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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 127 records · Page 7
All sourcesNASA NTRSDOE OSTI
DOE OSTI2020

Direct drive with the argon fluoride laser as a path to high fusion gain with sub-megajoule laser energy

Argon fluoride (ArF) is currently the shortest wavelength laser that can credibly scale to the energy and power required for high gain inertial fusion. ArF's deep ultraviolet light and capability to provide much wider bandwidth than other contemporary inertial confinement fusion (ICF) laser drivers would drastically improve the laser target coupling efficiency and enable substantially higher pressures to drive an implosion. Our radiation hydrodynamics simulations indicate gains greater than 100 are feasible with a sub-megajoule ArF driver. Our laser kinetics simulations indicate that the electron beam-pumped ArF laser can have intrinsic efficiencies of more than 16%, versus about 12% for the next most efficient krypton fluoride excimer laser. We expect at least 10% ‘wall plug' efficiency for delivering ArF light to target should be achievable using solid-state pulsed power and efficient electron beam transport to the laser gas that was demonstrated with the U.S. Naval Research Laboratory's Electra facility. These advantages could enable the development of modest size and lower cost fusion power plant modules. This would drastically change the present view on inertial fusion energy as being too expensive and the power plant size too large.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2020

Beating absorption in solid-state high harmonics

Since the new millennium coherent extreme ultra-violet and soft x-ray radiation has revolutionized the understanding of dynamical physical, chemical and biological systems at the electron’s natural timescale. Unfortunately, coherent laser-based upconversion of infrared photons to vacuum-ultraviolet and soft x-ray high-order harmonics in gaseous, liquid and solid targets is notoriously inefficient. In dense nonlinear media, the limiting factor is strong re-absorption of the generated high-energy photons. Here we overcome this limitation by generating high-order harmonics from a periodic array of thin one-dimensional crystalline silicon ridge waveguides. Adding vacuum gaps between the ridges avoids the high absorption loss of the bulk and results in a ~ 100-fold increase of the extraction depth. As the grating period is varied, each high harmonic shows a different and marked modulation, indicating their waveguiding in the vacuum slots with reduced absorption. Looking ahead, our results enable bright on-chip coherent short-wavelength sources and may extend the usable spectral range of traditional nonlinear crystals to their absorption windows. Potential applications include on-chip chemically-sensitive spectro-nanoscopy.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗
DOE OSTI2023

Plasma flows during the ablation stage of an over-massed pulsed-power-driven exploding planar wire array

We characterize the plasma flows generated during the ablation stage of an over-massed exploding planar wire array, fielded on the COBRA pulsed-power facility (1 MA peak current, 250 ns rise time). The planar wire array is designed to provide a driving magnetic field (80–100 T) and current per wire distribution (about 60 kA), similar to that in a 10 MA cylindrical exploding wire array fielded on the Z machine. Over-massing the arrays enables continuous plasma ablation over the duration of the experiment without implosion. The requirement to over-mass on the Z machine necessitates wires with diameters of 75–100μm, which are thicker than wires usually fielded on wire array experiments. To test ablation with thicker wires, we perform a parametric study by varying the initial wire diameter between 33 and 100 μm. The largest wire diameter (100 μm) array exhibits early closure of the cathode-wire gap, while the gap remains open over the duration of the experiment for wire diameters between 33 and 75 μm. Laser plasma interferometry and time-gated extreme-ultraviolet (XUV) imaging are used to probe the plasma flows ablating from the wires. The plasma flows from the wires converge to generate a pinch, which appears as a fast-moving (V≈100kms−1) column of increased plasma density (n¯e≈2×1018cm−3) and strong XUV emission. Finally, we compare the results with three-dimensional resistive-magnetohydrodynamic (MHD) simulations performed using the code GORGON, the results of which reproduce the dynamics of the experiment reasonably well.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2023

Time-resolving state-specific molecular dissociation with XUV broadband absorption spectroscopy

The electronic and nuclear dynamics inside molecules are essential for chemical reactions, where different pathways typically unfold on ultrafast timescales. Extreme ultraviolet (XUV) light pulses generated by free-electron lasers (FELs) allow atomic-site and electronic-state selectivity, triggering specific molecular dynamics while providing femtosecond resolution. Yet, time-resolved experiments are either blind to neutral fragments or limited by the spectral bandwidth of FEL pulses. Here, we combine a broadband XUV probe pulse from high-order harmonic generation with an FEL pump pulse to observe dissociation pathways leading to fragments in different quantum states. We temporally resolve the dissociation of a specific O 2 + state into two competing channels by measuring the resonances of ionic and neutral fragments. This scheme can be applied to investigate convoluted dynamics in larger molecules relevant to diverse science fields.

