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DOE OSTI2021

Observation of Quasiparticle Pair Production and Quantum Entanglement in Atomic Quantum Gases Quenched to an Attractive Interaction

We report observation of quasiparticle pair-production and characterize quantum entanglement created by a modulational instability in an atomic superfluid. By quenching the atomic interaction to attractive and then back to weakly repulsive, we produce correlated quasiparticles and monitor their evolution in a superfluid through evaluating the in situ density noise power spectrum, which essentially measures a 'homodyne' interference between ground state atoms and quasiparticles of opposite momenta. We observe large amplitude growth in the power spectrum and subsequent coherent oscillations in a wide spatial frequency band within our resolution limit, demonstrating coherent quasiparticle generation and evolution. Here, the spectrum is observed to oscillate below a quantum limit set by the Peres-Horodecki separability criterion of continuous-variable states, thereby confirming quantum entanglement between interaction quench-induced quasiparticles.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

NASA NTRS1994

Meso-beta scale numerical simulation studies of terrain-induced jet streak mass and momentum perturbations

An in-depth analysis of observed gravity waves and their relationship to precipitation bands over the Montana mesonetwork during the 11-12 July 1981 CCOPE case study indicated two episodes of coherent waves. While geostrophic adjustment, shearing instability, and terrain were all implicated separately or in combination as possible wave generation mechanisms, the lack of upper-air data within the wave genesis region made it difficult to define the genesis processes from observations alone. The first part of this paper, 3D Numerical Modeling Studies of Terrain-Induced Mass/Momentum Perturbations, employs a mesoscale numerical model to help diagnose the intricate early wave generation mechanisms during the first observed gravity wave episode. The meso-beta scale numerical model is used to study various simulations of the role of multiple geostrophic adjustment processes in focusing a region for gravity wave genesis. The second part of this paper, Linear Theory and Theoretical Modeling, investigates the response of non-resting rotating homogeneous and continuously stratified Boussinesq models of the terrestrial atmosphere to temporally impulsive and uniformly propagating three-dimensional localized zonal momentum sources representative of midlatitude jet streaks. The methods of linear perturbation theory applied to the potential vorticity (PV) and wave field equations are used to study the geostrophic adjustment dynamics. The total zonal and meridional wind perturbations are separated into geostrophic and ageostrophic components in order to define and follow the evolution of both the primary and secondary mesocirculations accompanying midlatitude jetogenesis forced by geostrophic adjustment processes. This problem is addressed to help fill the gap in understanding the dynamics and structure of mesoscale inertia-gravity waves forced by geostrophic adjustment processes in simple two-dimensional quiescent current systems and those produced by mesoscale numerical models simulating the orographic and diabatic perturbation of three-dimensional quasi-geostrophically balanced synoptic scale jet streaks associated with complex baroclinic severe storm producing environments.

Lin, Yuh-Lang↗

DOE OSTI2020

Imaging the Phase Transformation in Single Particles of Lithium Titanate Anode for Lithium-ion Batteries

Lithium uptake and release in lithium titanate (LTO) anode materials during a discharge and charge cycle is one of the fundamental processes of a Lithium-ion battery (LIB), still not fully understood at the microscopic level.During discharge cycle, LTO undergoes a phase transformation between Li 4 Ti 5 O 12 and Li 7 Ti 5 O 12 states within a cubic crystal lattice. To reveal the details of the microscopic mechanism,it is necessary to track the sequence of phase transformation sat different discharge/charge states under operating conditions.Here we use in-situ Bragg Coherent Diffraction Imaging (BCDI) and in-situ X-ray diffraction (XRD) experiments to examine the lithium insertion-induced materials phase transformation within a single LTO particle anda bulk battery analogue,respectively. BCDI analysis from (111) Bragg peak, shows the two-phase transformation manifesting as a distinct image phase modulation within a single LTO nanoparticle occurring in the middle of the discharge region then subsiding towards the end of the discharge cycle. We observe the biggest phase variation at the two-phase stage,indicating the formation of phase domains of 200 nm in size during the discharge process. Additionally, we also observe a lattice contraction of >0.2% in a single LTO nanoparticle at the (400) Bragg peak measurement, larger than that in the corresponding bulk material. Our observation of this phase transformation at a single particle level has implications for the understanding of the microscopic/mesoscale picture of the phase transformation in anode and cathode LIBs materials.

