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DOE OSTI2025

Dynamic nanodomains dictate macroscopic properties in lead halide perovskites

Lead halide perovskites have emerged as promising materials for solar energy conversion and X-ray detection owing to their remarkable optoelectronic properties. However, the microscopic origins of their superior performance remain unclear. Here we show that low-symmetry dynamic nanodomains present in the high-symmetry average cubic phases, whose characteristics are dictated by the A-site cation, govern the macroscopic behaviour. We combine X-ray diffuse scattering, inelastic neutron spectroscopy, hyperspectral photoluminescence microscopy and machine-learning-assisted molecular dynamics simulations to directly correlate local nanoscale dynamics with macroscopic optoelectronic response. Our approach reveals that methylammonium-based perovskites form densely packed, anisotropic dynamic nanodomains with out-of-phase octahedral tilting, whereas formamidinium-based systems develop sparse, isotropic, spherical nanodomains with in-phase tilting, even when crystallography reveals cubic symmetry on average. We demonstrate that these sparsely distributed isotropic nanodomains present in formamidinium-based systems reduce electronic dynamic disorder, resulting in a beneficial optoelectronic response, thereby enhancing the performance of formamidinium-based lead halide perovskite devices. By elucidating the influence of the A-site cation on local dynamic nanodomains, and consequently, on the macroscopic properties, we propose leveraging this relationship to engineer the optoelectronic response of these materials, propelling further advancements in perovskite-based photovoltaics, optoelectronics and X-ray imaging.

Materials Science↗

DOE OSTI2026

Effects of Composition and Oxidation States on the Structures of Chromium-Containing Sodium Silicate Glasses: Molecular Dynamics Simulations using Machine Learning Interatomic Potentials

Chromium represents a significant challenge for the vitrification of high-level nuclear waste into silicate and borosilicate glasses due to its low solubility and variable oxidation states, which can limit the waste loading due to promotion of crystallization or phase separation during processing. In this study, we modeled chromium containing silicate glasses using molecular dynamics simulations with three machine learning interatomic potentials (MLIPs), MACE, CHGNet, and PFP were employed, to gain insights on glass composition and oxidation states on the structures of these glasses. One of the goals is to evaluate their ability of these MLIPs to accurately represent the general structure of silicate glasses and chromium local environments as a function of chromium oxidation states. Density Functional Theory (DFT) based calculations and experimental data such as neutron structure factors were used to validate the structural models. It was found that the foundation models of all three MLIPs are able to reproduce general structural features of the sodium silicate glass structure consistent with experimental and DFT data, but only CHGNet and PFP can accurately capture the oxidation states and local environment of chromium: tetrahedral for Cr6+ and octahedral for Cr3+. Furthermore, we studied the effect of varying Cr3+/ Cr6+ (Cr3+/Crtotal) ratio and total chromium content using PFP. Our results show that Cr6+ enhances network polymerization by reducing non-bridging oxygens through Na? charge compensation required due to the formation of chromate (CrO42-) species, while Cr³? acts as a network modifier that disrupts connectivity. System size effects on the structural characteristics and chromium environments were also tested using the PFP potential. This work highlights the importance of careful validation on the precision, transferability, and potential of MLIPs for modeling glasses containing transition metal elements that can exist in multiple oxidation states. It is also encouraging to see the foundational models are all three MLFFs are able to reproduce the basic sodium silicate glass structures, while suggesting additional training or refining is needed to improve the description of more complex systems containing transition metals.

Puga, Christina L.↗

DOE OSTI2026

Quantum control of Hubbard excitons

Quantum control of the many-body wavefunction is a central challenge in quantum materials research, as it could yield a precise control knob to manipulate emergent phenomena. Floquet engineering, the coherent dressing of quantum states with periodic non-resonant optical fields, has become an important strategy for quantum control. Most applications to solid-state systems have targeted weakly interacting or single-ion states, leaving the manipulation of many-body wavefunctions largely unexplored. Here, in this work, we use Floquet engineering to achieve quantum control of a strongly correlated Hubbard exciton in the one-dimensional Mott insulator Sr 2 CuO 3 . A nonresonant midinfrared optical field coherently dresses the exciton wavefunction, driving its rotation between bright and dark states. We use resonant third-harmonic generation to quantify ultrafast π/2 rotations on the Bloch sphere spanned by these exciton states. Our work advances the quest towards programmable control of correlated states and exciton-based quantum sensing.