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

Single-shot measurements of shaped XUV FEL pulses with frequency-resolved optical gating

The ability to control the amplitude and phase of extreme ultraviolet (XUV) and X-ray free-electron laser (FEL) pulses can allow for the extension of optical techniques, such as multidimensional spectroscopy or coherent control, to higher photon energies, for probing and controlling core electronic transitions. However, this requires the ability to make single-shot, and complete, electric field measurements of potentially complex FEL pulses, in order to develop, and verify, pulse shaping strategies. Here, we present direct, single-shot measurements of XUV pulses generated under special operating configurations for producing specific pulse shapes from a laser-seeded XUV FEL. To do this, we built upon our past work using transient grating (TG) cross correlation frequency-resolved optical gating (FROG), where an optical reference pulse is diffracted from an XUV TG produced by a pair of interfering FEL pulses. The resulting nonlinear signal versus frequency and delay, i.e., the FROG trace, contains the electric field of the FEL pulse. The FEL pulse electric field is reconstructed from the FROG trace using a phase retrieval algorithm. Here we confirmed three different pulse shaping strategies for generating chirped, double and multiple FEL pulses by tuning the seed laser and FEL parameters and measuring the resulting shaped FEL pulses with TG XFROG. This work paves the way for generating on-demand pulse shapes with a seeded FEL by improving the characterization of FEL pulses, for transform-limited to more complex shapes.

Elverson, Francesca↗
DOE OSTI2024

Double diffraction imaging of x-ray induced structural dynamics in single free nanoparticles

Abstract Because of their high photon flux, x-ray free-electron lasers (FEL) allow to resolve the structure of individual nanoparticles via coherent diffractive imaging (CDI) within a single x-ray pulse. Since the inevitable rapid destruction of the sample limits the achievable resolution, a thorough understanding of the spatiotemporal evolution of matter on the nanoscale following the irradiation is crucial. We present a technique to track x-ray induced structural changes in time and space by recording two consecutive diffraction patterns of the same single, free-flying nanoparticle, acquired separately on two large-area detectors opposite to each other, thus examining both the initial and evolved particle structure. We demonstrate the method at the extreme ultraviolet (XUV) and soft x-ray Free-electron LASer in Hamburg (FLASH), investigating xenon clusters as model systems. By splitting a single XUV pulse, two diffraction patterns from the same particle can be obtained. For focus intensities of about 2 × 10 12 W cm −2 we observe still largely intact clusters even at the longest delays of up to 650 picoseconds of the second pulse, indicating that in the highly absorbing systems the damage remains confined to one side of the cluster. Instead, in case of five times higher flux, the diffraction patterns show clear signatures of disintegration, namely increased diameters and density fluctuations in the fragmenting clusters. Future improvements to the accessible range of dynamics and time resolution of the approach are discussed.

Sauppe, M. (ORCID:0000000163123102)↗
DOE OSTI2020

Phase-matching analysis in high-order harmonic generation with nonzero orbital angular momentum Laguerre-Gaussian beams

Through high-order harmonic generation driven by intense ultrashort vortex infrared or midinfrared lasers, a nonzero orbital angular momentum can be imprinted onto extreme ultraviolet (XUV) or soft-x-ray (SXR) light pulses. Here we simulate the generation of vortex XUV harmonics in the gas medium as well as their propagation in vacuum till reaching the far field. In this work, we find that the intensity and phase of generated high harmonics are very sensitive to the position of gas jet with respect to the laser focus. The topological charge of the $\textit{q}$th harmonic is found to be $\textit{q}$ times that of the driving Laguerre-Gaussian beam. Each harmonic in the far field appears as a single ring in the transverse plane with an invariant diameter which is scalable with the fundamental topological charge only when the gas jet is placed after the laser focus. The underlying phase-matching mechanism is analyzed by examining the spatial map of the coherence length and by calculating the evolution of harmonic emission in the medium. We anticipate this work to stimulate interest in generating intense vortex XUV or SXR attosecond pulses for probing dynamics of molecules where special molecular features are difficult to be detected with linear or circular XUV or SXR pulses.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2024

