Abstract

Two-dimensional (2D) magnetic layered materials have gained significant interest in spintronic for memory storage devices. Herein, the electronic and magnetic properties of high-quality single crystals of chromium (Cr)-doped hafnium diselenide were studied. The electronic study indicated that the Cr-doped HfSe2 reveals the semiconducting nature with a proper bandgap as identified by angle-resolved photoemission spectroscopy and first-principle density functional theory (DFT) calculations. The magnetic results indicate that the HfSe₂ exhibited ferromagnetic characteristics with the substitution of Cr atoms in a perpendicular direction. The Cr-doped HfSe2 sample shows a ferromagnetic phase below ∼58 K, indicating the critical temperature (Tc) of magnetic order, while above this temperature, it shows a paramagnetic phase that can follow the Curie-Weiss Law. It can be seen that the magnetic moment is approximately 0.16 emu/g at 5 K, which further decreases with increasing temperature until 60 K and then transforms to a paramagnetic phase. The sample can clearly show a weak out-of-plane magnetic anisotropy with a coercivity of around 50.56 Oe and a saturation magnetization value of 0.029 emu/g. Convincingly, it was observed from the ARPES results that the valence band is split due to the spin-orbit interaction of Cr atoms, which can induce ferromagnetic order. At the same time, the temperature-dependent ARPES data shows that the splitting is higher below the Tc, while it is weaker above the Tc. The DFT results revealed that near the Fermi level, the spin-up and spin-down are spin-polarized with asymmetric trends. It can be observed that substituting Cr on the octahedral sites of Hf atoms influences the electron spin order created by Hf vacancies (as validated by the magnetic coupling measured by electron paramagnetic resonance spectroscopy experiments), which can change the magnetic alignment to induce the magnetism in HfSe2. This study highlights that doping transition metal in HfSe2 has promising potential for future applications, especially in memory devices and spintronic technologies.