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At least 451 records · Page 25

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DOE OSTI2025

Correlated Lattice Fluctuations in CsPbBr 3 Quantum Dots Give Rise to Long-Lived Electronic Coherence

Electronic coherence is central to numerous areas of science, from quantum biology to quantum materials. In quantum materials, lead-halide perovskite (LHP) quantum dots (QDs) have been shown to support electronic coherence through observation of coherent single-photon emission and superfluorescence arising from spatial coherence at low temperatures. In contrast, direct measurement of temporal coherence between exciton states has been lacking. Here, we employ coherent multi-dimensional spectroscopy to observe an electronic coherence between exciton states in CsPbBr 3 QDs that is long-lived at room temperature, surviving nearly three times longer than the electronic dephasing time. This observation of a long-lived electronic coherence at room temperature points to nearly perfectly correlated lattice fluctuations for each excitonic state in the superposition. In conclusion, these experiments reveal that the properties of LHP QDs extend to lattice dynamics that give rise to correlated fluctuations in the basis exciton states, a process that may next be optimized by design.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

DOE OSTI2022

Anomalous phase separation in a correlated electron system: Machine-learning–enabled large-scale kinetic Monte Carlo simulations

Significance Phase separation is crucial to the functionalities of many correlated electron materials with notable examples including colossal magnetoresistance in manganites and high- T c superconductivity in cuprates. However, the nonequilibrium phase-separation dynamics in such systems are poorly understood theoretically, partly because the required multiscale modeling is computationally very demanding. With the aid of machine-learning methods, we have achieved large-scale dynamical simulations in a representative correlated electron system. We observe an unusual relaxation process that is beyond the framework of classical phase-ordering theories. We also uncover a correlation-induced freezing behavior, which could be a generic feature of phase separation in correlated electron systems.

Zhang, Sheng↗

DOE OSTI2026

Molecular origin of negative lithium transference in electrolytes with star-shaped multivalent anions

Large-scale molecular dynamics simulations illustrate that highly correlated cation–anion motion leads to negative t 0+ on the order of 1 in lithium electrolytes with star-shaped multivalent anions. Large multivalent anions have gained increasing attention for their potential to improve lithium transference in electrolytes. We employ large-scale molecular dynamics simulations based on the Onsager transport framework to investigate ion transport in a lithium electrolyte with star-shaped multivalent anions. The simulations show that t 0+, the cation transference number with respect to solvent velocity, is negative over a wide range of concentration. This is consistent with experimental data reported previously. The simulation-based Onsager transport coefficients reveal that the magnitudes of the cation–cation, anion–anion, and cation–anion correlations are comparable, a signature of highly correlated motion in the electrolyte. Examination of the cation solvation environment indicates the presence of strong cation–anion association across the entire concentration range, which leads to negative t 0+ on the order of −1. Both simulation and experiment also show that the maximum value of t 0+ reaches 0 when the cation concentration is c + = 0.4 M. This is the concentration at which the anions begin to spatially overlap, and lithium ions serve as dynamic linkers to balance cation–cation and cation–anion correlations. Our results provide molecular-level insights into the origin of transference in multivalent electrolytes.

Fang, Chao↗

DOE OSTI2024

Unveiling the Structural Origins of Dynamic Diversity in Pd-Based Metallic Glasses

The β -relaxation is one of the major dynamic behaviors in metallic glasses (MGs) and exhibits diverse features. Despite decades of efforts, the understanding of its structural origin and contribution to the overall dynamics of MG systems is still unclear. Here two palladium-based Pd—Cu—P and Pd—Ni—P MGs are reported with distinct different β -relaxation behaviors and reveal the structural origins for the difference using the advanced X-ray photon correlation spectroscopy and absorption fine structure techniques together with the first-principles calculations. The pronounced β -relaxation and fast atomic dynamics in the Pd—Cu—P MG mainly come from the strong mobility of Cu atoms and their locally favored structures. In contrast, the motion of Ni atoms is constrained by P atoms in the Pd—Ni—P MG, leading to the weakened β -relaxation peak and sluggish dynamics. Finally, the correlation of atomic dynamics with microscopic structures provides a way to understand the structural origins of different dynamic behaviors as well as the nature of aging in disordered materials.

