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Broadband absorption in the visible spectrum is essential in optoelectronic applications that involve power conversion such as photovoltaics and photocatalysis. Most ultrathin broadband absorbers use parasitic plasmonic structures that maximize absorption using surface plasmons and/or Fabry-Perot cavities, which limits the weight efficiency of the device. Here, we show the theoretical and experimental realization of an unpatterned/planar semiconductor thin-film absorber based on monolayer transition metal dichalcogenides (TMDCs). We experimentally demonstrate an average total absorption in the visible range (450 nm - 700 nm) of > 70% using > 4 nm of semiconductor absorbing materials scalable over large areas with vapor phase growth techniques. Our analysis suggests that a power conversion efficiency (PCE) of 15.54% and a specific power > 300 W g^-1 may be achieved in a photovoltaic cell based on this metamaterial absorber.

A method for solving elasticity problems based on separable physics-informed neural networks (SPINN) in conjunction with the deep energy method (DEM) is presented. Numerical experiments have been carried out for a number of problems showing that this method has a significantly higher convergence rate and accuracy than the vanilla physics-informed neural networks (PINN) and even SPINN based on a system of partial differential equations (PDEs). In addition, using the SPINN in the framework of DEM approach it is possible to solve problems of the linear theory of elasticity on complex geometries, which is unachievable with the help of PINNs in frames of partial differential equations. Considered problems are very close to the industrial problems in terms of geometry, loading, and material parameters.

The vast high entropy alloy (HEA) composition space is promising for discovery of new material phases with unique properties. We explore the potential to achieve rare-earth-free high magnetic anisotropy materials in single-phase HEA thin films. Thin films of FeCoNiMnCu sputtered on thermally oxidized Si/SiO$_{2}$ substrates at room temperature are magnetically soft, with a coercivity on the order of 10 Oe. After post-deposition rapid thermal annealing (RTA), the films exhibit a single face-centered-cubic phase, with an almost 40-fold increase in coercivity. Inclusion of 50 at.% Pt in the film leads to ordering of a single L1$_{0}$ high entropy intermetallic phase after RTA, along with high magnetic anisotropy and 3 orders of magnitude coercivity increase. These results demonstrate a promising HEA approach to achieve high magnetic anisotropy materials using RTA., Comment: 28 pages, including 4 figures and 6 pages of supporting information (5 SI figures and 2 SI tables)

We report the results of polarization-dependent Raman spectroscopy of phonon states in single-crystalline quasi-one-dimensional NbTe$_4$ and TaTe$_4$ van der Waals materials. The measurements were conducted in the wide temperature range from 80 K to 560 K. Our results show that although both materials have identical crystal structures and symmetries, there is a drastic difference in the intensity of their Raman spectra. While TaTe4 exhibits well-defined peaks through the examined frequency and temperature ranges, NbTe4 reveals extremely weak Raman signatures. The measured spectral positions of the phonon peaks agree with the phonon band structure calculated using the density-functional theory. We offer possible reasons for the in-tensity differences between the two van der Waals materials. Our results provide insights into the phonon properties of NbTe$_4$ and TaTe$_4$ van der Waals materials and indicate the potential of Raman spectroscopy for studying charge-density-wave quantum condensate phases., Comment: 24 pages; 6 figures; 1 table

Two-dimensional materials, such as transition metal dichalcogenides (TMDCs), have the potential to revolutionize the field of electronics and photonics due to their unique physical and structural properties. This research presents a novel method for synthesizing crystalline TMDCs crystals with < 10 nm size using ultra-fast migration of vacancies at elevated temperatures. Through in-situ and ex-situ processing and using atomic-level characterization techniques, we analyze the shape, size, crystallinity, composition, and strain distribution of these nanocrystals. These nanocrystals exhibit electronic structure signatures that differ from the 2D bulk i.e., uniform mono and multilayers. Further, our in-situ, vacuum-based synthesis technique allows observation and comparison of defect and phase evolution in these crystals formed under van der Waals heterostructure confinement versus unconfined conditions. Overall, this research demonstrates a solid-state route to synthesizing uniform nanocrystals of TMDCs and lays the foundation for materials science in confined 2D spaces under extreme conditions., Comment: MS+SI