25 ENERGY STORAGE↗

DOE OSTI2026

Nanoscale ultrafast lattice modulation with a free-electron laser

Ultrafast optical laser-based techniques have enabled the probing of atomistic processes at their intrinsic temporal scales with femto- and attosecond resolution. However, the long wavelengths of optical lasers have prevented their interrogation and manipulation with nanoscale spatial specificity. Advances in hard X-ray free-electron lasers have enabled progress in developing X-ray transient-grating spectroscopy, a technique that aims to coherently control elementary excitations with nanoscale X-ray standing waves. Thus far, the realization of this technique at the nanoscale has been a challenge. Here we demonstrate X-ray transient-grating spectroscopy with spatial periods of the order of 10 nm via the subfemtosecond synchronization of two hard X-ray pump pulses at a precisely controlled crossing angle. This creates a thermal grating and preferentially excites coherent longitudinal acoustic phonon modes with the transient-grating wavevector. On probing with a third, variably delayed, X-ray pulse with the same photon energy, time-and-wavevector-resolved measurements of the modulation of the induced scattering intensity provide evidence of ballistic thermal transport at nanometre scales. Finally, these results highlight the potential of X-ray transient gratings as a powerful platform for studying nanoscale transport in condensed matter and the coherent control of nanoscale dynamics.

nonlinear optics↗

DOE OSTI2024

Persistence of Spin Coherence in a Crystalline Environment

Here, we analyze quantum interference in the triplet-exciton pair generated by singlet exciton fission in a molecular crystal and introduce transport-induced dephasing (TID) as a key effect that can suppress the expected fluorescence quantum beats when the triplet-exciton wave function can localize on inequivalent sites. TID depends on the triplet-exciton hopping rate between inequivalent sites and on the energy shifts among the stationary states of the entangled triplet pair in different spatial configurations. The theoretical model is confirmed by experiments in rubrene single crystals, where triplet pairs remain entangled for more than 50 ns but quantum beats are suppressed by TID within a few nanoseconds when the magnetic field is misaligned by just a few degrees from specific symmetric directions. Our experiments deliver the zero-field parameters for the rubrene molecule in its orthorhombic lattice and information on triplet-exciton transport, in particular, the triplet-exciton hopping rate between inequivalent sites, which we evaluate to be of the order of 150 ps in rubrene.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

DOE OSTI2025

Non-Equilibrium in a Dust-Forming Low-Temperature Plasma: A CARS Study

Dust-forming low-temperature plasmas are versatile systems for the production of nanoparticles with tunable functionalities. While attractive from a materials processing point of view, these systems are inherently complex, with several plasma-induced phenomena determining the properties of the produced materials. Here, we characterize a carbon nanoparticle-forming plasma using coherent anti-Stokes Raman spectroscopy (CARS), with the primary goal of measuring gas temperature. While gas temperature is typically assumed to be at or slightly above room temperature in these reactors, we measure gas temperatures exceeding 1000 K under typical process conditions. We find a correlation between the gas temperature and the nanoparticle yield, suggesting that the particle nucleation and growth process releases energy within the reaction volume, leading to significant gas heating. In addition, we find that the relaxation of vibrationally excited species at the particle surfaces is a major contributor to their heating. In conclusion, these results underscore the complexity of these systems and the need for their more in-depth characterization using advanced techniques such as CARS.

Basic Plasma Phenomena and Gas Discharges↗

DOE OSTI2023

Giant self-driven exciton-Floquet signatures in time-resolved photoemission spectroscopy of MoS 2 from time-dependent GW approach

Time-resolved, angle-resolved photoemission spectroscopy (TR-ARPES) is a one-particle spectroscopic technique that can probe excitons (two-particle excitations) in momentum space. We present an ab initio, time-domain GW approach to TR-ARPES and apply it to monolayer MoS 2 . We show that photoexcited excitons may be measured and quantified as satellite bands and lead to the renormalization of the quasiparticle bands. These features are explained in terms of an exciton-Floquet phenomenon induced by an exciton time–dependent bosonic field, which are orders of magnitude stronger than those of laser field–induced Floquet bands in low-dimensional semiconductors. Our findings imply a way to engineer Floquet matter through the coherent oscillation of excitons and open the new door for mechanisms for band structure engineering.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

DOE OSTI2021

Distributed Acoustic Sensing Based on Coherent Microwave Photonics Interferometry

