arXiv subjects

Angela R. Hight Walker

Publications and source records attributed to Angela R. Hight Walker.

At least 37 records · Page 2Linked to original sources

arXiv2022

Nonconventional Quantized Hall Resistances Obtained with $ν= 2$ Equilibration in Epitaxial Graphene $p-n$ Junctions

We have demonstrated the millimeter-scale fabrication of monolayer epitaxial graphene $p-n$ junction devices using simple ultraviolet photolithography, thereby significantly reducing device processing time compared to that of electron beam lithography typically used for obtaining sharp junctions. This work presents measurements yielding nonconventional, fractional multiples of the typical quantized Hall resistance at $ν=2$ ($R_H\approx 12906 Ω$) that take the form: $\frac{a}{b}R_H$. Here, $a$ and $b$ have been observed to take on values such 1, 2, 3, and 5 to form various coefficients of $R_H$. Additionally, we provide a framework for exploring future device configurations using the LTspice circuit simulator as a guide to understand the abundance of available fractions one may be able to measure. These results support the potential for drastically simplifying device processing time and may be used for many other two-dimensional materials.

cond-mat.mes-hall↗

arXiv2022

Review of Theoretical and Computational Methods for 2D Materials Exhibiting Charge Density Waves

Two-dimensional (2D) materials that exhibit charge density waves (CDWs) have generated many research endeavors in the hopes of employing their exotic properties for various quantum-based technologies. Early investigations surrounding CDWs were mostly focused on bulk materials. However, applications for quantum devices have since required devices to be constructed from few-layer material to fully utilize the material's properties. This field has greatly expanded over the decades, warranting a focus on the computational efforts surrounding CDWs in 2D materials. In this review, we will cover ground in the following relevant, theory-driven subtopics for TaS2 and TaSe2: summary of general computational techniques and methods, atomic structures, Raman modes, and effects of confinement and dimensionality. Through understanding how the computational methods have enabled incredible advancements in quantum materials, one may anticipate the ever-expanding directions available for continued pursuit as the field brings us through the 21st century.

cond-mat.mtrl-sci↗

arXiv2021

Analysis of Raman and Ellipsometric Responses of Nb$_{x}$W$_{1-x}$Se$_{2}$ alloys

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.

cond-mat.mtrl-sci↗

arXiv2021

Bonding characteristics of the interfacial buffer layer in epitaxial graphene via density functional theory

Monolayer epitaxial graphene is an appropriate candidate for a wide variety of electronic and optical applications. One advantage of growing graphene on the Si face of SiC is that it develops as a single crystal, as does the layer underneath, commonly referred to as the interfacial buffer layer. The properties of this supporting layer include a band gap, making it of interest to groups seeking to build devices with on-off capabilities. In this work, using density functional theory, we have calculated the bonding characteristics of the buffer layer to the SiC substrate beneath. These calculations were used to determine a periodic length between the covalent bonds acting as anchor points in this interface. Additionally, it is evident that the formation of these anchor points depends on the lattice mismatch between the graphene layer and SiC.

cond-mat.mtrl-sci↗

arXiv2021

Influence of Dimensionality on the Charge Density Wave Phase of 2H-TaSe$_{2}$

Metallic transition metal dichalcogenides like tantalum diselenide (TaSe$_{2}$) exhibit exciting behaviors at low temperatures, including the emergence of charge density wave (CDW) states. In this work, density functional theory (DFT) is used to investigate how structural, electronic, and Raman spectral properties of the CDW configuration change as a function of thickness. Such findings highlight the influence of dimensionality change (from 2D to 3D) and van der Waals (vdW) interactions on the system properties. The vdW effect is most strongly present in bulk TaSe$_{2}$ in the spectral range 165 cm$^{-1}$ to 215 cm$^{-1}$. The phonons seen in the experimental Raman spectra are compared with the results calculated from the DFT models as a function of temperature and layer number. The matching of data and calculations substantiates the model's description of the CDW structural formation as a function of thickness, which is shown in depth for 1L through 6L systems. These results highlight the importance of understanding interlayer interactions, which are pervasive in many quantum phenomena involving two-dimensional confinement.

