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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 OSTI2023

DFT-Based Calculation of Molecular Hyperpolarizability and SFG Intensity of Symmetric and Asymmetric Stretch Modes of Alkyl Groups

Vibrational sum frequency generation (SFG) spectroscopy has been extensively used for obtaining structural information of molecular functional groups at two-dimensional (2D) interfaces buried in the gas or liquid medium. Although the SFG experiment can be done elegantly, interpreting the measured intensity in terms of molecular orientation with respect to the lab coordinate is quite complicated. One of the main reasons is the difficulty of determining the hyperpolarizability tensors of even simple molecules that govern their SFG responses. The single-bond polarizability derivative (SBPD) model has been proposed to estimate the relative magnitude of SFG-active hyperpolarizability by assuming that the perturbation associated to each vibration is negligible. In this study, density functional theory (DFT) was used to calculate the polarizability and dipole derivative tensors of the CH 3 stretch mode of CH 3 I, CH 3 CH 2 I, CH 3 OH, CH 3 CH 2 OH. Then, the hyperpolarizability tensors of symmetric and asymmetric vibration modes were calculated considering the Boltzmann distribution of representative conformers, which allowed theoretical calculation of their SFG intensities at all polarization combinations as a function of the tilt angle of the CH 3 group with respect to the surface normal direction. Then the ratios of the calculated SFG intensities for the CH 3 peaks used in experimental studies for the CH 3 tilt angle determination were compared. This comparison clearly showed the effect of vibrational coupling among neighboring functional groups. As a result, this study presents new parameters that can be used in determining the average tilt angle of the CH 3 group at the 2D interface with SFG measurements as well as limitations of the method.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2023

Photodissociation of H 2 on Ag and Au Nanoparticles: Effect of Size and Plasmon versus Interband Transitions on Threshold Intensities for Dissociation

This Article provides new insights concerning the simulation of plasmon-driven chemical reactions using real-time TDDFT based on the tight-binding electronic structure code DFTB+, with applications to the dissociation of H 2 on octahedral silver and gold nanoparticles with 19–489 atoms. A new component of these calculations involves sampling a 300 K canonical ensemble to determine the distribution of possible outcomes of the calculations, and with this approach we are able to determine the threshold for dissociation as a function of laser intensity, wavelength, and nanocluster size. We show that the threshold intensity varies as an inverse power of nanocluster size, which makes it possible to extrapolate the results to sizes that are more typical of experimental studies. The intensities obtained from this extrapolation are around a factor of 100 above powers used in the pulsed experiments. This is a closer comparison of theory and experiment than has been obtained in previous real-time simulations, and the remaining discrepancy can be understood in terms of electromagnetic hot spots that are associated with cluster formation. Here, we also compare the influence of plasmon excitation versus interband excitation on reaction thresholds, revealing that for silver clusters plasmon excitation leads to lower thresholds, but for gold clusters interband excitation is more effective. Our study also includes an analysis of charge transfer to and from the H 2 molecule, and a determination of orbital populations during and after the pulse, showing the correlation between metal excitations and the location of the antibonding level of H 2 .

77 NANOSCIENCE AND NANOTECHNOLOGY↗
DOE OSTI2023

Low-Energy Ion Scattering Intensities from Supported Nanoparticles: The Spherical Cap Model

Supported nanoparticles are of great importance to many technologies like fuel processing and chemical synthesis using catalysts and electrocatalysts, energy storage and generation using fuel cells and batteries, electrochemistry, magnetic information storage, and more. Low-energy ion scattering spectroscopy (LEIS) with noble gas ions like He+ is a powerful tool for the characterization of nanoparticles dispersed across flat support surfaces due to its ability to probe the elemental composition in the topmost atomic layer of a surface, providing quantitative information regarding the size and number density of nanoparticles. In this work, we present a derivation of the LEIS intensities expected from nanoparticles and the support material as a function of the average particle size, their number per unit area, and their contact angle with the support when modeled as spherical caps of the nanoparticle material dispersed over the surface of a flat support. The model assumes that the ion intensities are determined only by the physical blocking of linear ion trajectories and independent of the tilt angle of the local surface relative to the incident and scattered ion directions, an assumption we support by quantitative modeling of published data which tested tilt-angle effects. The model is a generalization to arbitrary contact angles of the hemispherical cap model, which assumes 90° contact angle and has been widely used to model spectroscopic signals in LEIS (and also in Auger and photoelectron spectroscopies) during nanoparticle growth. Here, this new model quantitatively reveals how LEIS signals are sensitive not only to the diameter and number density of the nanoparticle but also to their contact angle (or height/diameter ratio). With the use of additional data (e.g., from microscopy or adsorption microcalorimetry), the model presented here will enable more accurate determination of the average size, shape, and number density of supported nanoparticles based on LEIS intensity measurements.

