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DOE OSTI2023

Optically Enhanced Solid-State 1 H NMR Spectroscopy

Low sensitivity is the primary limitation to extending nuclear magnetic resonance (NMR) techniques to more advanced chemical and structural studies. Photochemically induced dynamic nuclear polarization (photo-CIDNP) is an NMR hyperpolarization technique where light is used to excite a suitable donor–acceptor system, creating a spin-correlated radical pair whose evolution drives nuclear hyperpolarization. Systems that exhibit photo-CIDNP in solids are not common, and this effect has, up to now, only been observed for 13 C and 15 N nuclei. However, the low gyromagnetic ratio and natural abundance of these nuclei trap the local hyperpolarization in the vicinity of the chromophore and limit the utility for bulk hyperpolarization. Here, we report the first example of optically enhanced solid-state 1 H NMR spectroscopy in the high-field regime. This is achieved via photo-CIDNP of a donor–chromophore–acceptor molecule in a frozen solution at 0.3 T and 85 K, where spontaneous spin diffusion among the abundant strongly coupled 1 H nuclei relays polarization through the whole sample, yielding a 16-fold bulk 1 H signal enhancement under continuous laser irradiation at 450 nm. These findings enable a new strategy for hyperpolarized NMR beyond the current limits of conventional microwave-driven DNP.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2020

Photonic methods and technologies for monitoring the ocean and atmosphere

In this paper, we review photonic methods and technologies that are promising for monitoring the ocean and atmosphere and have been implemented mainly in recent years at the Institute of Automation and Control Processes, Far Eastern Branch, Russian Academy of Sciences. We present results of lidar studies that have made it possible to understand key features of ocean – atmosphere interaction processes under continent – ocean transition conditions, which determine specific features of the atmospheric aerosol distribution, small gaseous components of the atmosphere and its optical characteristics. We consider methods and tools for combined optical and laser fluorescence monitoring of the ocean surface. Particular attention is paid to results of research on remote methods and tools for real-time laser-induced and laser fluorescence environmental monitoring of the ocean, including specialised fibre-optic probes and mobile underwater robotic systems. We present results of the development and investigation of highly sensitive, noise-proof fibre-optic hydro- and seismic/acoustic sensors for remote monitoring of the ocean and robotic systems for underwater laser protection of marine vessels, hydraulic structures and oceanographic instruments against the negative impact of biofouling. (invited paper)

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

NASA NTRS1966

Plasma physics

Calculations and experiments to determine ion wave instability in steady state discharge, laser breakdown in plasma, and microwave scattering from standing plasma waves

LASER OUTPUT↗

NASA NTRS1994

LASER Tech Briefs, Winter 1994

Topics include: Electronic Components and Circuits. Electronic Systems, Physical Sciences, Materials, Computer Programs, Mechanics, Machinery, Fabrication Technology, Mathematics and Information Sciences, Life Sciences, and Books and reports

Schnirring, Bill↗

DOE OSTI2022

Off-harmonic optical probing of high intensity laser plasma expansion dynamics in solid density hydrogen jets

Due to the non-linear nature of relativistic laser induced plasma processes, the development of laser-plasma accelerators requires precise numerical modeling. Especially high intensity laser-solid interactions are sensitive to the temporal laser rising edge and the predictive capability of simulations suffers from incomplete information on the plasma state at the onset of the relativistic interaction. Experimental diagnostics utilizing ultra-fast optical backlighters can help to ease this challenge by providing temporally resolved inside into the plasma density evolution. We present the successful implementation of an off-harmonic optical probe laser setup to investigate the interaction of a high-intensity laser at 5.4 x 10 21 W/cm 2 peak intensity with a solid-density cylindrical cryogenic hydrogen jet target of 5μm diameter as a target test bed. The temporal synchronization of pump and probe laser, spectral filtering and spectrally resolved data of the parasitic plasma self-emission are discussed. The probing technique mitigates detector saturation by self-emission and allowed to record a temporal scan of shadowgraphy data revealing details of the target ionization and expansion dynamics that were so far not accessible for the given laser intensity. Plasma expansion speeds of up to (2.3 ± 0.4)x 10 7 m/s followed by full target transparency at 1.4ps after the high intensity laser peak are observed. A three dimensional particle-in-cell simulation initiated with the diagnosed target pre-expansion at -0.2ps and post processed by ray tracing simulations supports the experimental observations and demonstrates the capability of time resolved optical diagnostics to provide quantitative input and feedback to the numerical treatment within the time frame of the relativistic laser-plasma interaction.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

