 3 AuO 45 , and CH 3 NH 3 PbI 3 46 .…”

Long-range electrostatic contribution to the electron-phonon couplings and mobilities of two-dimensional materials

“…In an effort to understand the nanoscopic mechanisms underlying the transport properties of TMDs and other 2D materials, density functional perturbation theory [15][16][17] provides a powerful tool by giving access to electron-phonon scattering rates fully from first principles. In particular, room-temperature resistive trans-port calculations based on such scattering rates are of key technological importance to orient experimental investigations and speed up materials discovery, and have therefore been widely exploited both in bulk [18][19][20][21][22][23][24][25][26][27][28][29][30][31][32][33][34][35] and 2D materials 13,14,18,24,[36][37][38][39][40][41][42][43][44][45][46] reaching remarkable accuracy with respect to experiments in prominent cases including graphene 40,47 .…”