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At least 91 records · Page 5

Imaging Electrons in Two Dimensional Materials (Final report)

Two-dimensional (2D) materials have extraordinary characteristics that offer promising new approaches for science and technology. Electrons in graphene can move ballistically through a sheet, even though it is only a single atom thick. And transition metal dichalcogenide materials can be cleaved into 2D flakes of all types – metals, semiconductors, insulators, magnetic materials, and superconductors. To benefit from these discoveries, the science needs to be understood to transform 2D materials into useful new devices and systems. The evolution in time of atomic scale graphene structures has been studied in time with a transmission electron microscope (TEM), and ballistic transport of electrons in graphene was been imaged using a cooled scanning probe microscope (SPM), as well as electron motion in MoS 2 . Graphene is only one atom thick but is extremely strong, creating the opportunity to fabricate atomic scale structures in the lateral direction. Using an atomic resolution TEM, a suspended sheet of graphene can be shaped by a Si impurity atom on its surface that acts like a chisel to open up apertures, one atom at a time. The electrons in the TEM provide both the chiseling energy and the ability to image the results. Electrons and holes in graphene form a new type of electronic system with conical conduction and valence bands that meet at the Dirac point, with no energy gap. For moderate densities, the carriers form a Fermi liquid with ballistic transport over micron-scale distances. Using a cooled SPM the cyclotron orbit of electrons in graphene has been imaged. In the magnetic focusing regime, electrons leaving a point contact circle around and leave from a second point contact when the cyclotron diameter is equal to the contact spacing. The paths of electrons are focused - they enter at different angles but converge again at the exiting contact. When the SPM tip knocks an electron out of its orbit, an imaging signal is created. The ballistic motion of carriers in graphene opens the way for ballistic devices that manipulate beams of electrons and holes. Our collaborator Gil-Ho Lee, in Philip Kim's group, created a collimating contact by placing zig-zag absorbers on either side of entering electrons. Our cooled SPM was used to image the electron beam and determine its 9-degree halfwidth. By changing the gate voltage, a collimated beam of holes was also created, opening the way for colliding beam experiments. Coherent beams of carriers are desirable for quantum information processing. Via Andreev reflection, superconducting contacts can covert Cooper pairs in a superconductor to an ingoing and outgoing electrons and holes. Using our cooled SPM, Andreev reflection was imaged from a superconducting contact on a graphene device. Magnetic focusing was used to create an incoming beam of electrons and an outgoing beam of holes, detected by a third point contact. The images show a clear transition from normal reflection above the superconducting transition temperature to Andreev reflection as the device is cooled. Transition metal dichalcogenides offer a wide array of materials that can be exfoliated into ultrathin 2D sheets. A cooled SPM can be used to detect quantum dots as well as to image electron flow. The tip charge capacitively couples to electrons on the dot, acting as a gate to tune the dot conductance. Coulomb blockade peaks appear as a bullseye pattern in an SPM image as the tip is raster scanned above the dot. This approach was used to detect quantum dots in a MoS 2 channel as the carrier density was reduced and electrons pooled in low energy points. Through our DOE supported research, cooled SPM imaging has proven to be a very useful tool to uncover the motion of electrons and holes in the new quantum materials graphene and MoS 2 .

36 MATERIALS SCIENCE↗

2021 Annual Progress Report: Vertical GaN Device Development

This project is part of a multi-lab consortium that leverages U.S. research expertise and facilities at national labs and universities to significantly advance electric drive power density and reliability, while simultaneously reducing cost. The final objective of the consortium is to develop a 100 kW traction drive system that achieves 33 kW/L, has an operational life of 300,000 miles, and a cost of less than 6 dollars/kW. One element of the system is a 100 kW inverter with a power density of 100 kW/L and a cost of 2.7 dollars/kW. New materials such as wide-bandgap semiconductors, soft magnetic materials, and ceramic dielectrics, integrated using multi-objective co-optimization design techniques, will be utilized to achieve these program goals. This project focuses on a subset of the power electronics work within the consortium, specifically the design, fabrication, and evaluation of vertical GaN power devices suitable for automotive applications.

