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Results for “coherent electronic phases”

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 91 records · Page 5
All sourcesNASA NTRSDOE OSTI
DOE OSTI2020

Quantum oscillations from networked topological interfaces in a Weyl semimetal

Layered transition metal chalcogenides are promising hosts of electronic Weyl nodes and topological superconductivity. MoTe 2 is a striking example that harbors both noncentrosymmetric T d and centrosymmetric T’ phases, both of which have been identified as topologically nontrivial. Applied pressure tunes the structural transition separating these phases to zero temperature, stabilizing a mixed T d –T’ matrix that entails a network of interfaces between the two nontrivial topological phases. Here, we show that this critical pressure range is characterized by distinct coherent quantum oscillations, indicating that the difference in topology between topologically nonvtrivial T d and T’ phases gives rise to an emergent electronic structure: a network of topological interfaces. A rare combination of topologically nontrivial electronic structures and locked-in transformation barriers leads to this counterintuitive situation, wherein quantum oscillations can be observed in a structurally inhomogeneous material. These results further open the possibility of stabilizing multiple topological phases coexisting with superconductivity.

36 MATERIALS SCIENCE↗
DOE OSTI2025

Coherently coupled carrier and phonon dynamics in elemental tellurium probed by extreme ultraviolet transient absorption

The narrow band-gap semiconductor elemental tellurium (Te) has a unique electronic structure due to strong spin-orbit splitting and a lack of inversion symmetry of its helical lattice. Using broadband extreme ultraviolet core-level transient absorption, we simultaneously measure the coherently coupled photoinduced carrier and lattice dynamics at the Te N4,5 edge initiated by a few-cycle NIR pulse. Ultrafast excitation of carriers leads to a coherently excited A1 phonon oscillation and the generation of a hot carrier population distribution that oscillates in temperature, and the phonon excursion and hot carrier temperature are π out of phase with respect to each other. The depths of modulation suggest a significant coupling between the electronic and lattice degrees of freedom in Te. A long-lived shift of the absorption edge suggests an excited state of Te in another equilibrium potential energy surface that lives on the order of the carrier recombination timescale. The observed phonon-induced oscillations of the hot carriers are supportive of a change in the metallicity, whereby Te becomes more metallic with increasing phonon-induced displacement. Additionally, near the Fermi level we observe an energy-dependent phase of the displacive excitation of the A1 phonon mode. The discovery of coherent coupling between the lattice and hot carriers in Te provides the basis to investigate coherent interactions between spin and orbital degrees of freedom. The results spectrally and temporally resolve the correlation between photoexcited hot carriers and coherent lattice excitations, providing insight on the optical manipulation of the Te electronic structure at high carrier densities exceeding 1021cm−3.

Adelman, Jonah R↗
DOE OSTI2024

Ultrafast Bragg coherent diffraction imaging of epitaxial thin films using deep complex-valued neural networks

Abstract Domain wall structures form spontaneously due to epitaxial misfit during thin film growth. Imaging the dynamics of domains and domain walls at ultrafast timescales can provide fundamental clues to features that impact electrical transport in electronic devices. Recently, deep learning based methods showed promising phase retrieval (PR) performance, allowing intensity-only measurements to be transformed into snapshot real space images. While the Fourier imaging model involves complex-valued quantities, most existing deep learning based methods solve the PR problem with real-valued based models, where the connection between amplitude and phase is ignored. To this end, we involve complex numbers operation in the neural network to preserve the amplitude and phase connection. Therefore, we employ the complex-valued neural network for solving the PR problem and evaluate it on Bragg coherent diffraction data streams collected from an epitaxial La 2-x Sr x CuO 4 (LSCO) thin film using an X-ray Free Electron Laser (XFEL). Our proposed complex-valued neural network based approach outperforms the traditional real-valued neural network methods in both supervised and unsupervised learning manner. Phase domains are also observed from the LSCO thin film at an ultrafast timescale using the complex-valued neural network.

