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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 1,801 records · Page 100
All sourcesNASA NTRSDOE OSTI
DOE OSTI2020

Measurement of the angular dependence of the spontaneous Raman scattering in anisotropic crystalline materials using spherical samples: Potassium dihydrogen phosphate as a case example

A specialized experimental configuration was created to allow for more-accurate characterization of the spontaneous Raman scattering properties in anisotropic materials. This need stems from the challenges, arising from the complexity of light propagation, in obtaining accurate measurements of the angular dependence of the Raman scattering cross section in birefringent materials. The nonlinear optical material KH 2 PO 4 (KDP) is used as a model medium. Our report is motivated by the need to improve our understanding and management of transverse stimulated Raman scattering in KDP crystals and its deuterated analog, DKDP, typically used for frequency conversion and polarization control in large-aperture laser systems. Key to this experimental platform is the use of high-quality spherical samples that enable one to measure the Raman scattering cross section in a wide range of geometries using only a single sample. The effect of polarization rotation of both the pump light and the collected Raman signal must be carefully considered in data analysis and can give rise to artifacts, which can, in part, be mitigated by reducing the input and collection cone angles.

47 OTHER INSTRUMENTATION↗
DOE OSTI2024

Empirical correlations between the function of entropy ( Z S ) and net artificial viscous work in a shock physics hydrocode

Entropy is a state variable that may be obtained from any thermodynamically complete equation of state (EOS). However, hydrocode calculations that output the entropy often contain numerical errors; this is not because of the EOS, but rather the solution techniques that are used in hydrocodes (especially Eulerian) such as convection, remapping, and artificial viscosity. Here, in this work, empirical correlations are investigated to reduce the errors in entropy without altering the solution techniques for the conservation of mass, momentum, and energy. Specifically, these correlations are developed for the function of entropy Z S , and they depend upon the net artificial viscous work, as determined via Sandia National Laboratories’ shock physics hydrocode CTH. These results are a continuation of a prior effort to implement the entropy-based CREST reactive burn model in CTH, and they are presented here to stimulate further interest from the shock physics community. Future work is planned to study higher-dimensional shock waves, shock wave interactions, and possible ties between the empirical correlations and a physical law.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2020

Contribution of cryogenic thermal cycling to the atomic dynamics in a La-based bulk metallic glass with different initial states

Structural rejuvenation in metallic glasses (MGs) induced by cryogenic thermal cycling has been intensively studied. However, the effect of thermal cycling on the atomic dynamics in MGs is still missing. In this work, we present a systematic study on the atomic dynamics in a La-based MG affected by sub-Tg annealing and thermal cycling. We find that the thermal cycling has little effect on the atomic dynamics in both as-cast and annealed MGs although it could significantly increase the free volume and change mechanical properties of the as-cast MG sample. In contrast, both the structure and mechanical properties of the well-relaxed sample are almost unchanged by thermal cycling. Further, the increased open volume, mainly in the form of atomic vacancies, does not greatly promote the atomic dynamics in the as-cast MG sample, indicating that the free volume induced by thermal cycling is not the key factor in stimulating the β-relaxation and the boson peak in the studied MG.

36 MATERIALS SCIENCE↗
DOE OSTI2020

Experimental determination of the thermal, turbulent, and rotational ion motion and magnetic field profiles in imploding plasmas

A tutorial is presented on advances in spectroscopic diagnostic methods developed for measuring key plasma properties in pulsed-power systems such as Z-pinches, magnetized-plasma compression devices, ion and electron diodes, and plasma switches. The parameters measured include the true ion temperature in Z-pinch implosions, which led to a discovery that much of the ion kinetic energy at stagnation is stored in hydrodynamic rather than in thermal motion. This observation contributed a new important insight into the understanding of the ion thermalization at stagnation and stimulated further investigations of turbulence at stagnation, discussed here too. The second part of this tutorial is devoted to the development of measurements for magnetic-field distributions in Z-pinches and in other pulsed-power systems, as well as their use in studying the plasma dynamics, resistivity, and pressure and energy balance. The latter study raises intriguing questions on the implosion process. In particular, in Z-pinches, the current during stagnation was found to largely flow at relatively large radii, outside the stagnation region. The magnetic-field measurements also enable investigations into the compression of a pre-magnetized cylindrical plasma that uncover striking phenomena related to the current flow, where the current was found to redistribute toward the outer regions during the implosion. Observation of the rotation of the magnetized plasma is also discussed. Lastly, experimental and theoretical investigations of a non-diffusive fast penetration of magnetic field into a low-density plasma, including its effect on the plasma dynamics, are described