33 ADVANCED PROPULSION SYSTEMS↗

VTO 2022 Annual Progress Report: Vertical GaN Device Development

This project is part of a multi-lab consortium that leverages U.S. research expertise and facilities at national labs and universities to significantly advance electric drive power density and reliability, while simultaneously reducing cost. The final objective of the consortium is to develop a 100 kW traction drive system that achieves 33 kW/L, has an operational life of 300,000 miles, and a cost of less than $\$$6/kW. One element of the system is a 100 kW inverter with a power density of 100 kW/L and a cost of $\$$2.7/kW. New materials such as wide bandgap semiconductors, soft magnetic materials, and ceramic dielectrics, integrated using multi-objective co optimization design techniques, will be utilized to achieve these program goals. This project focuses on a subset of the power electronics work within the consortium, specifically the design, fabrication, and evaluation of vertical GaN power devices suitable for automotive applications.

33 ADVANCED PROPULSION SYSTEMS↗

Ultranarrow electroluminescence from magnetic excitons in the van der Waals antiferromagnetic semiconductor NiPS 3

Electrically driven light emission from two-dimensional (2D) semiconducting materials has enabled numerous optoelectronic technologies, including light-emitting diodes, solid-state lasers, and single-photon sources for quantum communication. Here we report ultranarrow electroluminescence from the magnetic excitonic state of the van der Waals antiferromagnetic semiconductor NiPS 3 . This electroluminescence is enabled by the fabrication of gate-tunable NiPS 3 devices that remain electrically conductive below the antiferromagnetic ordering temperature of 155 K, ultimately allowing field-effect mobilities of 1.3 cm 2 V –1 s –1 and 4.5 cm 2 V –1 s –1 to be directly measured at room temperature and 7 K, respectively. By applying a high-frequency square wave voltage to the gate electrode of the resulting field-effect transistors, electroluminescence is capacitively induced from the magnetic excitons of NiPS 3 . Due to the coupling of these excitons with the underlying NiPS 3 antiferromagnetic order, the electroluminescence has an ultranarrow linewidth of 1 meV and a high degree of linear polarization (ρ = 0.78). In addition to facilitating fundamental studies of the coupling between spin states and excitons in van der Waals magnetic semiconductors, this work will accelerate the development of emerging 2D opto-spintronic applications.

two-dimensional materials↗

Asymmetric magnetic proximity interactions in MoSe 2 /CrBr 3 van der Waals heterostructures

Magnetic proximity interactions between atomically thin semiconductors and two-dimensional magnets provide a means to manipulate spin and valley degrees of freedom in non-magnetic monolayers, without using applied magnetic fields. In such van der Waals heterostructures, magnetic proximity interactions originate in the nanometre-scale coupling between spin-dependent electronic wavefunctions in the two materials, and typically their overall effect is regarded as an effective magnetic field acting on the semiconductor monolayer. Here we demonstrate that magnetic proximity interactions in van der Waals heterostructures can in fact be markedly asymmetric. Valley-resolved reflection spectroscopy of MoSe2/CrBr3 van der Waals structures reveals strikingly different energy shifts in the K and K' valleys of the MoSe2 due to ferromagnetism in the CrBr3 layer. Density functional calculations indicate that valley-asymmetric magnetic proximity interactions depend sensitively on the spin-dependent hybridization of overlapping bands and as such are likely a general feature of hybrid van der Waals structures. Here, these studies suggest routes to control specific spin and valley states in monolayer semiconductors.

36 MATERIALS SCIENCE↗

Discovery of an Intrinsic Antiferromagnetic Semiconductor EuSc 2 Te 4 With Magnetism‐Driven Nonlinear Transport

Magnetic topological materials have recently emerged as a promising platform for studying quantum geometry by the nonlinear transport in thin film devices. In this work, an antiferromagnetic (AFM) semiconductor EuSc₂Te₄ as the first bulk crystal that exhibits quantum geometry-driven nonlinear transport is reported. This material crystallizes into an orthorhombic lattice with AFM order below 5.2 K and a bandgap of less than 50 meV. The calculated band structure aligns with the angle-resolved photoemission spectroscopy spectrum. The AFM order preserves combined space-time inversion symmetry but breaks both spatial inversion and time-reversal symmetry, leading to the nonlinear Hall effect (NLHE). Nonlinear Hall voltage measured in bulk crystals appears at zero field, peaks near the spin-flop transition as the field increases, and then diminishes as the spin moments align into a ferromagnetic order. This field dependence, along with the scaling analysis of the nonlinear Hall conductivity, suggests that the NLHE of EuSc₂Te₄ involves contributions from quantum metric, in addition to extrinsic contributions, such as spin scattering and junction effects. Furthermore, this NLHE is found to have the functionality of broadband frequency mixing, indicating its potential applications in electronics. This work reveals a new avenue for studying magnetism-induced nonlinear transport in magnetic materials.