Topological insulators (TI) and magnetic topological insulators (MTI) can apply highly efficient spin-orbit torque (SOT) and manipulate the magnetization with their unique topological surface states with ultra-high efficiency. Here, we demonstrate efficient SOT switching of a hard MTI, V-doped (Bi,Sb)2Te3 (VBST) with a large coercive field that can prevent the influence of an external magnetic field. A giant switched anomalous Hall resistance of 9.2 $k\Omega$ is realized, among the largest of all SOT systems, which makes the Hall channel a good readout and eliminates the need to fabricate complicated magnetic tunnel junction (MTJ) structures. The SOT switching current density can be reduced to $2.8\times10^5 A/cm^2$. Moreover, as the Fermi level is moved away from the Dirac point by both gate and composition tuning, VBST exhibits a transition from edge-state-mediated to surface-state-mediated transport, thus enhancing the SOT effective field to $1.56\pm 0.12 T/ (10^6 A/cm^2)$ and the interfacial charge-to-spin conversion efficiency to $3.9\pm 0.3 nm^{-1}$. The findings establish VBST as an extraordinary candidate for energy-efficient magnetic memory devices.

A method is presented that allows to reduce a problem described by differential equations with initial and boundary conditions to the problem described only by differential equations. The advantage of using the modified problem for physics-informed neural networks (PINNs) methodology is that it becomes possible to represent the loss function in the form of a single term associated with differential equations, thus eliminating the need to tune the scaling coefficients for the terms related to boundary and initial conditions. The weighted loss functions respecting causality were modified and new weighted loss functions based on generalized functions are derived. Numerical experiments have been carried out for a number of problems, demonstrating the accuracy of the proposed methods., Comment: 25 pages, 7 figures, 6 tables

Electric field control of the exchange bias effect across ferromagnet/antiferromagnet (FM/AF) interfaces has offered exciting potentials for low-energy-dissipation spintronics. In particular, the solid state magneto-ionic means is highly appealing as it may allow reconfigurable electronics by transforming the all-important FM/AF interfaces through ionic migration. In this work, we demonstrate an approach that combines the chemically induced magneto-ionic effect with the electric field driving of nitrogen in the Ta/Co$_{0.7}$Fe$_{0.3}$/MnN/Ta structure to electrically manipulate exchange bias. Upon field-cooling the heterostructure, ionic diffusion of nitrogen from MnN into the Ta layers occurs. A significant exchange bias of 618 Oe at 300 K and 1484 Oe at 10 K is observed, which can be further enhanced after a voltage conditioning by 5% and 19%, respectively. This enhancement can be reversed by voltage conditioning with an opposite polarity. Nitrogen migration within the MnN layer and into the Ta capping layer cause the enhancement in exchange bias, which is observed in polarized neutron reflectometry studies. These results demonstrate an effective nitrogen-ion based magneto-ionic manipulation of exchange bias in solid-state devices., Comment: 28 pages, 4 figures; supporting information: 17 pages, 11 figures

Ferromagnetism and superconductivity are two key ingredients to create non-Abelian quasiparticle excitations that are expected as building blocks to construct topological quantum computers. Adversely, ferromagnetism and superconductivity are typically also two hostile orderings competing to align spins in different configurations, making the material design and experimental implementation extremely challenging. Recently, iron-based superconductor Fe(Te,Se) has emerged as a connate topological superconductor (TSC), which differentiates itself from other hybrid TSCs by self-proximitizing its Dirac surface states with bulk superconductivity. So far, the efforts to search for Majorana states in this material are prevalently focused on spectroscopy techniques. In this paper, we present the global transport signature of interfacial magnetism coexisting with superconductivity. Time-reversal symmetry breaking superconducting states are confirmed through device level transport measurements for the first time in a van der Waals (vdW) Josephson junction structure. Magnetic hysteresis is observed in this device scheme, which only appears below the superconducting critical temperature, leading to potential Fulde-Ferrell (FF) superconducting pairing mechanisms. The 0-{\pi} phase mixing in the Fraunhofer patterns pinpoints the ferromagnetic state dwelling on the surface. Furthermore, a stochastic field-free superconducting diode effect also confirms the spontaneous time-reversal symmetry breaking which reflects the behavior of the ferromagnetism. Our work paves a new way to explore topological superconductivity in iron-based superconductors for future high Tc fault-tolerant qubit implementations from a device perspective., Comment: 23 pages, 5 figures

