This study investigates the compound system Mn5−xZnxGe3 (x = 0.1, 0.2, and 0.3) through experimental investigations and theoretical calculations. Zn doping lowers the Curie temperature and magnetic entropy change of Mn5−xZnxGe3 alloys. Analysis of phenomenological curves, including Landau theories, normalized curves, and Arrott curves during the study of isothermal magnetization curves, reveals a second-order phase transition in this system. Through an extensive investigation of critical behavior using critical isotherm curves and the Kouvel–Fisher (KF) method, the consistency and reliability of these critical indices are validated by the prediction of the scaling theory in the critical region. By scaling the dependence of |ΔSM| on M and applying crucial exponen21t values, an efficient new approach is utilized to calculate the spontaneous magnetization that agrees well with the values deduced from the KF method. Additionally, first-principles calculations reveal that the Mn atoms' 3d orbitals are more significantly close to the Fermi energy level, with Zn doping generally reducing both the electronic density of states and the total magnetic moment of the Mn 3d orbitals. Consequently, the introduction of Zn leads to a decrease in the Mn–Mn atom exchange coupling, resulting in a deterioration of the total exchange interaction. This phenomenon also explains the decrease in the Curie temperature TC due to Zn doping, aligning with experimental observations.
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