36 MATERIALS SCIENCE↗

Magnetic structure and exchange interactions in the layered semiconductor CrPS 4

Compounds with two-dimensional (2D) layers of magnetic ions weakly connected by van der Waals bonding offer routes to enhance quantum behavior, stimulating both fundamental and applied interest. CrPS 4 is one such magnetic van der Waals material, however, it has undergone only limited investigation. Here we present a comprehensive series of neutron scattering measurements to determine the magnetic structure and exchange interactions. The observed magnetic excitations allow a high degree of constraint on the model parameters not normally associated with measurements on a powder sample. The results demonstrate the 2D nature of the magnetic interactions, while also revealing the importance of interactions along 1D chains within the layers. The subtle role of competing interactions is observed, which manifest in a nontrivial magnetic transition and a tunable magnetic structure in a small applied magnetic field through a spin-flop transition. Our results on the bulk compound provide insights that can be applied to an understanding of the behavior of reduced layer CrPS 4 .

36 MATERIALS SCIENCE↗

Pressure induced modification of electronic and magnetic properties of MnCrNbAl and MnCrTaAl

Spin-gapless semiconductor (SGS) is a new class of material that has been studied recently for potential applications in spintronics. This material behaves as an insulator for one spin channel, and as a gapless semiconductor for the opposite spin. In this work, we present results of a computational study of two quaternary Heusler alloys, MnCrNbAl and MnCrTaAl that have been recently reported to exhibit spin-gapless semiconducting electronic structure. In particular, using density functional calculations we analyze the effect of external pressure on electronic and magnetic properties of these compounds. It is shown that while these two alloys exhibit nearly SGS behavior at optimal lattice constants and at negative pressure (expansion), they are half-metals at equilibrium, and magnetic semiconductors at larger lattice constant. At the same time, reduction of the unit cell volume has a detrimental effect on electronic properties of these materials, by modifying the exchange splitting of their electronic structure and ultimately destroying their half-metallic/semiconducting behavior. Thus, our results indicate that both MnCrNbAl and MnCrTaAl may be attractive for practical device applications in spin-based electronics, but a potential compression of the unit cell volume (e.g. in thin-film applications) should be avoided.

Materials Science↗

Ferromagnetic Double Perovskite Semiconductors with Tunable Properties

Abstract The authors successfully dope the magnetically silent double perovskite semiconductor Sr 2 GaSbO 6 to induce ferromagnetism and tune its bandgap, with Ga 3+ partially substituted by the magnetic trivalent cation Mn 3+ , in a rigid cation ordering with Sb 5+ . The new ferromagnetic semiconducting Sr 2 Ga 1− x Mn x SbO 6 double perovskite, which crystallizes in tetragonal symmetry (space group I 4/ m ) and has tunable ferromagnetic ordering temperature and bandgap, suggests that magnetic ion doping of double perovskites is a productive avenue toward obtaining materials for application in next‐generation oxide‐based spintronic devices.

36 MATERIALS SCIENCE↗

Defect Complexes in CrSBr Revealed Through Electron Microscopy and Deep Learning

Atomic defects underpin the properties of van der Waals materials, and their understanding is essential for advancing quantum and energy technologies. Scanning transmission electron microscopy is a powerful tool for defect identification in atomically thin materials, and extending it to multilayer and beam-sensitive materials would accelerate their exploration. Here, we establish a comprehensive defect library in a bilayer of the magnetic quasi-1D semiconductor CrSBr by combining atomic-resolution imaging, deep learning, and calculations. We apply a custom-developed machine learning work flow to detect, classify, and average point vacancy defects. This classification enables us to uncover several distinct Cr interstitial defect complexes, combined Cr and Br vacancy defect complexes, and lines of vacancy defects that extend over many unit cells. We show that their occurrence is in agreement with our computed structures and binding energy densities, reflecting the intriguing layer interlocked crystal structure of CrSBr. Our ab initio calculations show that the interstitial defect complexes give rise to highly localized electronic states. These states are of particular interest due to the reduced electronic dimensionality and magnetic properties of CrSBr and are, furthermore, predicted to be optically active. Our results broaden the scope of defect studies in challenging materials and reveal new defect types in bilayer CrSBr that can be extrapolated to the bulk and to over 20 materials belonging to the same FeOCl structural family.

deep learning↗

In-situ tunable giant electrical anisotropy in a grating gated AlGaN/GaN two-dimensional electron gas.

