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Search indexed NASA NTRS and DOE OSTI research on propulsion, heat transfer, battery materials and energy systems. Follow report and document links to the original sources.

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At least 55 records · Page 3

Joint Experimental and Computational Characterization of Sum-Frequency Generation between a Continuous Wave Laser and an Ultrafast Frequency Comb Laser for Tunable Laser Development

Ultrafast optical frequency combs allow for both high spectral and temporal resolution in molecular spectroscopy and have become a powerful tool in many areas of chemistry and physics. Ultrafast lasers and frequency combs generated from ultrafast mode-locked lasers often need to be converted to other wavelengths. Commonly used wavelength conversions are optical parametric oscillators, which require an external optical cavity, and supercontinuum generation combined with optical parametric amplifiers. Whether commercial or home-built, these systems are complex and costly. Here, we investigate an alternative, simple, and easy-to-implement approach to tunable frequency comb ultrafast lasers enabled by new continuous-wave laser technology. Sum-frequency generation between an Nd:YAG continuous-wave laser and a Yb:fiber femtosecond frequency comb in a beta-barium borate (BBO) crystal is explored. The resulting sum-frequency beam is a pulsed frequency comb with the same repetition rate as the Yb:fiber source. SNLO simulation software is used to simulate the results and provide benchmarks for designing future systems to achieve wavelength conversion and tunability in otherwise difficult-to-reach spectral regions.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

The role of ambient gas confinement, plasma chemistry, and focusing conditions on emission features of femtosecond laser-produced plasmas

Ultrafast laser ablation coupled with optical emission spectroscopy is currently under development for standoff detection of elements and their isotopes for a wide range of application areas. In this work, we explore the role of ambient air pressure during the interaction of an ultrafast laser beam with two metallic targets (brass and uranium) with significantly different oxygen gas-phase reactivity. Plasma plumes were generated by focusing ~800 nm, ~35 fs pulses from an ultrafast laser system using a long focal length lens with f = 1 m. Two-dimensional spectral imaging was performed over the pressure range of 30 mTorr-700 Torr air to evaluate emission dynamics, plasma chemistry, signal-to-background ratio, and characteristic parameters (i.e. excitation temperature, electron density). An increase in ambient air pressure during ultrafast laser ablation leads to plume confinement and subsequent changes in the emission dynamics due to plasma chemistry as well as changes in plasma generation conditions (i.e. focused fs laser ablation versus filament ablation). Ablation crater morphologies were also investigated via scanning electron microscopy. Results indicate atomic emission intensity and signal-to-background ratios peak at moderate pressure levels (~50-100 Torr air) for both targets studied, although plasma chemistry influences uranium emission signatures. The emission features of the uranium plasma at pressures = 10 Torr showed the presence of atoms and oxide molecules which are co-located within the plume. We also find filament ablation leads to wider, more shallow craters compared to focused laser ablation. Our study provides unique insight into the interplay between plume dynamics, confinement, and oxygen chemistry of fs laser-produced plasmas and how these phenomena evolve with changing ambient air pressure.

Laser-produced plasma↗

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↗

The interplay between laser focusing conditions, expansion dynamics, ablation mechanisms, and emission intensity in ultrafast laser-produced plasmas

The interplay between ultrafast laser focusing conditions, emission intensity, expansion dynamics, and ablation mechanisms is critical to the detection of light isotopes relevant to nuclear energy, forensics, and geochemistry applications. Here, we study deuterium (2Hα) emission in plasmas generated from femtosecond laser ablation of a Zircaloy-4 target with a deuterium concentration of ≈37 at. %. Changes in emission intensity, plume morphology, crater dimensions, and surface modifications were investigated for varying focusing lens positions, where the laser was focused behind, at, and in front of the target. Spatially resolved optical emission spectroscopy and spectrally integrated plasma imaging were performed to investigate emission spectral features and plume morphology. Laser ablation crater dimensions and morphology were analyzed via optical profilometry and scanning electron microscopy. The 2Hα emission intensity showed significant reduction at the geometrical focal point or when the focal point is in front of the target. For all laser spot sizes, a two-component plume was observed but with different temporal histories. At the best focal point, the plume was spherical. When the laser was focused behind the target, the plume was elongated and propagated to farther distances than for the best focal position. In contrast, when the laser was focused in front of the target, filaments were generated in the beam path, and filament-plasma coupling occurred. By focusing the laser behind the target, the amount of material removal in the laser ablation process can be significantly reduced while still generating a plasma with a sufficient 2Hα emission signal for analysis.

