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At least 73 records · Page 4

All hard X-ray transient grating spectroscopy

Optical-domain transient grating (TG) spectroscopy is the ideal tool to investigate transport phenomena in gases, liquids and solids, but it is limited to typically micron-size grating periods. Extreme-Ultraviolet TG has represented a major leap forward to access the mesoscopic scales. Hard X-ray TGs open access in principle to the nanoscale. Hard X-ray TGs were recently generated using the Talbot effect and probed by optical pulses, but these hinder exploiting the advantages of the nanoscale gratings. Here, we present an all-X-ray TG study, in which few-femtosecond hard X-ray pulses are used both for excitation and probing. Our experiment was performed on an amorphous film of an FeGd alloy and on a thin silicon single crystal. The results show a manifestation of the TG induced by the X-ray pump and probe pulses in the form of Talbot carpets, as well as temporal evolution of the grating in crystalline silicon showing coherent optical phonons. Ultrafast all-X-ray TG spectroscopy has the potential to study fundamental excitations with femtosecond time resolution and nanometer spatial sensitivity.

Ferrari, Eugenio [Deutsches Elektronen-Synchrotron↗

Enhancing Coherence Limits in Superconducting Quantum Systems for Computing and Sensing

This talk will highlight recent efforts at the SQMS Center to develop qudit-based quantum computing architectures using superconducting three-dimensional (3D) cavities, as well as the use of these ultra-coherent cavities for quantum sensing. I will present systematic studies of materials and devices aimed at identifying and mitigating the dominant sources of decoherence—including two-level systems (TLS), quasiparticles, and other noise mechanisms—in both transmons and 3D cavities. These investigations include microwave loss characterization of niobium, tantalum, aluminum, their native oxides, and substrate materials such as silicon and sapphire. By combining measurements on qubits and cavities, we disentangle subsystem-specific loss mechanisms and establish a hierarchy of mitigation strategies, leading to transmon coherence times exceeding one millisecond. I will also discuss studies of quasiparticle dynamics, including quasiparticle bursts observed in qubits operated both above ground and at the Gran Sasso underground laboratory, and the observation that applied magnetic fields can suppress temporal T₁ fluctuations. Building on these advances, we demonstrate a record-coherence two-cell cavity-qudit system with coherence times exceeding 20 milliseconds. Leveraging tunable sideband interactions together with error-resilient protocols, including measurement-based error correction and post-selection, we achieve high-fidelity quantum state control, including the preparation of Fock states up to N=20 with fidelities above 95% and the generation of high-fidelity two-mode entangled states. Finally, I will discuss how these ultra-coherent quantum systems are enabling emerging quantum sensing applications, including searches for dark matter and gravitational waves.

Roy, Tanay [Fermilab] (ORCID:000000019442862X)↗

Multitiered computational methodology for extracting three-dimensional rotational diffusion coefficients from x-ray photon correlation spectroscopy data without structural information

X-ray photon correlation spectroscopy (XPCS) is a powerful technique for analyzing particle systems by investigating their dynamics in suspensions across a broad range of temporal and spatial scales. This is done by illuminating samples with coherent x-ray beams and calculating the correlation function of the obtained x-ray scattering images. XPCS is uniquely suited for studying Brownian dynamics, consisting of translational and rotational diffusion. While traditional XPCS image analysis techniques can extract translational diffusion components, they are unable to estimate rotational diffusion coefficients. Here, we introduce a methodology that combines the angular-temporal cross-correlation analysis and a algorithmic framework called Multi-Tiered Estimation for Correlation Spectroscopy in 3D for estimating three-dimensional rotational diffusion coefficients from XPCS images of three-dimensional particle systems. We demonstrate our methodology for extracting rotational diffusion coefficients from XPCS data by applying it to simulated noisy x-ray images of systems of crossing nanotubes and proteins that evolve under translational and rotational Brownian motion for different diffusion rates. Furthermore, our results show that our approach determines rotational diffusion coefficients within a few percent error.

97 MATHEMATICS AND COMPUTING↗

Symmetry Protected Two-Photon Coherence Time

We report the observation of symmetry protected two-photon coherence time of biphotons generated from backward spontaneous four-wave mixing in laser-cooled 87 Rb atoms. When biphotons are nondegenerate, nonsymmetric photonic absorption loss results in exponential decay of the temporal waveform of the two-photon joint probability amplitude, leading to shortened coherence time. In contrast, in the case of degenerate biphotons, when both paired photons propagate with the same group velocity and absorption coefficient, the two-photon coherence time, protected by space-time symmetry, remains unaffected by medium absorptive losses. Furthermore, our experimental results validate these theoretical predictions. This outcome highlights the pivotal role of symmetry in manipulating and controlling photonic quantum states.