Monolayer transition metal dichalcogenide (TMDC) semiconductors exhibit strong excitonic optical resonances which serve as a microscopic, non-invasive probe into their fundamental properties. Like the hydrogen atom, such excitons can exhibit an entire Rydberg series of resonances. Excitons have been extensively studied in most TMDCs (MoS$_2$, MoSe$_2$, WS$_2$ and WSe$_2$), but detailed exploration of excitonic phenomena has been lacking in the important TMDC material molybdenum ditelluride (MoTe$_2$). Here, we report an experimental investigation of excitonic luminescence properties of monolayer MoTe$_2$ to understand the excitonic Rydberg series, up to 3s. We report significant modification of emission energies with temperature (4K to 300K), quantifying the exciton-phonon coupling. Furthermore, we observe a strongly gate-tunable exciton-trion interplay for all the Rydberg states governed mainly by free-carrier screening, Pauli blocking, and band-gap renormalization in agreement with the results of first-principles GW plus Bethe-Salpeter equation approach calculations. Our results help bring monolayer MoTe$_2$ closer to its potential applications in near-infrared optoelectronics and photonic devices., Comment: 5 figures (main text)

We report on the temperature evolution of the polarization-dependent Raman spectrum of exfoliated MoI$_3$, a van der Waals material with a "true one-dimensional" crystal structure that can be exfoliated to individual atomic chains. The temperature evolution of several Raman features reveals anomalous behavior suggesting a phase transition of a magnetic origin. Theoretical considerations indicate that MoI$_3$ is an easy-plane antiferromagnet with alternating spins along the dimerized chains and with inter-chain helical spin ordering. The calculated frequencies of the phonons and magnons are consistent with the interpretation of the experimental Raman data. The obtained results shed light on the specifics of the phononic and magnonic states in MoI$_3$ and provide a strong motivation for future study of this unique material with potential for spintronic device applications., Comment: 28 pages

Two-dimensional (2D) materials have great potential for use in future electronics due to their atomically thin nature which withstands short channel effects and thus enables better scalability. Device scaling is the process of reducing all device dimensions to achieve higher device density in a certain chip area. For 2D materials-based transistors, both the channel and contact scalability must be investigated. The channel scalability of 2D materials has been thoroughly investigated, confirming their resilience to short-channel effects. However, systematic studies on contact scalability remain rare and the current understanding of contact scaling in 2D FET is inconsistent and oversimplified. Here we combine physically scaled contacts and asymmetrical contact measurements to investigate the contact scaling behavior in 2D field-effect transistors (FETs). The asymmetrical contact measurements directly compare electron injection with different contact lengths while using the exact same channel, eliminating channel-to-channel variations. Compared to devices with long contact lengths, devices with short contact lengths (scaled contacts) exhibit larger variation, smaller drain currents at high drain-source voltages, and a higher chance of showing early saturation and negative differential resistance. Quantum transport simulations show that the transfer length of Ni-MoS2 contacts can be as short as 5 nm. Our results suggest that charge injection at the source contact is different from injection at the drain side: scaled source contacts can limit the drain current, whereas scaled drain contacts cannot. Furthermore, we clearly identified that the transfer length depends on the quality of the metal-2D interface. The asymmetrical contact measurements proposed here will enable further understanding of contact scaling behavior at various interfaces.

