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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 127 records · Page 7

Spin-valley locking and bulk quantum Hall effect in a noncentrosymmetric Dirac semimetal BaMnSb 2

Spin-valley locking in monolayer transition metal dichalcogenides has attracted enormous interest, since it offers potential for valleytronic and optoelectronic applications. Such an exotic electronic state has sparsely been seen in bulk materials. Here, we report spin-valley locking in a Dirac semimetal BaMnSb 2 . This is revealed by comprehensive studies using first principles calculations, tight-binding and effective model analyses, angle-resolved photoemission spectroscopy measurements. Moreover, this material also exhibits a stacked quantum Hall effect (QHE). The spin-valley degeneracy extracted from the QHE is close to 2. This result, together with the Landau level spin splitting, further confirms the spin-valley locking picture. In the extreme quantum limit, we also observed a plateau in the z-axis resistance, suggestive of a two-dimensional chiral surface state present in the quantum Hall state. These findings establish BaMnSb 2 as a rare platform for exploring coupled spin and valley physics in bulk single crystals and accessing 3D interacting topological states.

36 MATERIALS SCIENCE↗

Flat band carrier confinement in magic-angle twisted bilayer graphene

Abstract Magic-angle twisted bilayer graphene has emerged as a powerful platform for studying strongly correlated electron physics, owing to its almost dispersionless low-energy bands and the ability to tune the band filling by electrostatic gating. Techniques to control the twist angle between graphene layers have led to rapid experimental progress but improving sample quality is essential for separating the delicate correlated electron physics from disorder effects. Owing to the 2D nature of the system and the relatively low carrier density, the samples are highly susceptible to small doping inhomogeneity which can drastically modify the local potential landscape. This potential disorder is distinct from the twist angle variation which has been studied elsewhere. Here, by using low temperature scanning tunneling spectroscopy and planar tunneling junction measurements, we demonstrate that flat bands in twisted bilayer graphene can amplify small doping inhomogeneity that surprisingly leads to carrier confinement, which in graphene could previously only be realized in the presence of a strong magnetic field.

36 MATERIALS SCIENCE↗

Coherent control of asymmetric spintronic terahertz emission from two-dimensional hybrid metal halides

Abstract Next-generation terahertz (THz) sources demand lightweight, low-cost, defect-tolerant, and robust components with synergistic, tunable capabilities. However, a paucity of materials systems simultaneously possessing these desirable attributes and functionalities has made device realization difficult. Here we report the observation of asymmetric spintronic-THz radiation in Two-Dimensional Hybrid Metal Halides (2D-HMH) interfaced with a ferromagnetic metal, produced by ultrafast spin current under femtosecond laser excitation. The generated THz radiation exhibits an asymmetric intensity toward forward and backward emission direction whose directionality can be mutually controlled by the direction of applied magnetic field and linear polarization of the laser pulse. Our work demonstrates the capability for the coherent control of THz emission from 2D-HMHs, enabling their promising applications on the ultrafast timescale as solution-processed material candidates for future THz emitters.

36 MATERIALS SCIENCE↗

Temperature dependence of quantum oscillations from non-parabolic dispersions

The phase offset of quantum oscillations is commonly used to experimentally diagnose topologically nontrivial Fermi surfaces. This methodology, however, is inconclusive for spin-orbit-coupled metals where π -phase-shifts can also arise from non-topological origins. Here, we show that the linear dispersion in topological metals leads to a T 2 -temperature correction to the oscillation frequency that is absent for parabolic dispersions. We confirm this effect experimentally in the Dirac semi-metal Cd 3 As 2 and the multiband Dirac metal LaRhIn 5 . Both materials match a tuning-parameter-free theoretical prediction, emphasizing their unified origin. For topologically trivial Bi 2 O 2 Se, no frequency shift associated to linear bands is observed as expected. However, the π -phase shift in Bi 2 O 2 Se would lead to a false positive in a Landau-fan plot analysis. Our frequency-focused methodology does not require any input from ab-initio calculations, and hence is promising for identifying correlated topological materials.

36 MATERIALS SCIENCE↗

In-plane quasi-single-domain BaTiO 3 via interfacial symmetry engineering

The control of the in-plane domain evolution in ferroelectric thin films is not only critical to understanding ferroelectric phenomena but also to enabling functional device fabrication. However, in-plane polarized ferroelectric thin films typically exhibit complicated multi-domain states, not desirable for optoelectronic device performance. Here we report a strategy combining interfacial symmetry engineering and anisotropic strain to design single-domain, in-plane polarized ferroelectric BaTiO 3 thin films. Theoretical calculations predict the key role of the BaTiO 3 /PrScO 3 (110) O substrate interfacial environment, where anisotropic strain, monoclinic distortions, and interfacial electrostatic potential stabilize a single-variant spontaneous polarization. A combination of scanning transmission electron microscopy, piezoresponse force microscopy, ferroelectric hysteresis loop measurements, and second harmonic generation measurements directly reveals the stabilization of the in-plane quasi-single-domain polarization state. This work offers design principles for engineering in-plane domains of ferroelectric oxide thin films, which is a prerequisite for high performance optoelectronic devices.