cond-mat.mtrl-sci↗

arXiv2021

The Joint Automated Repository for Various Integrated Simulations (JARVIS) for data-driven materials design

The Joint Automated Repository for Various Integrated Simulations (JARVIS) is an integrated infrastructure to accelerate materials discovery and design using density functional theory (DFT), classical force-fields (FF), and machine learning (ML) techniques. JARVIS is motivated by the Materials Genome Initiative (MGI) principles of developing open-access databases and tools to reduce the cost and development time of materials discovery, optimization, and deployment. The major features of JARVIS are: JARVIS-DFT, JARVIS-FF, JARVIS-ML, and JARVIS-Tools. To date, JARVIS consists of 40,000 materials and 1 million calculated properties in JARVIS-DFT, 1,500 materials and 110 force-fields in JARVIS-FF, and 25 ML models for material-property predictions in JARVIS-ML, all of which are continuously expanding. JARVIS-Tools provides scripts and workflows for running and analyzing various simulations. We compare our computational data to experiments or high-fidelity computational methods wherever applicable to evaluate error/uncertainty in predictions. In addition to the existing workflows, the infrastructure can support a wide variety of other technologically important applications as part of the data-driven materials design paradigm. The JARVIS datasets and tools are publicly available at the website: https://jarvis.nist.gov .

cond-mat.mtrl-sci↗

arXiv2020

Examining Experimental Raman Mode Behavior in Mono- and Bi-layer 2H-TaSe$_{2}$ via Density Functional Theory

Tantalum diselenide (TaSe$_{2}$) is a metallic transition metal dichalcogenide whose equilibrium structure and vibrational behavior strongly depends on temperature and thickness, including the emergence of charge density wave (CDW) states at very low T. In this work, observed modes for mono- and bi-layer are described across several spectral regions and com-pared to the bulk ones. Such modes, including an experimentally observed forbidden Raman mode and low frequency CDW modes, are then matched to corresponding density functional theory (DFT) predicted vibrations, to unveil their inner working. The excellent match between experimental and computational results justifies the presented vibrational visualizations of these modes. Additional support is provided by experimental phonons seen in Raman spectra as a function of temperature and thickness. These results highlight the importance of understanding interlayer interactions and their effects on mode behaviors.

cond-mat.mtrl-sci↗

arXiv2020

Distinct magneto-Raman signatures of spin-flip phase transitions in CrI3

The discovery of 2-dimensional (2D) materials, such as CrI3, that retain magnetic ordering at monolayer thickness has resulted in a surge of research in 2D magnetism from both pure and applied perspectives. Here, we report a magneto-Raman spectroscopy study on multilayered CrI3, focusing on two new features in the spectra which appear at temperatures below the magnetic ordering temperature and were previously assigned to high frequency magnons. We observe a striking evolution of the Raman spectra with increasing magnetic field in which clear, sudden changes in intensities of the modes are attributed to the interlayer ordering changing from antiferromagnetic to ferromagnetic at a critical magnetic field. Our work highlights the sensitivity of the Raman modes to weak interlayer spin ordering in CrI3. In addition, we theoretically examine potential origins for the new modes, which we deduce are unlikely single magnons.

cond-mat.mes-hall↗

arXiv2020

High-throughput Density Functional Perturbation Theory and Machine Learning Predictions of Infrared, Piezoelectric and Dielectric Responses