Layered transition metal dichalcogenides have rich phase diagram and they feature two dimensionality on numerous physical properties. Co1/3NbS2 is one of the newest members of this family where Co atoms are intercalated into the Van der Waals gaps between NbS2 layers. We study the three-dimensional electronic band structure of Co1/3NbS2 using both surface and bulk sensitive angle-resolved photoemission spectroscopy. We show that the electronic bands do not fit into the rigid-band-shift picture after the Co intercalation. Instead, Co1/3NbS2 displays a different orbital character near the Fermi level compared to the pristine NbS2 compound and has a clear band dispersion in kz direction despite its layered structure. Our photoemission study demonstrates the out-of-plane electronic correlations introduced by the Co intercalation, thus offering a new perspective on this compound. Finally, we propose how Fermi level tuning could lead to exotic phases such as spin density wave instability., Comment: Accepted by Physical Review B

The electronic properties of two-dimensional (2D) materials depend sensitively on the underlying atomic arrangement down to the monolayer level. Here we present a novel strategy for the determination of the band gap and complex dielectric function in 2D materials achieving a spatial resolution down to a few nanometers. This approach is based on machine learning techniques developed in particle physics and makes possible the automated processing and interpretation of spectral images from electron energy-loss spectroscopy (EELS). Individual spectra are classified as a function of the thickness with $K$-means clustering and then used to train a deep-learning model of the zero-loss peak background. As a proof-of-concept we assess the band gap and dielectric function of InSe flakes and polytypic WS$_2$ nanoflowers, and correlate these electrical properties with the local thickness. Our flexible approach is generalizable to other nanostructured materials and to higher-dimensional spectroscopies, and is made available as a new release of the open-source EELSfitter framework., Comment: 52 pages, 15 figures, EELSfitter code and documentation available from https://lhcfitnikhef.github.io/EELSfitter/, matches published version

Terahertz (THz) technologies have been of interest for many years due to the variety of applications including gas sensing, nonionizing imaging of biological systems, security and defense, etc. To date, scientists have used different classes of materials to perform different THz functions. However, to assemble an on-chip THz integrated system, we must understand how to integrate these different materials. Here, we explore the growth of Bi2Se3, a topological insulator (TI) material that could serve as a plasmonic waveguide in THz integrated devices, on technologically-important GaAs (001) substrates. We explore surface treatments and find that atomically smooth GaAs surface is critical to achieving high-quality Bi2Se3 films despite the relatively weak film/substrate interaction. Calculations indicate that the Bi2Se3/GaAs interface is likely selenium-terminated and shows no evidence of chemical bonding between the Bi2Se3 and the substrate. These results are a guide for integrating van der Waals materials with conventional semiconductor substrates and serve as the first steps toward achieving an on-chip THz integrated system.

Graphene nanoplatelets (GnPs) are promising candidates for gas sensing applications because they have a high surface area to volume ratio, high conductivity, and a high temperature stability. Also, they cost less to synthesize, and they are lightweight, making them even more attractive than other 2D carbon-based materials. In this paper, the surface and structural properties of pristine and functionalized GnPs, specifically with carboxyl, ammonia, carboxyl, nitrogen, oxygen, fluorocarbon, and argon, were examined with Raman spectroscopy, Fourier transform infrared spectroscopy, X-ray photoelectron spectroscopy and X-ray diffraction (XRD) to determine the functional groups present and effects of those groups on the structural and vibrational properties. We attribute certain features in the observed Raman spectra to the variations in concentration of the functionalized GnPs. XRD results show smaller crystallite sizes for functionalized GnPs samples that agree with images acquired with scanning electron microscopy. Lastly, a molecular dynamics simulation is employed to gain a better understanding of the Raman and adsorption properties of pristine GnPs.

The growth of transition metal dichalcogenide (TMDC) alloys provides an opportunity to experimentally access information elucidating how optical properties change with gradual substitutions in the lattice compared with their pure compositions. In this work, we performed growths of alloyed crystals with stoichiometric compositions between pure forms of NbSe2 and WSe2, followed by an optical analysis of those alloys by utilizing Raman spectroscopy and spectroscopic ellipsometry.

Given the importance of incorporating various superconducting materials to device fabrication or substrate development, studying the interface for possible interactions is warranted. In this work, NbN films sputter-deposited on 4H-SiC were heat-treated at 1400 C and 1870 C and were examined with transmission electron microscopy to assess whether the interfacial interactions undergo temperature-dependent behavior. We report the diffusion of NbN into the SiC substrate and the formation of NbN nanocrystallites therein during the 1400 C treatment. After the 1870 C treatment, tiered porosity and the formation of voids are observed, likely due to catalytic reactions between the two materials and accelerated by the stresses induced by the differences in the materials' coefficients of thermal expansion. Lastly, Raman spectroscopy is employed to gain an understanding of the interface lattices' optical responses.

