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At least 145 records · Page 8

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DOE OSTI2024

A parametrically programmable delay line for microwave photons

Delay lines that store quantum information are crucial for advancing quantum repeaters and hardware efficient quantum computers. Traditionally, they are realized as extended systems that support wave propagation but provide limited control over the propagating fields. Here, we introduce a parametrically addressed delay line for microwave photons that provides a high level of control over the stored pulses. By parametrically driving a three-wave mixing circuit element that is weakly hybridized with an ensemble of resonators, we engineer a spectral response that simulates that of a physical delay line, while providing fast control over the delay line’s properties. We demonstrate this novel degree of control by choosing which photon echo to emit, translating pulses in time, and even swapping two pulses, all with pulse energies on the order of a single photon. We also measure the noise added from our parametric interactions and find it is much less than one photon.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

DOE OSTI2024

Nanometer-Scale Acoustic Wave Packets Generated by Stochastic Core-Level Photoionization Events

We demonstrate that the absorption of femtosecond hard x-ray pulses excites quasispherical, high-amplitude, and high-wave-vector coherent acoustic phonon wave packets using an all hard-x-ray pump-probe scattering experiment. The time- and momentum-resolved diffuse scattering signal is consistent with an ensemble of 3D strain wave packets induced by the rapid electron cascade dynamics following photoionization at uncorrelated excitation centers. We quantify key parameters of this process, including the localization size of the stress field and the photon energy conversion efficiency into elastic energy. The parameters are determined by the photoelectron and Auger electron cascade dynamics, as well as the electron-phonon interaction. In particular, we obtain the localization size of the observed strain wave packet to be 1.5 and 2.5 nm for bulk SrTiO 3 and KTaO 3 single crystals, respectively. The results provide crucial information on the mechanism of x-ray energy deposition into matter and shed light on the shortest collective length scales accessible to coherent acoustic phonon generation using x-ray excitation. Published by the American Physical Society 2024

36 MATERIALS SCIENCE↗

DOE OSTI2020

Scattering of an utlrashort laser pulse by a spherical air bubble

The scattering of an ultrashort laser pulse by an air bubble in water is investigated by means of the Lorenz-Mie theory and the Debye expansion. A 70 fs, 800 nm pulse is considered as a plane wave with a Gaussian temporal envelope. The transient response is treated with the theory derived from Gouesbet and Gréhan [ Part. Part. Syst. Charact. 17 , 213 –224 ( 2000 ) ], taking now into account chromatic dispersion and absorption of water. It is observed that contrary to the case of water droplet in air, the Debye modes p ≥ 1 start their transient scattering at the same time and the same angle (≈90 ° ) and for a large size parameter, they differentiate as time elapses. A parametric study on the size parameter and the spatial extension of the pulse is performed to identify regimes where the different Debye mode are distinguishable in time. Dependence on the scattering angle is also treated. Finally, by considering pulse chirp, it is shown that the laser/bubble distance has an influence on the separability of modes p = 0 and p = 1.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

DOE OSTI2021

Laser-plasma acceleration beyond wave breaking

Laser wakefield accelerators rely on the extremely high electric fields of nonlinear plasma waves to trap and accelerate electrons to relativistic energies over short distances. When driven strongly enough, plasma waves break, trapping a large population of the background electrons that support their motion. Aside from limiting the maximum electric field, this trapping can lead to accelerated electron bunches with large energy spreads. Here we introduce a novel regime of plasma wave excitation and wakefield acceleration that allows for arbitrarily high electric fields while avoiding the deleterious effects of unwanted trapping. Here, the regime, enabled by spatiotemporal shaping of laser pulses, exploits the property that nonlinear plasma waves with superluminal phase velocities cannot trap charged particles and are therefore immune to wave breaking.