Materials with in-plane electrical anisotropy have great potential for designing artificial synaptic devices. However, natural materials with strong intrinsic in-plane electrical anisotropy are rare. We introduce a simple strategy to produce extremely large electrical anisotropy via grating gating of a semiconductor two-dimensional electron gas (2DEG) of AlGaN/GaN. We show that periodically modulated electric potential in the 2DEG induces in-plane electrical anisotropy, which is significantly enhanced in a magnetic field, leading to an ultra large electrical anisotropy. This is induced by a giant positive magnetoresistance and a giant negative magnetoresistance under two orthogonally oriented in-plane current flows, respectively. This giant electrical anisotropy is in situ tunable by tailoring both the grating gate voltage and the magnetic field. Our semiconductor device with controllable giant electrical anisotropy will stimulate new device applications, such as multi-terminal memtransistors and bionic synapses.

36 MATERIALS SCIENCE↗

Photoluminescence spectra of point defects in semiconductors: Validation of first-principles calculations

Optically and magnetically active point defects in semiconductors are interesting platforms for the development of solid state quantum technologies. Their optical properties are usually probed by measuring photoluminescence spectra, which provide information on excitation energies and on the interaction of electrons with lattice vibrations. We present a combined computational and experimental study of photoluminescence spectra of defects in diamond and SiC, aimed at assessing the validity of theoretical and numerical approximations used in first-principles calculations, including the use of the Franck-Condon principle and the displaced harmonic oscillator approximation. We focus on prototypical examples of solid state qubits, the divacancy centers in SiC and the nitrogen-vacancy in diamond, and we report computed photoluminescence spectra as a function of temperature that are in very good agreement with the measured ones. As expected we find that the use of hybrid functionals leads to more accurate results than semilocal functionals. Interestingly our calculations show that constrained density functional theory (CDFT) and time-dependent hybrid DFT perform equally well in describing the excited state potential energy surface of triplet states; our findings indicate that CDFT, a relatively cheap computational approach, is sufficiently accurate for the calculations of photoluminescence spectra of the defects studied here. Finally, we find that only by correcting for finite-size effects and extrapolating to the dilute limit can one obtain a good agreement between theory and experiment. Our results provide a detailed validation protocol of first-principles calculations of photoluminescence spectra, necessary both for the interpretation of experiments and for robust predictions of the electronic properties of point defects in semiconductors.

36 MATERIALS SCIENCE↗

Electrical Interrogation of Thickness‐Dependent Multiferroic Phase Transitions in the 2D Antiferromagnetic Semiconductor NiI 2

Abstract 2D magnetic materials hold promise for quantum and spintronic applications. 2D antiferromagnetic materials are of particular interest due to their relative insensitivity to external magnetic fields and higher switching speeds compared to 2D ferromagnets. However, their lack of macroscopic magnetization impedes detection and control of antiferromagnetic order, thus motivating magneto‐electrical measurements for these purposes. Additionally, many 2D magnetic materials are ambient‐reactive and electrically insulating or highly resistive below their magnetic ordering temperatures, which imposes severe constraints on electronic device fabrication and characterization. Herein, these issues are overcome via a fabrication protocol that achieves electrically conductive devices from the ambient‐reactive 2D antiferromagnetic semiconductor NiI 2 . The resulting gate‐tunable transistors show band‐like electronic transport below the antiferromagnetic and multiferroic transition temperatures of NiI 2 , revealing a Hall mobility of 15 cm 2 V −1 s −1 at 1.7 K. These devices also allow direct electrical probing of the thickness‐dependent multiferroic phase transition temperature of NiI 2 from 59 K (bulk) to 28 K (monolayer).

