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Recent advances in tools for crystal structure analysis enabled us todescribe a new phenomenon in structural chemistry, which, to this day, hasremained hidden. Here we describe a crystal structure with an incommensuratecompositional modulation, Mn0.6Ni0.4As. The sample adopts the NiAs typestructure, but in contrast to a normal solid solution, we observe thatmanganese and nickel separate into layers of MnAs and NiAs with thickness of2-4 face-shared octahedra. Experimentally, results are obtained by combinationof 3D electron diffraction, scanning transmission electron microscopy andneutron diffraction. The distribution of octahedral units between the manganeseand nickel layers is perfectly described by a modulation vector q = 0.360(3)c*. An additional periodicity is thus present in the compound. Positionalmodulation is observed of all elements as a consequence of the occupationalmodulation.

Exotic compositional ordering in Mn-Ni-As intermetallics