Thin film quantum materials

Abstract:

Abstract:

Magnetic domain formation in two-dimensional (2D) materials gives perspectives into the fundamental origins of 2D magnetism and also motivates the development of advanced spintronics devices. However, the characterization of magnetic domains in atomically thin van der Waals (vdW) flakes remains challenging. Here, we employ X-ray photoemission electron microscopy (XPEEM) to perform layer-resolved imaging of the domain structures in the itinerant vdW ferromagnet Fe₅GeTe₂ which shows near room temperature bulk ferromagnetism and a weak perpendicular magnetic anisotropy (PMA). In the bulk limit, we observe the well-known labyrinth-type domains. Thinner flakes, on the other hand, are characterized by increasingly fragmented domains. While PMA is a characteristic property of Fe₅GeTe₂, we observe a spin-reorientation transition with the spins canting in-plane for flakes thinner than six layers. Notably, a bubble phase emerges in four-layer flakes. This thickness dependence, which clearly deviates from the single-domain behavior observed in other 2D magnetic materials, demonstrates the exciting prospect of stabilizing complex spin textures in 2D vdW magnets at relatively high temperatures.

Abstract:

The study of magnetic order in few- and monolayer van der Waals materials poses a challenge to the most commonly employed magnetic characterization techniques as they normally lack magnetic sensitivity and/or lateral resolution enabling their thickness-dependent probing. Here we demonstrate the usefulness of x-ray absorption spectroscopy (XAS) and x-ray magnetic circular dichroism (XMCD) measurements, carried out at the Cr L2,3 and Te M5 edges, for the study of the ferromagnetic semiconductor CrSiTe3 (CST) in the form of single- and few-layer flakes. By scanning the sample under the incident x-ray beam, a map of the exfoliated system was obtained, which reproduced the optical micrographs showing the detailed distribution and thicknesses of the flakes. In this way, XAS/XMCD was performed at selected sample areas, revealing the thickness-resolved spectroscopic and magnetic properties of the flakes, such as the spin and orbital magnetic moments. The spin moment, in line with the saturation field, is decreasing with film thickness, revealing a single-domain and out-of-plane magnetization for the thinnest films. For CST, the electronic properties are governed by the strong covalent bond between the Cr 3d(eg ) and Te 5p states, giving rise to a superexchange scenario. We observed a gradually increasing ratio of orbital to spin moment for thinner flakes, which could be due to a further increase of the covalent mixing. Hysteresis loops were recorded at the Cr L3 edge, showing an open loop for 10 down to ∼3 layers, while the bulk shows a wasp-waist shaped loop. With the transition temperature from the soft to the hard ferromagnetic state decreasing with thickness, the monolayer shows a narrowed, closed loop at 10 K, suggesting its transition temperature >10 K. Our study demonstrates the unique capabilities of XAS/XMCD for the study of few-layer van der Waals magnets, highlighting the interplay between electron correlation and ferromagnetism in CST.

Abstract:

The study of magnetic order in few- and monolayer van der Waals materials poses a challenge to the most commonly employed magnetic characterization techniques as they normally lack magnetic sensitivity and/or lateral resolution enabling their thickness-dependent probing. Here we demonstrate the usefulness of X-ray absorption spectroscopy (XAS) and X-ray magnetic circular dichroism (XMCD) measurements, carried out at the Cr L2,3 and Te M5 edges, for the study of the ferromagnetic semiconductor CrSiTe3 (CST) in the form of single- and few-layer flakes. By scanning the sample under the incident X-ray beam, a map of the exfoliated system was obtained, which reproduced the optical micrographs showing the detailed distribution and thicknesses of the flakes. In this way, XAS/XMCD was performed at selected sample areas, revealing the thickness-resolved spectroscopic and magnetic properties of the flakes, such as the spin and orbital magnetic moments. The spin moment, in line with the saturation field, is decreasing with film thickness, revealing a single-domain and out-of-plane magnetization for the thinnest films. For CST, the electronic properties are governed by the strong covalent bond between the Cr 3d(eg) and Te 5p states, giving rise to a superexchange scenario. We observed a gradually increasing ratio of orbital to spin moment for thinner flakes, which could be due to a further increase of the covalent mixing. Hysteresis loops were recorded at the Cr L3 edge, showing an open loop for 10 down to ~3 layers, while the bulk shows a wasp-waist shaped loop. With the transition temperature from the soft to the hard ferromagnetic state decreasing with thickness, the monolayer shows a narrowed, closed loop at 10 K, suggesting its transition temperature >10 K. Our study demonstrates the unique capabilities of XAS/XMCD for the study of few-layer van der Waals magnets, correlation and ferromagnetism in CST.

Abstract:

An elegant approach to overcome the intrinsic limitations of magnetically doped topological insulators is to bring a topological insulator in direct contact with a magnetic material. The aspiration is to realize the quantum anomalous Hall effect at high temperatures where the symmetry-breaking magnetic field is provided by a proximity-induced magnetization at the interface. Hence, a detailed understanding of the interfacial magnetism in such heterostructures is crucial, yet its distinction from structural and magnetic background effects is a rather nontrivial task. Here, we combine several magnetic characterization techniques to investigate the magnetic ordering in MnTe/Bi2Te3 heterostructures. A magnetization profile of the layer stack is obtained using depth-sensitive polarized neutron reflectometry. The magnetic constituents are characterized in more detail using element-sensitive magnetic x-ray spectroscopy. Magnetotransport measurements provide additional information about the magnetic transitions. We find that the supposedly antiferromagnetic MnTe layer does not exhibit an x-ray magnetic linear dichroic signal, raising doubt that it is in its antiferromagnetic state. Instead, Mn seems to penetrate into the surface region of the Bi2Te3 layer. Furthermore, the interface between MnTe and Bi2Te3 is not abrupt, but extending over ∼2.2 nm. These conditions are the likely reason that we do not observe proximity-induced magnetization at the interface. Our findings illustrate the importance of not solely relying on one single technique as proof for proximity-induced magnetism at interfaces. We demonstrate that a holistic, multitechnique approach is essential to gain a more complete picture of the magnetic structure in which the interface is embedded.