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Results of fundamental and third order ac susceptibility measurements in a Ni49Mn29Ga22 single crystal demonstrate that higher harmonics of ac-susceptibility measurement is an excellent tool to identify transitions/anomalies originating from different magnetic substructures that remain undetected by usual dc susceptibility measurements. Anomaly observed at low temperature (∼150 K) has also been explored by differential scanning calorimetry, temperature dependent x-ray diffraction, and transmission electron microscopy measurements. The results demonstrate that the magnetic subsystem in Ni–Mn–Ga is unstable at low temperatures not only for metastable modulated crystal structure but also for very stable nonmodulated tetragonal structure.

Magnetic and structural properties of Ni–Mn–Al thin films are investigated. It is demonstrated that the annealed film shows L21 phase at room temperature. Magnetometry measurements reveal that the annealed film is ferromagnetic and a first order transition in magnetization versus temperature measurement confirms that the martensite to austenite transition occurs around room temperature. Transmission electron microscopy measurements confirm that this structural change occurs just below room temperature. The splitting of Mn 2p3/2 level in x-ray photoelectron spectroscopy core level spectra of the annealed Ni–Mn–Al film, confirms that the origin of magnetism is definitely correlated with the local magnetic moment at the Mn atoms.