74 ATOMIC AND MOLECULAR PHYSICS↗

Pushing the Boundaries of Coherence in Superconducting Quantum Systems at the SQMS Center for Computing, Sensing, and Metrology

This talk will highlight recent advances at the SQMS Center in understanding and mitigating decoherence in superconducting quantum systems, focusing on both transmon qubits and 3D superconducting cavities. I will present results from systematic studies of materials and devices, aimed at identifying key sources of loss: including two-level systems (TLS), quasiparticles, and other noise mechanisms. These studies span microwave loss characterization in materials such as niobium, tantalum, aluminum, and their native oxides, as well as substrate losses in silicon and sapphire. Using both qubits and cavities, we disentangle subsystem contributions to loss and develop a hierarchy of mitigation strategies. Through these efforts, we have achieved transmon coherence times exceeding one millisecond. I will also present investigations into quasiparticle dynamics, including bursts observed in qubits located above ground and in the Gran Sasso underground laboratory. Additional studies explore temperature dependence to distinguish between TLS and quasiparticle losses, and reveal that applying a magnetic field can reduce temporal T1 fluctuations in transmons. Building on these results, we demonstrate a record-coherence two-cell cavity-qudit system with coherence times exceeding 20 milliseconds. By leveraging sideband interactions and error-resilient protocols including measurement-based correction and post-selection, we achieve high-fidelity quantum state control. This includes preparation of Fock states up to N = 20 with fidelities over 95%, and two-mode entanglement with coherence-limited fidelities reaching 99.9% after post-selection. These achievements position the SQMS platform as a powerful foundation for scalable quantum information processing and high-dimensional qudit encodings. Finally, I will discuss how these ultra-coherent systems are being deployed in emerging quantum sensing applications, including dark matter searches and gravitational wave detection.

Roy, Tanay [Fermilab]↗

Intermittent cluster dynamics and temporal fractional diffusion in a bulk metallic glass

Glassy solids evolve towards lower-energy structural states by physical aging. This can be characterized by structural relaxation times, the assessment of which is essential for understanding the glass’ time-dependent property changes. Conducted over short times, a continuous increase of relaxation times with time is seen, suggesting a time-dependent dissipative transport mechanism. By focusing on micro-structural rearrangements at the atomic-scale, we demonstrate the emergence of sub-diffusive anomalous transport and therefore temporal fractional diffusion in a metallic glass, which we track via coherent x-ray scattering conducted over more than 300,000 s. At the longest probed decorrelation times, a transition from classical stretched exponential to a power-law behavior occurs, which in concert with atomistic simulations reveals collective and intermittent atomic motion. Our observations give a physical basis for classical stretched exponential relaxation behavior, uncover a new power-law governed collective transport regime for metallic glasses at long and practically relevant time-scales, and demonstrate a rich and highly non-monotonous aging response in a glassy solid, thereby challenging the common framework of homogeneous aging and atomic scale diffusion.

42 ENGINEERING↗

Light-wave-controlled Haldane model in monolayer hexagonal boron nitride

In recent years, the stacking and twisting of atom-thin structures with matching crystal symmetry has provided a unique way to create new superlattice structures in which new properties emerge. In parallel, control over the temporal characteristics of strong light fields has allowed researchers to manipulate coherent electron transport in such atom-thin structures on sublaser-cycle timescales. Here we demonstrate a tailored light-wave-driven analogue to twisted layer stacking. Tailoring the spatial symmetry of the light waveform to that of the lattice of a hexagonal boron nitride monolayer and then twisting this waveform result in optical control of time-reversal symmetry breaking and the realization of the topological Haldane model in a laser-dressed two-dimensional insulating crystal. Further, the parameters of the effective Haldane-type Hamiltonian can be controlled by rotating the light waveform, thus enabling ultrafast switching between band structure configurations and allowing unprecedented control over the magnitude, location and curvature of the bandgap. This results in an asymmetric population between complementary quantum valleys that leads to a measurable valley Hall current, which can be detected by optical harmonic polarimetry. The universality and robustness of our scheme paves the way to valley-selective bandgap engineering on the fly and unlocks the possibility of creating few-femtosecond switches with quantum degrees of freedom.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

The MOSAiC Distributed Network: Observing the coupled Arctic system with multidisciplinary, coordinated platforms

