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At least 1,369 records · Page 76

Ultrafast Dynamics of Excited Electronic States in Nitrobenzene Measured by Ultrafast Transient Polarization Spectroscopy

We investigate ultrafast dynamics of the lowest singlet excited electronic state in liquid nitrobenzene using ultrafast transient polarization spectroscopy, extending the well-known technique of optical Kerr effect spectroscopy to excited electronic states. The third-order nonlinear response of the excited molecular ensemble is measured using a pair of femtosecond pulses following a third femtosecond pulse that populates the S 1 excited state. By measuring this response, which is highly sensitive to details of the excited state character and structure, as a function of time delays between the three pulses involved, we extract the dephasing time of the wave packet on the excited state. The dephasing time, measured as a function of time delay after pump excitation, shows oscillations indicating oscillatory wave packet dynamics on the excited state. Finally, from the experimental measurements and supporting theoretical calculations, we deduce that the wave packet completely leaves the S 1 state potential energy surface after three traversals of the intersystem crossing between the singlet S 1 and triplet T 2 states.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Hydrogen retention in lithium on metallic walls from “in vacuo” analysis in LTX and implications for high-Z plasma-facing components in NSTX-U

The application of lithium to plasma-facing components (PFCs) has long been used as a technique for wall conditioning in magnetic confinement devices to improve plasma performance. Determining the characteristics of PFCs at the time of exposure to the plasma, however, is difficult because they can only be analyzed after venting the vacuum vessel and removing them at the end of an operational period. The Materials Analysis and Particle Probe (MAPP) addresses this problem here by enabling PFC samples to be exposed to plasmas, and then withdrawn into an analysis chamber without breaking vacuum. The MAPP system was used to introduce samples that matched the metallic PFCs of the Lithium Tokamak Experiment (LTX). Lithium that was subsequently evaporated onto the walls also covered the MAPP samples, which were then subject to LTX discharges. In vacuo extraction and analysis of the samples indicated that lithium oxide formed on the PFCs, but improved plasma performance persisted in LTX. The reduced recycling this suggests is consistent with separate surface science experiments that demonstrated deuterium retention in the presence of lithium oxide films. Since oxygen decreases the thermal stability of the deuterium in the film, the release of deuterium was observed below the lithium deuteride dissociation temperature. This may explain what occurred when lithium was applied to the surface of the NSTX Liquid Lithium Divertor (LLD). The LLD had segments with individual heaters, and the deuterium-alpha emission was clearly lower in the cooler regions. The plan for NSTX-U is to replace the graphite tiles with high-Z PFCs, and apply lithium to their surfaces with lithium evaporation. Experiments with lithium coatings on such PFCs suggest that deuterium could still be retained if lithium compounds form, but limiting their surface temperatures may be necessary.

42 ENGINEERING↗

Anisotropy and probe-medium interactions in the microrheology of nematic fluids.

A theoretical formalism is presented to analyze and interpret microrheology experiments in anisotropic fluids with nematic order. The predictions of that approach are examined in the context of a simple coarse-grained molecular model which is simulated using nonequilibrium molecular dynamics calculations. The proposed formalism is used to study the effect of confinement, the type of anchoring at the probe-particle surface, and the strength of the nematic field on the rheological response functions obtained from probe-particle active microrheology. As expected, a stronger nematic field leads to increased anisotropy in the rheological response of the material. It is also found that the defect structures that arise around the probe particle, which are determined by the type of anchoring and the particle size, have a significant effect on the rheological response observed in microrheology simulations. Independent estimates of the bulk dynamic modulus of the model nematic fluid considered here are obtained from small-amplitude oscillatory shear simulations with Lees Edwards boundary conditions. The results of simulations indicate that the dynamic modulus extracted from particle-probe microrheology is different from that obtained in the absence of the particle, but that the differences decrease as the size of the defect also decreases. Importantly, the results of the nematic microrheology theory proposed here are in much closer agreement with simulations than those from earlier formalisms conceived for isotropic fluids. As such, it is anticipated that the theoretical framework advanced in this study could provide a useful tool for interpretation of microrheology experiments in systems such as liquid crystals and confined macromolecular solutions or gels.

