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Materials exhibiting zero thermal expansion (ZTE), namely, volume invarianceduring temperature change, can resist thermal shock and are highly desired inmodern industries as high-precision components. However, pure ZTE materials arerare, especially those that are metallic. Here, we report the discovery of apure metallic ZTE material: an orthorhombic Mn1-xNixCoSi spiral magnet. Theintroduction of Ni can efficiently enhance the ferromagnetic exchangeinteraction and construct the transition from a spiral magnetic state to aferromagnetic-like state in MnCoSi-based alloys. Systematic in situ neutronpowder diffraction revealed a new cycloidal spiral magnetic structure in bcplane at ground state which would transform to the helical spiral in the abplane with increasing temperature. Combined with Lorentz transmission electronmicroscopy techniques, the cycloidal and helical spin order coherently rotatedat varying periods along the c axis during the magnetic transition. This spinrotation drove the continuous movement of the coupled crystalline lattice andinduced a large negative thermal expansion along the a axis, eventually leadingto a wide-temperature ZTE effect. Our work not only introduces a new ZTE alloybut also presents a new mechanism by which to discover or design ZTE magnets.

Coherent spin rotation-induced zero thermal expansion in MnCoSi-based spiral magnets