36 MATERIALS SCIENCE↗

DOE OSTI2026

A scalable variational method for estimating the latent infection-rate field of an outbreak

In this paper, we explore whether the infection-rate of a disease can serve as a robust monitoring variable in epidemiological surveillance algorithms. The infection-rate is dependent on population mixing patterns that do not vary erratically day-to-day; in contrast, daily case-counts used in contemporary surveillance algorithms are corrupted by reporting errors. The technical challenge lies in estimating the latent infection-rate from case-counts. Here we devise a Bayesian method to estimate the infection-rate across multiple adjoining areal units, and then use it, via an anomaly detector, to discern a change in epidemiological dynamics. We extend an existing model for estimating the infection-rate in an areal unit by incorporating a Markov random field model, so that we may estimate infection-rates across multiple areal units, while preserving spatial correlations observed in the epidemiological dynamics. To carry out the high-dimensional Bayesian inverse problem, we develop an implementation of mean-field variational inference specific to the infection model and integrate it with the random field model to incorporate correlations across counties. The method is tested on estimating the COVID-19 infection-rates across all 33 counties in New Mexico using data from the summer of 2020, and then employing them to detect the arrival of the Fall 2020 COVID-19 wave. We perform the detection using a temporal algorithm that is applied county-by-county. We also show how the infection-rate field can be used to cluster counties with similar epidemiological dynamics.

60 APPLIED LIFE SCIENCES↗

DOE OSTI2021

Modeling Microstructural Effects on Heterogeneous Temperature Fields within Polycrystalline Explosives

The paper addresses the role of crystal anisotropy on the evolution of heterogeneous temperature fields in plastic-bonded explosives (PBXs) under conditions of weak shock. The modeling approach is based on simplified idealizations of PBX microstructure including RDX grains and estane binder regions subjected to velocity boundary conditions representative of impact conditions in situ. The constitutive description of the microstructure constituents includes a dislocation-based, anisotropic, single crystal plasticity model for the explosive grains and a linear viscoelastic model to represent the estane binder. Large suites of simulations were used to systematically study the correlation in heating of the grains with local wave dynamics, crystal orientation, and the microstructural neighborhood. These correlations were identified through the selection of characteristics of crystal anisotropy including oriented wave speeds and Taylor factor. A key observation is that the wave dispersion within a certain distance from the impact interface plays a dominant role in the temperature field. Beyond this distance, individual crystal orientations play a more dominant role, but cannot entirely account for the observed heterogeneity without consideration of the local microstructure neighborhood.

42 ENGINEERING↗

DOE OSTI2021

Dynamics of Polymerization and Gelation in Epoxy Nanocomposites via X-ray Photon Correlation Spectroscopy

The details of the curing process of epoxy resins are notoriously difficult to ascertain, hampering polymer matrix composite manufacturing. Here, the curing of a series of six epoxy resins containing dilute spherical nanoparticles was investigated via X-ray photon correlation spectroscopy (XPCS). The resin formulation was varied to achieve a range of crosslink densities and topologies. Prior to gelation, the viscosities obtained from XPCS agreed with bulk rheology. A clear dynamic transition was detected in all samples, where the q-scaling changes from approximately q2 .2 to q 1 , indicating a transition from sub-diffusive to ballistic-like nanoparticle motion. For the samples with a high crosslink density, this change was abrupt and coincided with gelation, and there was no evidence of crosslink heterogeneity. Chain entanglement played a role in the transition for samples with lower crosslink density. Finally, this work reveals the potential of XPCS to deliver new quantitative insights into the curing process of thermosetting resins.

