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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 73 records · Page 4

Solid-to-plasma transition of polystyrene induced by a nanosecond laser pulse within the context of inertial confinement fusion

Laser Direct Drive (LDD) Inertial Confinement Fusion (ICF) involves irradiating a spherical target of thermonuclear fuel coated with an ablator, usually made of polystyrene. Laser energy absorption near the target surface leads to matter ablation, hydrodynamic shocks, and ultimately capsule implosion. The conservation of spherical symmetry is crucial for implosion efficiency, yet spatial modulations in laser intensity can induce nonuniformities, causing the laser imprint phenomenon. Understanding laser imprint, especially considering the initial solid state, is essential for advancing LDD ICF. A first microscopic model of solid-to-plasma transition was built in 2019, accounting for laser absorption in the solid state with a band structure based ionization model. This model has been improved to include chemical fragmentation and a more accurate description of electron collision frequency in various matter states. The latest development involves assessing the model reliability by comparing theoretical predictions with experimental observations. Despite the success of this approach, questions remain, leading to further investigations and observations under different irradiation conditions. This work presents an experiment with a nanosecond pulse, taking into account hydrodynamic effects, and measures transmission dynamics over the entire laser beam area to observe two-dimensional effects. As a result, the objective is to adapt the theoretical model, couple it with a hydrodynamic code, and observe additional effects related to the initial solid state.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Lasing from Finite Plasmonic Nanoparticle Lattices

Small lasers can generate coherent light for integrated photonics, in-vivo cellular imaging, and solid-state lighting. Unlike conventional lasers, plasmonic lasers can generate coherent light at sub-wavelength scales, although cavity architectures based on metal films and semiconducting gain exhibit large radiative losses and lack directional emission. In contrast, two-dimensional (2D) metal nanoparticle arrays surrounded by organic dyes can support lasing with high directionality at room temperature. Yet, the relationship between the number of nanoparticles in a finite lattice and their lasing emission characteristics is unknown. Here we show that the number of units in 2D gold nanoparticle lattices is critical to generate robust cavity resonances and lasing emission. Narrower lattice plasmons associated with stronger electromagnetic near fields are observed as nanoparticle number increases. Experimentally, we demonstrate lasing from a 30x30 nanoparticle lattice. Semi-quantum modeling indicates lower lasing thresholds and faster population inversion dynamics with higher nanoparticle numbers. These findings indicate that finite lattices of nanoparticles integrated with gain can function as independent, coherent light sources for optical multiplexing and lab-on-a-chip applications.

77 NANOSCIENCE AND NANOTECHNOLOGY↗

Photoinduced correlations in stochastic dynamics of a solid-state ionic conductor

Photoexcitation by ultrashort laser pulses plays a crucial role in controlling reaction pathways, creating nonequilibrium material properties, and probing complex molecular dynamics. The photoresponse following a laser pulse is generally nonidentical between exposures due to spatiotemporal fluctuations or the stochastic nature of dynamical pathways. However, most ultrafast pump-probe experiments struggle to distinguish intrinsic sample fluctuations from extrinsic apparatus noise, often missing deviations from the averaged response. Leveraging the stability and high photon flux of time-resolved X-ray micro-diffraction at a synchrotron, we characterized stochastic photoinduced dynamics in a solid-state ionic conductor. By analyzing temporal evolutions of the lattice parameter of a single grain, we found that shot-to-shot fluctuations are not independent. Instead, correlations exist between nonequilibrium lattice trajectories following adjacent shots, with a characteristic correlation length of approximately 1500 shots, corresponding to an energy barrier of 0.4 ± 0.1 eV, close to the activation energy of lithium-ion diffusion.

36 MATERIALS SCIENCE↗

Rapid Laser Reactive Sintering of Garnet Li 6.1 La 3 Zr 2 Al 0.3 O 12 Solid-State Electrolyte

All solid-state lithium-ion batteries (ASSLIBs) have gained significant interest in recent years due to their wide range of applications, including mobile devices, electric vehicles, and grid storage. Garnet-type Li 7 La 3 Zr 2 O 12 (LLZO) solid-state electrolyte (SSE) continues to be a significant player in the fabrication of ASSLIBs with excellent ionic conductivity on the order of 10 -3 S•cm -1 with the integration of dopants and sintering aids to assist conductivity and structural evolution during the sintering procedure. Traditional sintering techniques, such as solid-state sintering (SSS), have been proven to yield desirable crystal structures. However, the low ionic conductivity results from inferior microstructure, and lithium loss is a significant challenge. Recently, a relatively novel sintering process called rapid laser reactive sintering (RLRS) has shown great potential for achieving fully dense solid oxide electrolytes with less surface element loss, resulted in high ionic conductivity. Here, we applied the same RLRS method to fabricate LLZO dense electrolyte with different amounts of aluminum dopants. We hope the rapid high-temperature sintering can densify the electrolyte and avoid the lithium loss for achieving high lithium-ion conductivity. In this work, we optimized multiple combinations of laser parameters (speed, power, and defocus distance), initial precursor composition, and controlled atmospheres to discover the optimal conditions for reaching the efficacious crystal structure, microstructure, and ionic conductivity.

