Engineering Papers⌕ Search

SEARCH · Engineering Papers

Results for “layered materials”

Search indexed NASA NTRS and DOE OSTI research on propulsion, heat transfer, battery materials and energy systems. Follow report and document links to the original sources.

Quote a phrase for an exact phrase match. Source license links do not imply unrestricted reuse.

At least 397 records · Page 22
All sourcesNASA NTRSDOE OSTI
DOE OSTI2022

Low-dimensional physics of clay particle size distribution and layer ordering

Abstract Clays are known for their small particle sizes and complex layer stacking. We show here that the limited dimension of clay particles arises from the lack of long-range order in low-dimensional systems. Because of its weak interlayer interaction, a clay mineral can be treated as two separate low-dimensional systems: a 2D system for individual phyllosilicate layers and a quasi-1D system for layer stacking. The layer stacking or ordering in an interstratified clay can be described by a 1D Ising model while the limited extension of individual phyllosilicate layers can be related to a 2D Berezinskii–Kosterlitz–Thouless transition. This treatment allows for a systematic prediction of clay particle size distributions and layer stacking as controlled by the physical and chemical conditions for mineral growth and transformation. Clay minerals provide a useful model system for studying a transition from a 1D to 3D system in crystal growth and for a nanoscale structural manipulation of a general type of layered materials.

42 ENGINEERING↗
DOE OSTI2025

Intercalated chalcogenides Fe 1/4 TaS 2 and Fe 1/3 TaS 2 under extreme pressure—temperature conditions

Intercalation is an important strategy for enhancing functionality in complex chalcogenides. This is because layered materials can be endowed with intriguing properties by filling the van der Waals gap with various ions and molecules, which, in addition to their unique chemistry, break symmetry in new ways. In order to explore the properties of intercalated metal dichalcogenides under extreme pressure-temperature conditions, we combine diamond anvil cell techniques, Raman scattering spectroscopy, magnetic susceptibility, and first-principles calculations to reveal the pressure–temperature phase diagram of Fe 1/3 TaS 2 . This system hosts a compression-driven structural phase transition to a polar state as well as remnant charge density wave signatures deriving from the host lamella of the 2H-parent compound. We also explore the role of different A-site patterns and determine that, by comparison, Fe 1/4 TaS 2 is soft and flexible due to the lower metal density inside the van der Waals gap. These findings open the door to entirely new states of matter with exciting property combinations, including metallicity, polarity, chirality, and altermagnetism – depending upon the conditions – that can support a wide range of spintronics and phononics applications.

Materials science↗
DOE OSTI2020

Na ion dynamics in P2-Na x [Ni 1/3 Ti 2/3 ]O 2 : a combination of quasi-elastic neutron scattering and first-principles molecular dynamics study

In this work, the P2-type layered material Na 2/3 [Ni 1/3 Ti 2/3 ]O 2 was studied as a promising bi-functional electrode material for sodium-ion batteries. To assess the electrochemical performance of this material, we investigated the diffusion mechanism as well as ionic and electronic conductivity with a combination of experimental and computational techniques. The quasi-elastic neutron scattering (QENS) experiments and first-principles molecular dynamics (FPMD) simulations were performed to identify the diffusion mechanism. The QENS data showed that Na ion diffusion can be well described by the Singwi–Sjölander jump diffusion model, where the obtained mean jump length matched the distances between the neighboring edge-share and face-share Na sites. FPMD predicted diffusivity values similar to those from QENS. The computed composition dependence of ionic and electronic conductivity of Na x [Ni 1/3 Ti 2/3 ]O 2 suggested that electronic conductivity changes significantly when x deviates from 2/3 as the redox couple of Ni and Ti is activated, while the change of ionic conductivity with x is relatively small.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Thermal hysteresis controlled reconfigurable MoS 2 nanomechanical resonators

Two-dimensional (2D) structures from layered materials have enabled a number of novel devices including resonant nanoelectromechanical systems (NEMS). 2D NEMS resonators are highly responsive to strain, allowing their resonance frequencies to be efficiently tuned over broad ranges, which is a feature difficult to attain in conventional micromachined resonators. In electrically configured and tuned devices, high external voltages are typically required to set and maintain different frequencies, limiting their applications. Here we experimentally demonstrate molybdenum disulfide (MoS 2 ) nanomechanical resonators that can be reconfigured between different frequency bands with zero maintaining voltage in a non-volatile fashion. By leveraging the thermal hysteresis in these 2D resonators, we use heating and cooling pulses to reconfigure the device frequency, with no external voltage required to maintain each frequency. Here, we further show that the frequency spacing between the bands can be tuned by the thermal pulse strength, offering full control over the programmable operation. Such reconfigurable MoS 2 resonators may provide an alternative pathway toward small-form-factor and low-power tunable devices in future reconfigurable radio-frequency circuits with multi-band capability.

