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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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All sourcesNASA NTRSDOE OSTI
DOE OSTI2021

Auger Dynamics in InP/ZnSe/ZnS Quantum Dots Having Pure and Doped Shells

In this study, we report the negative trion and biexciton Auger dynamics in very high-quality InP/ZnSe/ZnS quantum dots (QDs) having varying amounts of indium-based traps in the ZnSe shell. Negative trion times are determined by time-correlated photon-counting measurements on QDs that have been photoreduced with lithium triethylborohydride. We find that the Auger times vary from 280 to 425 ps and scale linearly with the total particle volume. Excess indium in the ZnSe shell gives rise to hole traps that are transiently populated following photoexcitation. Comparing stoichiometric and nonstoichiometric particles, we find that the negative trion lifetimes are independent of the presence of indium in the ZnSe shell. Biexciton dynamics are determined from transient absorption (TA) bleach recovery measurements. Absorption of two photons results in the formation of two types of biexcitons: those having both holes in the InP core (XX state) and those having one hole trapped in the ZnSe shell (XT state). XX state Auger times are measured in stoichiometric QDs, and for these particles, the Auger times are ~80 ps. Nonstoichiometric QDs show an additional long TA decay component, assigned to Auger recombination of the XT state. Here, a previous study (J. Phys. Chem. C 2021, 125, 4110–4118) found that hole trapping at indium-based shell traps results in a slow photoluminescence (PL) rise component. We find that the fraction of the XT state formed by the absorption of two photons correlates with the product of the fraction of slow PL rise and the rise time constant following one-photon excitation.

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

Radiative lifetime-encoded unicolour security tags using perovskite nanocrystals

Traditional fluorescence-based tags, used for anticounterfeiting, rely on primitive pattern matching and visual identification; additional covert security features such as fluorescent lifetime or pattern masking are advantageous if fraud is to be deterred. Herein, we present an electrohydrodynamically printed unicolour multi-fluorescent-lifetime security tag system composed of lifetime-tunable lead-halide perovskite nanocrystals that can be deciphered with both existing time-correlated single-photon counting fluorescence-lifetime imaging microscopy and a novel time-of-flight prototype. We find that unicolour or matching emission wavelength materials can be prepared through cation-engineering with the partial substitution of formamidinium for ethylenediammonium to generate “hollow” formamidinium lead bromide perovskite nanocrystals; these materials can be successfully printed into fluorescence-lifetime-encoded-quick-read tags that are protected from conventional readers. Furthermore, we also demonstrate that a portable, cost-effective time-of-flight fluorescence-lifetime imaging prototype can also decipher these codes. A single comprehensive approach combining these innovations may be eventually deployed to protect both producers and consumers.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2020

Aging of Concrete for the Evaluation of Repair Materials to Protect the Walls of the HCAEX Tunnel at Savannah River - 20301

H-Canyon, located in the Savannah River site, is a unique facility for chemical reprocessing of plutonium, highly-enriched uranium, and other radioactive materials. The exhaust gases of the H-Canyon are sent through the H-Canyon Exhaust (HCAEX) tunnel for contamination removal. Robotic inspections of the tunnel revealed significant degradation of the reinforced concrete structure that was associated with acid attack, and could compromise the structural stability of the tunnel. Thus, the identification and evaluation of potential repair materials that could be applied on the degraded walls to mitigate and prevent further degradation is of significant interest to the Department of Energy and the Savannah River representatives. This research effort has been divided into two phases: 1) Development and evaluation of aged concrete under accelerated aging conditions (which is the focus of this paper) and 2) Evaluation of potential repair materials applied on aged and non-aged concrete under simulated aggressive conditions. In order to develop and evaluate concrete samples exposed to accelerated aging conditions in simulated aggressive environments, a literature review of the HCAEX tunnel was conducted that included 1) characterization and extent of the concrete damage, 2) environmental conditions inside the tunnel and 3) primary deterioration mechanisms. In addition, potential coatings and/or repair materials for degraded concrete surfaces exposed to aggressive environments (primarily acidic) were selected from the literature review and the most common testing and measurements for evaluating acid attack phenomena, erosion, etc. were reviewed. From the literature review findings, a preliminary bench-scale test plan for the concrete aging was developed, including accelerated aging tests with aggressive conditions (acid fumes, humidity, etc.). Concrete samples were exposed to the aging accelerated conditions (e.g. immersion in acid solutions) and visual inspection, mass loss and pH change (acid solution) were recorded over time. Correlations between the visual inspection, mass loss and pH changes results and the aging time or the aging conditions were developed. Specimens submitted to the highest acid concentration showed the fastest and most intense degradation. The type of coarse aggregate (limestone) used for the concrete seemed to be the cause of the fastest aging observed, compared to the cement paste. The research findings created the foundation for the ongoing investigation, in which new concrete samples with a mix design similar to the HCAEX tunnel will be tested and will serve as the substrate for testing the selected coatings and /or repair materials. In this paper, the literature review and preliminary results from the aging tests are provided. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2025