DOE OSTI2021

Ultrafast multi-cycle terahertz measurements of the electrical conductivity in strongly excited solids

Key insights in materials at extreme temperatures and pressures can be gained by accurate measurements that determine the electrical conductivity. Free-electron laser pulses can ionize and excite matter out of equilibrium on femtosecond time scales, modifying the electronic and ionic structures and enhancing electronic scattering properties. The transient evolution of the conductivity manifests the energy coupling from high temperature electrons to low temperature ions. Here we combine accelerator-based, high-brightness multi-cycle terahertz radiation with a single-shot electro-optic sampling technique to probe the evolution of DC electrical conductivity using terahertz transmission measurements on sub-picosecond time scales with a multi-undulator free electron laser. Our results allow the direct determination of the electron-electron and electron-ion scattering frequencies that are the major contributors of the electrical resistivity.

36 MATERIALS SCIENCE↗

DOE OSTI2023

In-Situ Observation of the Formation of Laser-Induced Periodic Surface Structures with Extreme Spatial and Temporal Resolution

Irradiation of solid surfaces with intense ultrashort laser pulses represents a unique way of depositing energy into materials. It allows to realize states of extreme electronic excitation and/or very high temperature and pressure and to drive materials close to and beyond fundamental stability limits. As a consequence, structural changes and phase transitions often occur along unusual pathways and under strongly nonequilibrium conditions. Furthermore, due to the inherent multiscale nature—both temporally and spatially—of these irreversible processes, their direct experimental observation requires techniques that combine high temporal resolution with the appropriate spatial resolution and the capability to obtain good quality data on a single pulse/event basis. In this respect, fourth-generation light sources, namely, short wavelength and short pulse free electron lasers (FELs), are offering new and fascinating possibilities. As an example, this chapter will discuss the results of scattering experiments carried out at the FLASH free electron laser at DESY (Hamburg, Germany), which allowed us to resolve laser-induced structure formation at surfaces on the nanometer to submicron length scale and in temporal regimes ranging from picoseconds to several nanoseconds with sub-picosecond resolution.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

DOE OSTI2023

Strong collisionless coupling between an unmagnetized driver plasma and a magnetized background plasma

Fast-exploding plasmas traveling though magnetized, collisionless plasmas can occur in a variety of physical systems, such as supernova remnants, coronal mass ejections, and laser-driven laboratory experiments. To study these systems, it is important to understand the coupling process between the plasmas. Here, in this work, we develop a semi-analytical model of the parameters that characterize the strong collisionless coupling between an unmagnetized driver plasma and a uniformly and perpendicularly magnetized background plasma. In particular, we derive analytical expressions that describe the characteristic diamagnetic cavity and magnetic compression of these systems, such as their corresponding velocities, the compression ratio, and the maximum size of the cavity. The semi-analytical model is compared with collisionless 1D particle-in-cell simulations and experimental results with laser-driven plasmas. The model allows us to provide bounds for parameters that are otherwise difficult to diagnose in experiments with similar setups.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

DOE OSTI2020

Spectroscopy of atoms in an optical dipole trap using spectrally selective heating by a probe laser field

Spectral properties of atoms localised in an optical dipole trap are studied using the method of spectrally selective heating by a probe field. The method is based on measuring the number of atoms in a trap after they interact with a probe field. The dependence of the number of atoms on the frequency of the probe field fully characterises the shift and width of the spectral absorption line of trapped atoms. (paper)

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

DOE OSTI2025

Coherent frequency combs from electrons colliding with a laser pulse

Highly coherent and powerful light sources capable of generating soft x-ray frequency combs are essential for high precision measurements and rigorous tests of fundamental physics. In this work, we derive the analytical conditions required for the emission of coherent radiation from an electron beam colliding with a laser pulse, modeled as a plane wave. These conditions are applied in a series of numerical simulations, where we show that a soft x-ray frequency comb can be produced if the electrons are regularly-spaced and sufficiently monoenergetic. High quality beams of this kind may be produced in the near future from laser-plasma interactions or linear accelerators. Furthermore, we highlight the advantageous role of employing few-cycle laser pulses in relaxing the stringent monoenergeticity requirements for coherent emission. The conditions derived here can also be used to optimize coherent emission in other frequency ranges, such as the terahertz domain.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