Circularly Polarized Attosecond Pulses Enabled by an Azimuthal Phase and Polarization Grating

High-harmonic generation (HHG) is an extreme nonlinear optical process that can map the properties of an infrared driving laser beam onto short wavelength attosecond pulse trains. However, current techniques for generating circularly polarized high harmonics for probing magnetic materials and chiral systems have limitations: two-color collinear counter-rotating driving lasers result in a low cutoff photon energy, while single-color non-collinear counter-rotating schemes suffer from low conversion efficiency. In this work, we generate circularly polarized attosecond pulse trains by using a structured laser driver which has a rotating polarization and phase grating along the azimuthal coordinate. Furthermore, our experimental and numerical results demonstrate the production of left and right circularly polarized harmonics, which naturally separate upon propagation. Our approach uses a single laser color in a collinear geometry, that can be scaled for high efficiency. Simulations show this scheme can extend into the soft x-ray region when driven by mid-infrared driving lasers, while preserving the same high phase-matching cutoff photon energy as for linearly-polarized high harmonics.

attosecond science↗
DOE OSTI2020

Laser-Plasma Spectroscopy of Hydroxyl with Applications

This article discusses laser-induced laboratory-air plasma measurements and analysis of hydroxyl (OH) ultraviolet spectra. The computations of the OH spectra utilize line strength data that were developed previously and that are now communicated for the first time. The line strengths have been utilized extensively in interpretation of recorded molecular emission spectra and have been well-tested in laser-induced fluorescence applications for the purpose of temperature inferences from recorded data. Moreover, new experiments with Q-switched laser pulses illustrate occurrence of molecular recombination spectra for time delays of the order of several dozen of microseconds after plasma initiation. The OH signals occur due to the natural humidity in laboratory air. Centrifugal stretching of the Franck-Condon factors and r-centroids are included in the process of determining the line strengths that are communicated as a Supplementary File. Laser spectroscopy applications of detailed OH computations include laser-induced plasma and combustion analyses, to name but two applications. This work also includes literature references that address various diagnosis applications.

47 OTHER INSTRUMENTATION↗
DOE OSTI2021

Ultraviolet photodissociation of gas-phase iron pentacarbonyl probed with ultrafast infrared spectroscopy

It is well known that ultraviolet photoexcitation of iron pentacarbonyl results in rapid loss of carbonyl ligands leading to the formation of coordinatively unsaturated iron carbonyl compounds. Here we employ ultrafast mid-infrared transient absorption spectroscopy to probe the photodissociation dynamics of gas-phase iron pentacarbonyl following ultraviolet excitation at 265 and 199 nm. After photoexcitation at 265 nm, our results show evidence for sequential dissociation of iron pentacarbonyl to form iron tricarbonyl via a short-lived iron tetracarbonyl intermediate. Photodissociation at 199 nm results in the prompt production of Fe(CO) 3 within 0.25 ps via several energetically accessible pathways. An additional 15 ps time constant extracted from the data is tentatively assigned to intersystem crossing to the triplet manifold of iron tricarbonyl or iron dicarbonyl. Mechanisms for formation of iron tetracarbonyl, iron tricarbonyl, and iron dicarbonyl are proposed and theoretically validated with one-dimensional cuts through the potential energy surface as well as bond dissociation energies. Ground state calculations are computed at the CCSD(T) level of theory and excited states are computed with EOM-EE-CCSD(dT).

