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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 199 records · Page 11
All sourcesNASA NTRSDOE OSTI
DOE OSTI2021

Imaging local discharge cascades for correlated electrons in WS 2 /WSe 2 moiré superlattices

Transition metal dichalcogenide moiré heterostructures provide an ideal platform to explore the extended Hubbard model, where long-range Coulomb interactions play a critical role in determining strongly correlated electron states. This has led to experimental observations of Mott insulator states at half filling as well as a variety of extended Wigner crystal states at different fractional fillings. However, a microscopic understanding of these emerging quantum phases is still lacking. Here we describe a scanning tunnelling microscopy (STM) technique for the local sensing and manipulation of correlated electrons in a gated WS 2 /WSe 2 moiré superlattice, which enables the experimental extraction of fundamental extended Hubbard model parameters. We demonstrate that the charge state of the local moiré sites can be imaged by their influence on the STM tunnelling current. In addition to imaging, we are also able to manipulate the charge state of correlated electrons. When we ramp the bias on the STM tip, there is a local discharge cascade of correlated electrons in the moiré superlattice, which allows us to estimate the nearest-neighbour Coulomb interaction. Two-dimensional mapping of the moiré electron charge states also enables us to determine the on-site energy fluctuations at different moiré sites. Furthermore, our technique should be broadly applicable to many semiconductor moiré systems, offering a powerful tool for the microscopic characterization and control of strongly correlated states in moiré superlattices.

36 MATERIALS SCIENCE↗
DOE OSTI2020

Effect of Anisotropic Confinement on Electronic Structure and Dynamics of Band Edge Excitons in Inorganic Perovskite Nanowires

Inorganic lead halide perovskite nanostructures show promise as the active layers in photovoltaics, light emitting diodes, and other optoelectronic devices. They are robust in the presence of oxygen and water, and the electronic structure and dynamics of these nanostructures can be tuned through quantum confinement. Here we create aligned bundles of CsPbBr3 nanowires with widths resulting in quantum confinement of the electronic wave functions and subject them to ultrafast microscopy. We directly image rapid one-dimensional exciton diffusion along the nanowires, and we measure an exciton trap density of roughly one per nanowire. Using transient absorption microscopy, we observe a polarization-dependent splitting of the band edge exciton line, and from the polarized fluorescence of nanowires in solution, we determine that the exciton transition dipole moments are anisotropic in strength. Furthermore, our observations are consistent with a model in which splitting is driven by shape anisotropy in conjunction with long-range exchange.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2022

Magnetic Interactions in Substitutional Core-Doped Graphene Nanoribbons

The design of a spin imbalance within the crystallographic unit cell of bottom-up engineered 1D graphene nanoribbons (GNRs) gives rise to nonzero magnetic moments within each cell. Here, we demonstrate the bottom-up assembly and spectroscopic characterization of a one-dimensional Kondo spin chain formed by a chevron-type GNR (cGNR) physisorbed on Au(111). Substitutional nitrogen core doping introduces a pair of low-lying occupied states per monomer within the semiconducting gap of cGNRs. Charging resulting from the interaction with the gold substrate quenches one electronic state for each monomer, leaving behind a 1D chain of radical cations commensurate with the unit cell of the ribbon. In this work, scanning tunneling microscopy (STM) and spectroscopy (STS) reveal the signature of a Kondo resonance emerging from the interaction of $\textit{S}$ = 1/2 spin centers in each monomer core with itinerant electrons in the Au substrate. STM tip lift-off experiments locally reduce the effective screening of the unpaired radical cation being lifted, revealing a robust exchange coupling between neighboring spin centers. First-principles DFT-LSDA calculations support the presence of magnetic moments in the core of this GNR when it is placed on Au.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2021

Photon-Sparse, Poisson Light-Sheet Microscopy

Light-sheet microscopy has revolutionized bioimaging by enabling approximately an order of magnitude reduction in specimen irradiance compared to confocal imaging. Here, we introduce a light-sheet imaging system that enables an additional order of magnitude reduction in specimen irradiance by operating at the Poisson limit. To operate at this limit, we integrated classical illumination with single-photon detection and wavelet-based image reconstruction. This integration enabled brightness quantification and object recognition from fewer than one detected photon per image pixel, corresponding to more than 10-fold lower irradiance levels than modern systems. We demonstrate how such photon-sparse imaging can eradicate photobleaching and enable both dim and bright object imaging, thus, further enhancing the related gains of light-sheet microscopy.