A microwave photonics method has been developed for measuring distributed acoustic signals. This method uses microwave-modulated low coherence light as a probe to interrogate distributed in-fiber interferometers, which are used to measure acoustic-induced strain. By sweeping the microwave frequency at a constant rate, the acoustic signals are encoded into the complex microwave spectrum. The microwave spectrum is transformed into the joint time–frequency domain and further processed to obtain the distributed acoustic signals. The method is first evaluated using an intrinsic Fabry Perot interferometer (IFPI). Acoustic signals of frequency up to 15.6 kHz were detected. The method was further demonstrated using an array of in-fiber weak reflectors and an external Michelson interferometer. Two piezoceramic cylinders (PCCs) driven at frequencies of 1700 Hz and 3430 Hz were used as acoustic sources. The experiment results show that the sensing system can locate multiple acoustic sources. The system resolves 20 nε when the spatial resolution is 5 cm. The recovered acoustic signals match the excitation signals in frequency, amplitude, and phase, indicating an excellent potential for distributed acoustic sensing (DAS).

47 OTHER INSTRUMENTATION↗

NASA NTRS1988

Characterization of electron-beam induced damage structures in natural fluorite, CaF2, by analytical electron microscopy

This paper describes the damage structure induced in natural CaF2 by the electron beam when using TEM. The observed 10-20 nm periodic features with coherent fringe patterns and the pronounced loss of fluorine found after the TEM exposure of 100-line-oriented and 111-oriented sections of CaF2 provides support for the mechanism of damage by decomposition of CaF2 into 2F and Ca, with the Ca precipitates maintaining a close topotaxial relationship with the parent CaF2.

Blake, D. F.↗

NASA NTRS2014

Northern Late Winter Planetary Waves: MRO/MARCI Observations and Mars Climate Model Simulations

As does Earth, Mars presents pronounced global atmospheric circulation patterns. Solar differential heating drives mean meridional overturning (Hadley) circulations which are deep and intense, are hemispherically asymmetric, and where a cross-equatorial single cell dominates. Within middle and high latitudes, thermally indirect eddy-driven (Ferrel) circulation cells have been indicated. Differently, however, large-amplitude orography on planetary and continental scales on Mars can force very non-Earth-like hemispheric circulation patterns. Recent observations from the Mars Reconnaissance Orbiter, "Mars Color Imager" (MARCI) instrument are utilized that emphasize water ice clouds in ultra-violet (UV) wavelengths, and these measurements have been binned into "daily global maps" (DGMs) of water-ice cloud optical depth. The presence of large-scale, extratropical quasi-stationary atmospheric wave disturbances in middle and late winter of the northern hemisphere have been found to be present in such DGMs. In combination with such observations, a full-physics Mars global climate model (NASA ARC marsgcm 2.1) is applied to place the observations into context. During late northern winter, it is found that strong, forced Rossby modes (i.e., planetary waves) exist, and with direct correlation to columnintegrated cloud opacity undulating spatial patterns. At this season, zonal wavenumber s = 2 dominates (in contrast to wavenumber s = 1), consistent with MGS/TES analyses at this particular season (Banfield et al., 2003). Large-scale, planetary waves dictate the "coherence" of the northern polar vortex. Fundamentally, such forced planetary waves influence the polar vortex's impermeability (wave-induced) to tracer transport (e.g., dust and water-ice aerosol) and temporal mean water vapor spatial variations. The large-scale dynamical features of such planetary waves will be highlighted and discussed.

Northern polar vortex↗

DOE OSTI2022

Micro-strains, local stresses, and coherently diffracting domain size in shock compressed Al(100) single crystals

In situ x-ray diffraction (XRD) measurements and their analysis in Al single crystals shock compressed along the [100]-direction were utilized to examine shock wave induced microstructural heterogeneities. High-resolution XRD line profiles for the 200, 400, and 600 Al peaks were measured in uniaxial strain compression states to either 5.6 or 11.7 GPa and partial stress release to 3.5 or 6.6 GPa, respectively. Broadening of the XRD line profiles was analyzed to determine the magnitude of the longitudinal micro-strain distribution (0.195% and 0.28% full width at half maximum for 3.5 and 6.6 GPa stresses, respectively) and the size of coherently diffracting domains (CDDs) (0.125 and 0.07 μm for 3.5 and 6.6 GPa stresses, respectively). From the longitudinal micro-strain distributions, the distribution of local stress differences (or stress deviators) was obtained in the shocked state. The full width at half maximum of this distribution, a measure of the local stress inhomogeneities, is greater than half of the macroscopic stress difference for both 3.5 and 6.6 GPa peak stresses, suggesting considerable variation in local stress deviators. The CDD sizes determined here are comparable to characteristic length scales for defect-free regions determined from defect density measurements in post-shock recovery experiments. As a result, the present work represents an important step in understanding material microstructure and inhomogeneities in the shock-compressed state.

