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DOE OSTI2022

Excited-State-Selective Ultrafast Relaxation Dynamics and Photoisomerization of trans-4,4'-Azopyridine

Here, excited-state dynamics of trans-4,4’-azopyridine in ethanol is studied using femtosecond transient absorption with 30 fs temporal resolution. Exciting the system at three different wavelengths, 460- and 290-(275) nm, to access the S 1 n,π* and S 2 π,π* electronic states, respectively, reveals a 195 cm -1 vibrational coherence, that suggests that the same mode is active in both n,π* and π,π* relaxation channels. Following S 1 -excitation, relaxation proceeds via a nonrotational pathway, where a fraction of the n,π* population is trapped in a planar minimum (lifetime, 2.1 ps), while the remaining population travels further to a second shallow minimum (lifetime, 300 fs) prior to decay into the ground state. Population of the S 2 state leads to 30-fs non-rotational relaxation with a concurrent buildup of n,π* population and nearly simultaneous formation of hot ground state species. An increase in the cis-isomer quantum yield upon π,π* vs. n,π* excitation is observed, which is opposite to trans-azobenzene.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2023

Independence of Environmental and Mechanical Damages on Silicone Adhesive Stored in a Thermo-Oxidative Environment

Abstract Elastomeric polymer materials hold a special place in today’s industrial sectors with respect to structural application needs. Low quality materials are detrimental to industries like aerospace, and automotive engineering. Assessment of the durability of elastomers for structural applications has been of much interest among the literary circles for decades and new materials keep outperforming the existing ones. Polymeric adhesives are one of the most abundantly used materials in these industries. All polymeric materials get damaged when in contact with aggressive environments in presence of high temperature and oxygen. Commonly referred to as thermo-oxidation, this environment exposes the material to heat and oxidation reactions in presence of oxygen. Resultantly, during service life, the damage to the polymer matrix is primarily caused by two factors: mechanical damage and environmental aging. Environmental aging is an irreversible phenomenon caused by changes in the molecular structure while mechanical damage maintains the shape of the polymer matrix, and the deterioration is mostly due to polymer chain mobility. Environmental aging can be caused by a single environmental agent or by a synergized impact of several environmental elements. Increasing temperature is found to be proportional to decreasing tensile strength and toughness of material. The rate and extent of degradation can be accessed by scrutinizing the changes in constitutive behavior of material through mechanical and chemical properties. Accelerated thermal aging is among the most common modes of process related degradation, leading generally to chain scission, and crosslinking phenomena and reduced resistance to fracture stress, and strain. In this experimental study, our goal is to separate the environmental degradation from mechanical damage. A silicone-based adhesive was aged in thermo-oxidative at (0%RH) aging environment. The damage and decay mechanisms have been used to draw a distinction between environmental degradation and mechanical damage. Material characterization included uniaxial tensile test (failure and cyclic) and scanning electron microscopy (SEM) tests on as-received and aged samples. Aging was conducted at three different temperatures (60°C, 80°C and 95°C) and six different exposure durations (1, 3, 10, 30, 90 and 200 days). This work confirms that environmental damage is superposed on top of the mechanical damage, and thus, they are separable. The total mechanical and environmental damage is a synergized effect of all exposure conditions and parameters involved i.e., aging time, temperature, and oxygen. The chemistry and mechanics of the polymer degradation were found to be in good agreement with each other.

Alazhary, Sharif↗

DOE OSTI2021

Selection of $\Lambda^0$ Production Events in MicroBooNE

A selection to find Cabibbo suppressed Λ production events, $\overline{ν}_µ$ + Ar → $µ^+$ + $Λ^0$ + $X$, in the MicroBooNE detector is described. This channel is sensitive to cross section and final state interaction parameters in different ways and can help break their degeneracy. $Λ^0$ production events are distinguished from background by the existence of a secondary vertex created when the $Λ^0$ decays. The selection examines a list of reconstructed particles thought to be the result of a neutrino interaction, first finding a muon candidate, then a proton and $π^-$ candidate and testing their consistency with a $Λ^0 → p+π^-$ decay. The selection achieves an efficiency of approximately 7% while rejecting 99.9999% of the background. This selection is designed to study neutrino interactions in the NuMI flux. After applying the selection, Monte Carlo simulation predicts 9.0 ± 0.8 (MC stat.) signal and 3.1 ± 1.4 background events when combining 1.0 × 10 21 protons on target of neutrino mode flux and 1.3 × 10 21 protons on target of anti-neutrino mode flux, corresponding to a significance of 2.6 $σ$.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