Cordoba, Andres↗

Hydrogen Retention in Lithium on Metallic Walls from “In Vacuo” Analysis in LTX and Implications for High-Z Plasma-Facing Components in NSTX-U

The application of lithium to plasma-facing components (PFCs) has long been used as a technique for wall conditioning in magnetic confinement devices to improve plasma performance. Determining the characteristics of PFCs at the time of exposure to the plasma, however, is difficult because they can only be analyzed after venting the vacuum vessel and removing them at the end of an operational period. The Materials Analysis and Particle Probe (MAPP) addresses this problem by enabling PFC samples to be exposed to plasmas, and then withdrawn into an analysis chamber without breaking vacuum. The MAPP system was used to introduce samples that matched the metallic PFCs of the Lithium Tokamak Experiment (LTX). Lithium that was subsequently evaporated onto the walls also covered the MAPP samples, which were then subject to LTX discharges. In vacuo extraction and analysis of the samples indicated that lithium oxide formed on the PFCs, but improved plasma performance persisted in LTX. The reduced recycling this suggests is consistent with separate surface science experiments that demonstrated deuterium retention in the presence of lithium oxide films. Since oxygen decreases the thermal stability of the deuterium in the film, the release of deuterium was observed below the lithium deuteride dissociation temperature. This may explain what occurred when lithium was applied to the surface of the NSTX Liquid Lithium Divertor (LLD). The LLD had segments with individual heaters, and the deuterium-alpha emission was clearly lower in the cooler regions. The plan for NSTX-U is to replace the graphite tiles with high-Z PFCs, and apply lithium to their surfaces with lithium evaporation. Experiments with lithium coatings on such PFCs suggest that deuterium could still be retained if lithium compounds form, but limiting their surface temperatures may be necessary.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Validation of Thermodynamic Vent System Performance using Thermal Desktop

Cryogenic fluid management (CFM) for in-space propulsion systems is crucial to enabling future space missions. A means to control the pressure inside a propellant tank is necessary to prevent the venting of liquid propellant in microgravity environments. A thermodynamic vent system (TVS) is one way to regulate the pressure and temperature of the fluid inside a tank. A previous study created a simplified model of a TVS in a two-phase cryogenic heat exchanger. The TVS expands the working fluid across a Joule-Thomson (J-T) device and routes the cooled fluid through the heat exchanger to remove heat from the surrounding fluid. The model was able to predict the TVS heat extraction performance and was validated against experimental data using the same hardware. This study expands the model of the TVS into Thermal Desktop (TD) and recreates the results from both the original model and the experimental data. This new TD model has the potential to be used to predict TVS heat extraction performance in cryogenic propellant tanks for future space missions.

Cryogenic Fluid Management↗

An Improved Hf Vapor Etching Apparatus for Stardust Particle Extraction

Introduction: The NASA Stardust mission captured thousands of particles from the Jupiter-family comet 81P/Wild 2 in a collector composed of aluminum foil and blocks of silica aerogel [1]. To date, most Wild 2 particles available for study are relatively large and coherent particles extracted individually from the ends of hollow, carrot-shaped impact tracks produced during impact into aerogel. However, >65% of the impacting mass can be found in the ‘bulb’ of the track, including nearly all of the <1 μm size fraction [2]. This fraction contains organic-rich material and is likely to include presolar grains, representing a critical opportunity to constrain the organic and presolar inventory of primitive outer solar system materials. However, the small size and susceptibility of this fraction to melting or alteration during capture poses significant analytical challenges. Previous attempts to extract and concentrate fine-grained material from the bulb of Stardust tracks have attempted to develop techniques that efficiently destroy aerogel and leave impactor particles relatively unharmed. The low density and high porosity of silica aerogel makes it more susceptible to attack by etching with hydrofluoric acid (HF) [3] or CF4 plasma ashing [4] than collected cometary silicates. Previous studies of HF vapor etching used HF solutions varying between 5 to 49% and noted that at high concentrations and etch rates, a liquid droplet was produced according to the etching reaction 4HF + SiO2 → SiF4 (g) + 2H2O [3]. SiF4 readily decomposes into HF and silicic acid in water, which has the potential to alter the freed cometary silicates. The plasma ashing technique avoids production of a liquid droplet and minimizes damage to embedded silicates but requires specialized equipment [4]. In this abstract, we present recent improvements to the HF etching procedure with the aim of constructing an etching chamber capable of slowly etching silica aerogel using small quantities of dilute HF. The etching chamber can be assembled using readily available materials.