36 MATERIALS SCIENCE↗

DOE OSTI2025

Stretched exponential magnetic relaxation dynamics in artificial square ice revealed through x-ray photon correlation spectroscopy

X-ray photon correlation scattering measurements are undertaken on a thermally active artificial spin ice based on the square lattice, referred to as artificial square ice, to probe the fluctuation timescales as a function of temperature as the system passes through the paramagnetic-antiferromagnetic phase transition, which belongs to the two-dimensional Ising universality class. In the paramagnetic regime, a single exponential timescale is seen, whereas at and below the critical temperature, a stretched exponential decorrelation is observed, with the stretching exponent decreasing from unity down to below one-half as the temperature reduces. This trend is confirmed by kinetic Monte Carlo simulations of a simplified point-dipolar square ice system, and is in agreement with past theoretical work on the kinetic Ising model where stretched exponential relaxation due to equilibrium domain wall dynamics below the critical temperature was found.

36 MATERIALS SCIENCE↗

DOE OSTI2024

Solution-phase sample-averaged single-particle spectroscopy of quantum emitters with femtosecond resolution

Here, the development of many optical quantum technologies depends on the availability of solid-state single quantum emitters with near-perfect optical coherence. However, a standing issue that limits systematic improvement is the significant sample heterogeneity and lack of mechanistic understanding of microscopic energy flow at the single emitter level and ultrafast timescales. Here we develop solution-phase single-particle pump-probe spectroscopy with photon correlation detection that captures sample-averaged dynamics in single molecules and/or defect states with unprecedented clarity at femtosecond resolution. We apply this technique to single quantum emitters in two-dimensional hexagonal boron nitride, which suffers from significant heterogeneity and low quantum efficiency. From millisecond to nanosecond timescales, the translation diffusion, metastable-state-related bunching shoulders, rotational dynamics, and antibunching features are disentangled by their distinct photon-correlation timescales, which collectively quantify the normalized two-photon emission quantum yield. Leveraging its femtosecond resolution, spectral selectivity and ultralow noise (two orders of magnitude improvement over solid-state methods), we visualize electron-phonon coupling in the time domain at the single defect level, and discover the acceleration of polaronic formation driven by multi-electron excitation. Corroborated with results from a theoretical polaron model, we show how this translates to sample-averaged photon fidelity characterization of cascaded emission efficiency and optical decoherence time. Our work provides a framework for ultrafast spectroscopy in single emitters, molecules, or defects prone to photoluminescence intermittency and heterogeneity, opening new avenues of extreme-scale characterization and synthetic improvements for quantum information applications.

36 MATERIALS SCIENCE↗

DOE OSTI2025

Can increasing the size and flexibility of a molecule reduce decoherence and prolong charge migration?

Coherent superposition of electronic states, created by ionizing a molecule, can initiate ultrafast dynamics of the electron density. Correlation between nuclear and electron motions, however, typically dissipates the electronic coherence in only a few femtoseconds, especially in larger and more flexible molecules. We, therefore, use ab initio semiclassical dynamics to study decoherence in a sequence of analogous organic molecules of increasing size and find, surprisingly, that extending the carbon skeleton in propynal analogs slows down decoherence and prolongs charge migration. To elucidate this observation, we decompose the overall decoherence into contributions from individual vibrational modes and show that: 1) The initial decay of electronic coherence is caused by high- and intermediate-frequency vibrations via momentum separation of nuclear wavepackets evolving on different electronic surfaces. 2) At later times, the coherence disappears completely due to the increasing position separation in the low-frequency modes. 3) In agreement with another study, we observe that only normal modes that preserve the symmetry of the molecule induce decoherence. All together, we justify the enhanced charge migration by a combination of increased hole-mixing and the disappearance of decoherence contributions from specific vibrational modes—CO stretching in butynal and various H rockings in pentynal.