NASA NTRS1976

Theoretical evaluation of rigid baffles in the suppression of combustion instability

An analytical technique for the prediction of the effects of rigid baffles on the stability of liquid propellant combustors is presented. This analysis employs both two and three dimensional combustor models characterized by concentrated combustion sources at the chamber injector and a constant Mach number nozzle. An eigenfunction-matching method is used to solve the linearized partial differential equations describing the unsteady flow field for both models. Boundary layer corrections to this unsteady flow are in a mechanical energy dissipation model to evaluate viscous and turbulence effects within the flow. An integral instability relationship is then employed to predict the decay rate of the oscillations. Results of this analysis agree qualitatively with experimental observations and show that sufficient dissipation exists to indicate that the proper mechanism of baffle damping is a fluid dynamic loss. The response of the dissipation model to varying baffle blade length, mean flow Mach number, oscillation amplitude, baffle configuration, and oscillation mode is examined.

Combustion instability↗

NASA NTRS1991

Implications of solar p-mode frequency shifts

An expression is derived that relates solar p-mode frequency shifts to changes in the entropy and magnetic field of the sun. The frequency variations result from changes in path length and propagation speed. Path length changes dominate for entropy perturbations, and propagation speed changes dominate for most types of magnetic field peturbations. The p-mode frequencies increased along with solar activity between 1986 and 1989; these frequency shifts exhibited a rapid rise with increasing frequency followed by a precipitous drop. The positive component of the shifts can be accounted for by variations of the mean square magnetic field strength in the vicinity of the photosphere. The magnetic stress perturbation decays above the top of the convection zone on a length scale comparable to the pressure scale height and grows gradually with depth below. The presence of a resonance in the chromospheric cavity means that the transition layer maintains enough coherence to partially reflect acoustic waves even near cycle maximum.

Goldreich, Peter↗

NASA NTRS1994

Parameter estimation of the vibrational model for the SCOLE experimental facility

The objective of this study is to experimentally determine an empirical model of the vibrational dynamics of the Spacecraft COntrol Laboratory Experiment (SCOLE) facility. The first two flexible modes of this test article are identified using a linear least-square identification procedure and the data utilized for this procedure are obtained by exciting the structure from a quiescent state with torque wheels. The time history data of rate gyro sensors and accelerometers due to excitation and after excitation in terms of free-decay are used in the parameter estimation of the vibrational model. The free-decay portion of the data is analyzed using the Discrete Fourier transform to determine the optimal model order to use in modelling the response. Linear least-square analysis is then used to select the parameters that best fit the output of an Autoregressive (AR) model to the data. The control effectiveness of the torque wheels is then determined using the excitation portion of the test data, again using linear least squares.

Crotts, B. D.↗

DOE OSTI2026

Quark-universal U(1) breaking scalar at the LHC

If the quarks or leptons are charged under a new U(1) gauge symmetry, then besides a Z′ boson there must exist at least one new boson whose decay products include Standard Model particles. In the case of a minimal symmetry breaking sector, that new boson is a scalar ϕ that couples to the Z′ boson as well as to the new fermions required to cancel the U(1) gauge anomalies. The scalar may be produced at the Large Hadron Collider (LHC) in association with a Z′ boson, or through Z′ boson fusion, while its decays are typically into four jets or two photons. We analyze in detail the case where the Z′ boson is leptophobic, and all the quarks have the same charge under the new U(1). If ϕ mixes with the Standard Model Higgs boson, then the new scalar can also be produced via gluon fusion, and the discovery mode is likely to be a diphoton resonance.

Armbruster, Lorin [Mainz U., Inst. Phys.; U. Mainz↗

DOE OSTI2025

Rippled shock propagation in a laser-driven target at multimegabar pressures

The evolution of non-uniform shocks produced by modulated laser irradiation or surface perturbations is relevant to studies of inertial confinement fusion and material properties at high-energy-density conditions. We present results from an experiment conducted at the OMEGA EP laser facility, where a 300 GPa shock was driven into a fused silica sample with pre-fabricated single-mode surface modulations. Using time-resolved optical velocimetry, we captured the continuous evolution of rippled shock motion, enabling a comprehensive mapping of the spatial amplitude history from formation to phase reversal in a single experiment. Initially, the ablation-driven shock inherits a fraction of the surface modulation amplitude from the sample, which subsequently grows before decaying, ultimately leading to the flattening of the rippled shock and a phase reversal. We find that two-dimensional inviscid hydrodynamic simulation of the experiment is able to qualitatively capture many aspects of the rippled shock evolution but over-predicts the initial amplitude growth. This experimental platform, capable of accommodating varying ripple wavelengths, lays the groundwork for a potential viscometry method at extreme pressures, where viscous effects manifest as differences in shock flattening times between rippled shocks of two distinct wavelengths propagating through the sample.

