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At least 955 records · Page 53

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DOE OSTI2025

Time evolution of a pumped molecular magnet—A time-resolved inelastic neutron scattering study

Introducing an experimental technique of time-resolved inelastic neutron scattering (TRINS), we explore the time-dependent effects of resonant pulsed microwaves on the molecular magnet Cr 8 F 8 Piv 16 . The octagonal rings of magnetic Cr 3+ atoms with antiferromagnetic interactions form a singlet ground state with a weakly split triplet of excitations at 0.8 meV. A 4.6 tesla field was applied to tune the splitting between two members of the triplet excited level |1$\rangle$ ↔ |2$\rangle$ to resonance with 105 GHz (0.434 meV) microwaves. The time-dependent occupations of the ground state |0$\rangle$, lower lying levels |1$\rangle$ and |2$\rangle$, and higher energy states |λ ≥ 3$\rangle$ were extracted during and after 20 s long microwave pulses incident along the (101) direction of a Cr 8 F 8 Piv 16 crystal held at 1.9 K. At significantly elevated spin temperatures, we found underpopulation relative to thermal equilibrium of |2$\rangle$ and spin-lattice thermalization time scales ranging from 1.6(2) s to 5.7(2) s depending on the power level. This contrasts with the relaxation time τ 1 (T → 0) = 27(5) 𝛍 s inferred for |2$\rangle$ from in situ Electron Spin Resonance measurements. By probing a broad range of excited states during intense microwave pumping, TRINS thus provides a first view of long lived excited states in a molecular antiferromagnet.

Science & Technology - Other Topics↗

DOE OSTI2025

Resolving the dynamic correlated disorder in KTa 1- x Nb x O 3

Understanding the complex temporal and spatial correlations of ions in disordered perovskite oxides is critical to rationalize their functional properties. Here, in this study, we provide new insights into the longstanding controversy regarding the off-centering of transition metal ions in the archetypal ferroelectric alloy KTa 1-x Nb x O 3 (KTN). By mapping the full energy (E) and wavevector (Q) dependence of the dynamical structure factor S(Q, E) using neutron scattering, and rationalizing our observations with atomistic simulations leveraging machine learning, we fully resolve the static vs dynamic nature of diffuse scattering sheets, as well as their composition (x) and temperature dependence. Our first-principles simulations, extended with machine-learning molecular dynamics, reproduce both inelastic neutron spectra and diffuse features, and establish how dynamically-correlated transition metal off-centerings couple to phonons, unifying local and collective viewpoints. This study sheds new light into an exemplary ferroelectric systems and shows the importance of mapping the full S(Q, E) to reveal critical spatio-temporal correlations of atomic disorder from which functional properties emerge.

42 ENGINEERING↗

DOE OSTI2019

Interface-Resolved Simulations of Reactor Flows

The presented review paper outlines the recent progress of the high-resolution single- and two-phase flow simulations of reactor-relevant flows. Rapid development of high-performance computing capabilities is creating exciting opportunities to study complex reactor thermal hydraulic phenomena. Today’s advances in thermal hydraulic analysis, machine learning techniques and interface resolved simulations will help pave the way to the next level of understanding of two-phase flow behavior in complex geometries. This paper consists of two major parts: (i) history and review of interface tracking simulations for nuclear thermal hydraulics in recent years and (ii) several opportunities to apply those advanced tools in the future. First part will discuss typical computational methods used for those simulations, provide some examples of the past work, as well as computational cost estimates and affordability of such simulations for research and industrial applications. In the second part some specific examples are discussed which could be analyzed using exascale supercomputers being designed and projected to be online in the early 2020s. New generation methodologies are required in order to take full advantage of those capabilities to greatly enhance the scientific understanding of complex two-phase flow phenomena in nuclear reactors under normal operation and postulated accident conditions.