99 GENERAL AND MISCELLANEOUS↗
DOE OSTI2021

Immobilization of Cyanines in DNA Produces Systematic Increases in Fluorescence Intensity

Cyanines are useful fluorophores for a myriad of biological labeling applications, but their interactions with biomolecules are unpredictable. Cyanine fluorescence intensity can be highly variable due to complex photoisomerization kinetics, which are exceedingly sensitive to the surrounding environment. This introduces large errors in Förster resonance energy transfer (FRET)-based experiments where fluorescence intensity is the output parameter. However, this environmental sensitivity is a strength from a biological sensing point of view if specific relationships between biomolecular structure and cyanine photophysics can be identified. We describe a set of DNA structures that modulate cyanine fluorescence intensity through the insertion of adenine or thymine bases. These structures simultaneously provide photophysical predictability and tunability. We characterize these structures using steady-state fluorescence measurements, fluorescence correlation spectroscopy (FCS), and time-resolved photoluminescence (TRPL). Here, we find that the photoisomerization rate decreases over an order of magnitude across the adenine series, which is consistent with increasing immobilization of the cyanine moiety by the surrounding DNA structure.

59 BASIC BIOLOGICAL SCIENCES↗
DOE OSTI2020

Direct Observations of Field-Intensity-Dependent Dielectric Breakdown Mechanisms in TiO 2 Single Nanocrystals

One of the main challenges for next-generation electric power systems and electronics is to avoid premature dielectric breakdown in insulators and capacitors and to ensure reliable operations at higher electric fields and higher efficiencies. However, dielectric breakdown is a complex phenomenon and often involves many different processes simultaneously. Here we show distinctly different defect-related and intrinsic breakdown processes by studying individual, single crystalline TiO 2 nanoparticles using in-situ transmission electron microscopy (TEM). As the applied electric field intensity rises, rutile-to-anatase phase transition, local amorphization/melting, or ablation are identified as the corresponding breakdown processes, the field intensity thresholds of which are found to be related to the position of the intensified field and the duration of the applied bias relative to the time of charged defects accumulation. Our observations reveal an intensity-dependent dielectric response of crystalline oxides at breakdown and suggest possible routes to suppress the iniation of premature dielectric breakdown. Hence, they will aid the design and development of next generation robust and efficient solid dielectrics.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Ensemble‐Based Assimilation of Satellite All‐Sky Microwave Radiances Improves Intensity and Rainfall Predictions for Hurricane Harvey (2017)

Abstract Ensemble‐based data assimilation of radar observations across inner‐core regions of tropical cyclones (TCs) in tandem with satellite all‐sky infrared (IR) radiances across the TC domain improves TC track and intensity forecasts. This study further investigates potential enhancements in TC track, intensity, and rainfall forecasts via assimilation of all‐sky microwave (MW) radiances using Hurricane Harvey (2017) as an example. Assimilating Global Precipitation Measurement constellation all‐sky MW radiances in addition to GOES‐16 all‐sky IR radiances reduces the forecast errors in the TC track, rapid intensification (RI), and peak intensity compared to assimilating all‐sky IR radiances alone, including a 24‐hr increase in forecast lead‐time for RI. Assimilating all‐sky MW radiances also improves Harvey's hydrometeor fields, which leads to improved forecasts of rainfall after Harvey's landfall. This study indicates that avenues exist for producing more accurate forecasts for TCs using available yet underutilized data, leading to better warnings of and preparedness for TC‐associated hazards in the future.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2022

Load‐Balancing Intense Physics Calculations to Embed Regionalized High‐Resolution Cloud Resolving Models in the E3SM and CESM Climate Models

