High-Throughput Screening for Advanced Thermoelectric Materials: Diamond-Like ABX₂ Compounds

Abstract

High-throughput (HTP) calculations are a highly promising direction for the discovery of novel functional materials. Here we use an HTP framework to investigate the electronic structures and p-type thermoelectric properties of the ABX2 compounds with diamond-like structures. We show application of HTP both to identify compounds and also to identify underlying trends. A total of 65 entries out of 84 908 in the Materials Informatics Platform are selected for this study. The electronic structures and chemical-bonding analyses reveal that there exists a general conductive network consisting of the anion X sublattice, which dominates the electrical transport properties of the compounds. Electrical and thermal transport properties of the 41 pnictide and chalcogenide compounds with sufficient band gaps are studied. Pnictide compounds have relatively smaller Seebeck coefficients than the chalcogenide compounds. This is due to the smaller effective masses around the valence band maxima. The electrical conductivities and power factors, however, are better in pnictide compounds. This is because pnictide compounds have high electronic group velocities and electronic relaxation times. Combined with the predictions of lattice thermal conductivities based on the Slack model, 12 novel p-type and n-type ABX2 materials with high ZT values are predicted.

Lattice dynamics of Pnma Sn(S1–xSex) solid solutions: energetics, phonon spectra and thermal transport

“…Due to the record-breaking high-temperature ZT of SnS, the Te-free Sn(S, Se) alloys are of particular interest, and experimental studies have demonstrated a reduction in the thermal conductivity of mixed compositions [12,14].Thermoelectricity is unique in that all four of the terms in the figure of merit ZT are amenable to calculation using first-principles electronic-structure methods such as density-functional theory (DFT) [18]. There have been a number of theoretical studies on existing and potential new single-component bulk thermoelectrics [6,[19][20][21][22][23], and there have recently been efforts to use high-throughput modelling to screen large numbers of compounds in a bid to identify new candidate thermoelectrics [24,25].Studying multicomponent alloy systems with first-principles methods is challenging, however, as building a realistic model requires calculations on a large number of configurations that for complex systems with lowsymmetry unit cells can easily approach the cost of a screening study [26]. Ektarawong and Alling used a firstprinciples cluster expansion method to study the Pnma Sn(S 1-x Se x ) system and confirmed the stability of the mixed phases at finite temperature [27].…”

“…Thermoelectricity is unique in that all four of the terms in the figure of merit ZT are amenable to calculation using first-principles electronic-structure methods such as density-functional theory (DFT) [18]. There have been a number of theoretical studies on existing and potential new single-component bulk thermoelectrics [6,[19][20][21][22][23], and there have recently been efforts to use high-throughput modelling to screen large numbers of compounds in a bid to identify new candidate thermoelectrics [24,25].…”

Active learning for the power factor prediction in diamond-like thermoelectric materials

“…1a). The original 158 entries of chalcogenides and pnictides are quoted from our previous HTP works and referred in the DFT database later 10,11 . By exhausting all the possible combinations among the aforementioned cations and anions, we construct a search space of diamond-like compounds with 482 entries (158 DFT calculated and 324 uncalculated) 10 .…”

“…In 2018, Xi et al applied HTP ab initio calculation to 161 ptype chalcogenides and experimentally verified the recommended TE compound Cd 2 Cu 3 In 3 Te 8 with ZT >1.0 10 . Li et al studied both p-type pnictides and chalcogenides in the atomic ratio 1:1:2, and pnictides showed exceptionally high power factors (PFs) 11 .…”

Electronic structure as a guide in screening for potential thermoelectrics: Demonstration for half-Heusler compounds

“…An implication is that thermoelectricity is a particularly rich area for testing and demonstrating theory based materials search strategies. [18][19][20][21][22] Here we report and demonstrate a high throughput strategy that starts with a simple electronic structure based metric. Application to a set of half-Heusler compounds identifies previously known high performance materials.…”