22 GENERAL STUDIES OF NUCLEAR REACTORS↗

DOE OSTI2019

Mixing state evolution of agglomerating particles in an aerosol chamber: Comparison of measurements and particle-resolved simulations

This article introduces a validation study of the stochastic particle-resolved aerosol model PartMC with experimental data from an aerosol chamber experiment. For the experiment, a scanning mobility particle sizer and a single-particle soot photometer were used to monitor the aerosol mixing state evolution of two initially externally-mixed aerosol populations of ammonium sulfate and black carbon particles undergoing agglomeration. We applied an efficient optimization algorithm (ProSRS) to determine several unconstrained simulation parameters and were able to successfully reproduce number concentrations and size distributions of mixed particles that formed by agglomeration. The PartMC modeling method in conjunction with the optimization procedure provides a tool for detailed comparisons of chamber experiments and modeling, where aerosol mixing state is the focus of investigation.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2020

Element- and Time-Resolved Measurements of Spin Dynamics Using X-ray Detected Ferromagnetic Resonance

Although XFMR experiments have been carried out at a number of synchrotron radiation facilities since 2004, only a few facilities currently have XFMR setups available for user operation. Here in this review, we mainly focus on recent developments and work that has been carried out using time-resolved XFMR at beamline 4.0.2 of the Advanced Light Source and at beamline I10 of the Diamond Light Source. The experimental setup and the sample holder used at beamline I10 and beamline 4.0.2, respectively, are shown in Figure 1. We will first introduce the working principle of XFMR and then provide examples of the capabilities of this technique. Finally, we will briefly describe an outlook for the future development of and new opportunities for XFMR.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

DOE OSTI2025

Resolving Mixtures of Soot Characterized by SP-AMS Spectra Using a Latent Dirichlet Allocation Model

Soot produced by detonation or combustion events exhibits different chemical properties depending on the fuel, device construction, and environmental conditions in which the event occurs. These properties can be useful for defining relevant signatures for probabilistically identifying the different types of events that occurred, based on the soot that is produced from these events. However, it is rare to observe samples of soot from a detonation or combustion that are not contaminated by outside particles. In this paper, we present a method for resolving mixtures of soot to determine the contributions of sources that may be present in samples of recovered soot. We use Latent Dirichlet Allocation to describe the generative process for a sample of recovered soot, and use Variational Bayesian Inference to learn about the parameters associated with the generative model. We demonstrate the utility of this method by considering real samples of mixtures of soot under various frameworks to show that the model is able to identify the different components present in a sample of soot as well as their mixing proportions.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2017

Temperature Evolution of Energy Gap and Band Structure in the Superconducting and Pseudogap States of Bi 2 Sr 2 CaCu 2 O 8+ δ Superconductor Revealed by Laser-Based Angle-Resolved Photoemission Spectroscopy

For this study, we carry out detailed momentum-dependent and temperature-dependent measurements on Bi 2 Sr 2 CaCu 2 O 8+δ (Bi2212) superconductor in the superconducting and pseudogap states by super-high resolution laser-based angle-resolved photoemission spectroscopy. The precise determination of the superconducting gap for the nearly optimally doped Bi2212 (T c =91 K) at low temperature indicates that the momentum-dependence of the superconducting gap deviates from the standard d-wave form (cos(2Φ)). It can be alternatively fitted by including a high-order term (cos(6Φ)) in which the next nearest-neighbor interaction is considered. We find that the band structure near the antinodal region smoothly evolves across the pseudogap temperature without a signature of band reorganization which is distinct from that found in Bi 2 Sr 2 CuO 6+δ superconductors. This indicates that the band reorganization across the pseudogap temperature is not a universal behavior in cuprate superconductors. These results provide new insights in understanding the nature of the superconducting gap and pseudogap in high-temperature cuprate superconductors.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

DOE OSTI2020

Time-resolved quantum beats in the fluorescence of helium resonantly excited by XUV radiation

Abstract We report on the observation of time-resolved quantum beats in the helium fluorescence from the transition 1 s 3 p → 1 s 2 s , where the initial state is excited by XUV free electron laser radiation. The quantum beats originate from the Zeeman splitting of the magnetic substates due to an external magnetic field. We perform a systematic study of this effect and discuss the possibilities of studying this phenomenon in the XUV and x-ray regime.

