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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.

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At least 235 records · Page 13
All sourcesNASA NTRSDOE OSTI
DOE OSTI2021

Terahertz emission spectroscopy of ultrafast exciton shift current in the noncentrosymmetric semiconductor CdS

The charge-neutral exciton has been predicted to carry genuine photocurrent due to the geometric Berry phase of the electronic bands, if the inversion symmetry in a crystal is broken. Here we detect such exciton shift current in a prototypical polar semiconductor CdS by using terahertz emission spectroscopy. A distinct peak emerges in the photocurrent spectra at the energy of the exciton resonance, which is demonstrated to result from the distinct displacements of electrons and holes in real space within the excitons to produce a finite transient charge current at subpicosecond time scale. Our findings elucidate the Berry phase physics of the charge-neutral photoexcitations and also shed light on the novel energy harvesting mechanism by exciton generation.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2024

Double-domed temperature-pressure phase diagram of CePd 3 S 4

CePd 3 S 4 exhibits interplay between ferromagnetism (FM), quadrupolar order, and the Kondo effect at low temperatures with a FM transition temperature that is much higher than the value expected from the de Gennes scaling of the heavier RPd 3 S 4 compounds. In this work, we investigated the electrical transport and magnetic properties of CePd 3 S 4 under pressure up through 12 GPa so as to better understand the interplay between electronic and magnetic phases in this material. Our findings show that the low pressure FM state is suddenly replaced by a new magnetically ordered phase that is most likely antiferromagnetic that spans from ~ 7 GPa to ~ 11 GPa. Whereas this could be described as an example of avoided quantum criticality, given that clear changes in resistance and Hall data are detected near 6.3 GPa for all temperatures below 300 K, it is also possible that the change in ground state is a response to a pressure induced change in structure. Furthermore, the lack of any discernible change in the pressure dependence of the room temperature unit cell parameter/volume across this whole pressure range suggests that this change in structure is either more subtle than could be detected by our measurements (i.e. development of weak, new wave vector) or the transition is electronic (such as a Lifshitz transition).

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2022

Strain-modulated anisotropic electronic structure in superconducting RuO 2 films

The binary ruthenate, RuO 2 , has been the subject of intense interest due to its itinerant antiferromagnetism and strain-induced superconductivity. The strain mechanism and its effect on the microscopic electronic states leading to the normal and superconducting state, however, remain undisclosed. Here, we investigate highly strained epitaxial (110) RuO 2 films using polarization-dependent oxygen K-edge x-ray absorption spectroscopy (XAS). Through the detection of pre-edge peaks arising from O:2p - Ru:4d hybridization, we uncover the effects of epitaxial strain on the orbital/electronic structure near the Fermi level. Our data show robust strain-induced shifts of orbital levels and a reduction of hybridization strength. Furthermore, we reveal a pronounced in-plane anisotropy of the electronic structure along the [110] / [1$\bar{1}$0] directions naturally stemming from the symmetry-breaking epitaxial strain of the substrate. The B 2g symmetry component of the epitaxially enforced strain breaks a sublattice degeneracy, resulting in an increase of the density of states at the Fermi level (E F ), possibly paving the way to superconductivity. Finally, these results underscore the importance of the effective reduction from tetragonal to orthorhombic lattice symmetry in (110) RuO 2 films and its relevance towards the superconducting and magnetic properties.

36 MATERIALS SCIENCE↗
DOE OSTI2020

Measurement of the Low-Energy Electron Inelastic Mean Free Path in Monolayer Graphene

Measuring the electron-transport properties of substrate-supported nanomaterials with the traditional two-point comparison method is difficult at electron energies below 50 eV, where core-level signals are too feeble to be detected against the strong secondary-electron background. Herein, a data-driven spectral analysis technique is used to study the low-energy electron-transport properties of substrate-supported target nanomaterials, while eliminating the influence of the substrate signal. Applying this technique, the electron-transport properties of the effective attenuation length and the inelastic mean free path (IMFP) can be determined with extremely high efficiency over the entire measured energy range of 6–600 eV. Further, these results show excellent agreement with other experimental and theoretical results. In this work, significant differences are observed between monolayer graphene and the bulk graphite IMFP, which illustrates the importance of the nanometer effect in the electron-transport properties of the material. Furthermore, this technique is readily applicable to any ultrathin material that can be transferred onto a polycrystalline gold substrate.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2023