60 APPLIED LIFE SCIENCES↗
DOE OSTI2020

Proximity-induced superconducting gap in the quantum spin Hall edge state of monolayer WTe2

The quantum spin Hall insulator is characterized by a bandgap in the two-dimensional (2D) interior and helical 1D edge states 1 , 2 , 3 . Inducing superconductivity in the helical edge state results in a 1D topological superconductor, a highly sought-after state of matter at the core of many proposals for topological quantum computing 4 . In the present study, we report the coexistence of superconductivity and the quantum spin Hall edge state in a van der Waals heterostructure, by placing a monolayer of 1T'-WTe 2 , a quantum spin Hall insulator 1 , 2 , 3 , on a van der Waals superconductor, NbSe 2 . Using scanning tunnelling microscopy and spectroscopy (STM/STS), we demonstrate that the WTe 2 monolayer exhibits a proximity-induced superconducting gap due to the underlying superconductor and that the spectroscopic features of the quantum spin Hall edge state remain intact. Taken together, these observations provide conclusive evidence for proximity-induced superconductivity in the quantum spin Hall edge state in WTe 2 , a crucial step towards realizing 1D topological superconductivity and Majorana bound states in this van der Waals material platform.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2023

Observation of skyrmion bubbles in multilayer [Pt/Co/Cu] n using spin-polarized STM

Magnetic multilayers are a promising platform for storage and logic devices based on skyrmion spin textures, due to the large materials phase space for tuning properties. Epitaxial superlattice structures of [Pt/Co/Cu]n thin films were grown by molecular beam epitaxy at room temperature. Spin-polarized scanning tunneling microscopy (SP-STM) of these samples was used to probe the connection between surface structure and skyrmion morphology with nanoscale spatial resolution. Irregular-shaped skyrmion bubbles were observed, with effective diameters from 20 to 200 nm that are much larger than the nanoscale grain structure of the surface topography. Nucleation, annihilation, and motion of skyrmion bubbles could be driven using the stray field of the ferromagnetic tip in repeated imaging, and spin-polarized current/voltage pulses. Furthermore, our detailed comparison of STM topography and differential conductance images shows that there are no surface defects or inhomogeneities at length scales that could account for the range in skyrmion bubble size or shape observed in the measurements.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2022

Physically and chemically smooth cesium-antimonide photocathodes on single crystal strontium titanate substrates

The performance of x-ray free electron lasers and ultrafast electron diffraction experiments is largely dependent on the brightness of electron sources from photoinjectors. Here, the maximum brightness from photoinjectors at a particular accelerating gradient is limited by the mean transverse energy (MTE) of electrons emitted from photocathodes. For high quantum efficiency (QE) cathodes like alkali-antimonide thin films, which are essential to mitigate the effects of non-linear photoemission on MTE, the smallest possible MTE and, hence, the highest possible brightness are limited by the nanoscale surface roughness and chemical inhomogeneity. In this work, we show that high QE Cs 3 Sb films grown on lattice-matched strontium titanate (STO) substrates have a factor of 4 smoother, chemically uniform surfaces compared to those traditionally grown on disordered Si surfaces. We perform simulations to calculate roughness induced MTE based on measured topographical and surface-potential variations on the Cs 3 Sb films grown on STO and show that these variations are small enough to have no consequential impact on the MTE and, hence, the brightness.