Stardust↗

Vortex flux dynamics and harmonic ac magnetic response of Ba(Fe 0.94 Ni 0.06 ) 2 As 2 bulk superconductor

Vortex dynamics and nonlinear ac response are studied in a Ba(Fe 0.94 Ni 0.06 ) 2 As 2 ( T c = 18.5 K) bulk superconductor in magnetic fields up to 12 T via ac susceptibility measurements of the first ten harmonics. A comprehensive study of the ac magnetic susceptibility and its first ten harmonics finds shifts to higher temperatures with increasing ac measurement frequencies (10 to 10,000 Hz) for a wide range of ac (1, 5, and 10 Oe) and dc fields (0 to 12 T). The characteristic measurement time constant t1 is extracted from the exponential fit of the data and linked to vortex relaxation. The Anderson-Kim Arrhenius law is applied to determine flux activation energy E a /k as a function dc magnetic field. The de-pinning, or irreversibility lines, were determined by a variety of methods and extensively mapped. The ac response shows surprisingly weak higher harmonic components, suggesting weak nonlinear behavior. Lastly, our data does not support the Fisher model; we do not see an abrupt vortex glass to vortex liquid transition and the resistivity does not drop to zero, although it appears to approach zero exponentially.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

The effect of divalent salt in chondroitin sulfate solutions

Chondroitin-4 sulfate (CS4) is the main glycosaminoglycan extracted from bovine trachea. CS4 play an important role in osteoarthritis treatment, anticoagulant activity, reduces the degradation of cartilage matrix components, reduces necrosis and apoptosis of chondrocytes and reduces the activity of collagenase. Chondroitin sulfate is also responsible for proteoglycans degradation. Chondroitin sulfate can bind calcium ions with different affinities, depending on their sulfation position. The purpose of this study was to determine the structural properties and the influence of Ca{sup 2+} cations. We carried out measurements on CS4 solutions and mixtures of liquid CS4 with Ca{sup 2+} by Small-Angle Neutron Scattering (SANS). CS4 have a mass fractal behavior and the addition of a salt (CaCl{sub 2}) in CS4 solutions generates the appearance of a correlation peak due to local ordering between adjacent chains with inter-chain distances between 483 Å and 233 Å for a calcium concentration of 0.01% w/w.

60 APPLIED LIFE SCIENCES↗

Anisotropic susceptibilities in the honeycomb Kitaev system α - RuCl 3

The magnetic insulator α - RuCl 3 is a promising candidate to realize Kitaev interactions on a quasi-two-dimensional honeycomb lattice. We perform extensive susceptibility measurements on single crystals of α - RuCl 3 , including angle dependence of the in-plane longitudinal and transverse susceptibilities, which reveal a unidirectional anisotropy within the honeycomb plane. By comparing the experimental results to a high-temperature expansion of a Kitaev-Heisenberg-$\textbf{Γ}$ spin Hamiltonian with bond anisotropy, we find excellent agreement with the observed phase shift and periodicity of the angle-resolved susceptibilities. Within this model, we show that the pronounced difference between in-plane and out-of-plane susceptibilities as well as the finite transverse susceptibility are rooted in strong symmetric off-diagonal $\textbf{Γ}$ spin exchange. The $\textbf{Γ}$ couplings and relationships between other terms in the model Hamiltonian are quantified by extracting relevant Curie-Weiss intercepts from the experimental data.

36 MATERIALS SCIENCE↗

Analysis strategy for ultrafast X-ray photon correlation spectroscopy

We explain an analysis strategy for ultrafast X-ray photon correlation spectroscopy, a technique enabled by X-ray free electron lasers to probe nano- and atomic-scale dynamics in complex systems on nanosecond timescales or faster. Central to the technique is the methodology for extracting contrast in coherent X-ray diffraction patterns, known as speckle patterns. Guided by simulations, we analyze common challenges and examine errors encountered in contrast extraction. A method for accurately determining contrast amid shot noise across a wide range of count rates is presented.

36 MATERIALS SCIENCE↗

Measurement of neutral current single π 0 production on argon with the MicroBooNE detector

We report the first measurement of π 0 production in neutral current (NC) interactions on argon with average neutrino energy of ≲1 GeV. We use data from the MicroBooNE detector’s 85-tonne active volume liquid argon time projection chamber situated in Fermilab’s Booster Neutrino Beam and exposed to 5.89 &#x00D7; 10 20 protons on target for this measurement. Measurements of NC π 0 events are reported for two exclusive event topologies without charged pions. Those include a topology with two photons from the decay of the π 0 and one proton and a topology with two photons and zero protons. Flux-averaged cross-sections for each exclusive topology and for their semi-inclusive combination are extracted (efficiency-correcting for two-plus proton final states), and the results are compared to predictions from the GENIE, NEUT, and NUWRO neutrino event generators. We measure cross sections of 1.243 ± 0.185 (syst) ±0.076 (stat), 0.444 ± 0.098 ± 0.047, and 0.624 ± 0.131 ± 0.075 [10 -38 cm 2 /Ar] for the semi-inclusive NCπ 0 , exclusive NCπ 0 +1p, and exclusive NCπ 0 +0p processes, respectively.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

