Alloys are disordered solid solutions of two or more materials (metals or insulators), which could be iso-or hetero-structural. Such solid solutions may span the entire composition range (complete solid solutions) or may form in limited composition ranges with miscibility gap(s). Alloying has been utilized to design materials with superior structural and functional properties since time immemorial. From alloying copper with tin to improve the mechanical strength of tools and weaponry in the Bronze age to alloying of iron to produce steel during the Industrial Revolution, alloy design and optimization has become the cornerstone of human advancement. More recently, In x Ga 1 x N alloys have enabled tunable light emitting diodes, wherein the band gap of GaN is tuned by controlling the In content . Alloying is extensively used to optimize functional properties of materials for photovoltaics (e.g., CdSe x Te 1 x , 2 CsSn x Pb 1 x I 3 hybrid perovskites ), energy storage (e.g., Li 6 PS 5 x Se x Br argyrodite solid electrolytes ), ferroelectrics (e.g., Sc x Al 1 x N ), and thermoelectrics (e.g., PbSe x Te