Low power consumption in both static and dynamic modes of operation is a key requirement in modern, highly scaled nanoelectronics. Tunneling field-effect transistors (TFETs) that exploit direct band-to-band tunneling of charges and exhibit steep sub-threshold slope (SS) transfer characteristics are an attractive option in this regard. However, current generation of Si and III-V heterojunction based TFETs while suffer from low ON current density and ON/OFF current ratios for < 60 mV/dec operation. Semiconducting two-dimensional (2D) layers have recently renewed enthusiasm in novel device design for TFETs not only because of their atomically-thin bodies that favor superior electrostatic control but the same feature also favors higher ON current density and consequently high ON/OFF ratio. Here, we demonstrate gate-tunable heterojunction diodes (triodes) fabricated from InSe/Si 2D/3D van der Waals heterostructures, with a minimum subthreshold swing (SS) as low as 6.4 mV/dec and an SS average of 30 mV/dec over 4 decades of current. Further, the devices show a large current on/off ratio of approximately 10^6 and on-state current density of 0.3 uA/um at a drain bias of -1V. Our work opens new avenues for 2D semiconductors for 3D hetero-integration with Si to achieve ultra-low power logic devices., Comment: 5 figures and supporting information

Photodetectors converting light signals into detectable photocurrents are ubiquitously in use today. To improve the compactness and performance of next-generation devices and systems, low dimensional materials provide rich physics to engineering the light matter interaction. Photodetectors based on two dimensional (2D) material van der Waals heterostructures have shown high responsivity and compact integration capability, mainly in the visible range due to their intrinsic bandgap. The spectral region of near-infrared (NIR) is technologically important featuring many data communication and sensing applications. While some initial NIR 2D material-based detectors have emerged, demonstrating doping junction based 2D material photodetectors with the capability to harness the charge separation photovoltaic effect are yet outstanding. Here, we demonstrate a 2D p-n van der Waals heterojunction photodetector constructed by vertically stacking p type and n type few layer indium selenide (InSe) 2D flakes. This heterojunction charge separation based photodetector shows a three fold enhancement in responsivity at near infrared spectral region (980 nm) as compared to a photoconductor detector based on p or n only doped regions, respectively. We show, that this junction device exhibits self-powered photodetection operation and hence enables few pA-low dark currents, which is about 4 orders of magnitude more efficient than state of the art foundry based devices., Comment: 12 pages, 5 figures

In transport, the topological Hall effect (THE) presents itself as non-monotonic features (or humps and dips) in the Hall signal and is widely interpreted as a sign of chiral spin textures, like magnetic skyrmions. However, when anomalous Hall effect (AHE) is also present, the co-existence of two AHEs could give rise to similar artifacts, making it difficult to distinguish between genuine THE with AHE and two-component AHE. Here we confirm genuine THE with AHE by means of transport and magneto-optical Kerr effect (MOKE) microscopy, in which magnetic skyrmions are directly observed, and find that genuine THE occurs in the transition region of the AHE. In sharp contrast, the artifact "THE", or two-component AHE occurs well beyond the saturation of the "AHE component" (under the false assumption of THE+AHE). Furthermore, we distinguish artifact "THE" from genuine THE by three methods: 1. Minor loops, 2. Temperature dependence, 3. Gate dependence. Minor loops of genuine THE with AHE are always within the full loop, while minor loops of the artifact "THE" may reveal a single loop that cannot fit into the "AHE component". Besides, the temperature or gate dependence of the artifact "THE" may also be accompanied by a polarity change of the "AHE component", as the non-monotonic features vanish, while the temperature dependence of genuine THE with AHE reveals no such change. Our work may help future researchers to exercise cautions and use these methods to examine carefully in order to ascertain genuine THE.