36 MATERIALS SCIENCE↗

DOE OSTI2022

Real-time laser ultrasonic monitoring of laser-induced thermal processes

Abstract Intra- and inter-layer integrity of components fabricated with advanced manufacturing techniques, such as laser powder bed fusion, is dependent upon rapid heating, melting, and solidification processes. There is a need for new techniques to provide in situ feedback of these processes. Here a laser-based ultrasonic technique to probe thermal effects induced by a high-power continuous wave laser in titanium samples is described. Numerical simulations were performed to show that, for a spatially uniform heating beam, laser-induced surface acoustic waves are strongly influenced by surface heating conditions, are dispersive in the case of rapid heating, and that an abrupt velocity reduction happens upon the onset of surface melting. Furthermore, laser-based ultrasound experimental results which monitor the transient change of surface wave travel time associated with high power laser surface heating are provided. A pulsed laser is used to generate high frequency surface acoustic waves that propagate through the laser-heated region and are detected using a photorefractive crystal-based interferometer. Qualitative agreement is observed between theory and experiment with both showing a rapid reduction in the surface wave velocity at the onset of illumination and further decrease in surface wave velocity associated with melting. It is demonstrated that changes in the surface wave velocity can be used to track local heating and detect the onset of surface melting in real time.

36 MATERIALS SCIENCE↗

DOE OSTI2020

Broad band tunable energy electron beam pulser

An electromagnetic mechanical pulser implements a transverse wave metallic comb stripline TWMCS kicker having inwardly opposing teeth that retards a phase velocity of an RF traveling wave to match the kinetic velocity of a continuous electron beam, causing the beam to oscillate before being chopped into pulses by an aperture. The RF phase velocity is substantially independent of RF frequency and amplitude, thereby enabling independent tuning of the electron pulse widths and repetition rate. The TWMCS further comprises an electron pulse picker (EPP) that applies a pulsed transverse electric field across the TWMCS to deflect electrons out of the beam, allowing only selected electrons and/or groups of electrons to pass through. The EPP pulses can be synchronized with the RF traveling wave and/or with a pumping trigger of a transverse electron microscope (TEM), for example to obtain dynamic TEM images in real time.

42 ENGINEERING↗

DOE OSTI2025

Photon acceleration of high-intensity vector vortex beams into the extreme ultraviolet

Extreme ultraviolet (XUV) light sources allow for the probing of bound electron dynamics on attosecond scales, interrogation of high-energy-density matter, and access to novel regimes of strong-field quantum electrodynamics. Despite the importance of these applications, coherent XUV sources remain relatively rare, and those that do exist are limited in their peak intensity and spatio-polarization structure. Here, we demonstrate that photon acceleration of an optical vector vortex pulse in the moving density gradient of an electron beam–driven plasma wave can produce a high-intensity, tunable-wavelength XUV pulse with the same vector vortex structure as the original pulse. Quasi-3D, boosted-frame particlein- cell simulations show the transition of optical vector vortex pulses with 800-nm wavelengths and intensities below 10 18 W/cm 2 to XUV vector vortex pulses with 36-nm wavelengths and intensities exceeding 10 20 W/cm 2 over a distance of 1.2 cm. The XUV pulses have sub-femtosecond durations and nearly flat phase fronts. The production of such high-quality, high-intensity XUV vector vortex pulses could expand the utility of XUV light as a diagnostic and driver of novel light–matter interactions.

43 PARTICLE ACCELERATORS↗

DOE OSTI2025

Continuum-electron interferometry for enhancement of photoelectron circular dichroism and measurement of bound, free, and mixed contributions to chiral response

We develop photoelectron interferometry based on laser-assisted extreme ultraviolet ionization for flexible and robust control of photoelectron circular dichroism in randomly oriented chiral molecules. A comb of XUV photons ionizes a sample of chiral molecules in the presence of a time-delayed infrared or visible laser pulse promoting interferences between components of the XUV-ionized photoelectron wave packet. In striking contrast to multicolor phase control schemes relying on pulse shaping techniques, the magnitude of the resulting chiral signal is here controlled by the time delay between the XUV and laser pulses. Furthermore, we show that the relative polarization configurations of the XUV and IR fields allow for disentangling the contributions of bound and continuum states to the chiral response. Our proposal provides a simple, robust, and versatile tool for the control of photoelectron circular dichroism and experimentally feasible protocol for probing the individual contributions of bound and continuum states to the photoelectron circular dichroism in a time-resolved manner.