36 MATERIALS SCIENCE↗

DOE OSTI2025

Global Simulations of Gravitational Instability in Protostellar Disks with Full Radiation Transport. II. Locality of Gravitoturbulence, Clumpy Spirals, and Implications for Observable Substructure

Spiral perturbations in a gravitationally unstable accretion disk regulate disk evolution through angular momentum transport and heating and provide an observational signature of gravitational instability (GI). We use global 3D simulations to systematically characterize and understand these spiral perturbations. The spiral perturbations and the resulting transport are overall insensitive to the cooling type, with the exception that radiative cooling, especially in the optically thick regime, reduces the amplitude of temperature perturbations. Spiral perturbations are localized around corotation, allowing transport to be approximated by a local α viscosity to zeroth order in aspect ratio (H/R), but only after averaging over multiple orbits in time and/or multiple scale heights in space. Meanwhile, large-amplitude perturbations from strong gravitoturbulence can cause $\mathcal{O}$(α 1/2 ) deviation in the cooling rate of the disk. We develop empirical prescriptions for the angular momentum transport, heating, and cooling in a gravitoturbulent disk that capture the deviation from a viscous, unperturbed disk to first order in H/R and α 1/2 . The spiral perturbations in saturated gravitoturbulence are clumpy, with dense clumps forming through the nonlinear coupling between multiple modes at different m. Observationally, the clumpy gravitoturbulence produced by saturated GI can be mistaken with observational noise or embedded companions, especially under finite resolution. Meanwhile, grand-design spirals with m-fold symmetry may be uncommon among disks in saturated gravitoturbulence, and we speculate that they may instead be a signature of recently triggered or decaying GI.

Gravitational instability↗

DOE OSTI2025

Surface Carboxylate Sensitivity to Electron and Hole Relaxation in Photoexcited Cadmium Sulfide Nanocrystals

Understanding how passivating surface ligands couple to excitonic states in nanocrystal photocatalysts is crucial for controlling nonradiative relaxation pathways which compete with interfacial charge transfer. Here, we report femtosecond transient infrared (IR) spectroscopy to resolve ∼100 fs ligand-exciton coupling between 1S exciton states in oleate-capped cadmium sulfide (CdS) nanocrystals and vibrational modes of surface carboxylates. Differential mid-IR spectra show distinct negative amplitude and positive photoinduced absorption signals at ∼1540 cm –1 (carboxylate asymmetric stretch) and ∼1440 cm –1 (carboxylate symmetric stretch), respectively. Fluence-dependent transient IR measurements reveal that the symmetric stretch is uniquely sensitive to picosecond Auger recombination, while the asymmetric stretch shows no analogous decay. Our results provide direct measurement of femtosecond ligand-exciton coupling in CdS nanocrystals and demonstrate how surface-bound carboxylate ligands serve as carrier-specific reporters of nanocrystal photophysics. Furthermore, these findings offer critical insights for designing and developing predictive models for ligand-mediated strategies in next-generation nanocrystal photocatalysts.

Cadmium sulfide↗

DOE OSTI2024

Hidden quantum criticality and entanglement in quench dynamics

Entanglement exhibits universal behavior near the ground-state critical point where correlations are long ranged and the thermodynamic entropy is vanishing. On the other hand, a quantum quench imparts extensive energy and results in a build up of entropy, hence no critical behavior is expected at long times. In this work, we present a new paradigm in the quench dynamics of integrable spin chains which exhibit a ground-state order-disorder phase transition at a critical line. Specifically, we consider a quench along the critical line which displays a volume-law behavior of the entropy and exponentially decaying correlations; however, we show that quantum criticality is hidden in higher-order correlations and becomes manifest via measures such as the mutual information and logarithmic negativity. Furthermore, we showcase the scale invariance of the Rényi mutual information between disjoint regions as further evidence for genuine critical behavior. We attribute the emergent quantum criticality to the soft mode not getting excited in spite of the quench. Moreover, the results presented here are universal to models whose low-energy or long-wavelength dynamics are well described by a free-fermionic field theory. Our results are amenable to an experimental realization on different quantum simulator platforms, particularly the Rydberg simulators. Published by the American Physical Society 2024