43 PARTICLE ACCELERATORS↗
DOE OSTI2022

Direct measurement of storage and loss behavior in AFM force–distance experiments using the modified Fourier transformation

Force–distance curve experiments are commonly performed in atomic force microscopy (AFM) to obtain the viscoelastic characteristics of materials, such as the storage and loss moduli or compliances. The classic methods used to obtain these characteristics consist of fitting a viscoelastic material model to the experimentally obtained AFM data. Here, we demonstrate a new method that utilizes the modified discrete Fourier transform to approximate the storage and loss behavior of a material directly from the data, without the need for a fit. Additionally, one may still fit a model to the resulting storage and loss behavior if a parameterized description of the material is desired. In contrast to fitting the data to a model chosen a priori, departing from a model-free description of the material's frequency behavior guides the selection of the model, such that the user may choose the one that is most appropriate for the particular material under study. To this end, we also include modified Fourier domain descriptions of commonly used viscoelastic models.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2023

Ultrafast Nanoimaging of Spin-Mediated Shear Waves in an Acoustic Cavity

Strong spin–lattice coupling in van der Waals (vdW) magnets shows potential for innovative magneto-mechanical applications. Here, nanoscale and picosecond imaging by ultrafast electron microscopy reveal heterogeneous spin-mediated coherent acoustic phonon dynamics in a thin-film cavity of the vdW antiferromagnet FePS3. The harmonics of the interlayer shear acoustic modes are observed, in which the even and odd harmonics exhibit distinct nanoscopic dynamics. Corroborated by acoustic wave simulation, the role of defects in forming even harmonics is elucidated. Above the Néel temperature (T N ), the interlayer shear acoustic harmonics are suppressed, while the in-plane traveling wave is predominantly excited. The dominant acoustic dynamics shifts from the out-of-plane shear to the in-plane traveling wave across T N , demonstrating that magnetic properties can influence phonon scattering pathways. In conclusion, the spatiotemporally resolved structural characterization provides valuable nanoscopic insights for interlayer-shear-mode-based acoustic cavities, opening up possibilities for magneto-mechanical applications of vdW magnets.

36 MATERIALS SCIENCE↗
DOE OSTI2022

High resolution atomic force microscopy with an active piezoelectric microcantilever

Active microcantilevers with on-chip sensing and actuation provide significant advantages in tapping mode Atomic Force Microscopy (AFM). Collocated transduction allows for effective manipulation of cantilever dynamics through feedback control, enabling higher scan rates. However, the adjacency of the sensing and actuation electrodes is known to result in a high level of feedthrough, leading to a low imaging resolution. Readout circuit noise further deteriorates the imaging precision. Here, we investigate the noise sources that affect AFM microcantilevers with collocated aluminum nitride (AlN) actuator–sensor pairs. We reported these cantilevers in earlier work and demonstrated that they display a very low level of feedthrough between the actuation and sensing electrodes. We present a high signal-to-noise ratio (SNR) sensing method that enables us to demonstrate high-resolution AFM on a calibration grating with nm-step silicon carbide (SiC) terraces. In conclusion, measuring the Lorentzian response of the cantilever’s Brownian motion with the on-chip active sensor at resonance enables us to calibrate the dynamic stiffness at the first fundamental resonance mode, without utilizing an optical sensor.

47 OTHER INSTRUMENTATION↗
DOE OSTI2021

AFM-IR and s-SNOM-IR measurements of chemically addressable monolayers on Au nanoparticles

The performance of catalysts depends on their nanoscale properties, and local variations in structure and composition can have a dramatic impact on the catalytic reactivity. Therefore, probing the localized reactivity of catalytic surfaces using high spatial resolution vibrational spectroscopy, such as infrared (IR) nanospectroscopy and tip-enhanced Raman spectroscopy, is essential for mapping their reactivity pattern. Two fundamentally different scanning probe IR nanospectroscopy techniques, namely, scattering-type scanning near-field optical microscopy (sSNOM) and atomic force microscopy-infrared spectroscopy (AFM-IR), provide the capabilities for mapping the reactivity pattern of catalytic surfaces with a spatial resolution of ~20 nm. Herein, we compare these two techniques with regard to their applicability for probing the vibrational signature of reactive molecules on catalytic nanoparticles. For this purpose, we use chemically addressable self-assembled molecules on Au nanoparticles as model systems. We identified significant spectral differences depending on the measurement technique, which originate from the fundamentally different working principles of the applied methods. While AFM-IR spectra provided information from all the molecules that were positioned underneath the tip, the s-SNOM spectra were more orientation-sensitive. Due to its field-enhancement factor, the s-SNOM spectra showed higher vibrational signals for dipoles that were perpendicularly oriented to the surface. The s-SNOM sensitivity to the molecular orientation influenced the amplitude, position, and signal-to-noise ratio of the collected spectra. Ensemble-based IR measurements verified that differences in the localized IR spectra stem from the enhanced sensitivity of s-SNOM measurements to the adsorption geometry of the probed molecules.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2021