42 ENGINEERING↗
DOE OSTI2024

Predictions of delafossite-hosted honeycomb and kagome phases

Delafossites, typically denoted by the formula ABO 2 , are a class of layered materials that exhibit a wide range of electronic and optical properties. Recently, the idea of modifying these delafossites into ordered kagome or honeycomb phases via strategic doping has emerged as a potential way to tailor these properties. In this study, we use high-throughput density functional theory calculations to explore many possible candidate kagome and honeycomb phases by considering dopants selected from the parent compounds of known ternary delafossite oxides from the inorganic crystal structure database. Here our results indicate that while A-site in existing delafossites can host a limited range of elemental specifies, and display a low propensity for mixing or ordering, the oxide sub-units in the BO 2 much more readily admit guest species. Our study identifies four candidate B-site kagome and fifteen candidate B-site honeycombs with a formation energy more than 50 meV f.u. −1 below other competing phases. The ability to predict and control the formation of these unique structures offers exciting opportunities in materials design, where innovative properties can be engineered through the selection of specific dopants. A number of these constitute novel correlated metals, which may be of interest for subsequent efforts in synthesis. These novel correlated metals may have significant implications for quantum computing, spintronics, and high-temperature superconductivity, thus inspiring future experimental synthesis and characterization of these proposed materials.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2020

Anisotropic band structure of TiS 3 nanoribbon revealed by polarized photocurrent spectroscopy

A re-discovered member of the layered material family, Titanium Trisulfide (TiS 3 ), has attracted intense research interest recently for the possibility of realizing an exciton insulator in the monolayer limit. However, due to their quasi-one-dimensional nature, thin TiS 3 flakes are typically in the form of nanoribbons that are challenging to characterize by optical absorption spectra, due to their small cross section. Here, we employ a sensitive photocurrent spectroscopy technique to probe the absorption of a thin TiS 3 nanoribbon in a field-effect transistor configuration. We have found a significant modification of the band structure of the thin TiS 3 nanoribbon, compared to its bulk counterpart. In addition, the polarization-dependent photocurrent spectra of thin TiS 3 nanoribbons exhibit greatly enhanced anisotropy compared to that of a thick TiS 3 device. The atomically thin TiS 3 flake, thus, not only provides an exciting platform for investigating many-body physics but also enables anisotropic quantum optoelectronics.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2022

Charge density wave activated excitons in TiSe 2 –MoSe 2 heterostructures

Layered materials enable the assembly of a new class of heterostructures where lattice-matching is no longer a requirement. Interfaces in these heterostructures therefore become a fertile ground for unexplored physics as dissimilar phenomena can be coupled via proximity effects. In this article, we identify an unexpected photoluminescence (PL) peak when MoSe 2 interacts with TiSe 2 . A series of temperature-dependent and spatially resolved PL measurements reveal that this peak is unique to the TiSe 2 –MoSe 2 interface, is higher in energy compared to the neutral exciton, and exhibits exciton-like characteristics. The feature disappears at the TiSe 2 charge density wave transition, suggesting that the density wave plays an important role in the formation of this new exciton. We present several plausible scenarios regarding the origin of this peak that individually capture some aspects of our observations but cannot fully explain this feature. These results therefore represent a fresh challenge for the theoretical community and provide a fascinating way to engineer excitons through interactions with charge density waves.

36 MATERIALS SCIENCE↗
DOE OSTI2023

Multimodal microscopy of extended defects in β-Ga 2 O 3 (010) EFG crystals

Beta-phase gallium oxide (β-Ga 2 O 3 ) has attracted attention in recent years as a potentially low cost, large area substrate and active layer material for high power, high temperature power electronics and sensing devices. However, growth of β-Ga 2 O 3 crystals is complicated by easily activated (100) and (001) cleavage planes, the presence of low angle grain boundaries (LAGBs) and twins, and the potential formation of polycrystalline grains. In this study, β-Ga 2 O 3 crystals were grown by the edge-defined film-fed growth technique with an (010) principal face. Two crystals with apparently randomly formed high angle grain boundaries (HAGBs) were selected and analyzed by electron backscatter diffraction, electron channeling contrast imaging, and cathodoluminescence to investigate the nature of the LAGBs and the source of the HAGB formation. It was discovered that planar LAGBs lying parallel to the (010) plane exist in the region immediately preceding the start of an HAGB. Increased misorientation across the LAGB was observed, approaching the initiation of a new grain. We present multimodal microscopy characterization, correlating misorientation and variation in optoelectronic properties with LAGBs and the associated dislocations.