77 NANOSCIENCE AND NANOTECHNOLOGY↗
NASA NTRS1981

Dispersive Doppler measurement of the electron content of the torus of Io

As Voyager 1 made its swing-by of Io, it passed through and behind the satellite's plasma torus. The phase paths of the coherent 13 cm and 3.6-cm wavelength signals transmitted from the spacecraft were shortened differentially by the plasma, resulting in the observation of a dispersive Doppler signature in the signals received at the NASA/Jet Propulsion Laboratory (deep space network) stations. Ray path integration through three different models of the electron distribution of the torus of Io (Warwick et al. 1979; Birmingham et al. 1981; Bagenal et al., 1981) have been performed. The results of the integrations are compared with the dispersive Doppler data.

Levy, G. S.↗
DOE OSTI2023

Deep-Learning Electron Diffractive Imaging

Here, we report the development of deep-learning coherent electron diffractive imaging at subangstrom resolution using convolutional neural networks (CNNs) trained with only simulated data. We experimentally demonstrate this method by applying the trained CNNs to recover the phase images from electron diffraction patterns of twisted hexagonal boron nitride, monolayer graphene, and a gold nanoparticle with comparable quality to those reconstructed by a conventional ptychographic algorithm. Fourier ring correlation between the CNN and ptychographic images indicates the achievement of a resolution in the range of 0.70 and 0.55 Å. We further develop CNNs to recover the probe function from the experimental data. The ability to replace iterative algorithms with CNNs and perform real-time atomic imaging from coherent diffraction patterns is expected to find applications in the physical and biological sciences.

47 OTHER INSTRUMENTATION↗
DOE OSTI2020

Amplified spontaneous emission in the extreme ultraviolet by expanding xenon clusters

Focused short-wavelength free-electron laser (FEL) pulses interacting with gas phase samples can induce by inner-shell ionization a short-lived population inversion, followed by coherent collective emission of directed, short, and strong radiation bursts. We extend our studies into the warm-dense matter (WDM) regime by investigating the nanoplasmas produced in an ensemble of nanometer-sized clusters by FEL irradiation. Here, additional pathways can also lead to strong, laserlike emission: Electron-ion collisions can yield a long-lived population inversion, and subsequent amplified spontaneous emission. We observe amplified spontaneous emission (ASE) in the extreme ultraviolet in xenon clusters excited by soft x-ray FEL pulses, we diagnose the generated nanoplasmas by fluorescence spectroscopy, and we study under various cluster and FEL parameters the directed ASE from the Xe 2+ 65 nm line. We show its exponential increase as a function of FEL irradiation power, and an accompanying collisional broadening of the emission spectra. These findings are corroborated by extensive numerical simulations based on theory, combining detailed hydrodynamic and kinetic simulations with time-dependent calculations of radiation transport, amplification, and collective emission in the WDM nanoplasma. Furthermore, our theoretical findings underline that population inversion is due to electron-ion collisions and that the observed decoherence processes can be empirically characterized by a phenomenological decoherence time in the range of 100–200 fs.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2023

Nanoscale phase transition in impact indented Mo/Cu thin films

The study reveals a size effect in deformation mechanisms via unique structural transitions in sputter deposited fcc/bcc nanolayers under high strain rate impact nanoindentation as layer thickness is reduced from around 100-200 nm to around 5 nm. Here, the indented 5 nm Cu/5 nm Mo multilayer films characterized via cross-sectional scanning/transmission electron microscopy have revealed a phase transition in the 5 nm thick Mo layers from BCC to a coherent metastable FCC structure and fine deformation twins in the 5 nm Cu layers inside a shear band that is approximately 500 nm long and inclined to the layer interfaces. In contrast, thicker layers, 80 nm Cu/180 nm Mo, show different deformation behavior with uneven layer thickness reduction, shearing of Cu layers, and bending of the columnar Mo grains beneath the indentation without any sign of shear band and localized phase transformation.