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2024

Time-Resolved Probing of the Iodobenzene C-Band Using XUV-Induced Electron Transfer Dynamics

Time-resolved extreme ultraviolet spectroscopy was used to investigate photodissociation within the iodobenzene C-band. The carbon–iodine bond of iodobenzene was photolyzed at 200 nm, and the ensuing dynamics were probed at 10.3 nm (120 eV) over a 4 ps range. Two product channels were observed and subsequently isolated by using a global fitting method. Their onset times and energetics were assigned to distinct electron transfer dynamics initiated following site-selective ionization of the iodine photoproducts, enabling the electronic states of the phenyl fragments to be identified using a classical over-the-barrier model for electron transfer. In combination with previous theoretical work, this allowed the corresponding neutral photochemistry to be assigned to (1) dissociation via the 7B2, 8A2, and 8B1 states to give ground-state phenyl, Ph(X), and spin–orbit excited iodine and (2) dissociation through the 7A1 and 8B2 states to give excited-state phenyl, Ph(A), and ground-state iodine. The branching ratio was determined to be 87 ± 4% Ph(X) and 13 ± 4% Ph(A). Similarly, the corresponding amount of energy deposited into the internal phenyl modes in these channels was determined to be 44 ± 10 and 65 ± 21%, respectively, and upper bounds to the channel rise times were found to be 114 ± 6 and 310 ± 60 fs.

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

On-target uniformity of the OMEGA 60-beam inertial confinement fusion laser

Successful direct-drive inertial confinement fusion (ICF) experiments require excellent on-target laser 9 irradiance uniformity maintained over the duration of the pulse. Achieving this symmetry relies on maintaining an 10 energy, power, and fluence balance among all beams in a multibeam laser system. As a result of the improvements 11 described in this paper, the OMEGA 60-beam laser performance has been assessed at approximately 2% on-target 12 irradiance nonuniformity using an updated performance assessment metric that accounts for the laser diagnostic noise 13 floor. The performance is measurement-limited, prompting the need for an improved diagnostic suite. This manuscript 14 provides a comprehensive first-order assessment of extant status of on-target energy, power, and fluence uniformity 15 and explores avenues for improvements.

Diagnostics↗
DOE OSTI2022

Fragmentation Dynamics of Fluorene Explored Using Ultrafast XUV-Vis Pump-Probe Spectroscopy

We report on the use of extreme ultraviolet (XUV, 30.3 nm) radiation from the Free-electron LASer in Hamburg (FLASH) and visible (Vis, 405 nm) photons from an optical laser to investigate the relaxation and fragmentation dynamics of fluorene ions. The ultrashort laser pulses allow to resolve the molecular processes occurring on the femtosecond timescales. Fluorene is a prototypical small polycyclic aromatic hydrocarbon (PAH). Through their infrared emission signature, PAHs have been shown to be ubiquitous in the universe, and they are assumed to play an important role in the chemistry of the interstellar medium. Our experiments track the ionization and dissociative ionization products of fluorene through time-of-flight mass spectrometry and velocity-map imaging. Multiple processes involved in the formation of each of the fragment ions are disentangled through analysis of the ion images. The relaxation lifetimes of the excited fluorene monocation and dication obtained through the fragment formation channels are reported to be in the range of a few tens of femtoseconds to a few picoseconds.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2020

Population inversion X-ray laser oscillator

Oscillators are at the heart of optical lasers, providing stable, transform-limited pulses. Until now, laser oscillators have been available only in the infrared to visible and near-ultraviolet (UV) spectral region. In this paper, we present a study of an oscillator operating in the 5- to 12-keV photon-energy range. We show that, using the Kα 1 line of transition metal compounds as the gain medium, an X-ray free-electron laser as a periodic pump, and a Bragg crystal optical cavity, it is possible to build X-ray oscillators producing intense, fully coherent, transform-limited pulses. As an example, we consider the case of a copper nitrate gain medium generating ~ 5 × 10 10 photons per pulse with 37-fs pulse length and 48-meV spectral resolution at 8-keV photon energy. Our theoretical study and simulation of this system show that, because of the very large gain per pass, the oscillator saturates and reaches full coherence in four to six optical-cavity transits. We discuss the feasibility and design of the X-ray optical cavity and other parts of the oscillator needed for its realization, opening the way to extend X-ray–based research beyond current capabilities.