14 SOLAR ENERGY↗
DOE OSTI2022

Direct visualization of polaron formation in the thermoelectric SnSe

SnSe is a layered material that currently holds the record for bulk thermoelectric efficiency. The primary determinant of this high efficiency is thought to be the anomalously low thermal conductivity resulting from strong anharmonic coupling within the phonon system. Here we show that the nature of the carrier system in SnSe is also determined by strong coupling to phonons by directly visualizing polaron formation in the material. We employ ultrafast electron diffraction and diffuse scattering to track the response of phonons in both momentum and time to the photodoping of free carriers across the bandgap, observing the bimodal and anisotropic lattice distortions that drive carrier localization. Relatively large (18.7 Å), quasi-one-dimensional (1D) polarons are formed on the 300-fs timescale with smaller (4.2 Å) 3D polarons taking an order of magnitude longer (4 ps) to form. This difference appears to be a consequence of the profoundly anisotropic electron–phonon coupling in SnSe, with strong Fröhlich coupling only to zone-center polar optical phonons. These results demonstrate a high density of polarons in SnSe at optimal doping levels. Strong electron-phonon coupling is critical to the thermoelectric performance of this benchmark material and, potentially, high performance thermoelectrics more generally.

36 MATERIALS SCIENCE↗
DOE OSTI2022

Bibliometric review and recent advances in total scattering pair distribution function analysis: 21 years in retrospect

Global research activities have been driven by the quest to develop and characterize novel materials for technological advancements. The total scattering pair distribution function (TSPDF) is a powerful and versatile characterization technique for examining the structural details of diverse complex materials including liquid, amorphous, disordered crystalline, and nanostructured materials. Thus, it is critical to keep track of research progress, identify research gaps, and future research directions of the application of the TSPDF technique in materials development and discovery. In this work, a bibliometric analysis of literature regarding the TSPDF technique between 2000 and 2021 was conducted using datasets retrieved from the Web of Science database. The research trends based on publication outputs, research subject distribution, co-authorships among institutions, countries/regions, co-citation of referenced sources, and keyword co-occurrence are evaluated and discussed herein. The impact of the TSPDF technique is projected to increase due to its importance in probing emerging functional materials, and the advances in specialized facilities and instrumentation among the scientific communities engaged with it. Finally, current and emerging research hotspots related to TSPDF technique such as catalysis, computer modeling and simulation, pharmaceutics, machine learning, hydrogen storage, battery materials, and layered structured materials are also identified and discussed.

36 MATERIALS SCIENCE↗
DOE OSTI2022

Emergence of ferrimagnetism in Li-intercalated NiPS 3

AbstractIntercalation has become a powerful approach to tune the intrinsic properties and introduce novel phenomena in layered materials. Intercalating van der Waals (vdW) magnetic materials is a promising route to engineer the low-dimensional magnetism. Recently, metal thiophosphates, MPX 3 , has been widely studied because their magnetic orders are highly tunable and persist down to the two-dimensional limit. In this work, we used electrochemical technique to intercalate Li into NiPS 3 single crystals and found the emergence of ferrimagnetism at low temperature in Li-intercalated NiPS 3 . Such tuning of magnetic properties highlights the effectiveness of intercalation, providing a novel strategy to manipulate the magnetism in vdW magnets.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2025

Dome-like pressure-temperature phase diagram of the cooperative Jahn–Teller distortion in NaNiO 2