Determining hexavalent chromium transport properties in alkaline nuclear waste using nuclear magnetic resonance spectroscopy

This study focuses on the transport properties of hexavalent chromium, specifically the chromate anion, to improve predictive models and environmental remediation strategies for Cr(VI) migration. Using 53 Cr Nuclear Magnetic Resonance (NMR) spectroscopy, the research quantifies chromate in multicomponent electrolytes replicating nuclear waste conditions at the Hanford Site in Washington State. The consistency of the 53 Cr NMR signal integral with chromate concentration, despite varying matrix compositions, establishes it as a reliable concentration indicator. The transport properties of chromate in an alkaline solution were assessed using relaxation-based measurements via saturation recovery and Carr-Purcell-Meiboom-Gill experiments, determining spin-lattice and spin-spin relaxation times. These measurements, combined with the Bloembergen-Purcell-Pound equation, helped estimate the rotational correlation time and the 53 Cr self-diffusion coefficient using Stokes-Einstein-Debye and Stokes-Einstein equations. Direct measurements were obtained through pulsed field gradient stimulated echo 53 Cr NMR spectroscopy. Monte Carlo simulations further estimated uncertainty propagation. The results enhance comprehension of chromate transport and highlight prospects for identifying transport properties of NMR-active nuclei, traditionally considered unreachable.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗
DOE OSTI2025

Active-noise-induced dynamic clustering of passive colloidal particles

Active fluids generate spontaneous, often chaotic mesoscale flows. Harnessing these flows to drive soft materials embedded within an active fluid into structures with controlled length scales and lifetimes is a key challenge at the interface between the fields of active matter and nonequilibrium self-assembly. Here, we present a simple and efficient computational approach to model soft materials advected by active fluids, by simulating particles moving in a spatiotemporally correlated noise field. To illustrate our approach, we simulate the dynamical self-organization of repulsive colloids within such an active noise field. The colloids form structures whose sizes and dynamics can be tuned by the correlation time and length of the active fluid, and range from small rotating droplets to clusters with internal flows and system-spanning sizes that vastly exceed the active correlation length. Our results explain how the interplay between active fluid time and length scales and emergent driven assembly can be used to rationally design functional assemblies. More broadly, our approach can be used to efficiently simulate diverse active fluids and other systems with spatiotemporally correlated noise.

Brownian dynamics↗
DOE OSTI2026

Rotational memory function of SPC/E water

Memory effects are essential for the dynamics of condensed materials and are responsible for non-exponential relaxation of correlation functions of dynamic variables through the memory function. Memory functions of dipole rotations for water have never been calculated directly from molecular dynamics simulations. We present here calculations of memory functions for single-dipole rotations and for the overall dipole moment of the sample for SPC/E water. The normalized memory functions for single-particle and collective dipole dynamics turn out to be nearly identical. This result validates theories of dielectric spectroscopy in terms of single-particle time correlation functions and the connection between the collective and single-particle relaxation times through the Kirkwood factor. The dielectric function in this formalism contains no new dynamic information that does not exist in the single-dipole correlation function. A short memory time, ≲1 fs, justifies the use of the mathematics of rotational diffusion to describe the dynamics of a single molecular dipole moment in bulk water. Here, an analytical equation for the rotational memory time is derived.