36 MATERIALS SCIENCE↗

NASA NTRSDate not supplied

Dynamic Analysis of Reynolds Number Effects on Trailing Edge Transonic Vortex Shedding and Its Impact on Turbine Blade Aerodynamic Performance

In this work, we will discuss observations from images acquired from a time-resolved, high-speed self-aligned focusing Schlieren campaign that was performed at the CW-22 facility at NASA Glenn Research Center to understand the dynamic behavior of thick trailing-edge high-pressure turbine blades simulating a ceramic matrix composite (CMC) construction at high inlet turbulence conditions. For the CMC-9 blade, which has a trailing edge thickness of 9% of the axial chord, we identified a regime where an excessive total pressure loss (loss anomaly) is observed only for a narrow range of Reynolds numbers at a fixed exit Mach number of 0.74. The loss anomaly is qualitatively explained by our images, which were taken at 10 distinct blade Reynolds numbers spanning a factor of 6. The images show a significant increase in energy related to the oscillations due to transonic vortex shedding at the Reynolds numbers related to the high loss conditions. This increased energy leads to the formation of strong acoustic waves that turn into shock waves at the highest loss conditions. From our observations stemming from Spectral POD analysis of the high-speed images, we see the acoustic waves produced by the trailing edge vortex shedding exist in all conditions tested; but the shedding frequency has a very slight trend upwards as the Reynolds number is increased, varying about 6% in the range tested. Considering this variation of shedding frequency as a function of Reynolds number, which is well-established for other bluff-body flows, we stipulate there may be a potential feedback mechanism involving an acoustic information transfer path across neighboring blades that may explain why only a narrow range of Reynolds numbers displays strong, shock-forming vortex shedding. We consider a few feedback paths and examine the timing based on the mean flow field from a high-resolution LES simulation. It appears that all feedback mechanisms are viable, presenting an integer number of delay cycles with respect to disturbances generated at the trailing edge. Most noteworthy, however, is the acoustic/shock-boundary layer interaction mechanism at the blade geometric throat. Based on our analysis, this mechanism likely plays an important role in realistic, curved turbine blade passages.

Aerodynamics↗

DOE OSTI2025

230Th/234U radiochronometry for uranium materials by alpha spectrometry for nuclear forensics analysis

We have developed an alpha spectrometry method for 230Th/234U radiochronometry to determine the model separation age for uranium materials. This method offers an alternative to the more commonly used, but significantly more resource intensive multi-collector inductively coupled plasma mass spectrometry (MC-ICP-MS) while providing similar accuracy and precision. The development included radiochemical separation of uranium and thorium, calibration of the 232U tracer and the alpha spectrometry measurement. The method was validated by analyzing a certified reference material, CRM 125-A, which is a uranium oxide pellet assay, isotopic, and radiochronometric standard. The results were compared to those obtained by our routine MC-ICP-MS 230Th/234U radiochronometry analysis method to assess the performance parameters for alpha spectrometry compared to the state-of-the-art technique.

Macsik, Zsuzsanna [Los Alamos National Laboratory ↗

DOE OSTI2025

Monitoring Depolymerization in Mesopores Using Dynamic Properties of Polymeric Melt Accessed via Dielectric Spectroscopy

Traditional design principles for heterogeneous catalysis guide the use of catalytic particles with mesosized (∼2–50 nm) pores to increase the number of surface-active sites by way of an increased surface area. However, the entry of long-chain polymers into such pores may be significantly limited by the size and entanglement of polymers in the melt state, thereby decreasing the number of accessible sites. Assessment of catalyst performance from traditional reactor-based studies averages over intrapore reaction events as well as reactions on the surface of a particle, resulting in an inability to distinguish between differences in site accessibility and activity. Techniques that assess the intrapore performance can inform the design of future heterogeneous catalysts for polymer upcycling. In this work, we demonstrate the use of broadband dielectric spectroscopy to monitor depolymerization of a polymer melt within mesopores via changes in the segmental relaxation time scale of amorphous polymer chains. In particular, we highlight the use of an anodic aluminum oxide (AAO) membrane as a readily available model for catalyst pores with a well-characterized pore morphology. The decrease in the segmental relaxation (α-relaxation) time of the melt with increasing chain scission emerges as a measure of the extent of polymer deconstruction inside mesopores. To demonstrate the utility of this technique, we demonstrate the decomposition of two commercial poly(propylene carbonate) polymers with different decomposition rates within mesopores. As the polymers depolymerize, their segmental relaxation time decreases as the molecular weight decreases (as predicted by the Fox–Flory equation). The BDS-measured change in segmental relaxation time mirrors the expected trend based on change in molecular weight measured by size exclusion chromatography.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