Science & Technology - Other Topics↗

DOE OSTI2025

Defect-Driven Redox Interplay on Anatase TiO 2 : Surface-Structure Dependent Activation for CO 2 Hydrogenation Catalysis

Titanium dioxide (TiO 2 ) is one of the most extensively studied oxides as an active catalyst or catalyst support, particularly in energy and environmental applications, but the atomistic mechanisms governing its dynamic response to reactive environments and their correlation to reactivity remain largely elusive. Using in situ environmental transmission electron microscopy (ETEM), synchrotron X-ray diffraction (XRD), ambient-pressure X-ray photoelectron spectroscopy (AP-XPS), temperature-programmed reduction (TPR), reactivity measurements, and theoretical modeling, we reveal the dynamic interplay between oxygen loss and replenishment of anatase TiO 2 under varying reactive conditions. Under H 2 exposure, anatase TiO 2 undergoes surface reduction via lattice oxygen loss, forming Ti 3 O 5 . In contrast, CO 2 exposure induces oxygen replenishment, reversing stoichiometry. In mixed H2/CO 2 environments, the reverse water–gas shift (RWGS) reaction proceeds selectively on stepped and high-indexed TiO 2 surfaces, whereas the thermodynamically stable TiO 2 (101) surface remains inactive and intact. Critically, H 2 pretreatment generates oxygen vacancies on TiO 2 (101), transforming it into an active Ti 3 O 5 or defect-rich surface that catalyzes RWGS. By correlating surface structure, defect dynamics, and gas-phase interactions, this work deciphers the competition between H 2 -driven reduction and CO 2 -driven oxidation pathways at the atomic scale. Furthermore, these insights establish defect engineering as a strategic lever to activate inert TiO 2 facets, advancing the design of adaptive catalysts for sustainable fuel synthesis technologies.

36 MATERIALS SCIENCE↗

DOE OSTI2025

Year six photometric measurements of known Trans-Neptunian Objects and Centaurs by the Dark Energy Survey

ABSTRACT We identified known Trans-Neptunian Objects (TNOs) and Centaurs in the complete Dark Energy Survey (DES) year six catalogue (DES Y6) through the Sky Body Tracker (SkyBoT) tool. We classified our data set of 144 objects into a widely used 4-class taxonomic system of TNOs. No such previous classification was available in the literature for most of these objects. From absolute magnitudes and average albedos, an estimation of the diameters of all these objects is obtained. Correlations involving colours, orbital parameters, dynamical classes, and sizes are also discussed. In particular, our largest reddest object has a diameter of $390^{+68}_{-53}$ km and our largest cold classical, $255^{+19}_{-17}$ km. Also, a weak correlation between colour and inclination is found within the population of resonant TNOs in addition to weak correlations between colour and phase slope in different bands.

79 ASTRONOMY AND ASTROPHYSICS↗

DOE OSTI2025

Segmental Dynamics and Vitrification in Associating Copolymer Melts: Role of Cluster Formation, Microdomains, and Cross-Linking

A microscopic statistical mechanical theory of the structure, self-assembly, and activated segmental relaxation is employed to study associating copolymer melts with high attractive sticker fractions, local clustering, and disordered microphase ordering. The stickers are dynamically pinned in a manner that does not affect equilibrium structure which mimics the much slower physical bond breaking process or postassembly cross-linking of sticky monomers. Local sticker clustering and microdomain spatial correlations significantly modify the activated relaxation of nonstickers and glass transition temperature, T g . A re-entrant glass-melting feature is predicted as sticker attraction strength is initially increased corresponding to a speed up of segmental relaxation, and hence reduction of T g relative to the cross-linked homopolymer network. A mechanistic analysis reveals three competing effects: a purely kinetic slowing down of nonstickers down due to cross-linking, disordering of the nonsticker local cage and weakening of effective forces they experience due to sticker physical clustering, and a longer range impact of microdomain scale correlations that results in nonmonotonic dynamical effects. At high enough attraction strength, a qualitative change emerges corresponding to a sticker fraction dependent elevation of T g , which eventually surpasses that of the cross-linked homopolymer network. Dynamically, the new physics arises from a complex evolution of the amplitude of the collective elastic field that dresses the large amplitude mobile segment hopping within a coupled local-nonlocal description of the alpha relaxation. Furthermore, the results are qualitatively consistent with recent experiments on associating PDMS and PPG telechelics of fixed sticker fraction but with chemically different end groups of variable attraction strengths. Finally, possible tests using simulation and the influence of material or model specific interaction potentials and other real world complications are discussed.