25 ENERGY STORAGE↗

Demonstration of a 1 TW peak power, joule-level ultrashort Tm:YLF laser

Here we report on the demonstration of a diode-pumped, Tm:YLF-based, chirped pulse amplification laser system operating at λ ≈ 1.9 µm that produces amplified pulse energies exceeding 1.5 J using a single 8-pass power amplifier. The amplified pulses are subsequently compressed to sub-300 fs durations by a diffraction grating pair, producing record >1 TW peak power pulses. To the best of our knowledge, this is the highest peak power demonstrated for any solid-state, near-2 µm laser architecture and illustrates the potential of Tm:YLF for the next generation of high-power, diode-pumped ultrashort lasers.

47 OTHER INSTRUMENTATION↗

Differentiating multi-MeV, multi-ion spectra with CR-39 solid-state nuclear track detectors

The development of high intensity petawatt lasers has created new possibilities for ion acceleration and nuclear fusion using solid targets. In such laser-matter interaction, multiple ion species are accelerated with broad spectra up to hundreds of MeV. To measure ion yields and for species identification, CR-39 solid-state nuclear track detectors are frequently used. However, these detectors are limited in their applicability for multi-ion spectra differentiation as standard image recognition algorithms can lead to a misinterpretation of data, there is no unique relation between track diameter and particle energy, and there are overlapping pit diameter relationships for multiple particle species. In this report, we address these issues by first developing an algorithm to overcome user bias during image processing. Second, we use calibration of the detector response for protons, carbon and helium ions (alpha particles) from 0.1 to above 10 MeV and measurements of statistical energy loss fluctuations in a forward-fitting procedure utilizing multiple, differently filtered CR-39, altogether enabling high-sensitivity, multi-species particle spectroscopy. To validate this capability, we show that inferred CR-39 spectra match Thomson parabola ion spectrometer data from the same experiment. Filtered CR-39 spectrometers were used to detect, within a background of ~ 2 × 10 11 sr -1 J -1 protons and carbons, (1.3 ± 0.7) × 10 8 sr -1 J -1 alpha particles from laser-driven proton-boron fusion reactions.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

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↗

Solid-state optical refrigerator for cryogenic cooling of payloads

A solid-state optical refrigerator for cryogenic cooling of a payload, the solid-state optical refrigerator including a laser cooling crystal including a first material and a dopant material; a thermal link including a second material, the thermal link being bonded to the laser cooling crystal and the thermal link being configured to be thermally linked to the payload to transfer heat conductively from the payload to the laser cooling crystal via the thermal link; and a vacuum chamber housing the laser cooling crystal and the thermal link, the vacuum chamber and thermal link having a combination of shape and coating such that laser and fluorescence light reflected off a wall of the vacuum chamber and laser and fluorescence light propagating within the thermal link are not incident on the payload.

Hehlen, Markus Peter↗

Clarifying the formation of equiaxed grains and microstructural refinement in the additive manufacturing of Ti-Cu

Controlling microstructural evolution in metallic additive manufacturing (AM) is difficult, especially in producing refined as-built grains instead of coarse, directional grains. Traditional solutions involve adding inoculants to AM feedstocks, but titanium (Ti) alloys cannot employ this approach without producing detrimental secondary phases. Ti-Cu (Ti-copper) alloys offer a solution through constitutional supercooling and/or solid state thermal cycling under AM conditions. This work analyzes a compositionally graded directed energy deposition (DED) Ti-Cu build, single-melt laser tracks, and dilatometric heat treatments to evaluate if, when, and by what mechanism(s) microstructural refinement occurs. Refinement by inoculation of unmelted powder particles was also considered. Constitutional supercooling produced no net microstructural refinement as any equiaxed dendrites which form are remelted with new deposition. This finding agreed with solidification modeling of powder bed fusion-laser beam (PBF-LB) and DED builds. Solid state thermal cycling refined microstructures only during ex-situ dilatometric heat treatments, suggesting build parameter optimization is needed to achieve refinement in-situ. Accidental heterogeneous nucleation on unmelted Ti powder, originating from the different thermophysical properties of Ti and Cu, provided the most significant microstructural refinement. This work systematically assesses the microstructural refinement mechanisms of Ti-Cu in AM builds and offers insights into microstructural control in eutectoid alloys.