Central Arctic properties and processes are important to the regional and global coupled climate system. The Multidisciplinary drifting Observatory for the Study of Arctic Climate (MOSAiC) Distributed Network (DN) of autonomous ice-tethered systems aimed to bridge gaps in our understanding of temporal and spatial scales, in particular with respect to the resolution of Earth system models. By characterizing variability around local measurements made at a Central Observatory, the DN covers both the coupled system interactions involving the ocean-ice-atmosphere interfaces as well as three-dimensional processes in the ocean, sea ice, and atmosphere. The more than 200 autonomous instruments (“buoys”) were of varying complexity and set up at different sites mostly within 50 km of the Central Observatory. During an exemplary midwinter month, the DN observations captured the spatial variability of atmospheric processes on sub-monthly time scales, but less so for monthly means. They show significant variability in snow depth and ice thickness, and provide a temporally and spatially resolved characterization of ice motion and deformation, showing coherency at the DN scale but less at smaller spatial scales. Ocean data show the background gradient across the DN as well as spatially dependent time variability due to local mixed layer sub-mesoscale and mesoscale processes, influenced by a variable ice cover. The second case (May–June 2020) illustrates the utility of the DN during the absence of manually obtained data by providing continuity of physical and biological observations during this key transitional period. We show examples of synergies between the extensive MOSAiC remote sensing observations and numerical modeling, such as estimating the skill of ice drift forecasts and evaluating coupled system modeling. The MOSAiC DN has been proven to enable analysis of local to mesoscale processes in the coupled atmosphere-ice-ocean system and has the potential to improve model parameterizations of important, unresolved processes in the future.

54 ENVIRONMENTAL SCIENCES↗

Mapping the nonequilibrium order parameter of a quasi-two dimensional charge density wave system

The driving force of a charge density wave (CDW) transition in quasi-two dimensional systems is still debated, while being crucial in understanding electronic correlation in such materials. Here we use femtosecond time- and angle-resolved photoemission spectroscopy combined with computational methods to investigate the coherent lattice dynamics of a prototypical CDW system. The photo-induced temporal evolution of the periodic lattice distortion associated with the amplitude mode reveals the dynamics of the free energy functional governing the order parameter. Our approach establishes that optically-induced screening rather than CDW melting at the electronic level leads to a transiently modified potential which explains the anharmonic behaviour of the amplitude mode and discloses the structural origin of the symmetry-breaking phase transition.

electronic properties and materials↗

Invited article: X-ray phase contrast imaging in inertial confinement fusion and high energy density research

X-ray phase contrast imaging (XPCI) provides enhanced image contrast beyond absorption-based x-ray imaging alone due to refraction and diffraction from gradients in the object material density. It is sensitive to small variations in density, such as internal voids, cracks, grains, defects, and material flow, as well as to stronger density variations such as from a shock wave. Beyond its initial use in biology and materials science, XPCI is now routinely used in inertial confinement fusion (ICF) and high energy density (HED) research, first to characterize ICF capsules and targets, and later applied in dynamic experiments, where coherent x-ray sources, ultrafast x-ray pulses, and high temporal and spatial resolution are required. In this Review article, XPCI image formation theory is presented, its diverse use in ICF and HED research is discussed, the unique requirements for ultrafast XPCI imaging are given, as well as current challenges and issues in its use.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Quantifying the thermal effect and methyl radical production in nanosecond repetitively pulsed glow discharges applied to a methane-air flame

In this work, we investigated non-equilibrium plasma produced by nanosecond repetitively pulsed glow discharges applied across a lean premixed methane-air flame. The flame is stationary, axisymmetric, and laminar. The discharges are applied on the symmetry axis crossing the reactant gases, flame front, and product gases, allowing phase-locked averaged measurements and comparisons with axisymmetric numerical simulations. The thermal effect and methyl radical production are quantified in the discharge in the reactant gas region. One-dimensional, two-beam, hybrid, femtosecond-picosecond, coherent anti-Stokes Raman scattering is used to acquire spatial and temporal profiles of temperature and oxygen-to-nitrogen concentration ratio. Photo-fragmentation laser-induced fluorescence is used to acquire quantitative two-dimensional profiles of methyl radicals in the discharge providing the first quantitative imaging of methyl produced ahead of a flame by plasma-induced methane dissociation. The spatial profiles of temperature and oxygen-to-nitrogen concentration ratio are in steady state, indicating that individual discharges have an insignificant heating effect. Upper and lower bounds of the produced mole fraction of methyl radicals in the plasma are obtained due to uncertainties in the collisional quenching rates of excited state methylidyne radicals in the plasma. The discharges produce a maximum of 600–1100 ppm of methyl radicals upstream of the flame front within 25 ns. This amount is similar to the predicted methyl mole fraction for the flame without plasma and thus represents a significant chemical perturbation to the reactants upstream of the flame front. The produced methyl follows an exponential decay in the first microsecond after the discharge with a decay constant of 8 µs close to the flame, and 0.8 µs further from the flame. The decay then deviates from the exponential curve and the methyl persists for tens of microseconds. The results suggest that for the tested configuration, the thermal effect of individual discharges through fast gas heating is negligible, while active chemical species are produced in large quantities in the reactant gases, upstream of the flame front.