NASA NTRS1993

A SIMULINK Environment for Flight Dynamics and Control Analysis - Application to the DHC-2 'Beaver', Part 1. Implementation of a Model Library in SIMULINK

The design of advanced Automatic Aircraft Control Systems (AACS's) can be improved upon considerably if the designer can access all models and tools required for control system design and analysis through a graphical user-interface, from within one software environment. This MSc-thesis presents the first step in the development of such an environment, which is currently being done at the Section for Stability and Control of Delft University of Technology, Faculty of Aerospace Engineering. The environment is implemented within the commercially available software package MATLAB/SIMULINK. The report consists of two parts. Part I gives a detailed description of the AACS design environment. The heart of this environment is formed by the SIMULINK implementation of a nonlinear aircraft model in block-diagram format. The model has been worked out for the old laboratory aircraft of the Faculty, the De Havilland DHC-2 'Beaver', but due to its modular structure, it can easily be adapted for other aircraft. Part I also describes MATLAB programs which can be applied for finding steady-state trimmed-flight conditions and for linearization of the aircraft model, and it shows how the built-in simulation routines of SIMULINK have been used for open-loop analysis of the aircraft dynamics. Apart from the implementation of the models and tools, a thorough treatment of the theoretical backgrounds is presented. Part II of this report presents a part of an autopilot design process for the 'Beaver' aircraft, which clearly demonstrates the power and flexibility of the AACS design environment from part I. Evaluations of all longitudinal and lateral control laws by means of nonlinear simulations are treated in detail. The AACS design environment from part I proved to be a very useful tool for designing the control laws of the 'Beaver' autopilot within a very tight time-schedule. The autopilot design process itself will be used as a guideline for future AACS research at the Faculty of Aerospace Engineering. Flight tests of the 'Beaver' autopilot, done after evaluating the control laws in the SIMULINK package, proved to be quite successful. In the future, the AACS design package will evolve into a standardized, integrated design environment which can be applied to virtually any type of aircraft. The AACS design cycle will be shortened further by developing tools for automatically porting control laws from the MATLAB/SIMULINK environment to a piloted real-time flight simulator and the Flight Control Computers of the aircraft.

Aircraft Modelling↗

NASA NTRS1993

Experimental and analytical ion thruster research

The results of further spectroscopic studies on the plume from a 3 cm ion source operated on an argon propellant is reported on. In particular, it is shown that it should be possible to use the spectroscopic technique to measure the plasma density of the ion plume close to the grids, where it is difficult to use electrical probe measurements. How the technique, along with electrical probe measurements in the far downstream region of the plume, can be used to characterize the operation of a three-grid, 15 cm diameter thruster from NASA JPL is outlined. Pumping speed measurements on the Vacuum Research Facility have shown that this facility should be adequate for testing the JPL thruster at pressures in the low 10(exp -5) Torr range. Finally, we describe a simple analytical model which can be used to calculate the grid impingement current which results from charge-exchange collisions in the ion plume.

Wilhelmus M. Ruyten↗

DOE OSTI2024

Magnetically Arrested Circumbinary Accretion Flows

Abstract Binary systems with comparable masses and a surrounding accretion disk can accrete gas through spiral accretion streams penetrating the central cavity formed by tidal interactions. Using three-dimensional Newtonian magnetohydrodynamics simulations, we investigate the possibility of a magnetically arrested accretion flow through the cavity. Rather than solely continuously feeding the binary through spiral accretion streams, the accretion is regulated by the strong magnetic field inside the cavity. Transport of mass and angular momentum onto the binary then proceeds largely periodically in magnetic flux eruption episodes. The ejected flux tubes carry angular momentum outward and away from the binary, inject hot plasma into the disk, and can launch flares. This likely intermittent scenario could have potential implications for the emission signatures of supermassive black hole binaries and shed light onto the role magnetic fields play in the binary’s orbital evolution.

