Giant Baromagnetic Effect Induced by Spin Engineering in Mn3(Zn0.25Sn0.25Ga0.25Ge0.25)C

Baromagnetic effect (BME), arising from pressure-induced spin reorientation, holds great potential for next-generation information technologies owing to its strong multifield coupling characteristics. However, the practical implementation of BME is hindered by the small magnetization change and the large driving pressure required in conventional materials. Guided by spin-polarized calculations, this work successfully obtains a giant BME material Mn3(Zn0.25Sn0.25Ga0.25Ge0.25)C, which exhibits a remarkable pressure-induced maximum magnetization change (|ΔMmax|) of 2.63 μB·f.u.-1 and an exceptionally large baromagnetic coefficient (BMC, d) of 15.0 μB·f.u.-1·GPa-1. Temperature-dependent neutron powder diffraction (NPD) measurements reveal a clear evolution from the nearly collinear antiferromagnetic (cAFM) configuration with k = (1/2, 1/2, 1/2) to the ferromagnetic (FM) configuration, indicating that the spins are highly susceptible to reorientation under external perturbations. First-principles calculations further clarify that pressure modulates the energy difference (ΔE) between the cAFM and FM configurations via the Ruderman-Kittel-Kasuya-Yosida (RKKY) interaction, elucidating the microscopic origin of the giant BME. This demonstration establishes spin engineering, achieved through precise control of spin configurations via targeted element selection, as an effective strategy for realizing high-performance baromagnetic systems. It further provides clear guidance for designing materials with superior functional properties.