hybrid fs-ps CARS↗

Laser-Modulation-Driven X-Ray Pulse Shaping in Regenerative Amplifier Free-Electron Lasers

In this Letter, we present a robust method for generating custom-shaped, coherent hard x-ray pulses in regenerative amplifier free-electron lasers (RAFELs) using laser-induced energy modulation of the electron beam. A temporally shaped optical modulation imprints an optical-wavelength energy pattern on the beam, which interacts with the recirculated seed in the x-ray cavity to generate spectral sidebands. These sidebands lie outside the Bragg reflection bandwidth and are extracted as out-coupled radiation, while the seed is retained for continued amplification, enabling a novel mechanism for both output coupling and pulse shaping. Furthermore, this approach allows deterministic control over the spectral and temporal properties of the emitted x-rays, including multicolor generation, twin-pulse structures, pulse duration tuning, and complex temporal waveforms. Importantly, it does not require modification of the RAFEL cavity or optics and is fully compatible with high-repetition-rate operation, offering a practical pathway to deliver coherent, shaped, and on-demand x-ray pulses for advanced time-resolved and nonlinear x-ray science.

Free-electron lasers↗

Ultrafast all-optical coherence of molecular electron spins in room-temperature water solution

The tunability and spatial precision of paramagnetic molecules makes them attractive for quantum sensing. However, usual microwave-based detection methods have poor temporal and spatial resolution, and optical methods compatible with room-temperature solutions have remained elusive. In this study, we utilized pump-probe polarization spectroscopy to initialize and track electron spin coherence in a molecule. Designed to efficiently couple spins to light, aqueous potassium hexachloroiridate(IV) enabled detection of few-picosecond free-induction decay at room temperature and micromolar concentrations. Viscosity was found to strongly vary decoherence lifetimes. This approach has improved the experimental time resolution by up to five orders of magnitude, making it possible to observe molecular electron spin coherence in a system that only exhibits coherence below 25 kelvin with traditional techniques.

74 ATOMIC AND MOLECULAR PHYSICS↗

Intermittent Defect Fluctuations in Oxide Heterostructures

Abstract The heterogeneous nature, local presence, and dynamic evolution of defects typically govern the ionic and electronic properties of a wide variety of functional materials. While the last 50 years have seen considerable efforts into development of new methods to identify the nature of defects in complex materials, such as the perovskite oxides, very little is known about defect dynamics and their influence on the functionality of a material. Here, the discovery of the intermittent behavior of point defects (oxygen vacancies) in oxide heterostructures employing X‐ray photon correlation spectroscopy is reported. Local fluctuations between two ordered phases in strained SrCoO x with different degrees of stability of the oxygen vacancies are observed. Ab‐initio‐informed phase‐field modeling reveals that fluctuations between the competing ordered phases are modulated by the oxygen ion/vacancy interaction energy and epitaxial strain. The results demonstrate how defect dynamics, evidenced by measurement and modeling of their temporal fluctuations, give rise to stochastic properties that now can be fully characterized using coherent X‐rays, coupled for the first time to multiscale modeling in functional complex oxide heterostructures. The study and its findings open new avenues for engineering the dynamical response of functional materials used in neuromorphic and electrochemical applications.

36 MATERIALS SCIENCE↗

Overcoming energy limitation in post-compression of picosecond pulses by free beam propagation in air and temporal pulse splitting and recombining

Cryogenically cooled diode-pumped Yb:YAG has been demonstrated to efficiently generate pulses of >1 J energy and several picoseconds duration at a kilohertz repetition rate. Pulse broadening and post-compression techniques capable of operating at these high pulse energies will expand the use of these lasers in applications requiring shorter pulses. Towards this goal, we demonstrate the post-compression of 5.5 ps pulses with energy in the 0.1 J range by spectral broadening of self-collimated large area beams in air. In proof-of-principle experiments, pulses of 65 mJ energy from a cryogenically cooled Yb:YAG laser were compressed to 1.1 ps after 65 m propagation in a compact setup in which the beam was folded using flat mirrors. Further energy scaling was demonstrated by combining this spectral broadening technique with temporal pulse splitting and recombining. 120 mJ pulses were split into two pulses and coherently recombined with 85% efficiency after 50 m of propagation in air to yield 1.4 ps pulses.