Vector spin Seebeck effect and spin swapping effect in antiferromagnetic insulators with non-collinear spin structure

Antiferromagnets (AFs) are prospective for next-generation high-density and high-speed spintronic applications due to their negligible stray field and ultrafast spin dynamics, notwithstanding the challenges in detecting and manipulating AF order with no magnetization (M = 0). Among the AFs, non-collinear AFs are of particular interest because of their unique properties arising from the non-collinear spin structure and the small magnetization M. In this work, we describe the recently observed vector spin Seebeck effect in non-collinear LuFeO 3 , where the magneto-thermovoltage under an in-plane temperature gradient, not previously observed, is consistent with the predicted spin swapping effect. Our results shed light on the importance of the non-collinear spin structure in the emerging spin phenomena in non-collinear AFs and offer a new class of materials for AF spintronics and spin caloritronics.

36 MATERIALS SCIENCE↗
DOE OSTI2020

Detection of topology via entanglement oscillations

In this work, we introduce a characterization of topological order based on bulk oscillations of the entanglement entropy and the definition of an “entanglement gap,” showing that it is generally applicable to pure and disordered quantum systems. Using exact diagonalization and the strong disorder renormalization group method, we demonstrate that this approach gives results in agreement with the use of traditional topological invariants, especially in cases where topological order is known to persist in the presence of off-diagonal bond disorder. The entanglement gap is then used to analyze classes of quantum systems with alternating bond types, allowing us to construct their topological phase diagrams. The validity of these phase diagrams is verified in limiting cases of dominant bond types, where the solution is known.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2020

Large spin Hall effect in Si at room temperature

Silicon's weak intrinsic spin-orbit coupling and centrosymmetric crystal structure are a critical bottleneck to the development of Si spintronics, because they lead to an insignificant spin Hall effect (spin current generation) and inverse spin Hall effect (spin current detection). In this work, we undertake current, magnetic field, crystallography dependent magnetoresistance, and magnetothermal transport measurements to study the spin transport behavior in freestanding Si thin films. We observe a large spin Hall magnetoresistance in both $\mathcal{p}$ – Si and $\mathcal{n}$ – Si at room temperature and it is an order of magnitude larger than that of Pt. One explanation of the unexpectedly large and efficient spin Hall effect is spin-phonon coupling instead of spin-orbit coupling. The macroscopic origin of the spin-phonon coupling can be large strain gradients that can exist in the freestanding Si films. This discovery in a light, earth abundant and centrosymmetric material opens a new path of strain engineering to achieve spin dependent properties in technologically highly developed materials.

36 MATERIALS SCIENCE↗
DOE OSTI2025

Unit-density SU(3) Fermi-Hubbard model with spin-flavor imbalance

The advent of ultracold alkaline-earth atoms in optical lattices has established a platform for investigating correlated quantum matter with SU⁡(𝑁) symmetry, offering highly tunable model parameters that allow experiments to access phenomena that are unavailable in conventional materials. Understanding the ground-state physics of SU⁡(𝑁) Fermi-Hubbard models away from the Heisenberg limit and from the spin-flavor balanced setting is important, as examining the flavor imbalance reveals new physics in Fermi-Hubbard models and shows how SU⁡(𝑁) phases react to practical experimental imperfections in optical lattices. Here, in this study, mean-field phase diagrams are presented for the unit-density SU(3) Fermi-Hubbard model at two sets of flavor densities, ($\frac{1}{3}$ − 𝛿, $\frac{1}{3}$ + 𝛿, $\frac{1}{3}$) and ($\frac{1}{4}$ − 𝛿, $\frac{1}{4}$ +𝛿, $\frac{1}{2}$), with the flavor imbalance introduced as 𝛿. Novel phases are identified at moderate interaction strengths for both densities, and their robustness is investigated in the presence of flavor imbalance. Furthermore, we provide microscopic explanations of the phases found and their stability. Analysis of thermal ensembles of random mean-field solutions indicate that, at temperatures accessible in state-of-the-art cold atom experiments, some spin orders are hard for conventional scattering or local observable measurements to detect, but can be more accessible with quantum gas microscopy in optical lattice experiments. This work also shows that nesting and Mottness, intertwined in the usual SU(2) Hubbard model in stark contrast to generic materials, can be tuned in the SU(3) model and play distinct roles. The resulting phase diagrams not only deepen our understanding of SU⁡(𝑁) Fermi-Hubbard models but also inform future experimental search for new phases.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2022

