No Arabic abstract
Material research has been a major driving force in the development of modern nano-electronic devices. In particular, research in magnetic thin films has revolutionized the development of spintronic devices; identifying new magnetic materials is key to better device performance and new device paradigm. The advent of two-dimensional van der Waals crystals creates new possibilities. This family of materials retain their chemical stability and structural integrity down to monolayers and, being atomically thin, are readily tuned by various kinds of gate modulation. Recent experiments have demonstrated that it is possible to obtain two-dimensional ferromagnetic order in insulating Cr$_2$Ge$_2$Te$_6$ and CrI$_3$ at low temperatures. Here, we developed a new device fabrication technique, and successfully isolated monolayers from layered metallic magnet Fe$_3$GeTe$_2$ for magnetotransport study. We found that the itinerant ferromagnetism persists in Fe$_3$GeTe$_2$ down to monolayer with an out-of-plane magnetocrystalline anisotropy. The ferromagnetic transition temperature, $T_c$, is suppressed in pristine Fe$_3$GeTe$_2$ thin flakes. An ionic gate, however, dramatically raises the $T_c$ up to room temperature, significantly higher than the bulk $T_c$ of 205 Kelvin. The gate-tunable room-temperature ferromagnetism in two-dimensional Fe$_3$GeTe$_2$ opens up opportunities for potential voltage-controlled magnetoelectronics based on atomically thin van der Waals crystals.
The weak interlayer coupling in van der Waals (vdW) magnets has confined their application to two dimensional (2D) spintronic devices. Here, we demonstrate that the interlayer coupling in a vdW magnet Fe$_3$GeTe$_2$ (FGT) can be largely modulated by a protonic gate.With the increase of the protons intercalated among vdW layers,interlayer magnetic coupling increases.Because of the existence of antiferromagnetic layers in FGT nanoflakes, the increasing interlayer magnetic coupling induces exchange bias in protonated FGT nanoflakes. Most strikingly, a rarely seen zero-field cooled (ZFC) exchange bias with very large values (maximally up to 1.2 kOe) has been observed when higher positive voltages (Vg>4.36 V) are applied to the protonic gate, which clearly demonstrates that a strong interlayer coupling is realized by proton intercalation. Such strong interlayer coupling will enable a wider range of applications for vdW magnets.
Dilute magnetic semiconductors (DMSs) show great promise for applications in spin-based electronics, but in most cases continue to elude explanations of their magnetic behavior. Here, we combine quantitative x-ray spectroscopy and Anderson impurity model calculations to study ferromagnetic Fe-substituted In$_2$O$_3$ films, and we identify a subset of Fe atoms adjacent to oxygen vacancies in the crystal lattice which are responsible for the observed room temperature ferromagnetism. Using resonant inelastic x-ray scattering, we map out the near gap electronic structure and provide further support for this conclusion. Serving as a concrete verification of recent theoretical results and indirect experimental evidence, these results solidify the role of impurity-vacancy coupling in oxide-based DMSs.
To understand the magnetic properties of Fe$_3$GeTe$_2$, we performed the detailed first-principles study. Contrary to the conventional wisdom, it is unambiguously shown that Fe$_3$GeTe$_2$ is not ferromagnetic but antiferromagnetic carrying zero net moment in its stoichiometric phase. Fe defect and hole doping are the keys to make this material ferromagnetic, which are shown by the magnetic force response as well as the total energy calculation with the explicit Fe defects and the varied system charges. Further, we found that the electron doping also induces the antiferro- to ferromagnetic transition. It is a crucial factor to understand the notable recent experiment of gate-controlled ferromagnetism. Our results not only unveil the origin of ferromagnetism of this material but also show how it can be manipulated with defect and doping.
Two-dimensional (2D) van der Waals (vdWs) materials have gathered a lot of attention recently. However, the majority of these materials have Curie temperatures that are well below room temperature, making it challenging to incorporate them into device applications. In this work, we synthesized a room-temperature vdW magnetic crystal Fe$_5$GeTe$_2$ with a Curie temperature T$_c = 332$ K, and studied its magnetic properties by vibrating sample magnetometry (VSM) and broadband ferromagnetic resonance (FMR) spectroscopy. The experiments were performed with external magnetic fields applied along the c-axis (H$parallel$c) and the ab-plane (H$parallel$ab), with temperatures ranging from 300 K to 10 K. We have found a sizable Lande g-factor difference between the H$parallel$c and H$parallel$ab cases. In both cases, the Lande g-factor values deviated from g = 2. This indicates contribution of orbital angular momentum to the magnetic moment. The FMR measurements reveal that Fe$_5$GeTe$_2$ has a damping constant comparable to Permalloy. With reducing temperature, the linewidth was broadened. Together with the VSM data, our measurements indicate that Fe$_5$GeTe$_2$ transitions from ferromagnetic to ferrimagnetic at lower temperatures. Our experiments highlight key information regarding the magnetic state and spin scattering processes in Fe$_5$GeTe$_2$, which promote the understanding of magnetism in Fe$_5$GeTe$_2$, leading to implementations of Fe$_5$GeTe$_2$ based room-temperature spintronic devices.
Thermal ammonolysis of quasi-two-dimensional (quasi-2D) CoTa2O6 yields the O2-/N3- and anionic vacancy ordered Co2+Ta5+2O6-xN2x/3$Box$x/3 (x $leq$ 0.15) that exhibits a transition from antiferromagnetism to defect engineered above room-temperature ferromagnetism as evidenced by diffraction, spectroscopic and magnetic characterizations. First-principles calculations reveal the origin of ferromagnetism is a particular CoON configuration with N located at Wyckoff position 8j, which breaks mirror symmetry about ab plane. A pressure-induced electronic phase transition is also predicted at around 24.5 GPa, accompanied by insulator-to-metal transition and magnetic moment vanishing.