36 MATERIALS SCIENCE↗

DOE OSTI2022

Soot-particle core-shell and fractal structures from small-angle X-ray scattering measurements in a flame

We have characterized soot particles measured in situ in a laminar co-flow ethylene-air diffusion flame using small-angle X-ray scattering (SAXS). The analysis includes temperature measurements made with coherent anti-Stokes Raman spectroscopy (CARS) and complements soot volume-fraction and maturity measurements made with laser-induced incandescence (LII). We compared the results of fits to the SAXS measurements using a unified model and a fractal core-shell model. Power-law parameters yielded by the unified model indicate that aggregates of primary particles are in the mass-fractal regime, whereas the primary particles are in the surface-fractal regime in the middle of the flame. Higher and lower in the flame, the primary-particle power-law parameter approaches 4, suggesting smooth primary particles. Furthermore, these trends are consistent with fits using the fractal core-shell model, which indicate that particles have an established core-shell structure in the middle of the flame and are internally homogeneous at higher and lower heights in the flame. Primary-particle size distributions derived using the fractal core-shell model demonstrate excellent agreement with distributions inferred from transmission electron microscopy (TEM) images in the middle of the flame. Higher in the flame, a second small mode appears in the size distributions, suggesting particle fragmentation during oxidation. Surface oxidation would explain (1) aggregate fragmentation and (2) loss of core-shell structure leading to smoother primary-particle surfaces by removal of carbon overlayers. SAXS measurements are much more sensitive to incipient and young soot particles than LII and demonstrate significant volume fraction from particles low in the flame where the LII signal is negligible.

42 ENGINEERING↗

DOE OSTI2025

Competing conduction mechanisms in high performance carbon nanotube fibers

The performance of carbon nanotube (CNT) cables, a contender for copper-wire replacement, is tied to its metallic and semi-conducting-like conductivity responses with temperature; the origin of the semi-conducting-like response however is an underappreciated incongruity in literature. With controlled aspect-ratio and doping-degree, over 61 unique cryogenic experiments including anisotropy and Hall measurements, CNT cable performance is explored at extreme temperatures (65 mK) and magnetic-fields (60 T). A semi-conducting-like conductivity response with temperature becomes temperature-independent approaching absolute-zero, uniquely demonstrating for the first time the necessity of heterogeneous fluctuation induced tunneling; complete de-doping leads to localized hopping, contrasting graphite's pure metallic-like response. High-field magneto-resistance (including novel +22 % longitudinal magneto-resistance near room-temperature) is analyzed with hopping and classical two-band models, both yielding a similar parameter useful for conductor development. Varying field-orientation angle uncovers significant two- and four-fold symmetries that are shown to be from Aharonov-Bohm-like corrections to the curvature-induced bandgap, a first for macroscale CNT fibers. Tight-binding calculations using Green's Function formalism model the largest, coherent transport to-date in commensurate CNT bundles in magnetic-field, revealing non-uniform transmission across bundle cross-sections with doping restoring uniformity; independent of doping, transport in bundle-junction-bundle systems are predominantly from CNTs adjacent to the other bundle—demonstrating that smaller bundles are more efficient for electronic transport. The final impact is predicting the ultimate conductivity of heterogeneous CNT cables using temperature and field-dependent transport, surpassing conductivity of traditional metals.

36 MATERIALS SCIENCE↗

DOE OSTI2020

Hydrogenation of Pyrolysis Oil from Loblolly Pine Residue

Loblolly pine residue prepared with and without zeolite ZSM-5 was pyrolyzed at 60°C and the pyrolysis oil was hydrogenated using formic acid as a hydrogen source, in the presence of a Ru/activated carbon catalyst. As indicated by the pyrolysis yield, addition of the zeolite ZSM-5 increased the yield of light oil but decreased the yield of heavy oil. The pyrolysis oils were analyzed by 13 C, 31 P, 19 F, and heteronuclear single quantum coherence or heteronuclear single quantum correlation nuclear magnetic resonance (HSQC-NMR), demonstrating that the zeolite ZSM-5 can efficiently induce decarboxylation reactions and decrease the content of aliphatic hydroxyl groups in the heavy oil by 57%. After hydrogenation of the pyrolysis oil, the aromatic carbon content decreased by 78%, with a significant increase in the aliphatic carbon content.