Electronic and magnetic properties of the topological semimetal SmMg 2 Bi 2

Dirac semimetals show nontrivial physical properties and can host exotic quantum states like Weyl semimetals and topological insulators under suitable external conditions. Here, by combining angle-resolved photoemission spectroscopy measurements (ARPES) and first-principle calculations, we demonstrate that the Zintl-phase compound SmMg 2 Bi 2 is in close proximity to a topological Dirac semimetallic state. ARPES results show a Dirac-like band crossing at the zone center near the Fermi level (E F ), which is further confirmed by first-principle calculations. Theoretical studies also reveal that SmMg 2 Bi 2 belongs to a Z 2 topological class and hosts spin-polarized states around the E F . Zintl's theory predicts that the valence state of Sm in this material should be Sm 2+ , however, we detect many Sm-4f multiplet states (flat-bands) whose energy positions and relative intensities suggest the presence of both dominant Sm 2+ and minor Sm 3+ . The small concentration (2.5%) of Sm 3+ in the bulk of a crystal is inferred to arise from Sm vacancies in the crystal. It is also evident that these flat bands and other dispersive states are strongly hybridized when they cross each other. Due to the presence of Sm 3+ ions, the temperature dependence of the magnetic susceptibility χ (T) shows a Curie-Weiss-like contribution in the low-temperature region, in addition to the Van Vleck-like behavior expected for the Sm 2+ ions. The present study will help to better understand the electronic structure, magnetism, and transport properties of related materials.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2024

Unexpected Observation of Disorder and Multiple Phase-Transition Pathways in Shock-Compressed Zr

The response of materials under dynamic compression involves a complex interplay of various deformation mechanisms aimed at relieving shear stresses, yielding a remarkable diversity in material behavior. Here, in this Letter, we utilize femtosecond x-ray diffraction coupled with nanosecond laser compression to reveal an intricate competition between multiple shear-relieving mechanisms within an elemental metal. Our observations in shocked-compressed single-crystal Zr indicate a disorder-mediated shear relaxation at lower pressures. Above the phase-transition pressure, we observe the increasing contribution of structural phase transition in relieving shear stress. We detect not one but three concurrent pathways during the transition from the hcp to a hex-3 structure. These complex dynamics are partially corroborated through multimillion-atom molecular dynamics simulations employing a machine-learned interatomic potential. Our observation of multiple concurrent pathways and disorder during shock compression underscore the far greater intricacies in the dynamic response of metals than previously assumed.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2020

Optical high-order harmonic generation as a structural characterization tool

Structural characterization is essential to material engineering, but few tools can detect structural properties in the time domain. High harmonic generation (HHG) emerges as a new frontier that touches the heart of condensed-matter physics from the symmetry to quantum geometrical nature of electrons, but its capability in structural characterization has not been materialized. Here, we establish a crucial connection between the symmetry of a material and the helicity of light. We employ monolayer MoS 2 as an example. In this work, we show that a linearly polarized laser pulse used in experiments is not ideal for structural characterization because it only generates in-plane anisotropy. It is the circularly polarized laser field that is capable of producing four distinctive HHG signals from the four phases of MoS 2 . This finally links the laser helicity to the crystal structure. The results are generic and are not affected by the Berry curvature, the interband or intraband contribution. Our study unleashes the power of HHG as a structural characterization tool for technologically important materials.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2025