Copolymers↗

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 OSTI2020

Dynamics of Hydroxyl Anions Promotes Lithium Ion Conduction in Antiperovskite Li 2 OHCl

Li 2 OHCl is an exemplar of the antiperovskite family of ionic conductors, for which high ionic conductivities have been reported, but in which the atomic-level mechanism of ion migration is unclear. The stable phase is both crystallographically defective and disordered, having similar to 1/3 of the Li sites vacant, while the presence of the OH(- )anion introduces the possibility of rotational disorder that may be coupled to cation migration. In this work, complementary experimental and computational methods are applied to understand the relationship between the crystal chemistry and ionic conductivity in Li 2 OHCl , which undergoes an orthorhombic to cubic phase transition near 311 K (approximate to 38 degrees C) and coincides with the more than a factor of 10 change in ionic conductivity (from 1.2 x 10 -5 mS/cm at 37 degrees C to 1.4 x 10 -3 mS/cm at 39 degrees C). X ray and neutron experiments conducted over the temperature range 20-200 degrees C, including diffraction, quasi-elastic neutron scattering (QENS), the maximum entropy method (MEM) analysis, and ab initio molecular dynamics (AIMD) simulations, together show conclusively that the high lithium ion conductivity of cubic Li2OHCl is correlated to "paddlewheel" rotation of the dynamic OH - anion. The present results suggest that in antiperovskites and derivative structures a high cation vacancy concentration combined with the presence of disordered molecular anions can lead to high cation mobility.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2024

Virtual tower measurements during the American WAKE ExperimeNt (AWAKEN)

Dual-Doppler lidar measurements were made during the American WAKE ExperimeNt to provide height-resolved measurements of wind speed and direction at multiple locations immediately south of the leading row turbines in the King Plains wind farm in Oklahoma. These so-called virtual tower measurements were performed to characterize the inflow into the wind farm and to assess possible upwind blockage effects due to the collective action of the wind farm. The campaign was conducted from 12 November 2022 to 17 October 2023, during which time 14 unique virtual tower locations were sampled with heights ranging from 240 to 490 m AGL. The wind retrieval algorithm provided estimates of the horizontal winds and their uncertainties with a vertical resolution of about 10 m, while also accounting for the tilt of the lidar platform. The virtual tower results are compared to collocated lidar wind profiling data at the A1 site, which was located roughly 2.4 rotor diameters south of the nearest turbine. The wind speed difference between the wind profiler and the virtual tower was found to be quite sensitive to atmospheric stability and wind direction below 250 m AGL. The largest differences were observed for inflow under stable conditions, where the profiler wind speeds were observed to be about 22% lower than the virtual tower near hub height. These results suggest that there are persistent horizontal gradients in the flow upwind of the wind farm which result in biased estimates using standard ground-based lidar wind profiling methods.