atomic and molecular processes in external fields↗

DOE OSTI2023

Stability of the modulator in a plasma-modulated plasma accelerator

We explore the regime of operation of the modulator stage of a recently proposed laser-plasma accelerator scheme [Phys. Rev. Lett. 127, 184801 (2021)], dubbed the plasma-modulated plasma accelerator (P-MoPA). The P-MoPA scheme offers a potential route to high-repetition-rate, GeV-scale plasma accelerators driven by picosecond-duration laser pulses from, for example, kilohertz thin-disk lasers. The first stage of the P-MoPA scheme is a plasma modulator in which a long, high-energy “drive” pulse is spectrally modulated by copropagating in a plasma channel with the low-amplitude plasma wave driven by a short, low-energy “seed” pulse. The spectrally modulated drive pulse is converted to a train of short pulses, by introducing dispersion, which can resonantly drive a large wakefield in a subsequent accelerator stage with the same on-axis plasma density as the modulator. In this paper we derive the 3D analytic theory for the evolution of the drive pulse in the plasma modulator and show that the spectral modulation is independent of transverse coordinate, which is ideal for compression into a pulse train. We then identify a transverse mode instability (TMI), similar to the TMI observed in optical fiber lasers, which sets limits on the energy of the drive pulse for a given set of laser-plasma parameters. We compare this analytic theory with particle-in-cell (PIC) simulations and find that even higher energy drive pulses can be modulated than those demonstrated in the original proposal.

43 PARTICLE ACCELERATORS↗

DOE OSTI2022

Experimental Verification of Pulse Shaping in Elastic Metamaterials Under Impact Excitation

Here, we present experimental verification of pulse shaping in elastic metamaterials together with a procedure to design, fabricate, and verify metamaterial pulse shapers under impact excitation. The split Hopkinson pressure bar (SHPB) test, a fundamental dynamic test introduced more than 70 years ago, often incorporates pulse shaping as a means to alter a stress wave, providing the primary motivation for the presented study. Elastic metamaterials hold promise for enhancing conventional pulse shaping abilities and improving capabilities of the SHPB test. We first design the pulse shaper by numerically optimizing its response using finite element analysis. The pulse shaper consists of repeated unit cells based on a combination of a phononic crystal and a local resonator. Then, we fabricate and test pulse shaper candidates to validate the procedural efficacy. An iterative element corrects inaccuracies in input force and material properties and allows convergence on an appropriate pulse shaper. We carry out this procedure by designing pulse shapers fabricated from 3D-printed polylactic acid (PLA) to achieve an extended dwell acceleration pulse shape. In experimental impact tests, the procedure results in rise, dwell, and fall behaviors comparable to that predicted, effectively confirming the efficacy of the presented procedure and verifying the performance of metamaterial-based pulse shapers.