36 MATERIALS SCIENCE↗

Leveraging the redox activities of cerium and dibenzotetrathiafulvalene to discover a photo-responsive magnetic material

Stimuli-responsive changes in lanthanide-based materials are a promising research direction. In this study, [DBTTF] 4 [Ce 2 Cl 10 ] DBTTF = dibenzotetrathiafulvalene (1) was synthesized by a light-induced crystallization, where photo-oxidation of DBTTF enables formation of the cerium dimer [Ce 2 Cl 10 ] 4− . Intermolecular interactions between the stacked organic units of the crystal result in charge transfer bands in the visible-NIR (near-infrared) region, evident in the solid-state absorption spectrum upon comparison with the solution spectrum. The assignments of the sublattice oxidation states were made with single-crystal X-ray diffraction (SC-XRD) structural characterization, Raman spectroscopy, X-ray absorption spectroscopy, and magnetometry. Continuous 532 nm laser irradiation of the microcrystalline solid modulates the redox states in 1, leading to ∼40% reduction in the observed magnetization at 2 K. Density functional theory PBE+U/HSE06 band structure calculations predict Mott insulating behavior in 1, with a bandgap of 0.54/0.81 eV, and further support the conjecture that the observed photo-induced change in magnetization results from electron transfer from the [Ce 2 Cl 10 ] 4− anions to the π-stacked [DBTTF] 2 2+ organic dimer subunits. An enhancement in conductivity is similarly observed upon 532 nm irradiation, determined by single-crystal transport measurements. The findings reveal that photo-responsive lanthanide-based materials can be achieved by integration of redox-active organic moieties with redox-active lanthanide cations for the realization of switchable, photo-magnetic materials.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Time-Resolved X-ray Emission Spectroscopy and Resonant Inelastic X-ray Scattering Spectroscopy of Laser Irradiated Carbon

The existence of liquid carbon as an intermediate phase preceding the formation of novel carbon materials has been a point of contention for several decades. Experimental observation of such a liquid state requires nonthermal melting of solid carbon materials at various laser fluences and pulse properties. Reflectivity experiments performed in the mid-1980s reached opposing conclusions regarding the metallic or insulating properties of the purported liquid state. Time-resolved X-ray absorption studies showed shortening of C–C bonds and increasing diffraction densities, thought to evidence a liquid or glassy carbon state, respectively. Nevertheless, none of these experiments provided information on the electronic structure of the proposed liquid state. Herein, we report the results of time-resolved resonant inelastic X-ray scattering (RIXS) and time-resolved X-ray emission spectroscopy (XES) studies on amorphous carbon (a-C) and ultrananocrystalline diamond (UNCD) as a function of delay time between the irradiating pulse and X-ray probe. For both a-C and UNCD, we attribute decreases in RIXS or XES signals to transition blocking, relaxation, and finally, ablation. Increased signal at 20 ps following the irradiation of the UNCD is attributed to the probable formation of nanoscale structures in the ablation plume. Further, differences in the amount of signal observed between a-C and UNCD are explained by the difference in sample thickness and, specifically, incomplete melting of the UNCD film. Comparisons to spectral simulations based on MD trajectories at extreme conditions indicate that the carbon state in our experiments is crystalline. Normal mode analysis confirmed that symmetrical bending or stretching of the C–C bonds in the diamond lattice results in XES spectra with small intensity differences. Overall, we observed no evidence of melting to a liquid state, as determined by the lack of changes in the spectral properties for up to 100 ps delays following the melting pulses.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Ionization-Based Optical Structures for the Control of Short-Pulse Lasers (Abbreviated LDRD Report)

The intensity of light from the highest-power lasers is limited by the size of the optics required to amplify, compress, transport, and focus a laser beam. Indeed, optics damage puts strict constraints on the laser energy density that solid optics can sustain; this leads to enormous optics sizes and limits the maximum intensity that these lasers can achieve. In this project we investigated new types of diffractive optics based on mixtures of neutral gas and plasmas. The basic idea is to interfere laser beams in a gas near the ionization threshold, so that plasma is created in the constructive interference regions (i.e., the “bright” fringes of the interference pattern) while the destructive interference regions remain a neutral gas. The resulting refractive index modulation, due to the different indices in gas vs. plasma, effectively turns such structures into diffractive optics elements. We proposed several new types of optics based on this general concept: i) reflection gratings, which can act as mirrors of “pulse cleaners” to eliminate laser pre-pulse; ii) transmission gratings, as part of a new type of pulse compression scheme with the potential to achieve laser intensities orders of magnitude above what is currently feasible using solid-state optics; and iii) holographic lenses, to focus high-power lasers. We conducted laboratory experiments which demonstrated high efficiency reflection gratings, paving the way for practical applications of our new concepts.

