Computationally Directed High-Pressure Discovery of Transition Metal-Bismuth Materials*

Under applied pressures, fundamental elemental properties are renormalized, revealing compounds that challenge our understanding. To efficiently direct high-pressure synthetic efforts, it is useful to employ computational approaches that predict material stability. In this work, we used high throughput ab initio random structure searches to explore high-pressure transition metal (TM)–Bi phase space. We observed that the CuAl₂ type structure is common, including for combinations of elements that are not miscible under ambient conditions. Turning to high-pressure experiments, we discovered the first Mo–Bi intermetallic material. Experimental structural elucidation of this material revealed how the CuAl₂ structure type imposes strict electronic limits on its Bi members. This structure-property relationship determines the dynamic and magnetic properties of these materials, but in situ techniques are required to elucidate the high-pressure properties. Using the optical response of nitrogen vacancies embedded in our diamond anvils, we observed the predicted magnetic ordering. This result confirms the promise of this high-pressure approach for designing and understanding new functional materials.