Kautz, Elizabeth J. (ORCID:0000000263389223)↗

Ultrafast laser-driven many-body dynamics and Kondo coherence collapse

Ultrafast laser pulse has provided a systematic way to inspect the dynamics of electrons in condensed matter systems. In this paper, by means of time-dependent density matrix renormalization group, we study an ultrafast laser-driven Kondo lattice model, in which conduction electrons are strongly coupled with magnetically local moments. The single-particle spectral function due to strong correlation effects and photon emission in the nonequilibrium states under laser driving are calculated. We find laser field excited collective doublon-hole pairs and an associated transient melting of Kondo coherence phase, signifying the collapse of Kondo energy gap. Moreover, we show that the photon emission, induced by a strong laser field, exhibits a different intensity characteristics than in the equilibrium Kondo insulator, which could be explained by the Kondo collapse and related suppression of both intraband and interband contribution in Kondo melting liquid. This theoretical insight is accessible with time- and angle-resolved photoemission spectroscopy and high-harmonic generation spectroscopy and will stimulate the investigation of nonequilibrium dynamics and nonlinear phenomenon in heavy fermion systems.

36 MATERIALS SCIENCE↗

Direct visualization of electromagnetic wave dynamics by laser-free ultrafast electron microscopy

Integrating femtosecond lasers with electron microscopies has enabled direct imaging of transient structures and morphologies of materials in real time and space. Here, we report the development of a laser-free ultrafast electron microscopy (UEM) offering the same capability but without requiring femtosecond lasers and intricate instrumental modifications. We create picosecond electron pulses for probing dynamic events by chopping a continuous beam with a radio frequency (RF)–driven pulser with the pulse repetition rate tunable from 100 MHz to 12 GHz. As a first application, we studied gigahertz electromagnetic wave propagation dynamics in an interdigitated comb structure. We reveal, on nanometer space and picosecond time scales, the transient oscillating electromagnetic field around the tines of the combs with time-resolved polarization, amplitude, and local field enhancement. This study demonstrates the feasibility of laser-free UEM in real-space visualization of dynamics for many research fields, especially the electrodynamics in devices associated with information processing technology.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Enabling high rate capability, low internal resistance, and excellent cyclability for vanadium redox flow batteries utilizing ultrafast laser-structured graphite felt

The electrochemical performance of vanadium redox flow batteries (VRFBs) was enhanced via laser-patterned graphite felt (GF) electrodes. The laser-structured GF electrodes engineered via preparing a series of well-ordered microscopic channel structures with an average width of 200 μm, creating a three-dimensional carbon framework. The ultrafast laser patterning increased the porosity by 10%, as compared to pristine electrode. The analysis of the overpotential distribution using electrochemical impedance spectroscopy revealed that the electrode polarization involving charge transfer and diffusion resistance is strongly alleviated with the aid of carbon micro-perforation. The advanced design of laser-structured GF electrode also exhibits high rate capability, low internal resistance, and excellent cyclability. The improved performance was attributed to the synergistic effect involving (i) high electrochemically active surface area for rapid electrochemical reactions (i.e., V(II)/V(III) and V(IV)/V(V) redox couples) and (ii) excellent transport properties for facile electron/ion/species transport. The micro-scale channels created with the laser-ablation technique act as capillary structures and enabled homogeneous and rapid wetting of GF electrodes as formulated with the classical Washburn equation. The VRFB equipped with the laser-structured GF electrodes delivered a high discharge capacity with exceptional capacity retention upon extended cycling (>84.9%). In conclusion, accordingly, the design of laser-structured electrode paves the pathway towards finely tuning the electrode internal microstructure for improved cyclability, durability, and capacity retention in various electrochemical energy storage/conversion devices (e.g. all-vanadium redox flow batteries).