Abstract We design a new strategy to load‐balance high‐intensity sub‐grid atmospheric physics calculations restricted to a small fraction of a global climate simulation's domain. We show why the current parallel load balancing infrastructure of Community Earth System Model (CESM) and Energy Exascale Earth Model (E3SM) cannot efficiently handle this scenario at large core counts. As an example, we study an unusual configuration of the E3SM Multiscale Modeling Framework (MMF) that embeds a binary mixture of two separate cloud‐resolving model grid structures that is attractive for low cloud feedback studies. Less than a third of the planet uses high‐resolution (MMF‐HR; sub‐km horizontal grid spacing) relative to standard low‐resolution (MMF‐LR) cloud superparameterization elsewhere. To enable MMF runs with Multi‐Domain cloud resolving models (CRMs), our load balancing theory predicts the most efficient computational scale as a function of the high‐intensity work's relative overhead and its fractional coverage. The scheme successfully maximizes model throughput and minimizes model cost relative to precursor infrastructure, effectively by devoting the vast majority of the processor pool to operate on the few high‐intensity (and rate‐limiting) high‐resolution (HR) grid columns. Two examples prove the concept, showing that minor artifacts can be introduced near the HR/low‐resolution CRM grid transition boundary on idealized aquaplanets, but are minimal in operationally relevant real‐geography settings. As intended, within the high (low) resolution area, our Multi‐Domain CRM simulations exhibit cloud fraction and shortwave reflection convergent to standard baseline tests that use globally homogenous MMF‐LR and MMF‐HR. We suggest this approach can open up a range of creative multi‐resolution climate experiments without requiring unduly large allocations of computational resources.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2024

Synchrotron intensity gradient revealing magnetic fields in galaxy clusters

Magnetic fields and their dynamical interplay with matter in galaxy clusters contribute to the physical properties and evolution of the intracluster medium. However, the current understanding of the origin and properties of cluster magnetic fields is still limited by observational challenges. In this article, we map the magnetic fields at hundreds-kpc scales of five clusters RXC J1314.4-2515, Abell 2345, Abell 3376, MCXC J0352.4-7401, and El Gordo using the synchrotron intensity gradient technique in conjunction with high-resolution radio observations from the Jansky Very Large Array (JVLA) and the Karoo Array Telescope (MeerKAT). We demonstrate that the magnetic field orientation of radio relics derived from synchrotron intensity gradient is in agreement with that obtained with synchrotron polarization. Most importantly, the synchrotron intensity gradient is not limited by Faraday depolarization in the cluster central regions and allows us to map magnetic fields in the radio halos of RXC J1314.4-2515 and El Gordo. We find that magnetic fields in radio halos exhibit a preferential direction along the major merger axis and show turbulent structures at higher angular resolution. The results are consistent with expectations from numerical simulations, which predict turbulent magnetic fields in cluster mergers that are stirred and amplified by matter motions.

79 ASTRONOMY AND ASTROPHYSICS↗
DOE OSTI2020

Femtosecond electronic structure response to high intensity XFEL pulses probed by iron X-ray emission spectroscopy

We report the time-resolved femtosecond evolution of the K-shell X-ray emission spectra of iron during high intensity illumination of X-rays in a micron-sized focused hard X-ray free electron laser (XFEL) beam. Detailed pulse length dependent measurements revealed that rapid spectral energy shift and broadening started within the first 10 fs of the X-ray illumination at intensity levels between 10 17 and 10 18 W cm -2 . We attribute these spectral changes to the rapid evolution of high-density photoelectron mediated secondary collisional ionization processes upon the absorption of the incident XFEL radiation. These fast electronic processes, occurring at timescales well within the typical XFEL pulse durations (i.e., tens of fs), set the boundary conditions of the pulse intensity and sample parameters where the widely-accepted ‘probe-before-destroy’ measurement strategy can be adopted for electronic-structure related XFEL experiments.

99 GENERAL AND MISCELLANEOUS↗
DOE OSTI2021

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

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

Kautz, Elizabeth J. (ORCID:0000000263389223)↗
DOE OSTI2022

Experimental verification of TNSA protons and deuterons in the multi-picosecond moderate intensity regime