Astronomy & Astrophysics↗

DOE OSTI2026

Imaging a terahertz superfluid plasmon in a two-dimensional superconductor

The superconducting gap defines the fundamental energy scale for the emergence of dissipationless transport and collective phenomena in a superconductor. In layered high-temperature cuprate superconductors, in which the Cooper pairs are confined to weakly coupled two-dimensional (2D) copper–oxygen (CuO 2 ) planes, terahertz (THz) spectroscopy at subgap millielectronvolt (meV) energies has provided crucial insights into the collective superfluid response perpendicular to the superconducting layers. However, within the CuO 2 planes, the collective superfluid response manifests as plasmonic charge oscillations at energies far exceeding the superconducting gap, obscured by strong dissipation. Here, in this study, we present spectroscopic evidence of a below-gap, 2D superfluid plasmon in few-layer Bi 2 Sr 2 CaCu 2 O 8+x and spatially resolve its deeply subdiffractive THz electrodynamics. By placing the superconductor in the near field of a spintronic THz emitter, we reveal this distinct resonance—absent in bulk samples and observed only in the superconducting phase—and determine its plasmonic nature by mapping the geometric anisotropy and dispersion. Crucially, these measurements offer a direct view of the momentum-dependent and frequency-dependent superconducting transition in two dimensions.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

DOE OSTI2025

Ultrafast low-temperature metal–insulator interface phonon dynamics and heat transport in a Pt/Gd 3 Fe 5 O 12 heterostructure

Interfacial thermal and acoustic phenomena have an important role in quantum science and technology, including in spintronic and spincaloritronic materials and devices. Simultaneous measurements of the low-temperature thermal and acoustic properties of a metal/insulator heterostructure reveal distinct dynamics in the characteristic phonon frequency ranges of acoustic and thermal transport. The measurements probed a heterostructure consisting of a thin film of Pt on the ferrimagnetic insulator gadolinium iron garnet (Gd 3 Fe 5 O 12 , GdIG) grown epitaxially on a gadolinium gallium garnet substrate. Ultrafast structural dynamics within the Pt layer were tracked using time-resolved ultrafast x-ray diffraction and analyzed to probe interfacial acoustic and thermal properties. The rapid heating of the Pt layer by a 400 nm wavelength femtosecond-duration optical pulse produced transient structural changes that provided the stimulus for these measurements. Rapid heating produced a broadband acoustic pulse that was partially reflected by the Pt/GdIG interface. Temporal frequencies up to 740 GHz, corresponding to angular frequencies of several THz, were detected in a wavelet analysis of the acoustic oscillations of the strain in the Pt layer. The structural results were analyzed to determine (i) the acoustic damping coefficient and phonon mean free path in Pt at frequencies of hundreds of GHz and (ii) the Grüneisen anharmonicity parameter. The thermal conductance of the Pt/GdIG interface was tracked using the slower, tens-of-picosecond-scale, dynamics of the initial cooling of the heated Pt layer. Analysis using a model based on the Boltzmann transport equation shows that the phonon transmission is lower at the phonon frequencies relevant to thermal transport than for subterahertz regime acoustics.

Acoustic phenomena↗

DOE OSTI2026

Few is different: deciphering many-body dynamics in mesoscopic quantum gases

Emergent macroscopic descriptions of matter, such as hydrodynamics, are central to our description of complex physical systems across a wide spectrum of energy scales. The conventional understanding of these many-body phenomena has recently been shaken by a number of experimental findings. Collective behavior of matter has been observed in mesoscopic systems, such as high-energy hadron–hadron collisions, or ultracold gases with only a few strongly interacting fermions. In such systems, the separation of scales between macroscopic and microscopic dynamics (at the heart of any effective theory) is inapplicable. To address the conceptual challenges that arise from these observations and explore the universality of emergent descriptions of matter, the EMMI Rapid Reaction Task Force was assembled. This document summarizes the RRTF discussions on recent theoretical and experimental advances in this rapidly developing field. Leveraging technological breakthroughs in the control of quantum systems, we can now quantitatively explore what it means for a system to exhibit behavior beyond the sum of its individual parts. In particular, the report highlights how the (in)applicability of hydrodynamics and other effective theories can be probed across three principal frontiers: the size frontier, the equilibrium frontier, and the interaction frontier.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

DOE OSTI2026

Direct Observation of Elusive (DTBM‐SEGPHOS)CuH Monomer Enables Mechanistic Insights Into Hydrocupration, Aggregation, and Dynamics of Alkene Functionalization Catalysis