36 MATERIALS SCIENCE↗

Magneto-transport evidence for strong topological insulator phase in ZrTe5

Abstract The identification of a non-trivial band topology usually relies on directly probing the protected surface/edge states. But, it is difficult to achieve electronically in narrow-gap topological materials due to the small (meV) energy scales. Here, we demonstrate that band inversion, a crucial ingredient of the non-trivial band topology, can serve as an alternative, experimentally accessible indicator. We show that an inverted band can lead to a four-fold splitting of the non-zero Landau levels, contrasting the two-fold splitting (spin splitting only) in the normal band. We confirm our predictions in magneto-transport experiments on a narrow-gap strong topological insulator, zirconium pentatelluride (ZrTe 5 ), with the observation of additional splittings in the quantum oscillations and also an anomalous peak in the extreme quantum limit. Our work establishes an effective strategy for identifying the band inversion as well as the associated topological phases for future topological materials research.

36 MATERIALS SCIENCE↗

Visualizing band selective enhancement of quasiparticle lifetime in a metallic ferromagnet

Abstract Electrons navigate more easily in a background of ordered magnetic moments than around randomly oriented ones. This fundamental quantum mechanical principle is due to their Bloch wave nature and also underlies ballistic electronic motion in a perfect crystal. As a result, a paramagnetic metal that develops ferromagnetic order often experiences a sharp drop in the resistivity. Despite the universality of this phenomenon, a direct observation of the impact of ferromagnetic order on the electronic quasiparticles in a magnetic metal is still lacking. Here we demonstrate that quasiparticles experience a significant enhancement of their lifetime in the ferromagnetic state of the low-density magnetic semimetal EuCd 2 As 2 , but this occurs only in selected bands and specific energy ranges. This is a direct consequence of the magnetically induced band splitting and the multi-orbital nature of the material. Our detailed study allows to disentangle different electronic scattering mechanisms due to non-magnetic disorder and magnon exchange. Such high momentum and energy dependence quasiparticle lifetime enhancement can lead to spin selective transport and potential spintronic applications.

36 MATERIALS SCIENCE↗

Origin of giant electric-field-induced strain in faulted alkali niobate films

A large electromechanical response in ferroelectrics is highly desirable for developing high-performance sensors and actuators. Enhanced electromechanical coupling in ferroelectrics is usually obtained at morphotropic phase boundaries requiring stoichiometric control of complex compositions. Recently it was shown that giant piezoelectricity can be obtained in films with nanopillar structures. Here, we elucidate its origin in terms of atomic structure and demonstrate a different system with a greatly enhanced response. This is in non-stoichiometric potassium sodium niobate epitaxial thin films with a high density of self-assembled planar faults. A giant piezoelectric coefficient of ~1900 picometer per volt is demonstrated at 1 kHz, which is almost double the highest ever reported effective piezoelectric response in any existing thin films. The large oxygen octahedral distortions and the coupling between the structural distortion and polarization orientation mediated by charge redistribution at the planar faults enable the giant electric-field-induced strain. Our findings demonstrate an important mechanism for realizing the unprecedentedly giant electromechanical coupling and can be extended to many other material functions by engineering lattice faults in non-stoichiometric compositions.

36 MATERIALS SCIENCE↗

Control of electronic topology in a strongly correlated electron system

It is becoming increasingly clear that breakthrough in quantum applications necessitates materials innovation. In high demand are conductors with robust topological states that can be manipulated at will. This is what we demonstrate in the present work. We discover that the pronounced topological response of a strongly correlated “Weyl-Kondo” semimetal can be genuinely manipulated—and ultimately fully suppressed—by magnetic fields. We understand this behavior as a Zeeman-driven motion of Weyl nodes in momentum space, up to the point where the nodes meet and annihilate in a topological quantum phase transition. The topologically trivial but correlated background remains unaffected across this transition, as is shown by our investigations up to much larger fields. Our work lays the ground for systematic explorations of electronic topology, and boosts the prospect for topological quantum devices.

