The evolutions of the crystallographic structure and magnetic phase transition in Tb2In1−xAlx (0 ≤ x ≤ 0.6) alloys are investigated in this work. By gradually alloying antiferromagnetic orthorhombic Tb2Al, the crystalline structure of ferromagnetic Tb2In is gradually distorted from the hexagonal type for x ≤ 0.3 to orthorhombic one for x ≥ 0.4. The ferromagnetic ground state for x ≤ 0.4 is also gradually evolved into antiferromagnetic one for x ≥ 0.5. The phase transition temperature is decreased monotonously. At the critical composition of x = 0.4, the weak field-triggered metamagnetism is realized, leading into the enhanced maximum of magnetic entropy change from 6.6 J kg−1 K−1 in Tb2In to 10.6 J kg−1 K−1 in Tb2In0.6Al0.4 for a field of 5.6 × 106 A/m. The origin is supposed to be from the lattice distortion due to the critical composition at the phase borderline.
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