36 MATERIALS SCIENCE↗
DOE OSTI2024

Wave-packet manipulation of He Rydberg states by a seeded free-electron laser

We report a two-dimensional pump-control-probe spectroscopic study of the dynamics of singly excited He Rydberg-state wave packets with a seeded extreme ultraviolet (XUV) free-electron laser (FEL) source. A pair of coherent XUV pulses, defined by their coarse time separation and relative phase, created and manipulated the wave packets. The He atoms were postionized by infrared (IR) pulses, and the ion yield was measured as a function of XUV phase and IR arrival time. We tagged and sorted the relative phase of the XUV pulse pair on a single-shot basis by fitting each FEL spectrum with a suitable function that accounts for nonidealities of the XUV pulse pairs, associated with the seeding process; more generally, the fit returns the time-dependent electric field of the FEL spectra. The experimental two-dimensional maps of ion yields, measured as a function of IR (probe) delay and of XUV (pump-control) phase, were compared with the solution of the first-order time-dependent Schrödinger equation for this field. Despite the fact that the experimental conditions imply strong excitation, beyond the approximations of first-order perturbation theory, the simulated map satisfactorily reproduces the experimental one for temporally well-separated pulses. We show that by selecting data at appropriate values of pump-control phase, we enhance or suppress the amplitude of chosen wave-packet components consisting of two or more Rydberg states. When the temporal overlap of the pulse pair cannot be neglected, the phase reconstruction is underdetermined, and we provide a simplified comparison between data and simulations. Published by the American Physical Society 2024

Dumergue, Mathieu (ORCID:0000000236984406)↗
DOE OSTI2021

Electronic Structure Correspondence of Singlet-Triplet Scale Separation in Strained Sr2RuO4

At a temperature of roughly 1 K, Sr 2 RuO 4 undergoes a transition from a normal Fermi liquid to a superconducting phase. Even while the former is relatively simple and well understood, the superconducting state has not even been understood after 25 years of study. More recently, it has been found that critical temperatures can be enhanced by the application of uniaxial strain, up to a critical strain, after which it falls off. In this work, we take an “instability” approach and seek divergences in susceptibilities. This provides an unbiased way to distinguish tendencies to competing ground states. We show that in the unstrained compound, the singlet and triplet instabilities of the normal Fermi liquid phase are closely spaced. Under uniaxial strain, electrons residing on all orbitals contributing to the Fermiology become more coherent, while the electrons of the Ru-dxy character become heavier, and the electrons of the Ru d x z , y z characters become lighter. In the process, Im χ(q,ω) increases rapidly around q = ( 0.3 , 0.3 , 0 ) 2 π / a and q = ( 0.5 , 0.25 , 0 ) 2 π / a , while it gets suppressed at all other commensurate vectors, in particular at q = 0, which is essential for spin-triplet superconductivity. We observe that the magnetic anisotropy under strain drops smoothly, which is concomitant with the increment in singlet instability. Thus, the triplet superconducting instability remains the lagging instability of the system, and the singlet instability enhances under strain, leading to a large energy-scale separation between these competing instabilities. However, since this happens even without spin-orbit coupling, we believe it is primarily the enhancement in the spin fluctuation glue around quasi-anti-ferromagnetic vectors that drives the Cooper pairing instead of the magnetic anisotropy. At large strain, an instability to a spin density wave overtakes the superconducting one. The analysis relies on a high-fidelity, ab initio description of the one-particle properties and two-particle susceptibilities, based on the quasiparticle self-consistent GW approximation augmented by dynamical mean field theory. This approach is described and its high fidelity confirmed by comparing to observed one- and two-particle properties.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2020

Formation of Coherent 1H–1T Heterostructures in Single-Layer MoS 2 on Au(111)

Heterojunctions of semiconductors and metals are the fundamental building blocks of modern electronics. Coherent heterostructures between dissimilar materials can be achieved by composition, doping, or heteroepitaxy of chemically different elements. Here, we report the formation of coherent single-layer 1H–1T MoS 2 heterostructures by mechanical exfoliation on Au(111), which are chemically homogeneous with matched lattices but show electronically distinct semiconducting (1H phase) and metallic (1T phase) character, with the formation of these heterojunctions attributed to a combination of lattice strain and charge transfer. The exfoliation approach employed is free of tape residues usually found in many exfoliation methods and yields single-layer MoS 2 with millimeter (mm) size on the Au surface. Raman spectroscopy, X-ray photoelectron spectroscopy (XPS), atomic force microscopy (AFM), scanning tunneling microscopy (STM), and scanning tunneling spectroscopy (STS) have collectively been employed to elucidate the structural and electronic properties of MoS 2 monolayers on Au substrates. Bubbles in the MoS 2 formed by the trapping of ambient adsorbates beneath the single layer during deposition, have also been observed and characterized. Lastly, our work here provides a basis to produce two-dimensional heterostructures which represent potential candidates for future electronic devices.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2025

Prolonging All-Optical Molecular Electron Spin Coherence in the Tissue Transparency Window