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2020

Preparation of high orbital angular momentum Rydberg states by optical-millimeter-wave STIRAP

Rydberg states of molecules are intrinsically challenging to study due to the presence of fast non-radiative decay pathways, such as predissociation. However, selectively exciting Rydberg states with values of the orbital angular momentum (ℓ) ℓ ≳ 3 is a productive strategy to minimize this rapid decay and to populate molecular Rydberg states with lifetimes that approach those of atoms. Here, in this proof-of-principle demonstration, we transfer population to an nf Rydberg state of the calcium atom by stimulated Raman adiabatic passage, in which an optical and a millimeter-wave field couple the initial and final states via an intermediate nd Rydberg state. Numerical simulations reproduce the observed time and frequency dependences of the population transfer and suggest the utility of this scheme to populate high-ℓ Rydberg states of molecules.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2020

Fast rise breakdown in dielectric filled air gap for surge protection

Electric discharge across an air gap can be self-healing, providing a unique capability for repetitive, fast, high-voltage/current switching applications through arc conduction. Furthermore, incorporating dielectric granules in the air gap stimulates gas ionization, which lowers the breakdown voltage and narrows breakdown voltage distribution, thereby enabling engineered surge protection from multiple lightning strikes on aerospace vehicles and sensitive solid-state electronics in critical systems. This study investigates the effect of the permittivity of dielectric granules, gap filling, surface roughness, and metal work function on fast-rising, high-voltage breakdowns. In addition to the air gap width, these factors play important roles in gas ionization, field concentration, and initiation of electrical discharge and arcing. Therefore, they could potentially be used to control and narrow operational breakdown voltages for practical applications. Additionally, a modified Langevin–Debye model is developed to correlate the breakdown voltage and the permittivity of the dielectric filler. These investigations identify and highlight key underpinning mechanisms governing the gas discharge behavior across a dielectric filled air gap during voltage surge events.

42 ENGINEERING↗
DOE OSTI2020

Laser propagation in a subcritical foam: Subgrid model

Here, we present a subgrid model for laser propagation in a subcritical foam. Our model describes the expansion of laser-irradiated foam elements that are below the resolution of the simulation grid and predicts the plasma conditions that result from burning down the foam. Our model can be included as a module within a larger multiphysics code, and we have implemented it within the code pF3D, which is used for simulating a laser-plasma interaction. The model predicts a reduced propagation velocity for a laser through a subcritical foam compared to simulating that foam as a homogeneous gas. This is attributed to the laser energy that goes into burning down the foam microstructure. We compare our model against experimental data by simulating a 2 mg/cc SiO 2 foam shot performed at the Janus laser facility at the Lawrence Livermore National Laboratory. pF3D simulations with the foam model predict hot ion temperatures. This leads to a reduction in the level of stimulated Brillouin scattering (SBS), bringing the simulated level of SBS into agreement with the data. Intensity fluctuations at the foam front due to laser speckles and refraction result in ion temperature fluctuations when the foam burns down. These drive long-lived electron density fluctuations on scales that are large compared to the pore size.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2021

Laser transport and backscatter in low-density SiO 2 and Ta2O 5 foams

Experiments using a single 527 nm wavelength beam interacting with sub- and supercritical density SiO 2 and Ta 2 O 5 foams examined laser propagation and backscatter from laser–plasma instabilities such as Stimulated Brillouin Scattering (SBS). Two densities of each material were examined, and multiple diagnostics were used to characterize the propagation and backscatter. For 5 mg/cc SiO 2 (n e /n c = 0.375), the laser propagation distance was well approximated by treating the foam as a gas. However, for the 2 mg/cc SiO 2 foam (n e /n c = 0.15), the same model over-predicts the propagation distance by ~40%. Furthermore, existing analytical theories on propagation through subcritical foams were able to account for this difference. The laser heat wave propagated ~1/2 as far in Ta 2 O 5 than SiO 2 foams with similar electron density. We showed that this difference is due to the increased radiation losses in the higher Z foam. The fraction of backscattered light scales linearly with incident laser intensity for the range of intensities examined. Ta 2 O 5 foams had significantly lower levels of backscatter (1–3%) than the SiO 2 (4–8%), which is consistent with estimates of large Landau damping due to the presence of the oxygen atoms. The measured fraction of SBS backscattered laser energy for a 2 mg/cc SiO 2 foam shot was ~4 times lower than predicted by simulations assuming a gas-like foam. We found that we needed to assume increased ion heating such that T i /T e ~1.2–1.5 in the plasma to agree with the measured SBS reflectivity. Analytical models of laser-heated foams predict preferential heating of the ions as has been observed in previous experiments.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2021