Asthagiri, Dilipkumar N. [Oak Ridge National Labor↗
DOE OSTI2025

Hidden domain boundary dynamics toward crystalline perfection

A central paradigm of nonequilibrium physics concerns the dynamics of heterogeneity and disorder, impacting processes ranging from the behavior of glasses to the emergent functionality of active matter. Understanding these complex mesoscopic systems requires probing the microscopic trajectories associated with irreversible processes, the role of fluctuations and entropy growth, and the timescales on which nonequilibrium responses are ultimately maintained. Approaches that illuminate these processes in model systems may enable a more general understanding of other heterogeneous nonequilibrium phenomena, and potentially define ultimate speed and energy cost limits for information processing technologies. Here, we apply ultrafast single-shot X-ray photon correlation spectroscopy to resolve the nonequilibrium, heterogeneous, and irreversible mesoscale dynamics during a light-induced phase transition in a (PbTiO 3 ) 16 /(SrTiO 3 ) 16 superlattice. Such ferroelectric superlattice systems are a useful platform to study phase transitions and topological dynamics due to their high degree of tunability. This provides an approach for capturing the nucleation of the light-induced phase, the formation of transient mesoscale defects at the boundaries of the nuclei, and the eventual annihilation of these defects, even in systems with complex polarization topologies. We identify a nonequilibrium correlation response spanning >10 orders of magnitude in timescales, with multistep behavior similar to the plateaus observed in supercooled liquids and glasses. We further show how the observed time-dependent long-time correlations can be understood in terms of stochastic and non-Markovian dynamics of domain walls, encoded in waiting-time distributions with power-law tails. This work defines possibilities for probing the nonequilibrium and correlated dynamics of disordered and heterogeneous media.

36 MATERIALS SCIENCE↗
DOE OSTI2024

Machine Learning‐Assisted Microearthquake Location Workflow for Monitoring the Newberry Enhanced Geothermal System

Abstract Enhanced geothermal systems (EGS) offer a sustainable energy source but face challenges in accurately locating microearthquakes induced during reservoir stimulation. Locating these microearthquakes provides reliable feedback on the stimulation progress. Current deep learning methods for locating earthquakes require extensive data sets for training, which is problematic as detected microearthquakes are often limited. To address the scarcity of training data, we propose a practical workflow using probabilistic multilayer perceptron (PMLP) which predicts microearthquake locations from cross‐correlation time lags in waveforms. Utilizing a 3D velocity model of Newberry site derived from ambient noise interferometry, we generate numerous synthetic microearthquakes and 3D acoustic waveforms for PMLP training. Accurate synthetic tests prompt us to apply the trained network to the 2012 and 2014 stimulation field waveforms. To enhance the accuracy of source localization, we carefully handpick the P‐arrival times. Predictions on the 2012 stimulation data set show major microseismic activity at depths of 0.5–1.2 km, correlating with a known casing leakage scenario. In the 2014 data set, the majority of predictions concentrate at 2.0–2.9 km depths, consistent with results obtained from conventional physics‐based inversion, and align with the presence of natural fractures from 2.0 to 2.7 km. We validate our findings by comparing the synthetic and field picks, demonstrating a satisfactory match for the first arrivals. By combining the benefits of quick inference speeds and accurate location predictions, we demonstrate the feasibility of using realistic synthetic data set to locate microseismicity for EGS monitoring.

15 GEOTHERMAL ENERGY↗
DOE OSTI2023

Noise-specific beating in the higher-level Ramsey curves of a transmon qubit

We report: in the higher levels of superconducting transmon devices and more generally charge sensitive devices, T 2 * measurements made in the presence of low-frequency time-correlated 1/f charge noise and quasiparticle-induced parity flips can give an underestimation of the total dephasing time. The charge variations manifest as beating patterns observed in the overlay of several Ramsey fringe curves and are reproduced with a phenomenological Ramsey curve model, which accounts for the charge variations. T 2 * dephasing times, which more accurately represent the total dephasing time, are obtained. The phenomenological model is compared with a Lindblad master equation model. Both models are found to be in agreement with one another and the experimental data. Finally, the phenomenological formulation enables a simple method in which the power spectral density for the low-frequency noise can be inferred from the overlay of several Ramsey curves.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2023

Analysis of the MUSIC 3 He Multiplicity Data

A measurement campaign called the Measurement of Uranium Subcritical and Critical (MUSiC) was performed on a range of configurations of highly-enriched uranium (HEU) from December 2020 through April of 2021. While part of the focus was to measure reactor kinetics parameters on delayed supercritical systems, an additional focus was performing neutron noise measurements on subcritical configurations from deeply subcritical to nearly delayed critical. Multiple detector systems were used to perform these measurements, such as a 3 He multiplicity detector called the Neutron Multiplicity Array Detector (NoMAD) and a liquid scintillator system called the Rossi-α Measurement Rapid Organic Discriminating Detector (RAM-RODD). Also included were a scintillator system from the University of Michigan and a set of small 3He tubes that have previously been used to measure Rossi-α values on near-critical systems. The focus of this paper will be a comparison of prospective analysis methods for the NoMAD measurements. Previous subcritical measurements at the National Criticality Experiments Research Center (NCERC) submitted to the International Criticality Safety Benchmark Evaluation Project (ICSBEP) used the Hage-Cifarelli formalism of the Feynman Variance-to-Mean method. This relies on the time correlations of neutron detections to infer the spontaneous fission rate and neutron multiplication of a system through binning the time tagged detections and analyzing resulting histograms of the numbers of counts. However, there are other neutron noise methods that rely on similar processes, such as the Hansen-Dowdy formalism which uses a slightly different methodology to extract multiplication from the neutron multiplicity counting moments. Comparisons can be made between these experimental results and those obtained through simulations to validate or identify deficiencies in analysis, detection methods, or the underlying nuclear data. Different time gating strategies and their effects on count rate uncertainties are also investigated.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2023