Atomic-scale imaging of frequency-dependent phonon anisotropy

Directly visualizing vibrational anisotropy in individual phonon modes is essential for understanding a wide range of intriguing optical, thermal and elastic phenomena in materials. Although conventional optical and diffraction techniques have been used to estimate vibrational anisotropies, they fall short in achieving the spatial and energy resolution necessary to provide detailed information. Here, we introduce a new form of momentum-selective electron energy-loss spectroscopy, which enables the element-resolved imaging of frequency- and symmetry-dependent vibrational anisotropies with atomic resolution. Vibrational anisotropies manifest in different norms of orthogonal atomic displacements, known as thermal ellipsoids. Using the centrosymmetric strontium titanate as a model system, we observed two distinct types of oxygen vibrations with contrasting anisotropies: oblate thermal ellipsoids below 60 meV and prolate ones above 60 meV. In non-centrosymmetric barium titanate, our approach can detect subtle distortions of the oxygen octahedra by observing the unexpected modulation of q-selective signals between apical and equatorial oxygen sites near 55 meV, which originates from reduced crystal symmetry and may also be linked to ferroelectric polarization. These observations are quantitatively supported by theoretical modelling, which demonstrates the reliability of our approach. The measured frequency-dependent vibrational anisotropies shed new light on the dielectric and thermal behaviours governed by acoustic and optical phonons. Furthermore, the ability to visualize phonon eigenvectors at specific crystallographic sites with unprecedented spatial and energy resolution opens new avenues for exploring dielectric, optical, thermal and superconducting properties.

Ferroelectrics and multiferroics↗
DOE OSTI2021

Wide Dynamic Range, 10 kHz Framing Detector for 4D-STEM

Hybrid pixel array detectors (PADs) have expanded the fidelity, frame rate and dynamic range for diffractive imaging in electron microscopes. With their high detective quantum efficiencies (DQE), the noise performance limited is by counting statistics. Consequently, improving the precision and quality of high-speed images requires increasing the linear dynamic range and the maximum usable beam current. Here we describe a new prototype hybrid PAD, our next-generation electron microscope pixel array detector (NG-EMPAD) that expands both the framing speed and dynamic range of our earlier EMPAD design. Like the EMPAD, electrons are detected directly in a 500 μm thick silicon sensor bonded pixel-by-pixel to a custom signal processing integrated circuit (IC). Each pixel in the IC integrates charge carriers produced by the high-energy incident electrons. Here, in-pixel circuitry uses a combination of techniques to extend the dynamic range, including adaptive gain switching and the quantitative excess charge dumping similar to the EMPAD. In-pixel buffering of signals during readout allows acquiring a new image while reading out the previously collected image, yielding an image collection duty cycle of nearly 100%.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Spatially inhomogeneous superconductivity in UTe 2

The newly discovered superconductor UTe 2 is a strong contender for a topological spin-triplet state wherein a multicomponent order parameter arises from two nearly degenerate superconducting states. A key issue is whether both of these states intrinsically exist at ambient pressure. Through thermal expansion and calorimetry, we show that UTe 2 at ambient conditions exhibits two detectable transitions only in some samples, and the size of the thermal expansion jump at each transition varies when the measurement is performed in different regions of the sample. This result indicates that the two transitions arise from two spatially separated regions that are inhomogeneously mixed throughout the volume of the sample, each with a discrete superconducting transition temperature (T c ). Notably, samples with higher T c only show a single transition at ambient pressure. Above 0.3 GPa, however, two transitions are invariably observed in ac calorimetry. Our results not only point to a nearly vertical line (constant pressure) in the pressure-temperature phase diagram but also provide a consistent scenario for the sample dependence of UTe 2 .

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2020

Strongly correlated Chern insulators in magic-angle twisted bilayer graphene

Interactions between electrons and the topology of their energy bands can create unusual quantum phases of matter. Most topological electronic phases appear in systems with weak electron–electron interactions. The instances in which topological phases emerge only as a result of strong interactions are rare and mostly limited to those realized in intense magnetic fields. The discovery of flat electronic bands with topological character in magic-angle twisted bilayer graphene (MATBG) has created a unique opportunity to search for strongly correlated topological phases. Here we introduce a local spectroscopic technique using a scanning tunnelling microscope to detect a sequence of topological insulators in MATBG with Chern numbers C = ±1, ±2 and ±3, which form near filling factors of ±3, ±2 and ±1 electrons per moiré unit cell, respectively, and are stabilized by modest magnetic fields. One of the phases detected here (C = +1) was previously observed when the sublattice symmetry of MATBG was intentionally broken by a hexagonal boron nitride substrate, with interactions having a secondary role. We also demonstrate that strong electron–electron interactions alone can produce not only the previously observed phase, but also other unexpected Chern insulating phases in MATBG. The full sequence of phases that we observe can be understood by postulating that strong correlations favour breaking time-reversal symmetry to form Chern insulators that are stabilized by weak magnetic fields. Our findings illustrate that many-body correlations can create topological phases in moiré systems beyond those anticipated from weakly interacting models.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2021