Imaging two-dimensional generalized Wigner crystals

The Wigner crystal has fascinated condensed matter physicists for nearly 90 years. Signatures of two-dimensional (2D) Wigner crystals were first observed in 2D electron gases under high magnetic field, and recently reported in transition metal dichalcogenide moiré superlattices. Direct observation of the 2D Wigner crystal lattice in real space, however, has remained an outstanding challenge. Conventional scanning tunnelling microscopy (STM) has sufficient spatial resolution but induces perturbations that can potentially alter this fragile state. Here we demonstrate real-space imaging of 2D Wigner crystals in WSe 2 /WS 2 moiré heterostructures using a specially designed non-invasive STM spectroscopy technique. This employs a graphene sensing layer held close to the WSe 2 /WS 2 moiré superlattice. Local STM tunnel current into the graphene layer is modulated by the underlying Wigner crystal electron lattice in the WSe 2 /WS 2 heterostructure. Different Wigner crystal lattice configurations at fractional electron fillings of n = 1/3, 1/2 and 2/3, where n is the electron number per site, are directly visualized. The n = 1/3 and n = 2/3 Wigner crystals exhibit triangular and honeycomb lattices, respectively, to minimize nearest-neighbour occupations. The n = 1/2 state spontaneously breaks the original C3 symmetry and forms a stripe phase. Here our study lays a solid foundation for understanding Wigner crystal states in WSe 2 /WS 2 moiré heterostructures and provides an approach that is generally applicable for imaging novel correlated electron lattices in other systems.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2025

Laser-driven ultrafast transmission electron microscopy

Recent advances in lasers and electron optics technology have allowed transmission electron microscopes to achieve high spatial and temporal resolution, making them capable of tracking atoms, charges and spin motions down to the attosecond and nanometre scales. This Primer discusses the most common and practical experimental implementation of time-resolved transmission electron microscopy and the stroboscopic mode for evaluating ultrafast reversible dynamics. An in-depth discussion of photo-induced near-field electron microscopy, a technique unique to laser-assisted electron microscopy, is also provided, covering its prospective applications in the study of coherent phenomena in quantum materials. The experimental strategies and limitations in investigating the structural dynamics of materials and nanostructures by imaging, diffraction and spectroscopy are also described in detail, with a direct comparison with more conventional and established techniques. Here, we provide key information for new researchers who intend to use ultrafast transmission electron microscopy to address new challenges in specific materials science, condensed matter and nanophotonics.

Transmission electron microscopy↗
DOE OSTI2024

Fingerprints of composite fermion Lambda levels in scanning tunneling microscopy

A composite fermion (CF) is a topological quasiparticle that emerges from a nonperturbative attachment of vortices to electrons in strongly correlated two-dimensional materials. Similar to noninteracting fermions that form Landau levels in a magnetic field, CFs can fill analogous “Lambda” levels, giving rise to the fractional quantum Hall (FQH) effect of electrons. Here, we show that Lambda levels can be directly visualized through the characteristic peak structure in the signal obtained via spectroscopy with scanning tunneling microscopy (STM) on a FQH state. Complementary to transport, which probes the low-energy properties of CFs, we show that high-energy features in STM spectra can be interpreted in terms of Lambda levels. We numerically demonstrate that STM spectra can be accurately modeled using Jain's CF theory. Our results show that STM provides a powerful tool for revealing the anatomy of FQH states and identifying physics beyond the noninteracting CF paradigm.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗
DOE OSTI2022