Optics↗

DOE OSTI2017

Quantitative analysis of time-resolved microwave conductivity data

Flash-photolysis time-resolved microwave conductivity (fp-TRMC) is a versatile, highly sensitive technique for studying the complex photoconductivity of solution, solid, and gas-phase samples. The purpose of this paper is to provide a standard reference work for experimentalists interested in using microwave conductivity methods to study functional electronic materials, describing how to conduct and calibrate these experiments in order to obtain quantitative results. The main focus of the paper is on calculating the calibration factor, K, which is used to connect the measured change in microwave power absorption to the conductance of the sample. We describe the standard analytical formulae that have been used in the past, and compare them to numerical simulations. This comparison shows that the most widely used analytical analysis of fp-TRMC data systematically under-estimates the transient conductivity by ~60%. We suggest a more accurate semi-empirical way of calibrating these experiments. However, we emphasize that the full numerical calculation is necessary to quantify both transient and steady-state conductance for arbitrary sample properties and geometry.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

DOE OSTI2022

Spatiotemporally resolved measurements of electric field around a piezoelectric transformer using electric-field induced second harmonic (E-FISH) generation

When a piezoelectric transformer (PT) is actuated at its second harmonic frequency by a low input voltage, the generated electric field at the distal end can be sufficient to breakdown the surrounding gas, making them attractive power sources for non-equilibrium plasma generation. Understanding the potential and electric fields produced in the surrounding medium by the PT is important for effectively designing and using PT plasma devices. In this work, the spatiotemporally resolved characteristics of the electric field generated by a PT operating in open air have been investigated using the femtosecond electric field-induced second harmonic generation (E-FISH) method. Here, electric field components were determined by simultaneously conducting E-FISH measurements with the incident laser polarized in two orthogonal directions relative to the PT crystal. Results of this work demonstrate the spatial distribution of electric field around the PT’s output distal end and how it evolves as a function of time. Notably, the strongest electric field appears on the face of the PT’s distal surface, near the top and bottom edges and decreases by approximately 70% over 3 mm. The time delay between the PT’s input voltage and measured electric field indicates that there is an about 0.45 phase difference between the PT’s input voltage and output signal.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

DOE OSTI2021

Time-resolved particle image velocimetry

Time-resolved particle image velocimetry (TR-PIV) has become widespread in fluid dynamics. Essentially a velocity field movie, the dynamic content provides temporal as well as spatial information, in contrast to conventional PIV offering only statistical ensembles of flow quantities. From these time series arise further analyses such as accelerometry, space-time correlations, frequency spectra of turbulence including spatial variability, and derivation of pressure fields and forces. The historical development of TR-PIV is chronicled, culminating in an assessment of the current state of technology in high-repetition-rate lasers and high-speed cameras. Commercialization of pulse-burst lasers has expanded TR-PIV into more flows, including the compressible regime, and has achieved MHz rates. Particle response times and peak locking during image interrogation require attention but generally are not impediments to success. Accuracy considerations are discussed, including the risks of noise and aliasing in spectral content. Oversampled TR-PIV measurements allow use of multi-frame image interrogation methods, which improve the precision of the correlation and raise the velocity dynamic range of PIV. In combination with volumetric methods and data assimilation, a full four-dimensional description of a flow is not only achievable but becoming standardized. Lastly, a survey of exemplary applications is followed by a few predictions concerning the future of TR-PIV.

