Zero thermal expansion (ZTE) is an intriguing phenomenon by virtue of its peculiar lack of expansion and contraction with temperature. The achievement of ZTE in a metallic material is a desired but challenging task. Here we report the ZTE behavior of a single-phase metallic VB compound, stacking with the V and B atomic layers along the direction (α = 2.18 × 10 K, 5-150 K). Neutron powder diffraction demonstrates that the ZTE behavior is entangled in the direct blocking of the lattice expansion along all crystallographic directions with temperature. X-ray photoelectron spectroscopy and density functional theory calculations indicate that strong covalent binding adheres the nearest-neighbor B-B and V-B pairs, which is proposed to control the ZTE within both the basal plane and the direction. An intimate correlation is revealed between the covalent binding and the lattice parameters. Our work indicates the opportunity to design metallic ZTE with strong chemical binding in the future.
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