Accelerating Discovery of Vacancy Ordered 18-Valence Electron Half-Heusler Compounds: A Synergistic Approach of Machine Learning and Density Functional Theory

TL;DR

This paper combines machine learning and density functional theory to predict and validate vacancy-ordered half-Heusler compounds with enhanced thermoelectric properties, focusing on reducing thermal conductivity and improving figure of merit.

Contribution

It introduces a machine learning model trained on a large dataset to predict formation energies of vacancy-ordered compounds, validated by DFT calculations, advancing thermoelectric material discovery.

Findings

Predicted formation energies closely match DFT calculations.

Identified Zr0.75NiSb and Hf0.75NiSb as stable narrow band gap semiconductors.

Analyzed thermoelectric properties indicating potential for high performance.

Abstract

In this study, we attempted to model vacancy ordered half Heusler compounds with 18 valence electron count (VHH) derived from 19 VEC compounds such as TiNiSb such that the compositions will be Ti0.75NiSb, Zr0.75NiSb and Hf0.75NiSb with semiconducting behavior. The main motivation is that such a vacancy-ordered phase not only introduces semi conductivity but also it disrupts the phonon conducting path in HH alloys and thus reduces the thermal conductivity and as a consequence enhances the thermoelectric figure of merit. In order to predict the formation energy ({\Delta}Hf) from composition and crystal structure we have used 4684 compounds for their {\Delta}Hf values are available in the material project database and trained a machine learning model with R2 value of 0.943. Using this trained model, we have predicted the {\Delta}Hf of a list of VHH. From the predicted database of VHH we have selected Zr0.75NiSb and Hf0.75NiSb to validate the machine learning prediction using accurate DFT calculation. The calculated {\Delta}Hf for these two compounds from DFT calculation are found to be comparable with our ML prediction. The calculated electronic and lattice dynamics properties show that these materials are narrow band gap semiconductors and are dynamically stable as their all-phonon dispersion curves are having positive frequencies. The calculated Seebeck coefficient, electrical conductivity as well as thermal conductivity, power factor and thermoelectric figure of merit are analyzed.