hydrogenation↗

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 OSTI2025

Fast and High-Fidelity SNAP Gate Enabled by Optimal Control on Floquet-Engineered Systems

Superconducting cavities with high quality factors, coupled to nonlinear ancilla, provide a promising platform for quantum information storage and manipulation. However, the commonly used selective number-dependent arbitrary phase (SNAP) gate faces significant challenges in ultra-high-coherence cavities, where weak dispersive shifts result in prolonged gate times. Here, we propose a protocol to achieve high-fidelity SNAP gates that are orders of magnitude faster than the standard implementation, breaking the speed limit set by the bare dispersive shift. This enhancement is achieved by dynamically amplifying dispersive coupling via sideband interactions, followed by quantum optimal control on Floquet-engineered systems. Additionally, we present a unified perturbation theory that explains both the gate acceleration and associated benign drive-induced decoherence, corroborated by Floquet\textendash Markov simulations. These results pave the way for the experimental realization of high-fidelity control of weakly coupled, high-coherence cavities, and expanding the scope of optimal control techniques in Floquet quantum systems.

You, Xinyuan [Fermilab]↗

NASA NTRS2019

Radiative Feedbacks Associated with the Madden-Julian Oscillation

Radiative kernels derived from CloudSat/CALIPSO measurements are used to diagnose radiative feedbacks induced by the Madden-Julian oscillation (MJO). Over the Indo-Pacific warm pool, positive cloud and water vapor feedbacks are coincident with the convective envelope of the MJO during its active phases, whereas the lapse rate feedback shows less obvious correlation to the propagating disturbance. During phase 2/3, when the convective envelope is over the Indian Ocean, water vapor exhibits a vertically coherent response, with the largest anomalies and strongest feedback in the middle troposphere. Though spatial structures of the feedbacks vary, the most prominent difference lies in the magnitude. Cloud changes induce the largest radiative perturbations associated with the MJO. We also find that for individual MJO events, cloud feedback and precipitation are highly correlated, suggesting that the strength of individual MJO events is largely dictated by the magnitude of cloud radiative heating of the atmosphere. In addition, stronger radiative heating due to water vapor and clouds helps the MJO survive the barrier effect of the Maritime Continent, leading to further eastward propagation. These results offer process-oriented metrics that could help to improve model simulations and predictions of the MJO in the future.

radiative feedbacks↗

DOE OSTI2026

Topochemical Oxidation of Ruddlesden–Popper Nickelates Reveals Distinct Structural Family: Oxygen-Intercalated Layered Perovskites

Layered perovskites─including the Dion–Jacobson, Ruddlesden–Popper, and Aurivillius families─exhibit a wide range of correlated electron phenomena, from high-temperature superconductivity to multiferroicity. Here, in this study, we report a new family of layered perovskites realized through topochemical oxidation of La n+1 Ni n O 3n+1+δ (n = 1–4) Ruddlesden–Popper nickelate thin films. Postgrowth ozone annealing induces a substantial c-axis expansion─17.8% for La 2 NiO 4+δ (n = 1)─that monotonically decreases with increasing n. Surface synchrotron X-ray diffraction and coherent Bragg rod analysis (COBRA) reveal that this structural expansion arises from the intercalation of approximately δ ≈ 0.7–1.0 oxygen atoms into interstitial sites within the rock salt spacer layers, far exceeding the previous record of δ ≈ 0.3 for any Ruddlesden–Popper oxide. These oxygen-intercalated phases form a new class of layered perovskites with a spacer layer composition intermediate between the Ruddlesden–Popper and Aurivillius phases. Furthermore, oxygen intercalation induces metallicity, enhances nickel–oxygen hybridization, and suppresses oxygen octahedral rotations, a feature associated with high-temperature superconductivity in Ruddlesden–Popper nickelates. Our work establishes topochemical oxidation as a powerful approach to accessing highly oxidized, metastable phases across a broad range of layered oxide systems, offering new platforms to engineer electronic properties via intercalation chemistry.

Ferenc Segedin, Dan [Harvard Univ., Cambridge, MA ↗