Paul, Sanku↗

NASA NTRS1978

Skylab viscous damper study

The proposed magnetically anchored viscous fluid damper can maintain the Skylab in a gravity-gradient stabilized mode at the anticipated reboost altitudes. The parameters influencing damper performance (and thereby affecting the degree of risk) are: (1) amount of skylab pitch bias in the orbit plane which will result from aerodynamic trim conditions of the post-reboost configuration Skylab; (2) the lowest altitude to which the post-reboost Skylab will be allowed to decay prior to the next rendezvous; (3) maximum allowable weight and size of the proposed damper in order to match shuttle/TRS mission constraints; (4) the amount of magnetic materials expected to be in the vicinity of the damper.

Source record↗

DOE OSTI2020

Radio frequency and DC high voltage breakdown of high pressure helium, argon, and xenon

Motivated by the possibility of guiding daughter ions from double beta decay events to single-ion sensors for barium tagging, the NEXT collaboration is developing a program of R&D to test radio frequency (RF) carpets for ion transport in high pressure xenon gas. This would require carpet functionality in regimes at higher pressures than have been previously reported, implying correspondingly larger electrode voltages than in existing systems. This mode of operation appears plausible for contemporary RF-carpet geometries due to the higher predicted breakdown strength of high pressure xenon relative to low pressure helium, the working medium in most existing RF carpet devices. In this paper we present the first measurements of the high voltage dielectric strength of xenon gas at high pressure and at the relevant RF frequencies for ion transport (in the 10 MHz range), as well as new DC and RF measurements of the dielectric strengths of high pressure argon and helium gases at small gap sizes. We find breakdown voltages that are compatible with stable RF carpet operation given the gas, pressure, voltage, materials and geometry of interest.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

DOE OSTI2021

Spin waves and high-frequency response in layered superconductors with helical magnetic structure

Here, we evaluate the spin-wave spectrum and dynamic susceptibility in a layered superconductor with helical interlayer magnetic structure. We especially focus on the structure in which the moments rotate 90 degrees from layer to layer realized in the iron pnictide RbEuFe 4 As 4 . While in nonmagnetic superconductors low-frequency magnetic field decays on the distance of the order of the London penetration depth, spin waves mediate its propagation to much larger distances limited by external dissipation mechanisms. The spin-wave spectrum in superconductors is strongly renormalized due to the long-range electromagnetic interactions between the oscillating magnetic moments. This leads to strong enhancement of the frequency of the mode coupled with uniform field and this enhancement exists only within a narrow range of the c-axis wave vectors of the order of the inverse London penetration depth. The key feature of materials like RbEuFe 4 As 4 is that this uniform mode corresponds to the maximum frequency of the spin-wave spectrum with respect to the c-axis wave vector. As a consequence, the high-frequency surface resistance acquires a very distinct asymmetric feature spreading between the bare and renormalized frequencies. Finally, we also consider excitation of spin waves with the Josephson effect in a tunneling contact between helical-magnetic and conventional superconductors and study the interplay between the spin-wave features and geometrical cavity resonances in the current-voltage characteristics.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

DOE OSTI2021

Search for long-lived particles decaying to e± μ∓ ν

Long-lived particles decaying to e±μ∓ν, with masses between 7 and 50GeV/c 2 and lifetimes between 2 and 50 ps, are searched for by looking at displaced vertices containing electrons and muons of opposite charges. The search is performed using 5.4 fb -1 of p p collisions collected with the LHCb detector at a centre-of-mass energy of $\sqrt{s}$=13TeV. Three mechanisms of production of long-lived particles are considered: the direct pair production from quark interactions, the pair production from the decay of a Standard-Model-like Higgs boson with a mass of 125GeV/c 2 , and the charged current production from an on-shell W boson with an additional lepton. No evidence of these long-lived states is obtained and upper limits on the production cross-section times branching fraction are set on the different production modes.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

DOE OSTI2020

Distended clads gas pressurization and material failure timescales

This document presents timescales for additional failure modes, including pressurization of void space in the pellet to the estimated tensile strength of the pellet. Because helium is known to be captured in the fuel as well as evolved as gas, previous timescales are adjusted to account for the substantial dissolution of helium in the matrix of the fuel at normal fuel temperatures. Helium arises from the decay of the 238Pu in the fuel, and can appear as a gas, creating bubbles within the fuel. The majority of helium is known to be captured within the fuel matrix at the operating temperatures of an isolated clad.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