47 OTHER INSTRUMENTATION↗

Ultrafast time-resolved 2D imaging of laser-driven fast electron transport in solid density matter using an x-ray free electron laser

High-power, short-pulse laser-driven fast electrons can rapidly heat and ionize a high-density target before it hydrodynamically expands. The transport of such electrons within a solid target has been studied using two-dimensional (2D) imaging of electron-induced Kα radiation. However, it is currently limited to no or picosecond scale temporal resolutions. Here, we demonstrate femtosecond time-resolved 2D imaging of fast electron transport in a solid copper foil using the SACLA x-ray free electron laser (XFEL). An unfocused collimated x-ray beam produced transmission images with sub-micron and ~10 fs resolutions. The XFEL beam, tuned to its photon energy slightly above the Cu K-edge, enabled 2D imaging of transmission changes induced by electron isochoric heating. Time-resolved measurements obtained by varying the time delay between the x-ray probe and the optical laser show that the signature of the electron-heated region expands at ~25% of the speed of light in a picosecond duration. Time-integrated Cu Kα images support the electron energy and propagation distance observed with the transmission imaging. The x-ray near-edge transmission imaging with a tunable XFEL beam could be broadly applicable for imaging isochorically heated targets by laser-driven relativistic electrons, energetic protons, or an intense x-ray beam.

47 OTHER INSTRUMENTATION↗

Laser-based conversion electron Mössbauer spectroscopy of 229 ThO 2

The exceptionally low-energy 229 Th nuclear isomeric state is expected to provide several new and powerful applications, including the construction of a robust and portable solid-state nuclear clock, perhaps contributing to a redefinition of the second, exploration of nuclear superradiance and tests of fundamental physics. Further, analogous to the capabilities of traditional Mössbauer spectroscopy, the sensitivity of the nucleus to its environment can be used to realize laser Mössbauer spectroscopy and, with it, new types of strain and temperature sensors and a new probe of the solid-state environment, all with excellent sensitivity. However, current models for examining the nuclear transition in a solid require the use of a high-bandgap, vacuum ultraviolet (VUV) transmissive host, severely limiting the applicability of these techniques. Here we report the first, to the authors’ knowledge, demonstration of laser-induced conversion electron Mössbauer spectroscopy (CEMS) of the 229 Th isomer in a thin ThO 2 sample whose bandgap (approximately 6 eV) is considerably smaller than the nuclear isomeric state energy (8.4 eV). Unlike fluorescence spectroscopy of the 229 Th isomeric transition, this technique is compatible with materials whose bandgap is less than the nuclear transition energy, opening a wider class of systems to study and the potential of a conversion-electron-based nuclear clock.

36 MATERIALS SCIENCE↗

Enhanced Isomer Population via Direct Irradiation of Solid-Density Targets Using a Compact Laser-Plasma Accelerator

Excitation of long-lived states in bromine nuclei using a tabletop laser-plasma accelerator providing pulsed (<100 fs) electron beams provided a sensitive probe of γ strength and level densities in the nuclear quasicontinuum and may indicate angular momentum coupling through electron-nuclear interactions. Solid-density active $LaBr_{3}$ targets absorb real and virtual photons up to 35 ± 2.5 MeV and deexcite through γ cascade into different states. Here, a factor of 4.354 ± 0.932 enhancement of the $^{80}Br^{m}/^{80}Br^{g}$ isomeric ratio was observed following electron irradiation, as compared to bremsstrahlung. Additional angular momentum transfer could possibly occur through nuclear-plasma or electron-nuclear interactions enabled by the ultrashort electron beam. Further investigation of these mechanisms could have far-reaching impact including decreased storage of long-term nuclear waste and an improved understanding of heavy element formation in astrophysical settings.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

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↗

Photo-exfoliation of MoS 2 quantum dots from nanosheets: an in-situ transmission electron microscopy study

Fabrication of transition metal dichalcogenide (TMD) quantum dots (QDs) is complex and requires submerging of powders in binary solvents and the constant tuning of wavelength and pulsed frequency of light to achieve a desired reaction. Here,iInstead of liquid state photoexfoliation, we utilize infrared laser irradiation of free-standing MoS 2 flakes in transmission electron microscope (TEM) to achieve solid-state multi-level photoexfoliation of QDs. By investigating the steps involved in photochemical reaction between the surface of MoS 2 and the laser beam, we gain insight into each step of the photoexfoliation mechanism and observe high yield production of QDs, led by an inhomogeneous crystalline size distribution. Additionally, by using a laser with a lower energy than the indirect optical transition of bulk MoS 2 , we conclude that the underlying phenomena behind the photoexfoliation is from multi-photon absorption achieved at high optical outputs from the laser source. These findings provide an environmentally friendly synthesis method to fabricate QDs for potential applications in biomedicine, optoelectronics, and fluorescence sensing.

36 MATERIALS SCIENCE↗