Low mode implosion symmetry sensitivity in low gas-fill NIF cylindrical hohlraums

Achieving an efficient capsule implosion in National Ignition Facility indirect-drive target experiments requires symmetric hohlraum x-ray drive for the duration of the laser pulse. This is commonly achieved using two-sided two-cone laser irradiation of cylindrical hohlraums that, in principle, can zero the time average of all spherical harmonic asymmetry modes <6 as well as the time dependence of the usually dominant mode 2. In practice, experimental evidence indicates that maintaining symmetric drive becomes limited late in the pulse due to the inward expansion of the hohlraum wall and outward expansion of the capsule ablator plasmas impairing the propagation of the inner-cone laser beams. This effect is enhanced in hohlraums employing low gas-fill, now used almost exclusively as these provide the highest performing implosions and reduce Stimulated Brillouin and Raman backscatter losses, since the gas plasma provides less back pressure to limit blow-in of the hohlraum wall and capsule ablator plasmas. In order to understand this dynamic behavior, we combined multi-keV X-ray imaging of the wall and imploded fuel plasmas as we changed a single parameter at a time: hohlraum gas-fill, laser outer cone picket energy, radius of high density carbon capsules used, and laser beam polar and azimuthal pointing geometry. In this work, we developed a physics-based multi-parameter experimental scaling to explain the results that extend prior scalings and compare those to radiation hydrodynamic simulations to develop a more complete picture of how hohlraum, capsule, and laser parameters affect pole vs equator drive symmetry.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2021

Site-specific generation of excited state wavepackets with high-intensity attosecond x rays

High-intensity attosecond x rays can produce coherent superpositions of valence-excited states through two-photon Raman transitions. The broad-bandwidth, high-field nature of the pulses results in a multitude of accessible excited states. Multiconfigurational quantum chemistry with the time-dependent Schrödinger equation is used to examine population transfer dynamics in stimulated x-ray Raman scattering of the nitric oxide oxygen and nitrogen K-edges. Two pulse schemes initiate wavepackets of different characters and demonstrate how chemical differences between core-excitation pathways affect the dynamics. The population transfer to valence-excited states is found to be sensitive to the electronic structure and pulse conditions, highlighting complexities attributed to the Rabi frequency. The orthogonally polarized two- color-pulse setup has increased selectivity while facilitating longer, less intense pulses than the one-pulse setup. Population transfer in the 1s → Rydberg region is more effective but less selective at the nitrogen K-edge; the selectivity is reduced by double core-excited states. Result interpretation is aided by resonant inelastic x-ray scattering maps.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2021

Broadband 2DES detection of vibrational coherence in the S x state of canthaxanthin

The nonadiabatic mechanism that mediates nonradiative decay of the bright S 2 state to the dark S 1 state of carotenoids involves population of a bridging intermediate state, S x , in several examples. The nature of S x remains to be determined definitively, but it has been recently suggested that S x corresponds to conformationally distorted molecules evolving along out-of-plane coordinates of the isoprenoid backbone near a low barrier between planar and distorted conformations on the S 2 potential surface. Here, the electronic and vibrational dynamics accompanying the formation of S x in toluene solutions of the ketocarotenoid canthaxanthin (CAN) are characterized with broadband two-dimensional electronic spectroscopy (2DES) with 7.8 fs excitation pulses and detection of the linear polarization components of the third-order nonlinear optical signal. A stimulated-emission cross peak in the 2DES spectrum accompanies the formation of S x in <20 fs following excitation of the main absorption band. S x is prepared instantaneously, however, with excitation of hot-band transitions associated with distorted conformations of CAN’s isoprenoid backbone in the low frequency onset of the main absorption band. Vibrational coherence oscillation maps and modulated anisotropy transients show that S x undergoes displacements from the Franck–Condon S 2 state along out-of-plane coordinates as it passes to the S 1 state. The results are consistent with the conclusion that CAN’s carbonyl-substituted β-ionone rings impart an intramolecular charge-transfer character that frictionally slows the passage from S x to S 1 compared to carotenoids lacking carbonyl substitution. Despite the longer lifetime, the S 1 state of CAN is formed with retention of vibrational coherence after passing through a conical intersection seam with the S x state.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2021

