When Machine Learning Meets 2D Materials: A Review.

The availability of an ever-expanding portfolio of 2D materials with rich internal degrees of freedom (spin, excitonic, valley, sublattice, and layer pseudospin) together with the unique ability to tailor heterostructures made layer by layer in a precisely chosen stacking sequence and relative crystallographic alignments, offers an unprecedented platform for realizing materials by design. However, the breadth of multi-dimensional parameter space and massive data sets involved is emblematic of complex, resource-intensive experimentation, which not only challenges the current state of the art but also renders exhaustive sampling untenable. To this end, machine learning, a very powerful data-driven approach and subset of artificial intelligence, is a potential game-changer, enabling a cheaper - yet more efficient - alternative to traditional computational strategies. It is also a new paradigm for autonomous experimentation for accelerated discovery and machine-assisted design of functional 2D materials and heterostructures. Here, the study reviews the recent progress and challenges of such endeavors, and highlight various emerging opportunities in this frontier research area.

Two-dimensional ferromagnetic superlattices.

Mechanically exfoliated two-dimensional ferromagnetic materials (2D FMs) possess long-range ferromagnetic order and topologically nontrivial skyrmions in few layers. However, because of the dimensionality effect, such few-layer systems usually exhibit much lower Curie temperature (T C) compared to their bulk counterparts. It is therefore of great interest to explore effective approaches to enhance their T C, particularly in wafer-scale for practical applications. Here, we report an interfacial proximity-induced high-T C 2D FM Fe3GeTe2 (FGT) via A-type antiferromagnetic material CrSb (CS) which strongly couples to FGT. A superlattice structure of (FGT/CS)n, where n stands for the period of FGT/CS heterostructure, has been successfully produced with sharp interfaces by molecular-beam epitaxy on 2-inch wafers. By performing elemental specific X-ray magnetic circular dichroism (XMCD) measurements, we have unequivocally discovered that T C of 4-layer Fe3GeTe2 can be significantly enhanced from 140 K to 230 K because of the interfacial ferromagnetic coupling. Meanwhile, an inverse proximity effect occurs in the FGT/CS interface, driving the interfacial antiferromagnetic CrSb into a ferrimagnetic state as evidenced by double-switching behavior in hysteresis loops and the XMCD spectra. Density functional theory calculations show that the Fe-Te/Cr-Sb interface is strongly FM coupled and doping of the spin-polarized electrons by the interfacial Cr layer gives rise to the T C enhancement of the Fe3GeTe2 films, in accordance with our XMCD measurements. Strikingly, by introducing rich Fe in a 4-layer FGT/CS superlattice, T C can be further enhanced to near room temperature. Our results provide a feasible approach for enhancing the magnetic order of few-layer 2D FMs in wafer-scale and render opportunities for realizing realistic ultra-thin spintronic devices.

Metallic 1T Phase, 3d1 Electronic Configuration and Charge Density Wave Order in Molecular Beam Epitaxy Grown Monolayer Vanadium Ditelluride.

We present a combined experimental and theoretical study of monolayer vanadium ditelluride, VTe2, grown on highly oriented pyrolytic graphite by molecular-beam epitaxy. Using various in situ microscopic and spectroscopic techniques, including scanning tunneling microscopy/spectroscopy, synchrotron X-ray and angle-resolved photoemission, and X-ray absorption, together with theoretical analysis by density functional theory calculations, we demonstrate direct evidence of the metallic 1T phase and 3d1 electronic configuration in monolayer VTe2 that also features a (4 × 4) charge density wave order at low temperatures. In contrast to previous theoretical predictions, our element-specific characterization by X-ray magnetic circular dichroism rules out a ferromagnetic order intrinsic to the monolayer. Our findings provide essential knowledge necessary for understanding this interesting yet less explored metallic monolayer in the emerging family of van der Waals magnets.

Evidence of Spin Frustration in a Vanadium Diselenide Monolayer Magnet.

Monolayer VSe2 , featuring both charge density wave and magnetism phenomena, represents a unique van der Waals magnet in the family of metallic 2D transition-metal dichalcogenides (2D-TMDs). Herein, by means of in situ microscopy and spectroscopic techniques, including scanning tunneling microscopy/spectroscopy, synchrotron X-ray and angle-resolved photoemission, and X-ray absorption, direct spectroscopic signatures are established, that identify the metallic 1T-phase and vanadium 3d1 electronic configuration in monolayer VSe2 grown on graphite by molecular-beam epitaxy. Element-specific X-ray magnetic circular dichroism, complemented with magnetic susceptibility measurements, further reveals monolayer VSe2 as a frustrated magnet, with its spins exhibiting subtle correlations, albeit in the absence of a long-range magnetic order down to 2 K and up to a 7 T magnetic field. This observation is attributed to the relative stability of the ferromagnetic and antiferromagnetic ground states, arising from its atomic-scale structural features, such as rotational disorders and edges. The results of this study extend the current understanding of metallic 2D-TMDs in the search for exotic low-dimensional quantum phenomena, and stimulate further theoretical and experimental studies on van der Waals monolayer magnets.