Layer Hall effect in a 2D topological axion antiferromagnet

While ferromagnets have been known and exploited for millennia, antiferromagnets (AFMs) were only discovered in the 1930s. The elusive nature indicates AFMs' unique properties: At large scale, due to the absence of global magnetization, AFMs may appear to behave like any non-magnetic material; However, such a seemingly mundane macroscopic magnetic property is highly nontrivial at microscopic level, where opposite spin alignment within the AFM unit cell forms a rich internal structure. In topological AFMs, such an internal structure leads to a new possibility, where topology and Berry phase can acquire distinct spatial textures. Here, we study this exciting possibility in an AFM Axion insulator, even-layered MnBi 2 Te 4 flakes, where spatial degrees of freedom correspond to different layers. Remarkably, we report the observation of a new type of Hall effect, the layer Hall effect, where electrons from the top and bottom layers spontaneously deflect in opposite directions. Specifically, under no net electric field, even-layered MnBi 2 Te 4 shows no anomalous Hall effect (AHE); However, applying an electric field isolates the response from one layer and leads to the surprising emergence of a large layer-polarized AHE (~50e 2 /h). Such a layer Hall effect uncovers a highly rare layer-locked Berry curvature, which serves as a unique character of the space-time PT-symmetric AFM topological insulator state. Moreover, we found that the layer-locked Berry curvature can be manipulated by the Axion field, E∙B, which drives the system between the opposite AFM states. Our results achieve previously unavailable pathways to detect and manipulate the rich internal spatial structure of fully-compensated topological AFMs. The layer-locked Berry curvature represents a first step towards spatial engineering of Berry phase, such as through layer-specific moiré potential.

36 MATERIALS SCIENCE↗
DOE OSTI2025

Dataset for manuscript "Equipartition and the temperature of maximum density of TIP4P/2005 water"

We simulate TIP4P/2005 water in the temperature range of 257 K to 318 K with time-steps 0.25, 0.50, 1.00, 2.00, and 4.00 fs. The density-temperature behavior obtained using 0.25 or 0.50 fs are in excellent agreement with each other but differ from those obtained using time-steps that have been shown earlier to lead to a breakdown of equipartition. The temperature of maximum density (TMD) is 277.15 K with time-step 0.25 or 0.50 fs, but is shifted to progressively lower values for longer time-steps, a trend that holds for different thermostat/barostat combinations. Enhancing the water-water dispersion interaction, as has been recommended for simulating disordered proteins in TIP4P/2005, degrades the description of the liquid-vapor phase envelope. We present a simple physically transparent reasoning to highlight the separation of the time-scales between translational and rotational motion. We also develop a metric, Chi, that we term the equipartition anomaly, to detect equipartition violations in simulations that include molecules that are treated as rigid objects. Calculating Chi is shown to be straightforward and sensitive to equipartition violations. A key takeaway from this study is that using sufficiently short time-steps (less than or equal to 0.5 fs) to preserve equipartition is essential for obtaining meaningful liquid water properties and for producing reliable simulation data, as correct-ensemble sampling is fundamental to ensure reproducibility across codes and simulation alogrithms. The included dataset provides the raw data used in the preparation of the graphs noted in the manuscript.

36 MATERIALS SCIENCE↗
DOE OSTI2023

Evidence of Polaron Formation in Halide Perovskites via Carrier Effective Mass Measurements

Carrier effective mass is a central parameter in solid-state physics. It is a measure of the strength of the coupling between a carrier and excitations arising from its surrounding medium, and features prominently in transport and optical calculations. Experimental techniques employed to determine it are steady-state ones, and so are unable to detect any change in the effective mass after a strong perturbation to the system, e.g., strong optical excitation. By combining time-resolved terahertz spectroscopy and transient absorption spectroscopy, on a mixed-cation mixed-halide perovskite thin film, we observe a large and long-lived photoinduced enhancement of the carrier effective mass, and from it deduce a twofold increase of the carrier-phonon coupling constant, giving evidence of polaron formation. Our work demonstrates a new approach to track the strength and ultrafast lifetimes of photoinduced carrier-boson interactions down to picosecond timescales that can be applied to a wide range of solid-state systems.

36 MATERIALS SCIENCE↗