25 ENERGY STORAGE↗

Time-resolved absorption spectroscopic characterization of ultrafast laser-produced plasmas under varying background pressures

Time-resolved tunable laser absorption spectroscopy is used to characterize the physical properties of ultrafast laser-produced plasmas. The plasmas were produced from an Inconel target, with = 0.4 wt. % Al, using ~ 35 fs, ~800 nm laser pulses at varying Ar background pressures from 1-100 Torr. The absorption spectrum of atomic Al is measured with high spectral and temporal resolution when the probe laser is stepped across the selected Al transition at 394.4 nm. Spectral fitting is used to infer linewidths, kinetic temperature, Al column density, and pressure broadening coefficient. The late time physical properties of plasmas are compared for various pressure levels. Our studies highlight that a significant lower state population exists even at early times of ultrafast laser-produced plasma evolution and lower state population persistence decreases with increasing ambient pressure. We also show that the fundamental optical properties, such as pressure-broadening, can be measured using ultrafast laser-produced plasmas combined with laser absorption spectroscopy.

laser absorption spectroscopy, laser produced plas↗

Ultrafast Laser-Excited Optical Emission of Xe under Loose-Focusing Conditions

The optical filament-based radioxenon sensing can potentially overcome the constraints of conventional detection techniques that are relevant for nuclear security applications. This study investigates the spectral signatures of pure xenon (Xe) when excited by ultrafast laser filaments at near-atmosphericpressure and in short and loose-focusing conditions. The two focusing conditions lead to laser intensity differences of several orders of magnitude and different plasma transient behavior. The gaseous sample was excited at atmospheric pressure using ∼7 mJ pulses with a 35 fs pulse duration at 800 nm wavelength. The optical signatures were studied by time-resolved spectrometry and imaging in orthogonal light collection configurations in the ∼400 nm (VIS) and ∼800 nm (NIR) spectral regions. The most prominent spectral lines of atomic Xe are observable in both focusing conditions. An on-axis light collection from an atmospheric air–Xe plasma mixture demonstrates the potential of femtosecond filamentation for the remote sensing of noble gases.

47 OTHER INSTRUMENTATION↗

Laser-induced fluorescence of filament-produced plasmas

Self-guided ultrafast laser filaments are a promising method for laser beam delivery and plasma generation for standoff and remote detection of elements and isotopes via filament-induced breakdown spectroscopy (FIBS). Yet, there are several challenges associated with the practical application of FIBS, including delivery of sufficient laser energy at the target for generating plasma with a copious amount of emission signals for obtaining a high signal-to-noise ratio. Here, in this study, we use laser-induced fluorescence (LIF) to boost the emission signal and reduce self-reversal in the spectral profiles. Ultrafast laser filaments were used to produce plasmas from an Al 6061 alloy target at various standoff distances from 1 to 10 m. For LIF emission enhancement, a narrow linewidth continuous-wave laser was used in resonance with a 394.40 nm Al I resonant transition, and the emission signal was monitored from the directly coupled transition at 396.15 nm. Emission signal features of Al I are significantly enhanced by resonant excitation. In addition, LIF of filament ablation plumes reduces the self-reversal features seen in the thermally excited spectral profiles. Time-resolved two-dimensional fluorescence spectroscopy was performed for evaluating the optical saturation effects, which are found to be non-negligible due to high Al atomic densities in the filament-produced plasmas.

47 OTHER INSTRUMENTATION↗

Ultrafast Reactive Laser Sintering of Highly Conductive Garnet-Type LLZTO Solid Electrolytes