DOE OSTI2022

Thermal transport modeling of laser-irradiated spheres

Thermal transport of uniformly laser-irradiated spheres of various materials is investigated computationally. One-dimensional simulations of low- to mid-Z materials (Be, Al, and Cu) are performed to evaluate the impact of nonlocal electron transport on experimental observables under laser intensities of relevance to direct-drive inertial confinement fusion. Here we compare thermal transport models of different levels of fidelity: flux-limited Spitzer–Harm diffusion, the Schurtz–Nicolai–Busquet (SNB) reduced-order nonlocal model, and a Fokker–Planck description. Spitzer–Harm diffusion with different flux-limiter factors are compared with different implementations of the SNB model in the HYDRA radiation hydrodynamics code. Under the conditions of interest, the peak heat flux in the thermal front with the SNB model shows good agreement with Fokker–Planck calculations, with the largest errors below 10% at 10 15 W/cm 2 laser intensity. From HYDRA-SNB simulations, two experimentally relevant effects are observed from nonlocal heat transport when compared to flux-limited Spitzer–Harm modeling: coronal temperatures are cooler due to reduced heat fluxes in the expanding plasma and (for mid-Z materials) x-ray emissions are enhanced due to preheating in the dense plasma.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

DOE OSTI2023

Experimental demonstration of >20 kJ laser energy coupling in 1-cm hydrocarbon-filled gas pipe targets via inverse Bremsstrahlung absorption with applications to MagLIF

Laser propagation experiments using four beams of the National Ignition Facility to deliver up to 35 kJ of laser energy at 351 nm laser wavelength to heat magnetized liner inertial fusion-scale (1 cm-long), hydrocarbon-filled gas pipe targets to ~keV electron temperatures have demonstrated energy coupling >20 kJ with essentially no backscatter in 15% critical electron density gas fills with 0–19 T applied axial magnetic fields. The energy coupling is also investigated for an electron density of 11.5% critical and for applied field strengths up to 24 T at both densities. This spans a range of Hall parameters 0 < ω ce τ ei ≲ 2, where a Hall parameter of 0.5 is expected to reduce electron thermal conduction across the field lines by a factor of 4–5 for the conditions of these experiments. At sufficiently high applied field strength (and therefore Hall parameter), the measured laser propagation speed through the targets increases in the measurements, consistent with reduced perpendicular electron thermal transport; this reduces the coupled energy to the target once the laser burns through the gas pipe. In conclusion, the results compare well with a 1D analytic propagation model for inverse Bremsstrahlung absorption.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

DOE OSTI2021

Generation of Bright Soft X-ray Laser Beams (Final Report)

The project goal was to demonstrate new compact soft x-ray lasers emitting high energy ultrashort pulses at shorter wavelengths and increased repetition rates by amplification in atomic transitions in high density laser-created plasmas. To demonstrate these lasers we developed new high power solid state lasers. The project succeeded in demonstrating the shortest wavelength compact soft x-ray laser to date, 6.85 nm wavelength, and the highest repetition rate table-top soft x-ray laser, 400 Hz. We also applied these compact soft x-ray laser sources to determine the composition of materials with nanoscale resolution using a new technique that combines soft x-ray laser ablation with mass spectrometry, and we demonstrated that these lasers are capable of acquiring nanoscale resolution holograms with picosecond time resolution. The combination of an increased pumping efficiency with increased repetition rates can yield soft x-ray laser beams with an unprecedented average power on a table-top for applications demanding a high photon flux. We have demonstrated that the efficiency of plasma-based laser-pumped soft x-ray lasers can be significantly increased by detailed pulse shaping of the pump laser using a new pulse synthesizer. Results include the demonstration of 18.9 nm wavelength laser operation at a record 400 Hz repetition rate, and the extension of repetitive gain-saturated plasma-based table-top x-ray lasers to the shortest wavelength to date, 6.85 nm. Laser amplification was also observed at wavelengths as short at 5.8 nm by isolectronic scaling in Ni-like lanthanide ions. We have also conducted simulations to explore the possibility of demonstrating gain saturated atomic x-ray lasers near the carbon K-edge, in the “carbon window” for the first time. The work conducted under this program also includes the use of compact soft x-ray lasers in applications to problems of chemical interest, such as isotopic composition mapping of micron-size uranium particles with nanoscale resolution, and nanoscale resolution depth profiling analysis of CoNCN-coated electrodes for water oxidation catalysis. We also demonstrated single-shot high resolution soft x-ray Fourier transform holography over a broad 7 µm diameter field of view with ~ 5 ps temporal resolution.