NaNiO 2 is a Ni 3+ -containing layered material consisting of alternating triangular networks of Ni and Na cations, separated by octahedrally-coordinated O anions. At ambient pressure, it features a collinear Jahn–Teller distortion below $T^{JT}_{onset} ≈ 480$ K, which disappears in a first-order transition on heating to $T^{JT}_{onset} ≈ 500$ K, corresponding to the increase in symmetry from monoclinic to rhombohedral. It was previously studied by variable-pressure neutron diffraction (Nagle-Cocco et al 2022 ACS Inorg. Chem. 61 4312) and found to exhibit an increasing $T^{JT}_{onset}$ with pressure up to ∼5 GPa. In this work, powdered NaNiO 2 was studied via variable-pressure synchrotron x-ray diffraction up to pressures of ∼67 GPa at 294 K and 403 K. Suppression of the collinear Jahn–Teller ordering is observed via the emergence of a high-symmetry rhombohedral phase, with the onset pressure occurring at ∼18 GPa at both studied temperatures. Further, a discontinuous decrease in unit cell volume is observed on transitioning from the monoclinic to the rhombohedral phase. These results taken together suggest that in the vicinity of the transition, application of pressure causes the Jahn–Teller transition temperature, $T^{JT}_{onset}$, to decrease rapidly. We conclude that the pressure-temperature phase diagram of the cooperative Jahn–Teller distortion in NaNiO 2 is dome-like.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2023

The effectiveness of D 2 pellet injection in reducing intra-ELM and inter-ELM tungsten divertor erosion rates in DIII-D during the Metal Rings Campaign

Abstract Edge localized modes (ELMs) in H-mode plasmas erode plasma-facing components (PFCs) and lead to impurities in the core, reducing confinement. This study analyzes D 2 pellet injection on the DIII-D fusion experiment used as an ELM mitigation technique applied during the 2016 tungsten Metal Rings Campaign to reduce W erosion during ELMs. The 400.9 nm photon wavelength line emission intensity of tungsten atoms (WI) filterscope channels and Langmuir probes were used to infer the gross erosion rate of tungsten-coated tiles installed in the divertor of DIII-D. D 2 mass injection rates ranging from 34 to 41 arbitrary units (A.U.) and no D 2 injection resulted in a similar total W erosion rate during ELMs (intra-ELM). On average, results show a 29% increase in the total gross W erosion rate with intermediate mass injection rates (∼13–23 A.U.) compared to the no pellets and the highest injection rate cases. On average, the fast D 2 mass injection rate cases had 15% less erosion in the inter-ELM phase than the case with no pellets. Generally, higher D 2 mass injection rates increased the ELM frequency, and the highest injection rates reduced the average erosion per ELM and fractional carbon impurities at the top of the pedestal by nearly 40% when compared to the no-pellet case. As expected, a higher D 2 pellet injection rate led to a higher plasma density and lower plasma temperature in the divertor. Additionally, an increasing divertor inter-ELM plasma electron density directly correlated to more frequent pellet injection and a decrease in both the average gross intra-ELM W erosion and the total gross intra-ELM W erosion rate. Simulations of intra-ELM erosion using the ‘free-streaming plus recycling model’ (FSRM) underestimate W erosion during pellet injection by about 30% on average. The discrepancies between the experimental measurements and the FSRM intra-ELM W erosion predictions are postulated to be due to C/W material mixing. A simple analytic mixed-material model is presented and results in better agreement with the experimental data. These results highlight the importance of incorporating the effects of a mixed-material layer in the analysis of PFC erosion.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2022

Etched Silicon Planar CRL Optics for the High-Energy X-ray Diffraction Beamlines 11-ID-B and 11-ID-C at the APS

We report the focusing of high-energy X-rays is most commonly achieved by commercially available compound refractive lenses (CRL), which are added together in larger structures. There is a need for high-energy X-ray beamlines to enable focusing in only one dimension down to a few micrometers to study layered materials and thin films. High-energy X-rays above 50 keV require often 100 lenses or more, therefore it is more efficient to etch the complete arrays of lenses into a monolithic substrate like a silicon wafer. Custom lens arrays were fabricated for the high-energy x-ray beamlines 11-ID-B, and 11-ID-C at the Argonne National Laboratory. The fabrication required tuning parameters of the Bosch process to optimize the etching of deep vertical sidewalls at a reasonable speed without overheating. The beamline 11-ID-B is equipped with lens arrays of 85-110 lenses for 59 keV and 190-250 lenses for 87 keV photon energy, focusing the beam vertically below 5.0 µm at the sample positions between 1600 mm to 2100 mm. 11-ID-C has received arrays of 435 lenses that focus 106 keV X-rays to a vertical height of 2.0 µm at the sample position. In both cases, the flux density gain in the focal spot is larger than a factor of 20, relative to using slits to cut the beam size. The lens setup is permanently installed and can be moved in and out of the beam during the experiment without further alignment. The lenses have enabled operando diffraction studies on interfaces in batteries and the development of pair distribution function (PDF) analysis using grazing incidence geometry.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗
DOE OSTI2026