Looking at supersymmetric black holes for a very long time

We study correlation functions for extremal supersymmetric black holes. It is necessary to take into account the strongly coupled nature of the boundary supergraviton mode. We consider the case with {\cal N}=2 supercharges which is the minimal amount of supersymmetry needed to give a large ground state degeneracy, separated from the continuum. Using the exact solution for this theory we derive formulas for the two point function and we also give integral expressions for any n n -point correlator. These correlators are time independent at large times and approach constant values that depend on the masses and couplings of the bulk theory. We also explain that in the non-supersymmetric case, the correlators develop a universal time dependence at long times. This paper is the longer companion paper of arXiv:2207.00407.

79 ASTRONOMY AND ASTROPHYSICS↗
DOE OSTI2025

Characterization of 6 Li-loaded pulse-shape-discriminating plastic scintillators

Lithium-loaded organic plastic scintillators combine sensitivity to γ rays with the ability to detect both fast and slow neutrons, making them valuable for applications in nuclear security and in basic nuclear and particle physics. The goal of this work is to characterize the neutron response of two custom lithium-loaded organic plastic scintillators developed at Lawrence Livermore National Laboratory. Both are ternary polystyrene-based formulations containing 1.5 wt.% 6 Li salts of isobutyric acid, but they differ in their primary and secondary dye compositions: one uses m-terphenyl as the primary fluor and with Exalite 404 as the wavelength shifter, whereas the other uses 2,5-diphenyloxazole (PPO) and 9,10-diphenyl-anthracene, respectively. The temporal response of the scintillators was measured via time-correlated single photon counting for γ-ray and neutron events. The proton light yield was measured using the double time-of-flight technique from 1.3 to 15 MeV at the 88-Inch Cyclotron at Lawrence Berkeley National Laboratory. For the slow neutron response, an AmBe source moderated with polyethylene was used, and the light output from the 6 Li(n,α)t reaction was characterized. Differences in ionization quenching and temporal response were observed between the two materials with the PPO-containing scintillator exhibiting higher ionization quenching. These results provide performance benchmarks that can guide the design and optimization of future lithium-loaded plastic scintillators for use in basic science and applications.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗
DOE OSTI2022

Heating and Acceleration of Solar Wind by Parametric Decay Instability Mediated Turbulence

One of the main goals of this project to understand the origin of density fluctuations in the solar winds, as revealed by the NASA’s Flagship satellite Parker Solar Probe (PSP) measurements, which motivates us to simulate and analyze magnetohydrodynamic (MHD) turbulence in the compressible regime. To achieve this goal, we have developed a set of sophisticated turbulence driving methods to study how MHD turbulence will develop under different time-correlated fluctuations at large-scales. Another key advance is that we have developed a new 3+1 (three spatial plus time domain) 4D FFT analysis of simulation data-cubes so that we can perform the spatio-temporal spectrum and mode decomposition studies on MHD turbulence.

79 ASTRONOMY AND ASTROPHYSICS↗
DOE OSTI2025

Measurement of correlated charge noise in superconducting qubits at an underground facility

The charge environment of superconducting qubits may be studied through the introduction of controlled, quantified amounts of ionizing radiation. We measure space- and time-correlated charge jumps on a four-qubit device, operating 107 meters below the Earth’s surface in a low-radiation, cryogenic facility designed for the characterization of low-threshold particle detectors. The rock overburden of this facility reduces the cosmic ray muon flux by over 99% compared to laboratories at sea level. Combined with 4π coverage of a movable lead shield, this facility enables quantifiable control over the flux of ionizing radiation on the qubit device. Long-time-series charge tomography measurements on these weakly charge-sensitive qubits capture discontinuous jumps in the induced charge on the qubit islands, corresponding to the interaction of ionizing radiation with the qubit substrate. The rate of these charge jumps scales with the flux of ionizing radiation on the qubit package, as characterized by a series of independent measurements on another energy-resolving detector operating simultaneously in the same cryostat with the qubits. Using lead shielding, we achieve a minimum charge jump rate of $0.19^{+0.04}_{-0.03}$ mHz, almost an order of magnitude lower than that measured in surface tests, but a factor of roughly seven higher than expected based on reduction of ambient gammas alone. We operate four qubits for over 22 consecutive hours with zero correlated charge jumps at length scales above three millimeters.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗
DOE OSTI2026

