The correlation between the covalent bonds and magnetocaloric properties of the Mn2−xFexPyGe1−yMz compounds

Abstract

In recent years, MnFePGe magnetocaloric materials have been widely studied as promising candidates for magnetic refrigeration materials. The Curie temperature of MnFePGe can be adjusted to around room temperature by changing the element ratio or doping with other elements. Due to its first-order magnetic and structural transition, it engenders a large entropy change but unfortunately also exhibits a large thermal hysteresis during the phase transition, which leads to energy loss and lower refrigeration capability. In this paper, we establish a correlation between the in-plane covalent bonding and Curie temperature (TC), thermal hysteresis (ΔThys), two-phase coexistence zone (ΔTcoex), and entropy change (ΔSDSC) using 54 Mn2−xFexPyGe1−yMz (where M is a metallic or nonmetallic doped element) samples with different components. Neutron diffraction and XRD diffraction data and refinements have been employed to allow a detailed electron density reconstruction of six typical samples with the maximum entropy method. We find that the length of the in-plane bonding is closely correlated with the TC and ΔThys, while the TC, ΔThys, ΔTcoex, and ΔSDSC have no significant correlation with the length of the interlayer covalent bond. Moreover, we find that the ΔThys correlates most strongly with the change in the bond length when undergoing the paramagnetic-to-ferromagnetic phase transition rather than the absolute value of the bond length. These results provide an understanding of how to control the properties, enabling effective ways to tune the composition of magnetic refrigeration materials to tailor magnetocaloric properties for optimal performance.