Inferring Water Content from Neutron Die-away Curves for Planetary Science Applications

Signatures of liquid water on planetary bodies may provide evidence for past, present, or future life elsewhere in the solar system. Multiple current and upcoming planetary science missions are prioritizing the search for water, using innovative technologies and creative algorithms. For this project, we explore the capabilities of an instrument similar to the Dragonfly spacecraft to map water content on the surface of Titan, the largest moon of Saturn. We simulate Dragonfly’s neutron observations for a variety of soil compositions and develop multiple techniques to extract water content from the resultant neutron data. Additionally, we supplement neutron observations with gamma spectroscopy in an attempt to further refine water content estimates. This work is part of a larger study to employ Gaussian process regression to estimate a map of water content along the surface of Titan. Using the estimated map, an algorithm based on prediction difference mapping is employed to optimally move multiple Dragonfly detectors around the surface of Titan, fully autonomously.

79 ASTRONOMY AND ASTROPHYSICS↗

The roles of the binodal curve and the spinodal curve in expansions from the supercritical state with flashing

Data extracted from time-of-flight (TOF) measurements made on steady-state He free jets at Göttingen already in 1986 and for pulsed Ne free jets investigated recently at Tel Aviv have been added to an earlier plot of terminal condensed-phase mass fraction x{sub 2∞} as a function of the dimensionless scaling parameter Γ. Γ characterizes the source (fluid species, temperature, pressure and throat diameter); values of x{sub 2∞} are extracted from TOF measurements using conservation of energy in the free-jet expansion. For nozzles consisting of an orifice in a thin plate; the extracted data yield 22 data points which are correlated satisfactorily by a single curve. The Ne free jets were expanded from a conical nozzle with a 20° half angle; the three extracted data points stand together but apart from the aforementioned curve, indicating that the presence of the conical wall influences significantly the expansion and hence the condensation. The 22 data points for the expansions via an orifice consist of 15 measurements with expansions from the gas-phase side of the binodal curve which crossed the binodal curve downstream from the sonic point and 7 measurements with expansions of the gas-phase product of the flashing which occurred after an expansion from the liquid-phase side of the binodal curve crossed the binodal curve upstream from the sonic point. The association of these 22 points with a single curve supports the alternating-phase model for flows with flashing upstream from the sonic point proposed earlier. In order to assess the role of the spinodal curve in such expansions, the spinodal curves for He and Ne were computed using general multi-parameter Helmholtz-free-energy equation-of-state formulations. Then, for the several sets of source-chamber conditions used in the free-jet measurements, thermodynamic states at key locations in the free-jet expansions (binodal curve, sonic point and spinodal curve) were evaluated, with the expansion presumed to be metastable from the binodal curve to the spinodal curve. TOF distributions with more than two peaks (interpreted earlier as superimposed alternating-state TOF distributions) indicated flashing of the metastable flow downstream from the binodal curve but upstream from the sonic point. This relatively early flashing is due apparently to destabilizing interactions with the walls of the source. If the expansion crosses the binodal curve downstream from the nozzle, the metastable fluid does not interact with surfaces and flashing might be delayed until the expansion reaches the spinodal curve. It is concluded that, if the expansion crosses the binodal curve before reaching the sonic point, the resulting metastable fluid downstream from the binodal curve interacts with the adjacent surfaces and flashes into liquid and vapor phases which expand alternately through the nozzle; the two associated alternating TOF distributions are superposed by the chopping process so that the result has the appearance of a single distribution with three peaks.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Insights From Routine Microbiological Monitoring of Air in Astromaterials Curation Cleanrooms