17 WIND ENERGY↗

DOE OSTI2021

Improved natural convection heat transfer correlations for reactor cavity cooling systems of high-temperature gas-cooled reactors: From computational fluid dynamics to Pronghorn

The Reactor Cavity Cooling System (RCCS) is a common reactor safety system in High Temperature Gas Cooled Reactors (HTGR) that removes heat from the Reactor Pressure Vessel (RPV) by radiation ($\sim 80\%$) and natural convection ($\sim 20\%$). For simulation of accident scenarios of HTGRs, intermediate fidelity and system codes models must be employed for limiting the models' execution time. While accurate quantification of the radiative heat transfer is available in these models, quantification of natural convection must rely on correlations of questionable accuracy for the Nusselt number. Commonly used correlations are based in experiments performed at low Rayleigh numbers and/or using isothermal walls in simplified geometries. Here, this work improves on the accuracy of natural convection heat transfer correlations in support for HTGR designs. These correlations include both local and average Nusselt numbers as a function of the global Rayleigh number, the local Rayleigh number, and the temperature profile at the hot wall of the RCCS. In the absence of dedicated experiments and the difficulty of performing high-fidelity simulations at realistic Rayleigh numbers, the data to fit the correlations are generated with Computational Fluid Dynamics (CFD) using Reynolds Averaged Navier-Stokes (RANS) models. First, a careful selection of the RANS turbulence model is performed by comparing the results obtained with different RANS turbulence models against high fidelity simulations of natural convection at $Ra \ 1 \times 10^{11}$ in a rectangular cavity. Next, the selected model is used to perform simulations of an HTGR cavity at different high Rayleigh numbers $\in [6.1 \times 10^{11},2.9 \times 10^{13}]$ to encompass several HTGR designs, assuming an isothermal RPV wall. The results obtained are used to fit a correlation for the average and space-varying Nusselt number as a function of the global and local Rayleigh numbers via a sparsity-promoting least-squares method. The selected RANS model is then used to perform simulations of a PBMR 400 HTGR cavity with the temperature profiles at the RPV wall obtained during a PLOFC transient. We use the results obtained to fit a temperature-dependent correction to the space-varying Nusselt number with the sparsity-promoting least-squares method. The results obtained in this work, enable system-level codes, such as Pronghorn, to perform higher-fidelity simulations of the heat exchange process in the RCCS while still maintaining a low computational cost.

42 ENGINEERING↗

DOE OSTI2021

High-speed synchrotron X-ray phase-contrast imaging for evaluating microscale damage mechanisms and tracking cracking behaviors inside cross-ply GFRCs

In this study, we integrated the high-speed synchrotron X-ray phase-contrast imaging (PCI) with a modified Kolsky compression bar loading platform to visualize the dynamic failure processes of cross-ply glass fiber reinforced composites (GFRCs). Four S-2 glass/SC-15 composite specimens were prepared, having similar thicknesses but different stacking sequences, namely as [0 12 /90 12 ], [90 12 /0 12 ], [0 8 /90 8 /0 8 ], and [90 8 /0 8 /90 8 ]. Three-dimensional synchrotron X-ray computed tomography and scanning electron microscopy (SEM) were employed to examine the microstructures and quantify the fiber volume fractions. Each specimen was notched and subjected to a dynamic three-point flexural loading. The onset of cracking close to the notch tip, crack propagation in 0° or 90° plies and their interface, crack opening, and ultimately failure of the specimen were captured by high-speed synchrotron X-ray PCI. Additional dynamic experiments were performed to determine the average time when the stress wave propagated through the specimen and correlate the X-ray images with the specimen's force-deflection response. Finally, the surface morphology of each specimen after the dynamic loading was imaged by SEM. Comparison between real-time X-ray images and post-fracture SEM images demonstrated the capability of the X-ray method to record damage evolution inside composites. Furthermore, the high spatial and temporal resolutions of the X-ray setup and edge enhancement by PCI enabled the identification of microscale damage features within 1 μs. Two damaging processes were identified, crack growth was quantified, and fracture toughness of the composites was evaluated. The method is deemed useful to reveal microscale damage mechanisms and track cracking behaviors inside cross-ply GFRCs under dynamic loading in real time.

42 ENGINEERING↗