Coherent electron spin states within paramagnetic molecules hold significant potential for microscopic quantum sensing. However, all-optical coherence measurements amenable to high spatial and temporal resolution under ambient conditions remain a significant challenge. Here we conduct room-temperature, picosecond time-resolved Faraday ellipticity/rotation (TRFE/R) measurements of the electron spin decoherence time T 2 * in [IrBr 6 ] 2- . Decoherence is strongly sensitive to solution phase viscosity, pointing to molecular tumbling as an important decoherence mechanism. Accordingly, immobilization of [IrBr 6 ] 2- molecules in thin polymer films results in an order-of-magnitude increase in coherence lifetime and significantly greater magnetic field sensitivity. Here, by tuning energies of ligand-to-metal charge transfer (LMCT) states, TRFE/R enables spin initialization and readout in the tissue transparency window, paving the way toward all-optical, ultrafast molecular electron spin coherence imaging in biological systems.

Electron paramagnetic resonance spectroscopy↗
DOE OSTI2020

Multimode Storage of Quantum Microwave Fields in Electron Spins over 100 ms

In this work, we report long coherence times (up to 300 ms) for near-surface bismuth donor electron spins in silicon coupled to a superconducting microresonator, biased at a clock transition. This enables us to demonstrate the partial absorption of a train of weak microwave fields in the spin ensemble, their storage for 100 ms, and their retrieval, using a Hahn-echo-like protocol. Phase coherence and quantum statistics are preserved in the storage.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2023

Active Q-Switched X-Ray Regenerative Amplifier Free-Electron Laser

Despite tremendous progress in x-ray free-electron laser (FEL) science over the last decade, future applications still demand fully coherent, stable x-rays that have not been demonstrated in existing X-ray FEL facilities. Here in this Letter, we describe an active Q-switched x-ray regenerative amplifier FEL scheme to produce fully coherent, high-brightness, hard x rays at a high-repetition rate. By using simple electron-beam phase space manipulation, we show this scheme is flexible in controlling the x-ray cavity quality factor Q and hence the output radiation. We report both theoretical and numerical studies on this scheme with a wide range of accelerator, x-ray cavity, and undulator parameters.

47 OTHER INSTRUMENTATION↗
DOE OSTI2026

Influence of Disorder on the Electronic Properties and Magnetotransport of Ti 3 C 2 T x Single-Flake Devices

The exploration of MXenes for electronic applications is a rapidly growing field in materials science. However, most research has focused on MXene films, with only a limited number of studies addressing the characterization of single-flake devices. In this work, we investigate the electronic and magnetotransport properties of Ti 3 C 2 T x single-flake devices, exploring the influence of structural defectivity on their transport mechanisms. We show that negative magnetoresistance present at low temperatures in single flake samples arises from weak localization, which we analyze to extract the phase coherence length of single-layer and multi-layer flakes. The study of magnetoresistance for this metallic MXene shows that the material exhibits quantum transport phenomena when intrinsic electronic behavior dominates. Moreover, by increasing the defect density via thermal annealing in ultrahigh vacuum, we uncover and characterize the metal-to-disordered metal transition in Ti 3 C 2 T x , shedding light on new properties and enriching fundamental knowledge about MXenes.

MXenes↗
DOE OSTI2022

Femtosecond diffraction studies of the sodium chloride phase diagram under laser shock compression

The phase diagram of sodium chloride (NaCl) under laser shock compression has been studied at Linac Coherent Light Source (LCLS) at the x-ray free-electron laser facility. Both solid–solid (B1 → B2) and solid–liquid (B2 → liquid) transitions have been observed along the Hugoniot over nanosecond time scales. By combining structural measurements through in situ x-ray diffraction, pressure determination through velocimetry, and a thermal equation-of-state, the shock-compressed data are used to constrain the phase diagram of NaCl. Transformation into the B2 phase is found to occur at 28(2) GPa, and B2–liquid coexistence is observed between 54(4) and 66(6) GPa, with near full melt at 66(6) GPa. Late-time pressure release from an initial shocked B2-state results in a B2 → B1 back transformation. Our results show agreement with previous static compression data, suggesting that the time scale for melting is very rapid and that equilibrium states in NaCl are being accessed over nanosecond time scales. Finally, a multiphase equation-of-state description of NaCl incorporated into a one-dimensional hydrocode is used to interpret pressure and temperature evolution over these rapid time scales.

