Robust Design of High-Performance Optoelectronic ChalcogenideCrystals from High-Throughput ComputationYu

High-performance functional materials are thecornerstones of the continuous advance of modern science andtechnology, but the development of new materials is stillchallenging. Here, we propose a robust design strategy for novelcrystalline solids based on group-theory classification and high-throughput computation, as demonstrated by the successfulidentification of new optoelectronic semiconductors. First, bymeans of theoretical group analysis and composition engineering,we obtained 78 prototypical crystal structures and built acomputational materials database containing 21,060 ternarychalcogenide compounds. Our high-throughput screening of thecoordination characteristics, phase stability, and electronic structures provided 97 candidate semiconductors, including 93completely new compounds. Among them, 22 crystals with excellent dynamical and thermal stability are predicted to show highphotovoltaic conversion efficiency (>30%), comparable to the currently most efficient single-junction GaAs solar cell, owing to theiroptimal electronic properties and outstanding optical absorption. This discovery of new chalcogenide crystals offers excellentcandidates for optoelectronic applications and suggests that our design strategy is a promising way to search for unknown high-performance functional materials.

Automated summary

In this study, we propose a robust design strategy for novel crystalline solids based on group-theory classification and high-throughput computation, which has successfully led to the discovery of new optoelectronic semiconductors. This design strategy offers a promising way to search for unknown high-performance functional materials.