Mapping wave packet bifurcation at a conical intersection in CH 3 I by attosecond XUV transient absorption spectroscopy

Extreme ultraviolet (XUV) transient absorption spectroscopy has emerged as a sensitive tool for mapping the real-time structural and electronic evolution of molecules. Here, attosecond XUV transient absorption is used to track dynamics in the A-band of methyl iodide (CH 3 I). Gaseous CH 3 I molecules are excited to the A-band by a UV pump (277 nm, ~20 fs) and probed by attosecond XUV pulses targeting iodine I(4d) core-to-valence transitions. Owing to the excellent temporal resolution of the technique, passage through a conical intersection is mapped through spectral signatures of nonadiabatic wave packet bifurcation observed to occur at 15 ± 4 fs following UV photoexcitation. The observed XUV signatures and time dynamics are in agreement with previous simulations [H. Wang, M. Odelius, and D. Prendergast, J. Chem. Phys. 151, 124106 (2019)]. Furthermore, due to the short duration of the UV pump pulse, coherent vibrational motion in the CH 3 I ground state along the C-I stretch mode (538 ± 7 cm -1 ) launched by resonant impulsive stimulated Raman scattering and dynamics in multiphoton excited states of CH 3 I are also detected.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Adaptive four-level modeling of laser cooling of solids

Laser cooling of rare-earth doped solids has been demonstrated across a wide range of material platforms, inspiring the development of simple phenomenological models such as the four-level model to elucidate the universal properties of laser cooling under various operating conditions. However, these models usually require the input of full absorption spectra that must be provided experimentally or by additional complicated atomic modeling. In this Letter, we propose that a four-level model, when extended to admit effective energy levels adaptive to the pumping photon energy, can accurately predict the cooling efficiency as a function of temperature and pumping frequency using only few inputs such as the absorption coefficient measured at a single frequency and temperature. Our model exploits the quasi-equilibrium properties of the excitation of rare-earth ions for the determination of the effective four energy levels. The model is validated against published experimental results for a span of materials including ytterbium/thulium-doped glass and crystals. With the verified model, we derive explicit expressions for the optimal frequency and the operating bandwidth of pumping lasers. Our model significantly simplifies the modeling process of laser cooling and is expected to stimulate further development of optical refrigeration.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2021

Simultaneous mapping of nanoscale dielectric, electrochemical, and ferroelectric surface properties of van der Waals layered ferroelectric via advanced SPM

Ferroelectric surfaces involve a complex interplay between polarization and dielectric properties, internal and external surface charge screening, and ionic and electrochemical effects. There is currently no good way to simultaneously capture all the required information at appropriate length scales. To this end, we present an advanced scanning probe microscopy approach for simultaneously mapping surface potential, dielectric, and piezoelectric properties on the nanoscale. For quantitatively mapping electromechancial properties, we utilize interferometric displacement sensing piezoresponse force microscopy, which measures the effective piezoelectric coefficient free of background artifacts such as the cantilever body electrostatics. The dielectric and surface electrochemical properties are captured during G-mode electrostatic force microscopy/Kelvin probe force microscopy operated in the lift mode. We show the capabilities of this approach on the chemically phase separated composite sample consisting of a van der Waals layered ferroelectric CuInP 2 S 6 phase and a non-polar In 4/3 P 2 S 6 phase. Finally, we demonstrate domain structure evolution during thermally stimulated phase transition.

36 MATERIALS SCIENCE↗
DOE OSTI2022

Cross-beam energy transfer in direct-drive ICF. II. Theory and simulation of mitigation through increased laser bandwidth

