Prediction and accelerated laboratory discovery of previously unknown 18-electron ABX compounds

TL;DR

This study combines computational predictions and experimental synthesis to identify and realize previously unreported 18-electron ABX compounds with potential functional properties, expanding the known materials space.

Contribution

It introduces an integrated approach of first-principles thermodynamics prediction and laboratory synthesis to discover new stable compounds in the ABX family.

Findings

54 of 400 predicted compounds are stable

15 new compounds synthesized and structurally confirmed

Potential for discovering new functional materials like topological insulators

Abstract

Chemists and material scientists have often focused on the properties of previously reported compounds, leaving out numerous unreported but chemically plausible compounds that could have interesting properties. For example, the 18-valence electron ABX family of compounds includes the half-Heusler subgroup, and features examples of topological insulators, thermoelectrics and superconductors, but only 83 out of 483 of these possible compounds have been made. Using first-principles thermodynamics we have examined the theoretical stability of 400 unreported members and predict that 54 should be stable. 15 previously missing materials, now predicted stable, were grown in this study; X-ray studies agreed with the predicted crystal structure in all 15 cases. Among the characterized properties of the missing compounds are potential transparent conductors, thermoelectric materials and topological semimetals. This integrated process-prediction of functionality in unreported compounds followed by laboratory synthesis and characterization-could be a route to the systematic discovery of hitherto missing, realizable functional materials.