36 MATERIALS SCIENCE↗

Gate-tunable Veselago interference in a bipolar graphene microcavity

The relativistic charge carriers in monolayer graphene can be manipulated in manners akin to conventional optics. Klein tunneling and Veselago lensing have been previously demonstrated in ballistic graphene pn-junction devices, but collimation and focusing efficiency remains relatively low, preventing realization of advanced quantum devices and controlled quantum interference. Here, we present a graphene microcavity defined by carefully-engineered local strain and electrostatic fields. Electrons are manipulated to form an interference path inside the cavity at zero magnetic field via consecutive Veselago refractions. The observation of unique Veselago interference peaks via transport measurement and their magnetic field dependence agrees with the theoretical expectation. We further utilize Veselago interference to demonstrate localization of uncollimated electrons and thus improvement in collimation efficiency. Our work sheds new light on relativistic single-particle physics and provide a new device concept toward next-generation quantum devices based on manipulation of ballistic electron trajectory.

36 MATERIALS SCIENCE↗

Cesium-mediated electron redistribution and electron-electron interaction in high-pressure metallic CsPbI3

Abstract Electron-phonon coupling was believed to govern the carrier transport in halide perovskites and related phases. Here we demonstrate that electron-electron interaction enhanced by Cs-involved electron redistribution plays a direct and prominent role in the low-temperature electrical transport of compressed CsPbI 3 and renders Fermi liquid (FL)-like behavior. By compressing δ-CsPbI 3 to 80 GPa, an insulator-semimetal-metal transition occurs, concomitant with the completion of a slow structural transition from the one-dimensional Pnma (δ) phase to a three-dimensional Pmn 2 1 (ε) phase. Deviation from FL behavior is observed upon CsPbI 3 entering the metallic ε phase, which progressively evolves into a FL-like state at 186 GPa. First-principles density functional theory calculations reveal that the enhanced electron-electron coupling results from the sudden increase of the 5d state occupation in Cs and I atoms. Our study presents a promising strategy of cationic manipulation for tuning the electronic structure and carrier scattering of halide perovskites at high pressure.

36 MATERIALS SCIENCE↗

Order-disorder charge density wave instability in the kagome metal (Cs,Rb)V 3 Sb 5

The origin of the charge density wave phases in the kagome metal compound AV 3 Sb 5 is still under great scrutiny. Here, we combine diffuse and inelastic x-ray scattering to identify a 3-dimensional precursor of the charge order at the L point that condenses into a CDW through a first order phase transition. The quasi-elastic critical scattering indicates that the dominant contribution to the diffuse precursor is the elastic central peak without phonon softening. However, the inelastic spectra show a small broadening of the Einstein-type phonon mode on approaching T CDW . Our results point to the situation where the Fermi surface instability at the L point is of order-disorder type with critical growth of quasi-static domains. The experimental data indicate that the CDW consists on an alternating Star of David and trihexagonal distortions and its dynamics goes beyond the classical weak-coupling scenario and is discussed within strong-electron phonon coupling and non-adiabatic models.

36 MATERIALS SCIENCE↗

Signatures of the exciton gas phase and its condensation in monolayer 1T-ZrTe 2

The excitonic insulator (EI) is a Bose-Einstein condensation (BEC) of excitons bound by electron-hole interaction in a solid, which could support high-temperature BEC transition. The material realization of EI has been challenged by the difficulty of distinguishing it from a conventional charge density wave (CDW) state. In the BEC limit, the preformed exciton gas phase is a hallmark to distinguish EI from conventional CDW, yet direct experimental evidence has been lacking. Here we report a distinct correlated phase beyond the 2×2 CDW ground state emerging in monolayer 1T-ZrTe 2 and its investigation by angle-resolved photoemission spectroscopy (ARPES) and scanning tunneling microscopy (STM). The results show novel band- and energy-dependent folding behavior in a two-step process, which is the signatures of an exciton gas phase prior to its condensation into the final CDW state. Our findings provide a versatile two-dimensional platform that allows tuning of the excitonic effect.

36 MATERIALS SCIENCE↗

Layered metals as polarized transparent conductors

The quest to improve transparent conductors balances two key goals: increasing electrical conductivity and increasing optical transparency. To improve both simultaneously is hindered by the physical limitation that good metals with high electrical conductivity have large carrier densities that push the plasma edge into the ultra-violet range. Technological solutions reflect this trade-off, achieving the desired transparencies only by reducing the conductor thickness or carrier density at the expense of a lower conductance. Here we demonstrate that highly anisotropic crystalline conductors offer an alternative solution, avoiding this compromise by separating the directions of conduction and transmission. We demonstrate that slabs of the layered oxides Sr 2 RuO 4 and Tl 2 Ba 2 CuO 6+δ are optically transparent even at macroscopic thicknesses >2 μm for c-axis polarized light. Underlying this observation is the fabrication of out-of-plane slabs by focused ion beam milling. This work provides a glimpse into future technologies, such as highly polarized and addressable optical screens.