NASA NTRSDate not supplied

Application of High-Spatial Resolution LA-MC-ICP-MS in Planetary Materials

High-precision stable and radiogenic isotopic measurements of planetary materials can help elucidate processes taking place during early Solar System formation, as well as during subsequent planetary differentiation. Laser Ablation Multi Collector Inductively Coupled Plasma Mass Spectrometry (LA-MC-ICP-MS) adds the valuable ability of preserving the spatial context of these isotopic measurements, by sampling small sample volumes (~10 – 60 um diameter) using a pulsed laser system. In the Center for Isotope Cosmochemistry and Geochronology (CICG) at NASA Johnson Space Center, these in-situ isotopic measurements are primarily made using the Applied SpectraTM iX-fs-Tandem LA-LIBS Instrument coupled to the Nu InstrumentsTM SP1700 MC-ICP-MS. The instrumental set-up also provides simultaneous Laser Induced Breakdown Spectroscopy (LIBS) measurements and the potential use of a low energy path with a collision/reaction cell for additional interference removal, though we focus here on the typical high-energy LA-MC-ICP-MS operation. We will provide examples of stable (e.g., Mg) and radiogenic (e.g., Lu-Hf) isotopic systems measured in planetary materials and their terrestrial analogs. The measurement of mass dependent Mg isotopic variations is an important tool for reconstructing processes such as evaporation and condensation of solids in the solar nebula. For early Solar System samples, Mg isotope measurements are also important for the short-lived (t1/2 = 0.7 Ma) Al-Mg chronometer. During laser ablation analyses, the measurement of the Al-Mg isotopic system is made in medium mass resolution (RP ~9500 at ~20% transmission) to limit interferences from 48Ti2+ and 48Ca2+ on 24Mg+, in addition to 52Cr2+ and 12C14N+ on 26Mg+. Measured in the mineral zircon, the 176Lu-176Hf decay system is often used for understanding the growth of continents on Earth, and is also a vital aid in deciphering early large-scale planetary differentiation processes, such as the crystallization of the lunar magma ocean, which is thought to be responsible for much of the Moon’s crust. Lu-Hf measurements are made in low resolution mode (RP <2000), with 10 ion masses (from 171Yb to 180Hf) measured simultaneously to facilitate corrections for isobaric interferences from 176Yb and 176Lu on 176Hf.

Jacob B Setera↗

DOE OSTI2022

Entanglement and seniority

In quantum mechanics entanglement is the most striking phenomenon which has no counterpart in classical systems. Although, different approaches have already been developed to study correlations in the case of indistinguishable particles, the exploration of the so-called mode entanglement is still in its initial stage in nuclear physics. Study of mode-entanglement in the seniority model, derivation of analytic formulas for the one-body reduced density matrix of states with seniority $ν$ = 0, 1, 2, and $ν$ = 3, and also determination of the particle number dependence of the one-body reduced density matrix for arbitrary seniority. In addition, comparison of the predictions of the seniority model with the results of the shell model to gain insight into the structure and correlations of the ground and lowest yrast states. In the seniority model the analytic results are calculated using the quasi-spin formalism. The numerical shell model calculations are carried out in the standard shell model framework using an inert core. The applied realistic effective interactions are derived earlier using the $G$-matrix formalism. The density matrix renormalization group method is also applied in order to directly calculate the mode entropies. In the seniority model simple analytical expressions are given for the mode entropies. The peculiar behavior of the half-filled shells and the seniority-zero states are revealed. Numerical results are presented for the lightest stable calcium isotopes and for 94 Ru nucleus. For 94 Ru, the seniority model accounts for the 0$g$ 9/2 mode entropies, but seniority mixing is important for certain yrast states. Furthermore, interaction induced quantum fluctuations decrease the occupation of the 0$f$ 5/2 , 1$p$ 3/2 and 1$p$ 1/2 shells, and amount in non-negligible mode entropies on these shells, too, clearly outside the scope of the simple (0$g$ 9/2 ) 4 seniority model. The 0$f$ 7/2 shell-based seniority model is more accurate for the Ca isotopes, but seniority mixing is substantial for some 44 Ca yrast states, too. Mode and one-body entanglement entropies are useful tools to investigate the structure of quantum correlations in nuclei.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