Nanoscale imaging of phonon dynamics by electron microscopy

Spatially resolved vibrational mapping of nanostructures is indispensable to the development and understanding of thermal nanodevices, modulation of thermal transport and novel nanostructured thermoelectric materials. Through the engineering of complex structures, such as alloys, nanostructures and superlattice interfaces, one can significantly alter the propagation of phonons and suppress material thermal conductivity while maintaining electrical conductivity. There have been no correlative experiments that spatially track the modulation of phonon properties in and around nanostructures due to spatial resolution limitations of conventional optical phonon detection techniques. Here we demonstrate two-dimensional spatial mapping of phonons in a single silicon–germanium (SiGe) quantum dot (QD) using monochromated electron energy loss spectroscopy in the transmission electron microscope. Tracking the variation of the Si optical mode in and around the QD, we observe the nanoscale modification of the composition-induced red shift. We observe non-equilibrium phonons that only exist near the interface and, furthermore, develop a novel technique to differentially map phonon momenta, providing direct evidence that the interplay between diffuse and specular reflection largely depends on the detailed atomistic structure: a major advancement in the field. Our work unveils the non-equilibrium phonon dynamics at nanoscale interfaces and can be used to study actual nanodevices and aid in the understanding of heat dissipation near nanoscale hotspots, which is crucial for future high-performance nanoelectronics.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Magneto-Optical Sensing Beyond the Shot Noise Limit

Magneto-optical sensors including spin noise spectroscopies and magneto-optical Kerr effect microscopies are now ubiquitous tools for materials characterization that can provide new understanding of spin dynamics, hyperfine interactions, spin-orbit interactions, and charge-carrier g-factors. Both interferometric and intensity-difference measurements can provide photon-shot-noise-limited sensitivity, but further improvements in sensitivity with classical resources require either increased laser power that can induce unwanted heating and electronic perturbations or increased measurement times that can obscure out-of-equilibrium dynamics and slow experimental throughput. Proof-of-principle measurements have already demonstrated quantum enhanced spin noise measurements with a squeezed readout field that are likely to be critical to the nonperturbative characterization of spin excitations in quantum materials that emerge at low temperatures. Here, a truncated nonlinear interferometric readout for low-temperature magneto-optical Kerr effect and related magneto-optical microscopies that is accessible with today's quantum optical resources is proposed. 10 nrad/$\sqrt{Hz}$ sensitivity is achievable with optical power as small as 1 µW. As a result, measurements may be performed at temperatures as low as 83 mK in commercially available dilution refrigerators. This combination of high sensitivity and low operating temperature is impossible to achieve with any classical measurement. The quantum advantage for the proposed measurements persists even in the limit of large loss and small squeezing parameters.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2024

Imaging the Breakdown and Restoration of Topological Protection in Magnetic Topological Insulator MnBi 2 Te 4

Quantum anomalous Hall (QAH) insulators transport charge without resistance along topologically protected chiral 1D edge states. Yet, in magnetic topological insulators to date, topological protection is far from robust, with zero-magnetic field QAH effect only realized at temperatures an order of magnitude below the Néel temperature T N , though small magnetic fields can stabilize QAH effect. Understanding why topological protection breaks down is therefore essential to realizing QAH effect at higher temperatures. Here a scanning tunneling microscope is used to directly map the size of exchange gap (E g,ex ) and its spatial fluctuation in the QAH insulator 5-layer MnBi 2 Te 4 . Long-range fluctuations of E g,ex are observed, with values ranging between 0 (gapless) and 70 meV, appearing to be uncorrelated to individual surface point defects. The breakdown of topological protection is directly imaged, showing that the gapless edge state, the hallmark signature of a QAH insulator, hybridizes with extended gapless regions in the bulk. Finally, it is unambiguously demonstrated that the gapless regions originate from magnetic disorder, by demonstrating that a small magnetic field restores E g,ex in these regions, explaining the recovery of topological protection in magnetic fields. The results indicate that overcoming magnetic disorder is the key to exploiting the unique properties of QAH insulators.

36 MATERIALS SCIENCE↗