74 ATOMIC AND MOLECULAR PHYSICS↗

NASA NTRS1976

Study report on laser storage and retrieval of image data

The theoretical foundation is presented for a system of real-time nonphotographic and nonmagnetic digital laser storage and retrieval of image data. The system utilizes diffraction-limited laser focusing upon thin metal films, melting elementary holes in the metal films in laser focus. The metal films are encapsulated in rotating flexible mylar discs which act as the permanent storage carries. Equal sized holes encompass two dimensional digital ensembles of information bits which are time-sequentially (bit by bit) stored and retrieved. The bits possess the smallest possible size, defined by the Rayleigh criterion of coherent physical optics. Space and time invariant reflective read-out of laser discs with a small laser, provides access to the stored digital information. By eliminating photographic and magnetic data processing, which characterize the previous state of the art, photographic grain, diffusion, and gamma-distortion do not exist. Similarly, magnetic domain structures, magnetic gaps, and magnetic read-out are absent with a digital laser disc system.

Becker, C. H.↗

DOE OSTI2022

The Influence of Environment on Post-Detonation Chemistry and Debris Formation (Abbreviated Final Report: 20-SI-006)

Predicting, responding to, or interpreting the chemical record preserved in debris derived from nuclear events can be challenging due to chemical fractionation. Chemical fractionation is where different species of the evolving radionuclide inventory segregate and/or are lost from the system over the timescales of debris formation. Both historic data and recent research suggest that the interaction and character of the local environment may exert controls on chemical fractionation by influencing the cooling and evolution of the associated fireball as well as the composition of the vapor term and resultant speciation. Prior to this work, an integrated platform permitting dynamic and concurrent consideration of physical and chemical evolution of early time post-detonation event environments did not exist. Our work merged historic data and experimental approaches to support development of a computational framework able to simulate fundamental processes (e.g., entrainment of local environment, oxidation chemistry, and cooling time scales) that may perturb the radionuclide inventory captured in post-detonation debris. Work with historic debris confirmed that entrained environmental material affect debris composition, structure, and radionuclide incorporation. Complementary work utilizing a readily controllable and tunable benchtop setup (a plasma flow reactor) simulated the late cooling of a nuclear fireball (e.g., T < 6000 K) and bounded the sensitivity of actinide speciation and particle size distribution to variations in oxygen concentration and cooling rates. Concurrent laser ablation and laser heating experiments were used to investigate the chemistry and physics of processes occurring in vaporized and/or rapidly heated actinides and other elements in the presence of oxygen. A more computationally efficient microphysical model was developed for predicting and evolving size distributions of particles forming from mixed vapor terms and simulating particle formation processes under a variety of extreme conditions. Continued study of historic nuclear event film confirmed that shockwave data and physics codes agree to within the uncertainty of the data. Good agreement was achieved for thermal emission from an airburst, however the paucity of low-temperature molecular opacity data for mixtures of air, bomb debris, entrained dirt, and water vapor complicate agreement for more elaborate scenarios. A multiphysics code (ALE3D) was modified to bring the necessary physics and chemistry, including these new data and insights, onto a single platform. Code development included improved initialization of large physical systems, modernization of chemistry capabilities, and modifications to enable inclusion of particle transport.

