Role of the structure order in the transport and magnetic properties of high-entropy alloy films

The fabrication and development of high-entropy alloys (HEAs) with exceptional functionalities is a rapidly expanding field with numerous applications. When the role of entropy in HEAs is considered, the extrinsic factors, such as the existence of grains and different phases, need to be separated from the intrinsic configurations of the atomic lattice. Here, we fabricated the CoCrFeNi₂Al_0.5 HEA/muscovite heterostructures, and some were prepared as epitaxial bilayers and others were prepared as an amorphous system. These two systems are classified into atomic-site disordered (ASD) and structurally disordered (SD) states, respectively, without the extrinsic effects for the determination of the crystal lattice role in high-entropy states. In this study, we determined the role of the structure order in correlation with the structural, electronic, and magnetic properties of HEAs using a combination of energy-dispersive X-ray spectrometry, X-ray diffraction, transmission electron microscopy, magneto-transport, ac magnetometry, and X-ray absorption spectroscopy with magnetic circular dichroism. The ASD state showed fully metallic behavior. In contrast, the SD state showed a metallic behavior with intense magnetic saturation, which was called Kondo-like behavior, under 50 K with a low-temperature coefficient of resistivity of ~64 ppm/°C. The difference between the saturation magnetic moment and the electron relaxation behavior in the ASD and SD states resulted from the existence of the structural order affecting the atomic distance and periodicity to modify the exchange interaction and tune the electron-phonon interaction for scattering. The ferromagnetic behavior contributed by Co, Fe, and Ni atoms was probed by X-ray absorption and magnetic circular dichroism to understand the magnetic interactions in the ASD and SD states.