Rapid and scalable fabrication of garnet-type solid electrolytes remains a major challenge for the practical deployment of lithium metal batteries. Here, we report reactive laser sintering (RLS) as an ultrafast and potentially scalable strategy for fabricating garnet-type Li 6.4 La 3 Zr 1.4 Ta 0.6 O 12 (LLZTO) solid electrolytes. RLS of LLZTO enables simultaneous reaction and densification, achieving ∼95% relative density while minimizing lithium loss and suppressing secondary phase formation. Compared to conventional furnace sintering, RLS promotes enhanced grain growth and improved densification, leading to improved ionic conductivity (0.36 ± 0.08 mS cm −1 ) while maintaining comparable activation energies for Li + transport. Structural characterization by X-ray diffraction (XRD), Raman spectroscopy, and solid-state 6 Li/ 7 Li NMR confirms the formation of cubic garnet LLZTO with homogeneous microscale elemental distribution. In addition, nanoindentation measurements demonstrate that RLS preserves the mechanical properties of the garnet framework despite ultrafast localized thermal processing. By integrating simultaneous reaction and densification with tunable microstructural control, reactive laser sintering provides a promising manufacturing pathway for high-performance garnet solid electrolytes toward next-generation solid-state batteries.

CO2 laser↗

Ultra-high energy density relativistic plasmas from nanostructures: scaling to ultra-high intensities (Final Report)

This project investigated the ultra-high energy density (UHED) regime of matter found in the center of stars, using a compact PW-class laser. These extreme conditions are typically only obtained in the laboratory in the central hot-spot of spherically imploded capsules in inertial confinement fusion experiments driven by the world’s largest lasers. We have shown that near-solid density arrays of aligned nanostructures can be volumetrically heated to multi-keV temperatures by irradiation at relativistic intensity with ultrafast laser pulses of modest energy, opening a path for the generation of UHED plasmas with compact lasers. This new UHED plasma generation approach promises to create an environment with extreme energy densities and degrees of ionization, record conversion of optical laser light into ultrafast x-ray pulses, gigantic magnetic fields and pressures, and directed beams of high energy particles . In this project we achieved record degree of ionization in volumetric heating solid density and near-solid density plasmas. Gold plasmas which spectra is characterized by L shell transition emission from ions with charge up to the Ne-like state, Au+ 72 were generated using ultrafast laser pulses of less than 10 J of energy from a compact laser focused to an intensity of ~ 3x10 21 Wcm -2 . We also conducted measurements to determine the heat penetration depth in Ni nanowire arrays as compared to Ni foil targets by monitoring the line emission of a Co buried tracer underneath a variable amount of Ni. The measurements revealed that the nanowire plasmas are roughly six times larger in depth than the solid density target plasmas. A result of this increased plasma in nanowire arrays is a greatly increased conversion of optical laser light into > 1 KeV x-rays, a record conversion efficiency of 20 %. Critical to the realization of the proposed experiments was the generation of ultrafast laser pulses with ultra-high contrast that can deposit the energy deep into the nanowire arrays before the nanowires explode to create a continuous plasma. Supporting the proposed experiments was the recent demonstration at Colorado State University of a Petawatt-class laser that emits 30 fs pulses at high repetition rates. The experiments combined this unique laser tool with a variety of tailored nanowire arrays fabricated in house and with an extensive suite of diagnostics. The experiments were accompanied by 3-dimensional particle-in-cell simulations and detailed atomic physics simulations with transient kinetics and radiation transport. The proposed research allowed us to continue training Ph.D students and post-docs with broad experience in HEDP Science.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Laser-driven ultrafast transmission electron microscopy

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

Transmission electron microscopy↗

Laser-Induced Ultrafast Demagnetization and Spin Switching (Final Report)

The information technology revolution demands bigger and faster magnetic storage devices. The funded research focuses on a new frontier - Laser-induced ultrafast all-optical spin switching (AOS), where a single laser pulse can switch spins from one direction to another permanently, without a magnetic field, on a time scale of 1-10 picoseconds, 2-3 orders of magnitude faster than the existing technology. The funded research has successfully resolved a long-standing issue in ultrafast demagnetization whether the lattice contributes to the demagnetization. We developed a high level first-principles theory and employed a massively parallel computer to pin down the details of the physical mechanisms that are inaccessible to other methods. This unique feature allows us to compute the force on each atom in both bulk and monolayer systems. We find that it is indeed true there is a nonzero force on each atom, but the idea of vibration contribution is not crucial to our basic understanding of physics. This paves the way to future experimental, theoretical and technological developments.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