36 MATERIALS SCIENCE↗

DOE OSTI2025

Characterizing IHE Response to Multiple Shock Loading

The response of high explosives to shock loading is traditionally measured with a steady loading pressure. In many accident scenarios involving fragment impact, however, a loading duration that is shorter than the build up to detonation may occur. Fragments passing through multiple materials before reaching a high explosive charge may produce loading that is comprised of more than one shock wave. Additionally, the build up to detonation in high explosive corner turning loads the explosive a short duration pressure pulse, since rarefactions can often rapidly overtake the reactive wave. For these reasons, we have studied the response of the insensitive high explosive (IHE) materials PBX 9502 and LX-17 to complex loadings of varied intensity and duration. We refer to a single loading of limited duration as a “thin pulse”, whereas more complex scenarios were studied with an impactor that produces a double shock in the explosive. The following report presents experimental data and analyses of thin pulse shock initiation and double shock experiments designed to guide development of models of Insensitive High Explosives (IHEs) under controlled one-dimensional conditions relevant to accident scenarios and corner turning. Thin pulse shock initiation data on PBX 9502 and LX-17 were obtained under varied pulse duration, pressed density, and temperature conditions in order to probe various parameters essential for the development of a physics-based Cheetah reactive flow hotspot model. In situ pressure gauges provide insight into the degree of reaction in the explosive that are not obtainable with optical PDV measurements or distance measurements such as run to detonation. Double shock data was obtained to inform a Composition Aware Cheetah model which can be applied to any TATB-based IHEs. This model supports efforts to find a new IHE formulation and potentially incorporate new binders into IHE formulations. Simulations of each experiment are included to demonstrate the utility of these focused experiments to developing models of HE behavior. One-dimensional gas gun experiments are essential for characterizing shocked HE behavior and informing HE models.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2020

Electron plasma wave Thomson scattering on laboratory plasma jets

Plasma jets created from a 15 lm thick Al foil on a 1 MA pulsed power machine were studied using a new electron plasma wave (EPW) Thomson scattering system in conjunction with previously developed ion acoustic wave (IAW) Thomson scattering and interferometry. These diagnostics give multiple ways of measuring the electron temperature and density of the jet. Analysis of the EPW feature found the on-axis density of the jet to be between 5 X 10 18 and 1.4 X 10 19 cm -3 , which either matched or was higher than interferometry measurements. Outside of the jet, both of these diagnostics measured a density of 7 X 10 17 cm -3 . On one shot, the EPW spectral feature showed two pairs of peaks within a 250 lm scattering length on the edge of the jet, which shows that the boundary of the jet ~1 mm radius jet is 0.1 mm. While electron temperature measurements of the plasma jet are complicated by the probe beam producing inverse bremsstrahlung heating of the jet, comparison of the electron temperature measured between IAW and EPW Thomson scattering showed the EPW feature to imply significantly higher electron temperatures than the IAW feature (e.g., 160 eV vs 70 eV in one case). Various sources of this discrepancy (for example, density gradients, collisions, and a lag in ionization) and their impact on the plasma are discussed.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

DOE OSTI2021

Strain wave pathway to semiconductor-to-metal transition revealed by time-resolved X-ray powder diffraction

One of the main challenges in ultrafast material science is to trigger phase transitions with short pulses of light. Here we show how strain waves, launched by electronic and structural precursor phenomena, determine a coherent macroscopic transformation pathway for the semiconducting-to-metal transition in bistable Ti 3 O 5 nanocrystals. Employing femtosecond powder X-ray diffraction, we measure the lattice deformation in the phase transition as a function of time. We monitor the early intra-cell distortion around the light absorbing metal dimer and the long range deformations governed by acoustic waves propagating from the laser-exposed Ti 3 O 5 surface. We developed a simplified elastic model demonstrating that picosecond switching in nanocrystals happens concomitantly with the propagating acoustic wavefront, several decades faster than thermal processes governed by heat diffusion.

36 MATERIALS SCIENCE↗

DOE OSTI2023

Entangled Photon Correlations Allow a Continuous-Wave Laser Diode to Measure Single-Photon, Time-Resolved Fluorescence

Fluorescence lifetime experiments are a standard approach for measuring excited state dynamics and local environment effects. Here, we show that entangled photon pairs produced from a continuous-wave (CW) laser diode can replicate pulsed laser experiments without phase modulation. As a proof of principle, picosecond fluorescence lifetimes of indocyanine green are measured in multiple environments. Here, the use of entangled photons has three unique advantages. First, low power CW laser diodes and entangled photon source design lead to straightforward on-chip integration for a direct path to distributable fluorescence lifetime measurements. Second, the entangled pair wavelength is easily tuned by temperature or electric field, allowing a single source to cover octave bandwidths. Third, femtosecond temporal resolutions can be reached without requiring major advances in source technology or external phase modulation. Entangled photons could therefore provide increased accessibility to time-resolved fluorescence while also opening new scientific avenues in photosensitive and inherently quantum systems.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2023