NASA maintains nine separate cleanrooms at the Johnson Space Center to curate and preserve astromaterials samples. Routine microbial monitoring of the surfaces in these cleanrooms began in 20181. Until recently, materials compatibility requirements prevented monitoring airborne biological particles in all but one of these cleanrooms. New astromaterials collections from carbon rich asteroids are more susceptible to biological degradation than previous collections. Therefore, it is important to monitor the bioburden in the air and on surfaces in these labs. Establishing a comprehensive microbial monitoring program will help inform the monitoring and curation plans for Mars sample return which will include samples that are extremely biologically sensitive. In April of 2022 we began routinely collecting air samples in seven of the nine curation cleanrooms (Meteorite ISO 7 equivalent, Lunar ISO 6 equivalent, Stardust, Hayabusa2, OSIRIS-REx ISO 5 equivalent, and Genesis ISO 4 equivalent) using a sampling device that collects airborne biological particles on an electret filter instead conventional sampler that collect cells in a liquid media or onto organic rich Petri dishes. Electret is a generic term for electrostatically charged media. The charge on these materials increases particle trapping when compared to non-charged filters of similar thickness. N95 respirators also use electret filters. This dry sample collection method allows us to meet materials requirements for all the curation labs and reduces the risk of inadvertently introducing contamination as part of our monitoring effort. This method also allows us to preserve a portion of each sample for DNA extraction and next generation sequencing. DNA sequencing helps us to characterize the portion of the cleanroom microbiome that we cannot culture. We will present the results of our first 8 months of monitoring, compare these results to particle counts in the labs and to measurements made directly onto Petri dishes when possible. We will also make recommendations for modifications to the sampling method to improve sampling efficiency and preserve diversity.

A. B. Regberg↗

Magnetic field induced evolution of intertwined orders in the Kitaev magnet β – Li 2 IrO 3

Recent scattering experiments in the 3D Kitaev magnet β–Li 2 IrO 3 have shown that a relatively weak magnetic field along the crystallographic b axis drives the system from its incommensurate counter-rotating order to a correlated magnet, with a significant uniform ‘zigzag’ component superimposing the magnetization along the field. Here it is shown that the zigzag order is not emerging from its linear coupling to the field (via a staggered, off-diagonal element of the g tensor) but from its intertwining with the incommensurate order and the longitudinal magnetization. The emerging picture explains all qualitative experimental findings at zero and finite fields, including the rapid decline of the incommensurate order with field and the so-called intensity sum rule. The latter are shown to be independent signatures of the smallness of the Heisenberg exchange J, compared to the Kitaev coupling K and the off-diagonal anisotropy Γ. Remarkably, in the regime of interest, the field H* at which the incommensurate component vanishes, depends essentially only on J, which allows us to extract an estimate of J≃4 K from reported measurements of H*. Lastly, we also comment on recent experiments in pressurized β–Li 2 IrO 3 and conclude that J decreases with pressure.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Measurements of the Prompt Fission Neutron Spectrum at LANSCE: The Chi-Nu Experiment

The goal of the Chi-Nu experiment at the Los Alamos Neutron Science Center is to measure the prompt fission neutron spectra from major actinides using a double time-of-flight method with a pulsed, white incoming neutron source. Fission events are detected with a parallel-plate avalanche counter and outgoing neutrons are detected with either a 6 Li-glass or liquid scintillator detector array for low- or high-energy neutrons, respectively. A detector response matrix for the interaction of neutrons with the experimental environment for neutrons measured with the Chi-Nu 6 Li-glass detector array has been calculated to obtain a full understanding of the measured Chi-Nu data and also to allow for nearly instantaneous production of simulated Chi-Nu data spectra. Prompt fission neutron spectra corresponding to 19 incoming neutron energy ranges from 0.7-20 MeV have been extracted using the ratio-of-ratios method with Chi-Nu 6 Li-glass data on the neutron-induced fission of 235 U.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

A method for analyzing the non-stationary nucleation and overall transition kinetics: A case of water

We present the statistical method as a direct extension of the mean first-passage time concept to the analysis of molecular dynamics simulation data of a phase transformation. According to the method, the mean first-passage time trajectories for the first (i = 1) as well as for the subsequent (i = 2, 3, 4,…) nucleation events should be extracted that allows one to calculate the time-dependent nucleation rate, the critical value of the order parameter (the critical size), the waiting times for the nucleation events, and the growth law of the nuclei – i.e., all the terms, which are usually necessary to characterize the overall transition kinetics. There are no restrictions in the application of the method by the specific thermodynamic regions; and the nucleation rate parameters are extracted according to their basic definitions. The method differs from the Wedekind-Bartell scheme and its modification [A. V. Mokshin and B. N. Galimzyanov, J. Phys. Chem. B 116, 11959 (2012)], where the passage-times for the first (largest) nucleus are evaluated only and where the average waiting time for the first nucleation event is accessible instead of the true steady-state nucleation time scale. We demonstrate an efficiency of the method by its application to the analysis of the vapor-to-liquid transition kinetics in water at the different temperatures. The nucleation rate/time characteristics and the droplet growth parameters are computed on the basis of the coarse-grained molecular dynamics simulation data.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