2D magnets↗

Epitaxial Electrodeposition of Wide Bandgap Semiconductors for Energy Conversion and Storage

The focus of this project was to electrodeposit epitaxial films and nanostructures of inorganic materials. Although electrodeposition is normally associated with the electroplating of metals, the emphasis in this work was the deposition of compound materials such as metal oxides, semiconductors, catalysts, and magnetic materials. An electrochemical/chemical approach was used, in which an electrochemical redox reaction was followed by a chemical reaction to produce the product. The materials were deposited as epitaxial thin films or nanostructures onto a single-crystal substrate that determined their in-plane and out-of-plane orientation. Epitaxial films can have enhanced properties due to the lack of grain boundaries. They can also produce catalytic materials which have enhanced reactivity due to the exposure of the most catalytically active surface. A method was developed to produce inexpensive single-crystal-like metal foils that could be used as the substrate to deposit materials for applications such as flexible electronics. It was also demonstrated that epitaxial films of inorganic materials could be produced by a simple spin-coating technique.

36 MATERIALS SCIENCE↗

Ferromagnetism in a Semiconductor with Mobile Carriers via Low-Level Nonmagnetic Doping

We show that doped cubic iron pyrite, which is a diamagnetic semiconductor, becomes ferromagnetic when p-type doped. We furthermore find that this material can exhibit high spin polarization both for tunneling and transport devices. These results are based on first-principles electronic structure and transport calculations. This illustrates the use of p-type doping without magnetic impurities as a strategy for obtaining ferromagnetic semiconducting behavior, with implications for spintronic applications that require both magnetic ordering and good mobility. This is a combination that has been difficult to achieve by doping semiconductors with magnetic impurities. We show that phosphorus and arsenic may be effective dopants for achieving this behavior.

36 MATERIALS SCIENCE↗

Layered Antiferromagnetism Induces Large Negative Magnetoresistance in the van der Waals Semiconductor CrSBr

The recent discovery of magnetism within the family of exfoliatable van der Waals (vdW) compounds has attracted considerable interest in these materials for both fundamental research and technological applications. However, current vdW magnets are limited by their extreme sensitivity to air, low ordering temperatures, and poor charge transport properties. In this work, the magnetic and electronic properties of CrSBr are reported, an air-stable vdW antiferromagnetic semiconductor that readily cleaves perpendicular to the stacking axis. Below its Néel temperature, T N = 132 ± 1 K, CrSBr adopts an A-type antiferromagnetic structure with each individual layer ferromagnetically ordered internally and the layers coupled antiferromagnetically along the stacking direction. Scanning tunneling spectroscopy and photoluminescence (PL) reveal that the electronic gap is Δ E = 1.5 ± 0.2 eV with a corresponding PL peak centered at 1.25 ± 0.07 eV. Using magnetotransport measurements, strong coupling between magnetic order and transport properties in CrSBr is demonstrated, leading to a large negative magnetoresistance response that is unique among vdW materials. These findings establish CrSBr as a promising material platform for increasing the applicability of vdW magnets to the field of spin-based electronics.

36 MATERIALS SCIENCE↗

Nonvolatile Electric Control of the Anomalous Hall Effect in an Ultrathin Magnetic Metal

Abstract Low‐dimensional magnetism has been boosted by the recent discovery of the ferromagnetism in layered two‐dimensional (2D) semiconductors. Although the macroscopic magnetic moments of 2D ferromagnets are weak, the anomalous Hall effect (AHE) can serve as a versatile electric probe to their magnetic properties. Here, the nonvolatile electric‐field manipulation of the AHE in an ultrathin metallic ferromagnet with perpendicular magnetic anisotropy at room temperature is reported, which is achieved by the electrostatic modulation of the longitudinal resistivity via a ferroelectric substrate without varying magnetization. Therefore, this work demonstrates an electric‐field‐controlled room‐temperature memory device based on the zero‐magnetic‐field anomalous Hall resistance of an ultrathin ferromagnet. More importantly, the experimental results disentangle magnetization and anomalous Hall resistance. As a result, the study reveals a linear decrease of anomalous Hall conductivity with normal conductivity, which is distinct from previous scaling relations. Accordingly, this work manifests a universe avenue to harnessing the AHE in low‐dimensional magnetic materials.

Feng, Zexin↗