Many technological applications depend on the response of materials to electric fields, but available databases of such responses are limited. Here, we explore the infrared, piezoelectric and dielectric properties of inorganic materials by combining high-throughput density functional perturbation theory and machine learning approaches. We compute Γ-point phonons, infrared intensities, Born-effective charges, piezoelectric, and dielectric tensors for 5015 non-metallic materials in the JARVIS-DFT database. We find 3230 and 1943 materials with at least one far and mid-infrared mode, respectively. We identify 577 high-piezoelectric materials, using a threshold of 0.5 C/m2. Using a threshold of 20, we find 593 potential high-dielectric materials. Importantly, we analyze the chemistry, symmetry, dimensionality, and geometry of the materials to find features that help explain variations in our datasets. Finally, we develop high-accuracy regression models for the highest infrared frequency and maximum Born-effective charges, and classification models for maximum piezoelectric and average dielectric tensors to accelerate discovery.

cond-mat.mtrl-sci↗

arXiv2019

Quasi-Two-Dimensional Magnon Identification in Antiferromagnetic FePS3 via Magneto-Raman Spectroscopy

Recently it was discovered that van der Waals-bonded magnetic materials retain long range magnetic ordering down to a single layer, opening many avenues in fundamental physics and potential applications of these fascinating materials. One such material is FePS3, a large spin (S=2) Mott insulator where the Fe atoms form a honeycomb lattice. In the bulk, FePS3 has been shown to be a quasi-two-dimensional-Ising antiferromagnet, with additional features in the Raman spectra emerging below the Neel temperature of approximately 120 K. Using magneto-Raman spectroscopy as an optical probe of magnetic structure, we show that one of these Raman-active modes in the magnetically ordered state is actually a magnon with a frequency of of approximately 3.7 THz (122 cm-1). Contrary to previous work, which interpreted this feature as a phonon, our Raman data shows the expected frequency shifting and splitting of the magnon as a function of temperature and magnetic field, respectively, where we determine the g-factor to be approximately 2. In addition, the symmetry behavior of the magnon is studied by polarization-dependent Raman spectroscopy and explained using the magnetic point group of FePS3.

cond-mat.mtrl-sci↗

arXiv2019

Global alignment of solution-based single-wall carbon nanotube films via machine-vision controlled filtration

Over the past decade, substantial progress has been made in the chemical processing (chiral enrichment, length sorting, handedness selectivity, and filling substance) of single-wall carbon nanotubes (SWCNTs). Recently, it was shown that large, horizontally-aligned films can be created out of post-processed SWCNT solutions. Here, we use machine-vision automation and parallelization to simultaneously produce globally-aligned SWCNT films using pressure-driven filtration. Feedback control enables filtration to occur with a constant flow rate that not only improves the nematic ordering of the SWCNT films, but also provides the ability to align a wide range of SWCNT types and on a variety of nanoporous membranes using the same filtration parameters. Using polarized optical spectroscopic techniques, we show that meniscus combing produces a two-dimensional radial SWCNT alignment on one side of the film. After we flatten the meniscus through silanation, spatially-resolved nematicity maps on both sides of the SWCNT film reveal global alignment across the entire structure. From experiments changing ionic strength and membrane tribocharging, we provide evidence that the SWCNT alignment mechanism stems from an interplay of intertube interactions and ordered membrane charging. This work opens up the possibility of creating globally-aligned SWCNT film structures for a new-generation of nanotube electronics and optical control elements.

cond-mat.mes-hall↗

arXiv2018

Strain Controlled Magnetic and Optical Properties of Monolayer 2H-TaSe$_2$

First-principles calculations are used to probe the effects of mechanical strain on the magnetic and optical properties of monolayer (ML) 2H-TaSe$_2$. A complex dependence of these physical properties on strain results in unexpected behavior, such as ferromagnetism under uniaxial, in-plane, tensile strain and a lifting of the Raman-active E' phonon degeneracy. While ferromagnetism is observed under compression along x-axis and expansion along y-axis, no magnetic order occurs when interchanging the strain direction. The calculations show that the magnetic behavior of the system depends on the exchange within the 5d orbitals of the Ta atoms. The magnetic moment per Ta atom persists even when an additional compressive strain along the z-axis is added to a biaxially-strained ML, which suggests stability of the magnetic order. Exploring the effects of this mechanical strain on the Raman-active phonon modes, we find that the E$^"$ and E' modes are red-shifted due to Ta-Se bond elongation, and that strain lifts the E' mode degeneracy, except for the symmetrical biaxial tensile case. Our results demonstrate the possibility of tuning the properties of 2D-materials for nanoelectronic applications through strain.