High Energy Laser↗

Single-shot observation of nonlinear pulse splitting in a Kerr medium

We report single-shot, time-resolved observation of self-steepening and temporal splitting of near-infrared, 50 fs, micro-joule pulses propagating nonlinearly in flint (SF11) glass. A coherent, smooth-profiled, 60-nm-bandwidth probe pulse that propagated obliquely to the main pulse through the Kerr medium recorded a time sequence of longitudinal projections of the main pulse’s induced refractive index profile in the form of a phase-shift “streak,” in which frequency–domain interferometry recovered with ∼10 fs temporal resolution. A three-dimensional simulation based on a unidirectional pulse propagation equation reproduced observed pulse profiles.

Chang, Yen-Yu↗

Physics Goals of DWA Experiments at FACET-II

The dielectric wakefield acceleration (DWA) program at FACET produced a multitude of new physics results that range from GeV/m acceleration to the discovery of high field-induced conductivity in THz waves, and beyond, to a demonstration of positron-driven wakes. Here we review the rich program now developing in the DWA experiments at FACET-II. With increases in beam quality, a key feature of this program is extended interaction lengths, near 0.5 m, permitting GeV-class acceleration. Detailed physics studies in this context include beam breakup and its control through the exploitation of DWA structure symmetry. The next step in understanding DWA limits requires the exploration of new materials with low loss tangent, large bandgap, and improved thermal characteristics. Advanced structures with photonic features for mode confinement and exclusion of the field from the dielectric, as well as quasi-optical handling of coherent Cerenkov signals is discussed. Use of DWA for laser-based injection and advanced temporal diagnostics is examined.

43 PARTICLE ACCELERATORS↗

Space-Time Quantum Information from the Entangled States of Magnetic Molecule (STI Product)

This collaborative project combines synthesis, measurement, and theory by three faculty members at the Eddleman Quantum Institute of UC Irvine to effectively investigate the quantum properties of molecules in the space, time, and frequency domains. Through synthetic chemistry, molecules are tailored for their magnetic and coherent properties. By combining femtosecond (fs) terahertz (THz) light and a continuous wave (cw) THz laser with a low temperature scanning tunneling microscope (STM), quantum phenomena are probed with simultaneous femtosecond temporal and atomic-scale spatial resolution. In particular, the invention of the quantum superposition microscope (QSM) advances quantum sensing for enhanced spectroscopy and imaging capabilities. Coupling theory to the experimental efforts offers a deeper understanding and predictive power for the molecular systems. The phenomena of superposition, entanglement, and coherence is central to quantum information science and can be realized in qubit states. Many systems can be modeled by a double-well potential in which two levels are formed in the two lowest energy states interacting with the environment and external radiation. In focusing on molecules as two-level systems, the underlying expectation is that their tunable composition and structure allows an effective parameter space to optimize their use as qubits for quantum sensing and computing. The THz radiation induces the superposition between the two states, appearing as temporal oscillations that damp in amplitude. Enhanced spectroscopy and imaging in the time and frequency domains is achieved through the extreme sensitivity of the frequency and damping of coherence of two-level systems to its environment. A single hydrogen molecule trapped in the STM tunneling gap experiences a double-well potential and absorption of THz femtosecond pulses of light creates the superposition of its two levels, appearing as damped oscillations in the light induced direct current (DC). The oscillation frequency depends sensitively on the electric field distribution of the copper nitride (Cu 2 N) surface, through the Stark effect, and associated with the different charge distributions at the copper and nitrogen sites and in between. This QSM can resolve variation in the surface electric field with 0.02 nanometer resolution. In addition, the single hydrogen molecule entaes with nearby hydrogen molecules as seen in the avoided level crossings of energy (oscillation frequency) versus the voltage across the tunneling gap. Thus, the first application of the QSM senses and images the surface electric field at the atomic scale. Results from this project advance fundamental understanding of quantum phenomena, develop novel synthesis, measurement, and theory, provide the knowledge foundation for molecule-based qubits and sensing that enable the development of the QSM and emergent technologies. This project trained researchers in quantum information science, extended knowledge in classrooms, and outreached to the community.

47 OTHER INSTRUMENTATION↗