47 OTHER INSTRUMENTATION↗
DOE OSTI2021

Intense quasi-monochromatic resonant harmonic generation in the multiphoton ionization regime

Resonant high-order harmonics, which result in quasimonochromatic extreme ultraviolet light with coherent intensity enhancement involving autoionizing resonances, have been demonstrated from laser-ablated plumes in the tunnel-ionization regime. Here, we demonstrate resonant harmonics in the previously unexplored multiphoton-ionization regime. We demonstrate an intense resonant harmonic from gallium with an intensity enhancement ratio of 714 relative to the neighboring harmonics, achieved without the need for extreme ultraviolet filtering methods, thus preventing a typical photon flux loss of more than 70%. Three-dimensional time-dependent Schrödinger equation calculations reveal that this increase in the enhancement ratio is due to the lowelectron wave packet spreading in the multiphoton-ionization regime. These results reveal a method for increasing the intensity and monochromaticity of intense multimicrojoule femtosecond extreme ultraviolet light and will also facilitate understanding of the involvement of autoionizing resonances in generating resonant harmonics in the multiphoton-ionization regime.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2022

Noncolinear Synthesis of Picosecond Flat-Top Laser Pulses to Increase Electron Photoinjector Brightness

Next-generation electron photoinjector accelerators, such as the LCLS-II photoinjector, have increasingly tight requirements on the excitation lasers, often calling for tens of picosecond, temporally flat-top, ultraviolet (UV) pulse trains to be delivered at up to 1 MHz[1]. We present a numerical and experimental implementation of a non-colinear sum frequency generation scheme wherein the incident optical pulses have equal and opposite amounts of spectral dispersion resulting in a spectrally narrowband pulse with flat-top temporal profile[2]. In preliminary experiments we achieve upwards of 40% conversion efficiency with this process. We additionally demonstrate the ability for the narrowband pulses to be directly upconverted to the UV for driving a photocathode.

Lemons, R.↗
DOE OSTI2023

Modeling of transverse stimulated Raman scattering in KDP/DKDP in large-aperture plates suitable for polarization control

Transverse stimulated Raman scattering (TSRS) in potassium dihydrogen phosphate (KDP) and deuterated potassium dihydrogen phosphate (DKDP) plates for large-aperture, inertial confinement fusion (ICF)-class laser systems is a well-recognized limitation giving rise to parasitic energy conversion and laser-induced damage. The onset of TSRS is manifested in plates exposed to the ultraviolet section of the beam. TSRS amplification is a coherent process that grows exponentially and is distributed nonuniformly in the crystal and at the crystal surfaces. To understand the growth and spatial distribution of TSRS energy in various configurations, a modeling approach has been developed to simulate the operational conditions relevant to ICF-class laser systems. Specific aspects explored in this work include (i) the behavior of TSRS in large-aperture crystal plates suitable for third-harmonic generation and use as wave plates for polarization control in current-generation ICF-class laser system configurations; (ii) methods, and their limitations, of TSRS suppression and (iii) optimal geometries to guide future designs.

47 OTHER INSTRUMENTATION↗
DOE OSTI2021

Measuring an ultrashort, ultraviolet pulse in a slowly responding, absorbing medium

Frequency-resolved optical gating (FROG) is a common technique for measuring ultrashort laser pulses using an instantaneous, nonlinear-optical interaction as a fast time-gate to measure the pulse intensity and phase. But at high frequencies, materials are often absorbing and it is not always possible to find a medium with a fast nonlinear-optical response. Here we show that an ultrashort, ultraviolet (UV) pulse can be measured in a strongly absorbing medium, using the absorption as the nonlinear-optical time-gate. To do this, we build on our recent implementation of FROG, known as induced-grating cross-correlation FROG (IG XFROG), where an unknown, higher-frequency pulse creates a transient grating that is probed with a lower-frequency, more easily detectable reference pulse. We demonstrate this with an 800 nm reference pulse to characterize 400 nm or 267 nm pulses using ZnS as the nonlinear-optical medium, which is absorptive at and below 400 nm. By scanning the delay between the two UV pulses which create the transient grating, we show that the phase-sensitive instantaneous four-wave-mixing contribution to the nonlinear signal field can be detected and separated from the slower, incoherent part of the response. Measuring a spectrally-resolved cross-correlation in this way and then applying a simple model for the response of the medium, we show that a modified generalized projections (GP) phase-retrieval algorithm can be used to extract the pulse amplitude and phase. We test this approach by measuring chirped UV pulses centered at 400 nm and 267 nm. Since interband absorption (or even photoionization) is not strongly wavelength-dependent, we expect IG XFROG to be applicable deeper into the UV.

77 NANOSCIENCE AND NANOTECHNOLOGY↗