Anomalous specific heat and magnetic properties of TmxDy1-xAl2 (0 ≤ x ≤ 1)
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We study crystal structure, phase transitions and magnetism of pseudo-binary TmxDy1-xAl2 (0 ≤ x ≤ 1) compounds using temperature dependent X-ray powder diffraction, specific heat and magnetization measurements, first principles, and model calculations. In low external magnetic fields, Dy-rich compounds undergo continuous, second-order phase transitions at the respective Curie temperatures, TC. In contrast, the Tm-rich compounds exhibit discontinuous, first-order anomalies in the magnetically ordered states. These sharp transitions correlate with a substantial energy difference between the room temperature cubic and ground state rhombohedral structures of TmAl2. A clear anomaly in the lattice parameter is observed at ∼30 K for x = 0.5, which nearly coincides with TC = 31.2 K. The effective quadrupolar moment of the lanthanides changes sign around x = 0.5, which leads to a nearly zero anisotropy constant and approximately spherical effective 4f charge densities, providing an explanation for the lack of structural distortions below TC for x = 0.5. The calculations confirm  as the easy magnetization axis in the ground state tetragonal structure of DyAl2, and reveal collapse of the orbital magnetic moment when the easy magnetization direction changes to . Within the rhombohedral ground state of TmAl2  is the easy magnetization direction.