Ferromagnet/Two-Dimensional Semiconducting Transition-Metal Dichalcogenide Interface with Perpendicular Magnetic Anisotropy.

Ferromagnet/two-dimensional transition-metal dichalcogenide (FM/2D TMD) interfaces provide attractive opportunities to push magnetic information storage to the atomically thin limit. Existing work has focused on FMs contacted with mechanically exfoliated or chemically vapor-deposition-grown TMDs, where clean interfaces cannot be guaranteed. Here, we report a reliable way to achieve contamination-free interfaces between ferromagnetic CoFeB and molecular-beam epitaxial MoSe2. We show a spin reorientation arising from the interface, leading to a perpendicular magnetic anisotropy (PMA), and reveal the CoFeB/2D MoSe2 interface allowing for the PMA development in a broader CoFeB thickness-range than common systems such as CoFeB/MgO. Using X-ray magnetic circular dichroism analysis, we attribute generation of this PMA to interfacial d-d hybridization and deduce a general rule to enhance its magnitude. We also demonstrate favorable magnetic softness and considerable magnetic moment preserved at the interface and theoretically predict the interfacial band matching for spin filtering. Our work highlights the CoFeB/2D MoSe2 interface as a promising platform for examination of TMD-based spintronic applications and might stimulate further development with other combinations of FM/2D TMD interfaces.

Recent Advances in X-Ray Hydroxyl Radical Footprinting at the Advanced Light Source Synchrotron.

BACKGROUND: Synchrotron hydroxyl radical footprinting is a relatively new structural method used to investigate structural features and conformational changes of nucleic acids and proteins in the solution state. It was originally developed at the National Synchrotron Light Source at Brookhaven National Laboratory in the late nineties, and more recently, has been established at the Advanced Light Source at Lawrence Berkeley National Laboratory. The instrumentation for this method is an active area of development, and includes methods to increase dose to the samples while implementing high-throughput sample delivery methods. CONCLUSION: Improving instrumentation to irradiate biological samples in real time using a sample droplet generator and inline fluorescence monitoring to rapidly determine dose response curves for samples will significantly increase the range of biological problems that can be investigated using synchrotron hydroxyl radical footprinting.

XMCD characterization of the ferromagnetic state of Yb14MnSb11.

X-ray magnetic circular dichroism (XMCD) measurements on Yb14MnSb11 provide experimental evidence of a moment of 5 microB on Mn, with partial cancellation by an opposing moment on the Sb4 cage surrounding each Mn ion. The compound is isostructural to Ca14AlSb11, with Mn occupying the Al site in the AlSb4(9-) discrete tetrahedral, anionic unit. Bulk magnetization measurements indicate a saturation moment of 3.90 +/- 0.02 microB/formula unit consistent with four unpaired spins and implying a Mn3+, high-spin d4 state. XMCD measurements reveal that there is strong dichroism in the Mn L23 edge, the Sb M45 edge shows a weak dichroism indicating antialignment to the Mn, and the Yb N45 edge shows no dichroism. Comparisons of the Mn spectra with theoretical models for Mn2+ show excellent agreement. The bulk magnetization can be understood as Mn with a moment of 5 microB and a 2+ configuration, with cancellation of one spin by an antialigned moment from the Sb 5p band of the Sb4 cage surrounding the Mn.

Epitaxial electrodeposition of Fe(3)O(4) thin films on the low-index planes of gold.

Half-metallic ferrimagnetic materials such as Fe(3)O(4) are of interest for use in spintronic devices. These devices exploit both the spin and charge of an electron in spin-dependent charge transport. Epitaxial thin films of Fe(3)O(4) have been grown on the three low-index planes of gold by electrodeposition. On Au(110), a [110] Fe(3)O(4) orientation that is aligned with the underlying Au(110) substrate is observed. Thin films on Au(100) grow with three different orientations: [100], [111], and [511]. On Au(111), both [111] and [511] orientations of Fe(3)O(4) are observed. The [511] orientations are the result of twinning on [111] planes. A polarization value of approximately -40% at the Fermi level was measured by spin-polarized photoemission at room temperature for a thin film on Au(111).