Ion acceleration from high intensity short pulse laser interactions is of great interest due to a number of applications, and there has been significant work carried out with laser energies up to a few 100 J with 10's of femtosecond to 1 ps pulse durations. Here, we report results from an experiment at the OMEGA EP laser, where laser energy and pulse length were varied from 100 to 1250 J and 0.7–30 ps, respectively, in the moderate (2 × 10 17 –2 × 10 18 W/cm 2 ) laser intensity regime. Ions and electrons were simultaneously measured from disk targets made of CH and CD by a Thomson parabola and a magnetic spectrometer, respectively. Measurements showed that the electron temperature, T e (MeV), has a dependence on the laser energy, E L (J), and pulse duration, τ L (ps), and its empirical scaling was found to be 0.015 × E L 0.90 τ L –0.48. The maximum proton and deuteron energies are linearly dependent on the electron temperature, (5.60 ± 0.26) × T e and (3.17 ± 0.18) × T e , respectively. A significant increase in proton numbers with the laser energy was also observed. Furthermore, the increase in the maximum proton energy and proton count with higher energy longer duration pulses presented in this article shows that such laser conditions have a great advantage for applications, such as the proton radiograph, in the moderate laser intensity regime.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2023

Flexible tape-drive target system for secondary high-intensity laser-driven sources

Here, we present the development of a flexible tape-drive target system to generate and control secondary high-intensity laser-plasma sources. Its adjustable design permits the generation of relativistic MeV particles and x rays at high-intensity (i.e., ≥1 × 10 18 W cm —2 ) laser facilities, at high repetition rates (>1 Hz). The compact and robust structure shows good mechanical stability and a high target placement accuracy (<4 μm RMS). Its compact and flexible design allows for mounting in both the horizontal and vertical planes, which makes it practical for use in cluttered laser-plasma experimental setups. The design permits ~170° of access on the laser-driver side and 120° of diagnostic access at the rear. A range of adapted apertures have been designed and tested to be easily implemented to the targetry system. The design and performance testing of the tape-drive system in the context of two experiments performed at the COMET laser facility at the Lawrence Livermore National Laboratory and at the Advanced Lasers and Extreme Photonics (ALEPH) facility at Colorado State University are discussed. Experimental data showing that the designed prototype is also able to both generate and focus high-intensity laser-driven protons at high repetition rates are also presented.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2024

Multichannel Doppler fiber-imager spectrometer for spatiotemporal characterization of high-intensity laser-driven plasmas

Here, we demonstrate a flexible multichannel fiber-based imaging Doppler spectrometer to characterize plasmas in high intensity (≥1 × 10 18 W/cm 2 ) laser-plasma experiments at high repetition rates. This instrument collects data from ×21 different plasma locations combining optical fibers and a single imaging spectrometer. This diagnostic maps the plasma velocity evolution as a function of time with sub-pico-second resolution. Experimental results showing 2D velocity measurements of plasma with 20 μm spatial resolution are presented. Intensities of the order of 10 18 W/cm 2 were used to generate a plasma, while a much less intense, frequency doubled (400 nm), probe beam (10 11 W/cm 2 ) was used to measure the Doppler shift from the plasma critical surface. The instrument can be scaled to a larger number of channels (e.g., 100) still using a single spectrometer.

47 OTHER INSTRUMENTATION↗
DOE OSTI2026

Evaluation of a deuterated detector for gamma-ray beam intensity measurements

Laser-Compton scattering sources of quasi-monochromatic γ-ray beams have been in operation for over 30 years, with new facilities being under construction or proposed. To sustain a high-quality experimental physics program, continuous monitoring of these beams is essential by measuring the spectral, temporal, and spatial characteristics. In this work, we introduce a new method for determining the γ-ray beam intensity by using photodisintegration of deuterons in an active target detector approach. Measurements were performed using deuterated liquid scintillator detectors at several incident gamma energies between 4 and 13 MeV at the High Intensity γ-ray Source, Durham, USA. The results demonstrate that an instrument based on a deuterated active detector can be used to monitor the intensity of the γ-ray beam with high efficiency and operational simplicity.