cond-mat.mtrl-sci↗

arXiv2018

High-throughput assessment of vacancy formation and surface energies of materials using classical force-fields

In this work, we present an open access database for surface and vacancy-formation energies using classical force-fields (FFs). These quantities are essential in understanding diffusion behavior, nanoparticle formation and catalytic activities. FFs are often designed for a specific application, hence, this database allows the user to understand whether a FF is suitable for investigating particular defect and surface-related material properties. The FF results are compared to density functional theory and experimental data whenever applicable for validation. At present, we have 17,506 surface energies and 1,000 vacancy formation energies calculation in our database and the database is still growing. All the data generated, and the computational tools used, are shared publicly at the following websites https://www.ctcms.nist.gov/~knc6/periodic.html, https://jarvis.nist.gov and https://github.com/usnistgov/jarvis . Approximations used during the high-throughput calculations are clearly mentioned. Using some of the example cases, we show how our data can be used to directly compare different FFs for a material and to interpret experimental findings such as using Wulff construction for predicting equilibrium shape of nanoparticles. Similarly, the vacancy formation energies data can be useful in understanding diffusion related properties.

cond-mat.mtrl-sci↗

arXiv2018

Phase Modulators Based on High Mobility Ambipolar ReSe2 Field-Effect Transistors

We fabricated ambipolar field-effect transistors (FETs) from multi-layered triclinic ReSe2, mechanically exfoliated onto a SiO2 layer grown on p-doped Si. In contrast to previous reports on thin layers (~2 to 3 layers), we extract field-effect carrier mobilities in excess of 10^2 cm^2/Vs at room temperature in crystals with nearly ~10 atomic layers. These thicker FETs also show nearly zero threshold gate voltage for conduction and high ON to OFF current ratios when compared to the FETs built from thinner layers. We also demonstrate that it is possible to utilize this ambipolarity to fabricate logical elements or digital synthesizers. For instance, we demonstrate that one can produce simple, gate-voltage tunable phase modulators with the ability to shift the phase of the input signal by either 90^o or nearly 180^o. Given that it is possible to engineer these same elements with improved architectures, for example on h-BN in order to decrease the threshold gate voltage and increase the carrier mobilities, it is possible to improve their characteristics in order to engineer ultra-thin layered logic elements based on ReSe2.

cond-mat.mes-hall↗

arXiv2018

Confocal laser scanning microscopy: A tool for rapid optical characterization of 2D materials

Confocal laser scanning microscopy (CLSM) is a non-destructive, highly-efficient optical characterization method for large-area analysis of graphene on different substrates, which can be applied in ambient air, does not require additional sample preparation, and is insusceptible to surface charging and surface contamination. CLSM leverages optical properties of graphene and provides greatly enhanced optical contrast and mapping of thickness down to a single layer. We demonstrate the effectiveness of CLSM by measuring mechanically exfoliated and chemical vapor deposition graphene on Si/SiO2, and epitaxial graphene on SiC. In the case of graphene on Si/SiO2, both CLSM intensity and height mapping is powerful for analysis of 1-5 layers of graphene. For epitaxial graphene on SiC substrates, the CLSM intensity allows us to distinguish features such as dense, parallel 150 nm wide ribbons of graphene (associated with the early stages of the growth process) and large regions covered by the interfacial layer and 1-3 layers of graphene. In both cases, CLSM data shows excellent correlation with conventional optical microscopy, atomic force microscopy, Kelvin probe force microscopy, conductive atomic force microscopy, scanning electron microscopy and Raman mapping, with a greatly reduced acquisition time. We demonstrate that CLSM is an indispensable tool for rapid analysis of mass-produced graphene and is equally relevant to other 2D materials.