07 ISOTOPE AND RADIATION SOURCES↗

DOE OSTI2022

Analysis of the laser welding keyhole using inline coherent imaging

Laser beam welding is a widely used fusion welding process in many industrial applications such as automotive, aerospace, energy, defense, and medical products. Industry has a fundamental need to model the laser welding process to minimize experimental testing and improve confidence in production welds. However, computational models attempting to predict weld formation are limited by an incomplete understanding of the beam-material interactions. As a consequence, these models do not accurately predict the mechanisms associated with laser weld formation. To improve the current state of prediction capabilities, it is vital to better detect/measure the physical aspects of the weld pool during high energy density welding. In this work, a novel real-time laser weld monitoring device using inline coherent imaging (ICI) was used to provide a fundamental understanding of laser weld formation via vaporization. The objective of this work was to investigate and quantify the relationship relating laser weld parameters and the vapor capillary (keyhole) through a state-of-the-art measurement technique. Bead-on-plate laser beam welds were produced with partial penetration on 304L stainless steel, 2205 duplex stainless steel, and Ti-6Al-4V. Keyhole monitoring was performed using a commercially available ICI system to collect keyhole penetration data in real time. These measurements were reconstructed to generate the vapor capillary shape at different welding parameters. Process parameters significantly influenced the keyhole shape and the keyhole root position relative to the process beam. Finally, the keyhole geometry showed distinct differences between the stainless steel alloys and Ti-6Al-4V.

2205↗

DOE OSTI2020

The SuperCam Instrument Suite on the NASA Mars 2020 Rover: Body Unit and Combined System Tests

The SuperCam instrument suite provides the Mars 2020 rover, Perseverance, with a number of versatile remote-sensing techniques that can be used at long distance as well as within the robotic-arm workspace. These include laser-induced breakdown spectroscopy (LIBS), remote time-resolved Raman and luminescence spectroscopies, and visible and infrared (VISIR; separately referred to as VIS and IR) reflectance spectroscopy. A remote micro-imager (RMI) provides high-resolution color context imaging, and a microphone can be used as a stand-alone tool for environmental studies or to determine physical properties of rocks and soils from shock waves of laser-produced plasmas. SuperCam is built in three parts: The mast unit (MU), consisting of the laser, telescope, RMI, IR spectrometer, and associated electronics, is described in a companion paper. The on-board calibration targets are described in another companion paper. Here we describe SuperCam’s body unit (BU) and testing of the integrated instrument. The BU, mounted inside the rover body, receives light from the MU via a 5.8 m optical fiber. The light is split into three wavelength bands by a demultiplexer, and is routed via fiber bundles to three optical spectrometers, two of which (UV and violet; 245–340 and 385–465 nm) are crossed Czerny-Turner reflection spectrometers, nearly identical to their counterparts on ChemCam. The third is a high-efficiency transmission spectrometer containing an optical intensifier capable of gating exposures to 100 ns or longer, with variable delay times relative to the laser pulse. This spectrometer covers 535–853 nm ( $105\text{--}7070~\text{cm}^{-1}$ Raman shift relative to the 532 nm green laser beam) with $12~\text{cm}^{-1}$ full-width at half-maximum peak resolution in the Raman fingerprint region. The BU electronics boards interface with the rover and control the instrument, returning data to the rover. Thermal systems maintain a warm temperature during cruise to Mars to avoid contamination on the optics, and cool the detectors during operations on Mars.Results obtained with the integrated instrument demonstrate its capabilities for LIBS, for which a library of 332 standards was developed. Examples of Raman and VISIR spectroscopy are shown, demonstrating clear mineral identification with both techniques. Luminescence spectra demonstrate the utility of having both spectral and temporal dimensions. Finally, RMI and microphone tests on the rover demonstrate the capabilities of these subsystems as well.

47 OTHER INSTRUMENTATION↗

DOE OSTI2026

Scalings of laser-driven MeV electron sources with relativistic multi-picosecond laser pulses

We investigate the generation of MeV electrons in relativistic multi-picosecond laser–solid interactions, using two-dimensional particle-in-cell simulations. Scanning a parameter space of intensities from 10 18 to 10 20 W/cm 2 and pulse durations between 100 fs and 10 ps, we discuss scalings of the effective hot electron temperature and MeV electron dose relevant to applications, as well as the direct laser acceleration mechanism that drives electrons to energies much higher than the ponderomotive potential of the laser pulse.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