36 MATERIALS SCIENCE↗

Local spectroscopy of a gate-switchable moiré quantum anomalous Hall insulator

Abstract In recent years, correlated insulating states, unconventional superconductivity, and topologically non-trivial phases have all been observed in several moiré heterostructures. However, understanding of the physical mechanisms behind these phenomena is hampered by the lack of local electronic structure data. Here, we use scanning tunnelling microscopy and spectroscopy to demonstrate how the interplay between correlation, topology, and local atomic structure determines the behaviour of electron-doped twisted monolayer–bilayer graphene. Through gate- and magnetic field-dependent measurements, we observe local spectroscopic signatures indicating a quantum anomalous Hall insulating state with a total Chern number of ±2 at a doping level of three electrons per moiré unit cell. We show that the sign of the Chern number and associated magnetism can be electrostatically switched only over a limited range of twist angle and sample hetero-strain values. This results from a competition between the orbital magnetization of filled bulk bands and chiral edge states, which is sensitive to strain-induced distortions in the moiré superlattice.

36 MATERIALS SCIENCE↗

Uncovering spin-orbit coupling-independent hidden spin polarization of energy bands in antiferromagnets

Abstract Many textbook physical effects in crystals are enabled by some specific symmetries. In contrast to such ‘apparent effects’, ‘hidden effect X’ refers to the general condition where the nominal global system symmetry would disallow the effect X, whereas the symmetry of local sectors within the crystal would enable effect X. Known examples include the hidden Rashba and/or hidden Dresselhaus spin polarization that require spin-orbit coupling, but unlike their apparent counterparts are demonstrated to exist in non-magnetic systems even in inversion-symmetric crystals. Here, we discuss hidden spin polarization effect in collinear antiferromagnets without the requirement for spin-orbit coupling (SOC). Symmetry analysis suggests that antiferromagnets hosting such effect can be classified into six types depending on the global vs local symmetry. We identify which of the possible collinear antiferromagnetic compounds will harbor such hidden polarization and validate these symmetry enabling predictions with first-principles density functional calculations for several representative compounds. This will boost the theoretical and experimental efforts in finding new spin-polarized materials.

36 MATERIALS SCIENCE↗

Modulation-doping a correlated electron insulator

Abstract Correlated electron materials (CEMs) host a rich variety of condensed matter phases. Vanadium dioxide (VO 2 ) is a prototypical CEM with a temperature-dependent metal-to-insulator (MIT) transition with a concomitant crystal symmetry change. External control of MIT in VO 2 —especially without inducing structural changes—has been a long-standing challenge. In this work, we design and synthesize modulation-doped VO 2 -based thin film heterostructures that closely emulate a textbook example of filling control in a correlated electron insulator. Using a combination of charge transport, hard X-ray photoelectron spectroscopy, and structural characterization, we show that the insulating state can be doped to achieve carrier densities greater than 5 × 10 21 cm −3 without inducing any measurable structural changes. We find that the MIT temperature (T MIT ) continuously decreases with increasing carrier concentration. Remarkably, the insulating state is robust even at doping concentrations as high as ~0.2 e − /vanadium. Finally, our work reveals modulation-doping as a viable method for electronic control of phase transitions in correlated electron oxides with the potential for use in future devices based on electric-field controlled phase transitions.

36 MATERIALS SCIENCE↗

Anomalous excitonic phase diagram in band-gap-tuned Ta2Ni(Se,S)5

Abstract During a band-gap-tuned semimetal-to-semiconductor transition, Coulomb attraction between electrons and holes can cause spontaneously formed excitons near the zero-band-gap point, or the Lifshitz transition point. This has become an important route to realize bulk excitonic insulators – an insulating ground state distinct from single-particle band insulators. How this route manifests from weak to strong coupling is not clear. In this work, using angle-resolved photoemission spectroscopy (ARPES) and high-resolution synchrotron x-ray diffraction (XRD), we investigate the broken symmetry state across the semimetal-to-semiconductor transition in a leading bulk excitonic insulator candidate system Ta 2 Ni(Se,S) 5 . A broken symmetry phase is found to be continuously suppressed from the semimetal side to the semiconductor side, contradicting the anticipated maximal excitonic instability around the Lifshitz transition. Bolstered by first-principles and model calculations, we find strong interband electron-phonon coupling to play a crucial role in the enhanced symmetry breaking on the semimetal side of the phase diagram. Our results not only provide insight into the longstanding debate of the nature of intertwined orders in Ta 2 NiSe 5 , but also establish a basis for exploring band-gap-tuned structural and electronic instabilities in strongly coupled systems.

36 MATERIALS SCIENCE↗