Compton scattering↗
DOE OSTI2020

Effect of hydrothermal synthesis conditions on up-conversion luminescence intensity of β-NaYF{sub 4} : Er{sup 3+}, Yb{sup 3+} submicron particles

The differences in the luminescence intensities of up-conversion β-NaYF{sub 4} : Er{sup 3+}, Yb{sup 3+} particles synthesised by the hydrothermal method under various synthesis conditions are studied. The results of the study lead to the conclusion that in order to achieve the maximum luminescence intensity in such particles, it is necessary to use ammonium fluoride and a medium with pH = 3. In this case, the length of the particles increases, up to the formation of rod-shaped particles. Based on the data on the size of the coherent scattering region and on microstresses, we can assume that the particles are polycrystals. At the same time, limiting the size of the coherent scattering region is possible due to the defective structure. When the nanoparticles are synthesised in a medium with pH = 3, hydrolysed regions containing OH groups are formed on the crystallite surface. The presence of these groups does not affect the intensity of up-conversion luminescence of submicron-size particles. (paper)

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2020

Nonlinear Thomson scattering of a tightly focused relativistically intense laser pulse by an ensemble of particles

We report a study of the process of nonlinear Thomson scattering (NTS) of a tightly focused relativistically intense laser pulse by an ensemble of electrons simulating the result of ionisation of an ultrathin nanofoil. The description of all six components of a laser pulse is based on the Stratton – Chu integrals describing radiation focused by an off-axis parabolic mirror into a spot down to the diffraction limit, which is of practical interest for modern experiments with extreme-intensity lasers, including diagnostics of their parameters. The interaction of a laser pulse with electrons is simulated by the test-particle method, and the resulting trajectories are used to calculate the characteristics of secondary electromagnetic radiation. The effect of the laser-pulse focal spot diameter in the range λ – 6λ on the angular distributions of the radiated energy and NTS spectra, as well as of a laser-beam peak intensity of 10{sup 21} – 10{sup 22} W cm{sup −2} on the spectral width of the secondary radiation is studied in relation to the experimentally implemented focusing scheme using the example of a laser pulse with an initial homogeneous spatial distribution and a duration of ∼25 fs. (interaction of laser radiation with matter. laser plasma)

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2020

Specific features of fluorescence transfer in multiply scattering randomly inhomogeneous layers under intense laser pumping

Based on the analysis of experimental data on the effect of the pulsed laser pump intensity on the spectral properties and the size of the fluorescent response zone in randomly inhomogeneous fluorescent layers, we found that the amplification of spontaneous and stimulated emission significantly affects the statistical properties of the propagation lengths of the fluorescent field partial components in the layers. The experiments are performed with layers of SiO{sub 2} and TiO{sub 2} nanoparticles saturated with rhodamine 6G, pumped by 532-nm laser radiation in the intensity range corresponding to the transient regime from excitation of spontaneous fluorescence to random lasing in the layer. The experimental data are compared with the results of statistical modelling of fluorescence transfer. It is shown that, even at a pump intensity below the random lasing threshold, the spontaneous emission amplification in a layer leads to a significant increase in the contributions to the fluorescence response from partial components with propagation lengths much larger than the layer thickness. This can be interpreted as a manifestation of the quasi-waveguide effect, in which the probability of propagation of diffuse fluorescence components along the layer over distances many times greater than its thickness and the size of the pumped region increases significantly with a decrease in the characteristic radiation amplification length in the layer. (paper)

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2021

Astrophysics & cosmology from line intensity mapping vs galaxy surveys

Line intensity mapping (LIM) proposes to efficiently observe distant faint galaxies and map the matter density field at high redshift. Building upon the formalism in a companion paper, we first highlight the degeneracies between cosmology and astrophysics in LIM. We discuss what can be constrained from measurements of the mean intensity and redshift-space power spectra. With a sufficient spectral resolution, the large-scale redshift-space distortions of the 2-halo term can be measured, helping to break the degeneracy between bias and mean intensity. With a higher spectral resolution, measuring the small-scale redshift-space distortions disentangles the 1-halo and shot noise terms. Additionally, cross-correlations with external galaxy catalogs or lensing surveys further break degeneracies. We derive requirements for experiments similar to SPHEREx, HETDEX, CDIM, COMAP and CONCERTO. We then revisit the question of the optimality of the LIM observables, compared to galaxy detection, for astrophysics and cosmology. We use a matched filter to compute the luminosity detection threshold for individual sources. We show that LIM contains information about galaxies too faint to detect, in the high-noise or high-confusion regimes. We quantify the sparsity and clustering bias of the detected sources and compare them to LIM, showing in which cases LIM is a better tracer of the matter density. We extend previous work by answering these questions as a function of Fourier scale, including for the first time the effect of cosmic variance, pixel-to-pixel correlations, luminosity-dependent clustering bias and redshift-space distortions.

79 ASTRONOMY AND ASTROPHYSICS↗