The MnCoGe alloy can crystallize in either the hexagonal Ni2In- or the orthorhombic TiNiSi-type of structure. In both phases MnCoGe behaves like a typical ferromagnet with a second-order magnetic phase transition. For MnCoGeBx with B on interstitial positions, we discover a giant magnetocaloric effect associated with a single first-order magnetostructural phase transition, which can be achieved by tuning the magnetic and structural transitions to coincide. The results obtained on the MnCoGe-type alloys may be extensible to other types of magnetic materials undergoing a first-order structural transformation and can open up some possibilities for searching magnetic refrigerants for room-temperature applications.

Substitution of some Cr for Mn atoms in MnCoGe was employed to control the magnetic and structural transitions in this alloy to coincide, leading to a single first-order magnetostructural transition from the ferromagnetic to the paramagnetic state with a giant magnetocaloric effect observed near room temperature. Further increase in the Cr content in the Mn1−xCrxCoGe alloys can induce another first-order magnetoelastic transition from the antiferromagnetic to the ferromagnetic state occurring at lower temperature. The giant magnetocaloric effect as well as the simultaneous tunability of the two magnetic transitions make these materials promising for future cooling applications.

Using high-resolution neutron diffraction measurements for Mn-rich hexagonal Mn-Fe-P-Si compounds, we show that the substitution of Mn for Fe on the 3f sites results in a linear decrease of the Fe/Mn(3f ) magnetic moments, while the Mn(3g) magnetic moments remain constant. With increasing temperature, the Mn(3g) magnetic moments show almost no change, while the Fe/Mn(3f ) moments decrease quickly when the transition temperature is approached. The reduction of the magnetic moments at the transition temperature and in the high-temperature range is discussed based on changes in interatomic distances and lattice parameters and high-temperature magnetic-susceptibility measurement.

Neutron-diffraction experiments on the (Mn,Fe) 2 (P,Si)-type compounds have shown a site preference of Si atoms in the hexagonal structure. The degree of ordering of Si depends on the Si/P ratio, while it is independent of the Mn/Fe ratio. The ferromagnetic-paramagnetic magnetoelastic transition is closely related to the size of the magnetic moment on the 3f site. A preferred occupation of Si atoms on the 2c site stabilizes and decreases the magnetic moment on the 3f and 3g site, respectively, which is supported by our first-principles density functional theory calculations. This effect, together with the contribution from the Si substitution-induced changes in the interatomic distances, leads to a phase transition that is tunable in temperature and degree of first order in Mn 1.25 Fe 0.70 P 1−x Si x compounds. These results provide us with further insight into the relationship between the magnetoelastic phase transition and the local atomic coordination.

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