Coherent light control of a metastable hidden state

Metastable phases present a promising route to expand the functionality of complex materials. Of particular interest are light-induced metastable phases that are inaccessible under equilibrium conditions, as they often host new, emergent properties switchable on ultrafast timescales. However, the processes governing the trajectories to such hidden phases remain largely unexplored. Here, using time- and angle-resolved photoemission spectroscopy, we investigate the ultrafast dynamics of the formation of a hidden quantum state in the layered dichalcogenide 1T-TaS 2 upon photoexcitation. Our results reveal the nonthermal character of the transition governed by a collective charge-density-wave excitation. Using a double-pulse excitation of the structural mode, we show vibrational coherent control of the phase-transition efficiency. Our demonstration of exceptional control, switching speed, and stability of the hidden state are key for device applications at the nexus of electronics and photonics.

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

Visualization of shocked material instabilities using a fast-framing camera and XFEL four-pulse train

Many questions regarding dynamic materials could be answered by using time-resolved ultra-fast imaging techniques to characterize the physical and chemical behavior of materials in extreme conditions and their evolution on the nanosecond scale. In this work, we perform multi-frame phase-contrast imaging (PCI) of micro-voids in low density polymers under laser-driven shock compression. At the Matter in Extreme Conditions (MEC) Instrument at the Linac Coherent Light Source (LCLS), we used a train of four x-ray free electron laser (XFEL) pulses to probe the evolution of the samples. To visualize the void and shock wave interaction, here, we deployed the Icarus V2 detector to record up to four XFEL pulses, separated by 1-3 nanoseconds. In this work, we image elastic waves interacting with the micro-voids at a pressure of several GPa. Monitoring how the material’s heterogeneities, like micro-voids, dictate its response to a compressive wave is important for benchmarking the performances of inertial confinement fusion energy materials. For the first time in a single sample, we have combined an ultrafast x-ray framing camera and four XFEL pulse train to create an ultrafast movie of micro-void evolution under laser-driven shock compression. Eventually, we hope this technique will resolve the material density as it evolves dynamically under laser shock compression.

fusion↗

DOE OSTI2023

Quantum Emitter Formation Dynamics and Probing of Radiation-Induced Atomic Disorder in Silicon

Near-infrared color centers in silicon are emerging candidates for on-chip integrated quantum emitters, optical-access quantum memories, and sensing. We access ensemble G-color-center formation dynamics and radiation-induced atomic disorder in silicon for a series of megaelectronvolt proton-flux conditions. The photoluminescence results reveal that the G centers are formed more efficiently by pulsed-proton irradiation than by continuous-wave proton irradiation. The enhanced transient excitations and dynamic annealing within nanoseconds allows optimization of the ratio of G-center formation to nonradiative defect accumulation. The G centers preserve narrow line widths of about 0.1 nm when they are generated by moderate pulsed-proton fluences, while the line width broadens significantly as the pulsed-proton fluence increases. This implies vacancy or interstitial clustering by overlapping collision cascades. The tracking of G-center properties for a series of irradiation conditions enables sensitive probing of atomic disorder, serving as a complementary analytical method for sensing damage accumulation. Aided by ab initio electronic structure calculations, we provide insight into the atomic disorder induced inhomogeneous broadening by introducing vacancies, silicon interstitials, and oriented strain fields in the vicinity of a G center. A vacancy leads to a tensile strain and can result in either a red shift or a blue shift of the G-center emission, depending on its position relative to the G center. Meanwhile, Si interstitials lead to compressive strain, which results in a monotonic red shift. In conclusion, high-flux and tunable ion pulses enable the exploration of the fundamental dynamics of radiation-induced defects as well as methods for the optimization of G-center formation and qubit synthesis for quantum information processing.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