Evidence for an isomeric {pi}½{sup +}[411] state in {sup 183}Ta

We report on the identification of a new isomeric state in Ta populated via the ground-state -decay of Hf. The experiment was performed at the KISS setup at RIKEN, where neutron-rich hafnium isotopes were produced via multi-nucleon transfer (MNT) reactions, followed by laser ionization of hafnium atoms, mass separation, and detection using an electron-gamma coincidence system. Isomeric spectroscopy was carried out by gating on different electron-gamma time correlations. A 459.1 keV -ray transition was identified in delayed spectra, and a half-life of μ was extracted through time-distribution fitting. The 459.1 keV state in Ta is known from previous work and has been assigned a Nilsson orbital configuration of , while a proposed new isomeric state above it is interpreted as a configuration that decays to via a low-energy, unobserved E2 transition. This is consistent with the systematic trends in neighbouring odd-A nuclei and transition rate calculations. Similar content being viewed by others

Doshi, S.↗
DOE OSTI2020

Time-reversal symmetry breaking in two-dimensional nonequilibrium viscous fluids

In this work, we study the rheological signatures of departure from equilibrium in two-dimensional viscous fluids with and without internal spin. Under the assumption of isotropy, we provide the most general linear constitutive relations for stress and couple stress in terms of the velocity and spin fields. Invoking Onsager's regression hypothesis for fluctuations about steady states, we derive the Green-Kubo formulas relating the transport coefficients to time-correlation functions of the fluctuating stress. In doing so, we show that one of the nonequilibrium transport coefficients, the odd viscosity, requires time-reversal symmetry breaking in the case of systems without internal spin. However, the Green-Kubo relations for systems with internal spin also show that there is a possibility for nonvanishing odd viscosity even when time-reversal symmetry is preserved. Furthermore, we find that breakdown of equipartition in nonequilibrium steady states results in the decoupling of the two rotational viscosities relating the vorticity and the internal spin.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2024

Multivariate Machine Learning Models of Nanoscale Porosity from Ultrafast NMR Relaxometry

Abstract Nanoporous materials are of great interest in many applications, such as catalysis, separation, and energy storage. The performance of these materials is closely related to their pore sizes, which are inefficient to determine through the conventional measurement of gas adsorption isotherms. Nuclear magnetic resonance (NMR) relaxometry has emerged as a technique highly sensitive to porosity in such materials. Nonetheless, streamlined methods to estimate pore size from NMR relaxometry remain elusive. Previous attempts have been hindered by inverting a time domain signal to relaxation rate distribution, and dealing with resulting parameters that vary in number, location, and magnitude. Here we invoke well‐established machine learning techniques to directly correlate time domain signals to BET surface areas for a set of metal‐organic frameworks (MOFs) imbibed with solvent at varied concentrations. We employ this series of MOFs to establish a correlation between NMR signal and surface area via partial least squares (PLS), following screening with principal component analysis, and apply the PLS model to predict surface area of various nanoporous materials. This approach offers a high‐throughput, non‐destructive way to assess porosity in c.a. one minute. We anticipate this work will contribute to the development of new materials with optimized pore sizes for various applications.

Fricke, Sophia N.↗
DOE OSTI2024

Multivariate Machine Learning Models of Nanoscale Porosity from Ultrafast NMR Relaxometry

Abstract Nanoporous materials are of great interest in many applications, such as catalysis, separation, and energy storage. The performance of these materials is closely related to their pore sizes, which are inefficient to determine through the conventional measurement of gas adsorption isotherms. Nuclear magnetic resonance (NMR) relaxometry has emerged as a technique highly sensitive to porosity in such materials. Nonetheless, streamlined methods to estimate pore size from NMR relaxometry remain elusive. Previous attempts have been hindered by inverting a time domain signal to relaxation rate distribution, and dealing with resulting parameters that vary in number, location, and magnitude. Here we invoke well‐established machine learning techniques to directly correlate time domain signals to BET surface areas for a set of metal‐organic frameworks (MOFs) imbibed with solvent at varied concentrations. We employ this series of MOFs to establish a correlation between NMR signal and surface area via partial least squares (PLS), following screening with principal component analysis, and apply the PLS model to predict surface area of various nanoporous materials. This approach offers a high‐throughput, non‐destructive way to assess porosity in c.a. one minute. We anticipate this work will contribute to the development of new materials with optimized pore sizes for various applications.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