physics.app-ph↗

arXiv2017

Rapid characterization of wafer-scale 2D material: Epitaxial graphene and graphene nanoribbons on SiC

We demonstrate that the confocal laser scanning microscopy (CLSM) provides a non-destructive, highly-efficient characterization method for large-area epitaxial graphene and graphene nanostructures on SiC substrates, which can be applied in ambient air without sample preparation and is insusceptible to surface charging or surface contamination. Based on the variation of reflected intensity from regions covered by interfacial layer, single layer, bilayer, or few layer graphene, and through the correlation to the results from Raman spectroscopy and SPM, CLSM images with a high resolution (around 150 nm) reveal that the intensity contrast has distinct feature for undergrown graphene (mixing of dense, parallel graphene nanoribbons and interfacial layer), continuous graphene, and overgrown graphene. Moreover, CLSM has a real acquisition time hundreds of times faster per unit area than the supplementary characterization methods. We believe that the confocal laser scanning microscope will be an indispensable tool for mass-produced epitaxial graphene or applicable 2D materials.

physics.app-ph↗

arXiv2016

Epitaxial graphene homogeneity and quantum Hall effect in millimeter-scale devices

Quantized magnetotransport is observed in 5.6 x 5.6 mm^2 epitaxial graphene devices, grown using highly constrained sublimation on the Si-face of SiC(0001) at high temperature (1900 °C). The precise quantized Hall resistance of Rxy = h/2e^2 is maintained up to record level of critical current Ixx = 0.72 mA at T = 3.1 K and 9 T in a device where Raman microscopy reveals low and homogeneous strain. Adsorption-induced molecular doping in a second device reduced the carrier concentration close to the Dirac point(n ~ 1E10 (1/cm^2)), where mobility of 43700 cm^2/Vs is measured over an area of 10 mm^2. Atomic force, confocal optical, and Raman microscopies are used to characterize the large-scale devices, and reveal improved SiC terrace topography and the structure of the graphene layer. Our results show that the structural uniformity of epitaxial graphene produced by face-to-graphite processing contributes to millimeter-scale transport homogeneity, and will prove useful for scientific and commercial applications.

cond-mat.mtrl-sci↗

arXiv2015

Metal to insulator quantum-phase transition in few-layered ReS$_2$

In ReS$_2$ a layer-independent direct band-gap of 1.5 eV implies a potential for its use in optoelectronic applications. ReS$_2$ crystallizes in the 1T$^{\prime}$-structure which leads to anisotropic physical properties and whose concomitant electronic structure might host a non-trivial topology. Here, we report an overall evaluation of the anisotropic Raman response and the transport properties of few-layered ReS$_2$ field-effect transistors. We find that ReS$_2$ exfoliated on SiO$_2$ behaves as an $n$-type semiconductor with an intrinsic carrier mobility surpassing $μ_i$ ~30 cm$^2$/Vs at $T = 300$ K which increases up to ~350 cm$^2$/Vs at 2 K. Semiconducting behavior is observed at low electron densities $n$, but at high values of n the resistivity decreases by a factor > 7 upon cooling to 2 K and displays a metallic $T^2$-dependence. This indicates that the band structure of 1T$^{\prime}$-ReS$_2$ is quite susceptible to an electric field applied perpendicularly to the layers. The electric-field induced metallic state observed in transition metal dichalcogenides was recently claimed to result from a percolation type of transition. Instead, through a scaling analysis of the conductivity as a function of $T$ and $n$, we find that the metallic state of ReS$_2$ results from a second-order metal to insulator transition driven by electronic correlations. This gate-induced metallic state offers an alternative to phase engineering for producing ohmic contacts and metallic interconnects in devices based on transition metal dichalcogenides.

cond-mat.mes-hall↗