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Exploratory theoretical predictions in uncharted structural and compositional space are integral to materials discoveries. Inspired by M5SiB2 (T2) phases, the finding of a family of laminated quaternary metal borides, M′4M″SiB2, with out‐of‐plane chemical order is reported here. 11 chemically ordered phases as well as 40 solid solutions, introducing four elements previously not observed in these borides...
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