The response of the cross-beam energy transfer instability (CBET) to laser bandwidth is investigated through a combination of theory and simulation. Existing linear theory is generalized to treat broadband lasers, demonstrating that CBET is most effectively suppressed when the bandwidth exceeds the ion-acoustic wave (IAW) frequency. It is shown that for such bandwidths, reverse (seed to pump) transfer becomes possible, which reduces the net energy transfer rapidly as bandwidth is increased. The CBET gain exponent in this regime scales with bandwidth (Δω) as Δω−3 for Gaussian or Lorentzian laser spectra with different scalings possible for other spectra. Comparison of our theory with linearized fluid and particle-in-cell simulations, performed with the laser-plasma simulation environment (LPSE) and vector particle in cell (VPIC) codes, respectively, finds that the model is accurate in the absence of nonlinear processes. However, linear analysis also finds that the IAW energy density scales as Δω−1, implying that nonlinear effects may be more difficult to control than the CBET scaling would suggest. Indeed, nonlinear effects are found to be present in VPIC simulations with high-intensity lasers, despite minimal apparent CBET. Nonlinear processes in the VPIC cases include particle trapping, the two-ion wave decay, and ion wave self-focusing. In some high intensity VPIC cases, these effects lead to net energy transfer from seed to pump and increases to backscatter stimulated Brillouin scattering reflectivities. Finally, for a given bandwidth, we show that improved control of nonlinear processes can be achieved via smoothing by spectral dispersion.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2022

Magnetized laser–plasma interactions in high-energy-density systems: Parallel propagation

In this study, we investigate parametric processes in magnetized plasmas, driven by a large-amplitude pump light wave. Our focus is on laser–plasma interactions relevant to high-energy-density (HED) systems, such as the National Ignition Facility and the Sandia MagLIF concept. We present a self-contained derivation of a “parametric” dispersion relation for magnetized three-wave interactions, meaning the pump wave is included in the equilibrium, similar to the unmagnetized work of Drake et al., Phys. Fluids 17, 778 (1974). For this, we use a multi-species plasma fluid model and Maxwell's equations. The application of an external B field causes right- and left-polarized light waves to propagate with differing phase velocities. This leads to Faraday rotation of the polarization, which can be significant in HED conditions. Phase-matching and linear wave dispersion relations show that Raman and Brillouin scattering have modified spectra due to the background B field, though this effect is usually small in systems of current practical interest. We study a scattering process we call stimulated whistler scattering, where a light wave decays to an electromagnetic whistler wave (ω≲ω ce ) and a Langmuir wave. This only occurs in the presence of an external B field, which is required for the whistler wave to exist.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2022

Conical intersection and coherent vibrational dynamics in alkyl iodides captured by attosecond transient absorption spectroscopy

The photodissociation dynamics of alkyl iodides along the C–I bond are captured by attosecond extreme-ultraviolet (XUV) transient absorption spectroscopy employing resonant ∼20 fs UV pump pulses. The methodology of previous experiments on CH3I [Chang et al., J. Chem. Phys. 154, 234301 (2021)] is extended to the investigation of a C–I bond-breaking reaction in the dissociative A-band of C2H5I, i-C3H7I, and t-C4H9I. Probing iodine 4d core-to-valence transitions in the XUV enables one to map wave packet bifurcation at a conical intersection in the A-band as well as coherent vibrations in the ground state of the parent molecules. Analysis of spectroscopic bifurcation signatures yields conical intersection crossing times of 15 ± 4 fs for CH3I, 14 ± 5 fs for C2H5I, and 24 ± 4 fs for i-C3H7I and t-C4H9I, respectively. Observations of coherent vibrations, resulting from a projection of A-band structural dynamics onto the ground state by resonant impulsive stimulated Raman scattering, indirectly reveal multimode C–I stretch and CCI bend vibrations in the A-bands of C2H5I, i-C3H7I, and t-C4H9I.

Chang, Kristina F. (ORCID:000000022315039X)↗
DOE OSTI2022

Stochastic exciton-scattering theory of optical line shapes: Renormalized many-body contributions

Spectral line shapes provide a window into the local environment coupled to a quantum transition in the condensed phase. In this paper, we build upon a stochastic model to account for non-stationary background processes produced by broad-band pulsed laser stimulation, as distinguished from those for stationary phonon bath. In particular, we consider the contribution of pair-fluctuations arising from the full bosonic many-body Hamiltonian within a mean-field approximation, treating the coupling to the system as a stochastic noise term. Herein, using the Itô transformation, we consider two limiting cases for our model, which lead to a connection between the observed spectral fluctuations and the spectral density of the environment. In the first case, we consider a Brownian environment and show that this produces spectral dynamics that relax to form dressed excitonic states and recover an Anderson–Kubo-like form for the spectral correlations. In the second case, we assume that the spectrum is Anderson–Kubo like and invert to determine the corresponding background. Using the Jensen inequality, we obtain an upper limit for the spectral density for the background. The results presented here provide the technical tools for applying the stochastic model to a broad range of problems.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

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