Laser-assisted atom probe tomography (APT) was used to measure the indium mole fraction x of c-plane, MOCVD-grown, GaN/In(x)Ga(1-x)N/GaN test structures and the results were compared with Rutherford backscattering analysis (RBS). Four sample types were examined with (RBS determined) x = 0.030, 0.034, 0.056, and 0.112. The respective In(x)Ga(1-x)N layer thicknesses were 330 nm, 327 nm, 360 nm, and 55 nm. APT data were collected at (fixed) laser pulse energy (PE) selected within the range of (2-1000) fJ. Sample temperatures were = 54 K. PE within (2-50) fJ yielded x values that agreed with RBS (within uncertainty) and were comparatively insensitive to region-of-interest (ROI) geometry and orientation. By contrast, approximate stoichiometry was only found in the GaN portions of the samples provided PE was within (5-20) fJ and the analyses were confined to cylindrical ROIs (of diameters =20 nm) that were coaxial with the specimen tips. m-plane oriented tips were derived from c-axis grown, core-shell, GaN/In(x)Ga(1-x)N nanorod heterostructures. Compositional analysis along [0 0 0 1] (transverse to the long axis of the tip), of these m-plane samples revealed a spatial asymmetry in charge-state ratio (CSR) and a corresponding asymmetry in the resultant tip shape along this direction; no asymmetry in CSR or tip shape was observed for analysis along [-1 2-1 0]. Simulations revealed that the electric field strength at the tip apex was dominated by the presence of a p-type inversion layer, which developed under typical tip-electrode bias conditions for the n-type doping levels considered. Finally, both c-plane and m-plane sample types showed depth-dependent variations in absolute ion counts that depended upon ROI placement., Comment: 45 pages total, which includes 22 figures

Active learning - the field of machine learning (ML) dedicated to optimal experiment design, has played a part in science as far back as the 18th century when Laplace used it to guide his discovery of celestial mechanics [1]. In this work we focus a closed-loop, active learning-driven autonomous system on another major challenge, the discovery of advanced materials against the exceedingly complex synthesis-processes-structure-property landscape. We demonstrate autonomous research methodology (i.e. autonomous hypothesis definition and evaluation) that can place complex, advanced materials in reach, allowing scientists to fail smarter, learn faster, and spend less resources in their studies, while simultaneously improving trust in scientific results and machine learning tools. Additionally, this robot science enables science-over-the-network, reducing the economic impact of scientists being physically separated from their labs. We used the real-time closed-loop, autonomous system for materials exploration and optimization (CAMEO) at the synchrotron beamline to accelerate the fundamentally interconnected tasks of rapid phase mapping and property optimization, with each cycle taking seconds to minutes, resulting in the discovery of a novel epitaxial nanocomposite phase-change memory material., Comment: 30 pages and 13 figures in PDF including Methods section

Neutral and charged excitons (trions) in atomically-thin materials offer important capabilities for photonics, from ultrafast photodetectors to highly-efficient light-emitting diodes and lasers. Recent studies of van der Waals (vdW) heterostructures comprised of dissimilar monolayer materials have uncovered a wealth of optical phenomena that are predominantly governed by interlayer interactions. Here, we examine the optical properties in NbSe$_2$ - MoSe$_2$ vdW heterostructures, which provide an important model system to study metal-semiconductor interfaces, a common element in optoelectronics. Through low-temperature photoluminescence (PL) microscopy we discover a sharp emission feature, L1, that is localized at the NbSe$_2$-capped regions of MoSe$_2$. L1 is observed at energies below the commonly-studied MoSe$_2$ excitons and trions, and exhibits temperature- and power-dependent PL consistent with exciton localization in a confining potential. Remarkably, L1 is very robust not just in different samples, but also under a variety of fabrication processes. Using first-principles calculations we reveal that the confinement potential required for exciton localization naturally arises from the in-plane band bending due to the changes in the electron affinity between pristine MoSe$_2$ and NbSe$_2$ - MoSe$_2$ heterostructure. We discuss the implications of our studies for atomically-thin optoelectronics devices with atomically-sharp interfaces and tunable electronic structures., Comment: 30 pages, 5 figures, 2 tables