36 MATERIALS SCIENCE↗
DOE OSTI2022

Stroboscopic ultrafast imaging using RF strip-lines in a commercial transmission electron microscope

The development of ultrafast electron microscopy (UEM), specifically stroboscopic imaging, has brought the study of structural dynamics to a new level by overcoming the spatial limitations of ultrafast spectroscopy and the temporal restrictions of traditional TEM simultaneously. Combining the concepts governing both techniques has enabled direct visualization of dynamics with spatiotemporal resolutions in the picosecond-nanometer regime. Here, in this study, we push the limits of imaging using a pulsed electron beam via RF induced transverse deflection based on the newly developed 200 keV frequency-tunable strip-line pulser. We demonstrate 0.2 nm spatial resolution at high magnifications and elucidation of Lorentz imaging using the phase-microscopy method. We also present beam coherence measurements and expand our study using the breathing modes of a silicon interdigitated comb under RF excitation which achieves improved temporal synchronization between the electron pulse-train and electric field. A new RF holder has also been developed with impedance matching to the RF signal to minimize transmission power loss to samples and its performance is compared with a conventional sample holder.

47 OTHER INSTRUMENTATION↗
DOE OSTI2024

Highly Anisotropic Drude-Weight-Reduction and Enhanced Linear-Dichroism in van der Waals Weyl Semimetal T d -MoTe 2 with Coherent Interlayer Electronic Transport

Weyl semimetal (WSM) states can be achieved by breaking spatial-inversion symmetry or time reversal symmetry. However, the anisotropy of the energy reduction contributing to the emergence of WSM states has seldom been investigated by experiments. A van der Waals metal MoTe 2 exhibits a type-II WSM phase below the monoclinic-to-orthorhombic-phase-transition temperature T c ~ 250 K. Here, in this work, a combined linearly polarized optical-spectroscopy and electrical-transport study of MoTe 2 is reported at different temperatures. The Drude components in the a-axis, b-axis, and c-axis optical conductivity spectra, together with the metallic out-of-plane and in-plane electrical resistivities, indicate the coherent inter-layer and in-plane charge transports. Moreover, the Drude weight in σ 1a (ω), rather than the Drude weights in σ 1b (ω) and σ 1c (ω), decreases dramatically below T c , which exhibits a highly anisotropic decrease in its Drude weight and thus suggests a strongly anisotropic reduction of the electronic kinetic energy in the WSM phase. Furthermore, below T c , due to the in-plane anisotropic spectral-weight transfer from Drude component to high-energy region, the in-plane inter-band-absorption anisotropy increases remarkably ≈770 meV, and has the largest value (≈0.68) of normalized linear dichroism among the reported type-II WSMs. The work sheds light on seeking new WSMs and developing novel photonic devices based on WSMs.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2024

In‐Operando Spatiotemporal Imaging of Coupled Film‐Substrate Elastodynamics During an Insulator‐to‐Metal Transition

Abstract The drive toward non‐von Neumann device architectures has led to an intense focus on insulator‐to‐metal (IMT) and the converse metal‐to‐insulator (MIT) transitions. Studies of electric field‐driven IMT in the prototypical VO 2 thin‐film channel devices are largely focused on the electrical and elastic responses of the films, but the response of the corresponding TiO 2 substrate is often overlooked, since it is nominally expected to be electrically passive and elastically rigid. Here, in‐operando spatiotemporal imaging of the coupled elastodynamics using X‐ray diffraction microscopy of a VO 2 film channel device on TiO 2 substrate reveals two new surprises. First, the film channel bulges during the IMT, the opposite of the expected shrinking in the film undergoing IMT. Second, a microns thick proximal layer in the substrate also coherently bulges accompanying the IMT in the film, which is completely unexpected. Phase‐field simulations of coupled IMT, oxygen vacancy electronic dynamics, and electronic carrier diffusion incorporating thermal and strain effects suggest that the observed elastodynamics can be explained by the known naturally occurring oxygen vacancies that rapidly ionize (and deionize) in concert with the IMT (MIT). Fast electrical‐triggering of the IMT via ionizing defects and an active “IMT‐like” substrate layer are critical aspects to consider in device applications.

36 MATERIALS SCIENCE↗