47 OTHER INSTRUMENTATION↗

DOE OSTI2024

Resolving crystallographic geometrically necessary dislocations in three dimensions in a hexagonal close packed titanium alloy

Abstract Geometrically necessary dislocation (GND) content is measured from mm 3 -scaled Ti7Al three-dimensional (3D) microstructural data using a theory extended for hexagonal close packed crystals, which accounts for basal, prismatic and pyramidal ⟨ c + a ⟩ type dislocation content. The Ti7Al samples have been mechanically pre-strained to two different strain levels, and will then be strained along the same axis in uniaxial tension during simulation. Both inter- and intragranular GNDs across the microstructures have been characterized, with a large contribution of pyramidal ⟨ c + a ⟩ GNDs, consistent with the relative slip activity involved in pre-straining. The spatially resolved crystallographic GND distributions within the 3D microstructures are used to instantiate a microstructure model for forward modeling deformation simulations by a dislocation density hardening elasto-viscoplastic fast Fourier transform framework. Coarsening the voxel resolution during the initial microstructure construction procedure is shown to strongly impact both the magnitude and spatial distribution of the GNDs and in turn the forward deformation response of the pre-strained material. This study indicates that the voxel resolution desired when transferring from measured to model microstructures need not only be proportionally scaled with the microstructure but also sufficiently fine to capture the subgranular orientation gradients that may already be present in the material.

Materials Science↗

DOE OSTI2018

Characterizing the ionization potential depression in dense carbon plasmas with high-precision spectrally resolved x-ray scattering

We discuss here the possibility of obtaining highly precise measurements of the ionization potential depression in dense plasmas with spectrally resolved x-ray scattering, while simultaneously determining the electron temperature and the free electron density. A proof-of-principle experiment at the Linac Coherent Light Source, probing isochorically heated carbon samples, demonstrates the capabilities of this method and motivates future experiments at x-ray free electron laser facilities.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

DOE OSTI2019

Resolving interactions between ion-cyclotron range of frequencies heating and the scrape-off layer plasma in EAST using divertor probes

Waves in the ion-cyclotron range of frequencies (ICRF) used for tokamak heating are known to interact strongly with the scrape-off layer (SOL) plasma, potentially limiting ICRF performance. We present the effect of ICRF heating on triple-probe signals in the Experimental Advanced Superconducting Tokamak (EAST) experiment, an advanced superconducting tokamak with two ICRF antennas and 12 MW of ICRF source power in support of high-power and long-pulse operation. Applying time-resolved magnetic mapping to the divertor probe arrays enables detailed sensing of the spatial structure of the SOL modifications. We observe a sharp transition in floating potential from negative to positive over a length scale of a centimeter at a major radius just inboard of the ICRF antenna. The largest changes in floating potential are observed not for probes connecting to the active ICRF antennas but rather to the main limiter or limiters for inactive lower hybrid launchers. Ion saturation current can be greatly reduced for probes mapping just in front of an antenna. Where relevant, comparison with results from the National Spherical Torus Experiment are made. This work will provide insight into sputtering, impurity production and antenna coupling as higher ICRF power levels are attempted on EAST.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

DOE OSTI2025

Predictive outlook for experiments resolving prompt vs local redeposition of high- Z materials in tokamaks

High-Z plasma facing components redeposit within the sheath through a combination of two distinct mechanisms: prompt (or geometric-driven) and local (or sheath-driven) redeposition. Experimental efforts are needed to determine the leading-order parameters influencing prompt-vs-local trade-off, which sets the fraction of material entering the scrape-off layer. In preparation for such experiments, leading-order parameters are isolated within the PYEAD-RustBCA-GITR coupled net erosion code using Sobol’ sensitivity analysis. Then, experiments resolving prompt-vs-local trade-off under variation of these leading-order parameters are proposed using an isotopic coupon design with multifaceted diagnostic coverage. The measurability of these experiments is evaluated using synthetic diagnostics.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

DOE OSTI2026

Vibrationally resolved cross sections for proton collisions with hydrogen molecules

