
In high-entropy alloys (HEA), the configurational entropy arising from the presence of multiple elements, stabilizes a disordered solid solution in preference to the possible formation of compounds. In the current work, we identify cluster compounds (of the type AM4X8) as orientational analogues of HEA (as a first report on orientational high-entropy systems). In cluster compounds, orientational disorder increases the entropy and plays a role analogous to positional disorder in HEA. In the GaMo4S8 compound, at temperatures greater than 50 K, the entropic benefit more than makes up for the strain energy cost and stabilizes the disordered phase in preference to an orientationally ordered compound.
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