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All atomically laminated MAB phases (M = transition metal, A = A-group element, and B = boron) exhibit orthorhombic or tetragonal symmetry, with the only exception being hexagonal Ti 2 InB 2 . Inspired by the recent discovery of chemically ordered hexagonal carbides, i-MAX phases, we perform an extensive first-principles study to explore chemical ordering upon metal alloying of M 2 AlB 2 (M from groups 3 to 9) in orthorhombic and hexagonal symmetry. Fifteen stable novel phases with in-plane chemical ordering are identified, coined i-MAB, along with 16 disordered stable alloys. The predictions are verified through the powder synthesis of Mo 4/3 Y 2/3 AlB 2 and Mo 4/3 Sc 2/3 AlB 2 of space group R 3̅ m (no. 166), displaying the characteristic in-plane chemical order of Mo and Y/Sc and Kagomé ordering of the Al atoms, as evident from X-ray diffraction and electron microscopy. The discovery of i-MAB phases expands the elemental space of these borides with M = Sc, Y, Zr, Hf, and Nb, realizing an increased property tuning potential of these phases as well as their suggested potential two-dimensional derivatives.

Theoretical Prediction and Synthesis of a Family of Atomic Laminate Metal Borides with In-Plane Chemical Ordering