The semi-classical molecular convergent close-coupling approach has been applied to proton collisions with molecular hydrogen in the ground electronic and vibrational state. Cross sections for electron loss and electron capture agree well with the experimental data in the intermediate energy range where coupling between electronic reaction channels is strong and previously available calculations produce inconsistent results. Results for elastic scattering and total excitation are compared with effective one-electron coupled-channel calculations, showing that accurate target structure makes an important difference to these cross sections at intermediate energies. The excitation cross sections are calculated using both the fixed-nuclei and adiabatic-nuclei approximations for transitions from the $X^1Σ^+_{\textrm{g}}$ state to the $B^1Σ^+_{\textrm{u}}$, $B'$$^1Σ^+_{\textrm{u}}$, $B''$$^1Σ^+_{\textrm{u}}$, $EF$$^1Σ^+_{\textrm{g}}$, $GK$$^1Σ^+_{\textrm{g}}$, $H$$^1Σ^+_{\textrm{g}}$, $C$$^1Π_{\textrm{u}}$, $D$$^1Π_{\textrm{u}}$, $D'$$^1Π_{\textrm{u}}$, $I$$^1Π_{\textrm{u}}$, and $J$$^1Δ_{\textrm{g}}$ states for proton energies from to keV. We find significant differences between the present ab initio calculations and the equivelocity scaled electron-scattering data that is currently used for collisional-radiative modelling. Furthermore, the adiabatic-nuclei calculations enable us to resolve the final vibrational level after excitation, producing a complete set of cross sections for excitation of ground-state molecular hydrogen for all electronic states up to $n = 3$, where $n$ is the united-atoms-limit principle quantum number.

74 ATOMIC AND MOLECULAR PHYSICS↗

DOE OSTI2018

Characterization of time-resolved emission of N 2 (C) in an atmospheric pressure nanosecond pulsed air-plasma using streak spectroscopy

We present that a new optical emission spectroscopy (OES) system using a streak camera (streak-OES) is developed to obtain highly time-resolved OES measurements of nanosecond-duration pulsed air plasmas at atmospheric pressure. The newly developed system is used to measure the time evolution of the emission of N 2 (C), a critical species in the two-step mechanism of rapid heating characteristic of nanosecond pulsed discharges. Time resolution of less than 400 ps is achieved in the current system, a significant improvement over conventional OES measurements with ICCD cameras or photomultiplier tubes. In addition, as long as the driving voltage pulse lies within the streak camera sweep window, the entire plasma emission spectrum for a single discharge is acquired. This capability is in contrast to prior studies where the time-dependent emission is obtained by plotting measurements at single steps from separate discharges. The effect of pulse repetition frequency (PRF) on the N 2 (C) decay is investigated by recording emission spectra for single discharges at 5–100 kHz. The streak images clearly show that the decay time of the N 2 (C–B, 0–0) transition increases as the PRF is increased. The emission decay exhibits two distinct phases with significantly different decay rates, consistent with prior measurements. The 1/e lifetimes of the two decay regimes are found using exponential fits to the emission decay curves. Additionally, joint statistics relating the decay times and energy deposited in the plasma were also obtained.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

DOE OSTI2020

Time and space resolved diagnostics for plasma thermal-chemical instability of fuel oxidation in nanosecond plasma discharges

Here, an instability in a nanosecond pulsed dielectric barrier discharge plasma occurring in methane–oxygen–argon mixtures is experimentally observed and measured by 1D time-resolved in situ electric field measurements. This instability, which seems to be created by the positive feedback between plasma kinetics and plasma-assisted low temperature fuel oxidation, is studied using electric field induced second harmonic generation and direct ICCD imaging. The rapid formation of streamers from an originally uniform discharge appears to be caused by the chemical kinetics of plasma-assisted low temperature methane oxidation, which may be resulting in a new type of plasma instability: a thermal-chemical instability. The results also revealed that the occurrence of this possible thermal-chemical instability in a reactive flow drastically changes the plasma properties by forming multiple secondary discharges and possibly leads to micron-sized non-uniform electric distributions. Single shot uncalibrated measurements of the electric field of the micron sized streamers appears to show much greater strengths than the average electric field. Furthermore, one-dimensional data analysis shows the positive feedback loop between the streamers and the low temperature plasma assisted oxidation chemistry in the plasma thermal-chemical instability. The present finding advances the understanding plasma instability growth and provides a new way to control plasma uniformity in plasma-assisted combustion and plasma fuel reforming.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