Pairing around a single Dirac point: A unifying view of Kohn-Luttinger superconductivity in Chern bands, quarter metals, and topological surface states

Superconductivity of a single two-dimensional Dirac fermion offers a natural route to topological superconductivity. While usually considered extrinsic—arising from proximity to a conventional superconductor—we investigate when a doped Dirac cone can develop superconductivity from a short-range repulsive interaction 𝑈 via the Kohn–Luttinger mechanism. We show that an ideal, linear Dirac cone is immune to pairing at leading order in 𝑈 2 . Superconductivity instead emerges only through higher-order in 𝑘 corrections to the dispersion, which are unavoidable in any lattice realization and crucially dictate the pairing symmetry. The form of the pairing thus reflects how the well-known obstruction to realizing a single Dirac cone on a lattice is circumvented. When a Dirac cone arises from broken time-reversal symmetry—for instance, at a transition between Chern insulators or in a valley-polarized phase—we find a topological 𝑝−𝑖⁢𝑝 state whose chirality is opposite to that of the parent chiral metal above 𝑇 𝑐 . By contrast, for a surface Dirac cone of a 3D topological insulator, superconductivity is stabilized by anisotropies in the dispersion. For 𝐶 3⁢𝑣 -symmetric warping, as in , pairing is strongest when the Fermi surface becomes hexagonal, leading to order in the (𝑑±𝑖⁢𝑑)×(𝑝+𝑖⁢𝑝) channel with accidental near-nodes. In the highly anisotropic limit 𝑣 𝑥 ≫𝑣 𝑦 , relevant to side surfaces of layered materials, the Fermi surface splits into two branches, and nesting favors a pairing symmetry 𝛥∼s⁢g⁡n⁢(𝑘 𝑥 )⁢cos⁡(𝑘 𝑦 ) reminiscent of organic superconductors.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2022

Electronic structure of α - RuCl 3 by fixed-node and fixed-phase diffusion Monte Carlo methods

Layered material α-RuCl 3 has caught wide attention due to its possible realization of Kitaev's spin liquid and its electronic structure that involves the interplay of electron-electron correlations and spin-orbit effects. Several DFT+U studies have suggested that both electron-electron correlations and spin-orbit effects are crucial for accurately describing the band gap. This work studies the importance of these two effects using fixed-node and fixed-phase diffusion Monte Carlo calculations both in spin-averaged and explicit spin-orbit formalisms. In the latter, the Slater-Jastrow trial function is constructed from two-component spin orbitals using our recent quantum Monte Carlo (QMC) developments and thoroughly tested effective core potentials. Our results show that the gap in the ideal crystal is already accurately described by the spin-averaged case, with the dominant role being played by the magnetic ground state with significant exchange and electron correlation effects. We find qualitative agreement between hybrid DFT, DFT+U, and QMC. In addition, QMC results agree very well with available experiments, and we identify the values of exact Fock exchange mixing that provide comparable gaps. Explicit spin-orbit QMC calculations reveal that the effect of spin-orbit coupling on the gap is minor, of the order of 0.2 eV, which corresponds to the strength of the spin orbit of the Ru atom.

36 MATERIALS SCIENCE↗
DOE OSTI2024

Optically induced umklapp shift currents in striped cuprates

Motivated by recent experiments that observed low-frequency second-order optical responses in doped striped superconductors, here we investigate the nonlinear electrodynamics of systems exhibiting a charge density wave (CDW) order parameter. Due to the Bragg scattering off the CDW order, an incoming spatially homogeneous electric field in addition to zero momentum current generates umklapp currents that are modulated in space at momenta of the reciprocal CDW lattice. In particular, here we predict and microscopically evaluate the umklapp shift current, a finite momentum analog of the regular shift current which represents the second-order optical process that downconverts homogeneous AC electric field into low-frequency, zero momentum current. Specifically, we evaluate real-time response functions within mean-field theory via the Keldysh technique and use the Peierls substitution to compute observables at finite momenta in lattice models. We find that systems with certain lattice symmetries (such as inversion symmetry), where the regular shift current is disallowed, may give rise to the umklapp one. We apply our framework to investigate lattice symmetries in layered materials with helical-like stripes and show that both types of shift currents provide insight into the nature of intertwined phases of matter. Finally, we discuss the relation of our findings to recent experiments in striped superconductors. Published by the American Physical Society 2024

Materials Science↗