Computational discovery of semiconducting high-entropy chalcogenide alloys

High-entropy materials are formed by mixing typically five or more principal components into a single crystal structure and show improved thermodynamic stability due to the large configurational disorder. While significant progress has been made to synthesize entropy-stabilized metals and ceramics for structural applications, little attention has been paid to the discovery of new semiconducting materials using the design principle of entropy stabilization.  Here, we present a new class of entropy-stabilized semiconducting alloys based on the IV-VI binary chalcogenides, namely Ge_xSn_yPb_1–x–yS_zSe_tTe_1–z–t high-entropy chalcogenides (HECs). By utilizing high-throughput first-principles calculations, we investigate the thermodynamic stability of HECs over their entire composition space, and show that more than 50% of the investigated compositions are stable with respect to phase segregation to the competing binary ingredients at the experimental synthesis temperature. We further studied the enthalpic effect of the individual elements and showed that Sn and Se lower the enthalpy of mixing, while S is detrimental to the phase stability of HECs. Our work demonstrates the potential of entropy stabilization in the discovery of novel multicomponent semiconductor alloys.