The bulky diphosphine DTBM-SEGPHOS is widely employed in CuH-catalyzed transformations as it provides remarkably active catalyst systems. The transient (DTBM-SEGPHOS)CuH monomer (LCuH) is the often-invoked active species. However, its instability has prevented spectroscopic characterization and mechanistic elucidation, hindering mechanistic understanding. We report low-temperature NMR spectroscopic characterization of LCuH, enabling quantitative kinetic analysis of the stoichiometric hydrocupration and catalytic hydroboration of cyclopentene, as well as the structural identification of two CuH clusters. LCuH inserts cyclopentene at −43°C, reaffirming its high reactivity toward olefins. LCuH deactivates to form L 2 Cu 3 H 3 and L 2 Cu 4 H 4 clusters, in which LCuH dimerization initiates aggregation. Kinetic analysis of reactions of unactivated alkenes indicates that competing on-cycle alkene hydrocupration and LCuH dimerization impact performance, as catalyst deactivation and turnover occur on comparable timescales. Structure–activity analysis using atomistic simulations shows that the steric profile of DTBM-SEGPHOS increases the CuH dimerization barrier by ∼7.7 kcal mol−1 compared to that of SEGPHOS, rationalizing the unique ability of DTBM-SEGPHOS to stabilize a reactive monomer for hydrocupration of broader alkene substrates. These findings illustrate the fundamental design principle that steric control of aggregation governs CuH catalyst performance, explaining both the exceptional activity of (DTBM-SEGPHOS)CuH and the limitations imposed by competing deactivation.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2026

Stoichiometry dependent properties of cerium hydride: An active learning developed interatomic potential study

Cerium hydride has a variety of interesting properties, including a known lattice contraction and densification with increasing hydrogen content. However, precise stoichiometric control is not experimentally straightforward and ab initio approaches are not computationally feasible for many properties such as melting and low temperature diffusion. Therefore, we develop a machine-learned interatomic potential for cerium hydride that is valid for H to Ce ratios from 2.0 to 3.0. A query-by-committee active learning approach is used to develop the training set. Leveraging classical molecular dynamics simulations, we assess a range of properties and provide fundamental mechanisms for the trends with stoichiometry. Finally, a majority of the properties follow the trend of lattice contraction, being governed by the stronger lattice binding induced by adding octahedral atoms.

36 MATERIALS SCIENCE↗

NASA NTRS2024

Expansion of Check-Cases for 6DOF Simulation

This is the Appendix containing a description of the solution for Case 1 in the assessment, “Expansion of Check-Cases for 6DOF Simulation”. For cases of spherical gravity, it is possible to provide a two-body solution without recourse to numerical integration and thus it is accurate to machine precision. Python code for a Keplerian Propagator (propagate.py) which produced a reference trajectory for Case 1 is provided in this appendix. There is also code for generating test cases which was used as an independent verification of the propagator. This is a high-level description of the algorithm employed. The documentation of each function includes implementation details, including equations for each task.

Modeling↗

DOE OSTI2026

Nonequilibrium dynamics of two-level systems directly after cryogenic alternating bias

Two-level systems (TLSs) are a dominant decoherence mechanism in superconducting qubits, microwave kinetic inductance detectors, and quantum dots. TLSs are tunneling states commonly found in amorphous materials and interfaces, which interact electromechanically, leading to energy loss. Fluctuations in the frequency of the TLSs are a significant problem for qubit operation and force recalibration every few hours. In this study, we probe the effect of alternating bias at cryogenic temperatures on TLSs in a purpose-built LC oscillator. When an in situ alternating bias is applied, the steady-state spectra of the TLSs disappear. Spectroscopy reveals transient behavior, in which the TLS frequency fluctuates on the order of minutes. Thermal cycling above 10 K reverses these effects, restoring the TLS spectrum to its original state. Importantly, the intrinsic loss tangent of the LC oscillator remains unchanged before and after the application of the alternating bias. We propose that the disappearance of the steady-state spectrum is caused by nonequilibrium energy buildup from strain in the oxide film introduced by the pulsed voltage-bias sequence. Understanding this nonequilibrium energy could shed light on TLS fluctuations and reduce the calibration requirements for qubits.

general physics↗

DOE OSTI2026

Visualizing Crystallization Dynamics and Transformation Pathways of Disordered Rocksalt Oxides During Thermally Activated Sol–Gel Synthesis

Sol–gel synthesis is a wet-chemical processing route for fabricating functional materials with control over composition and microstructure at relatively low temperatures compared to conventional solid-state synthesis. While sol–gel process initiates with intermixed molecular precursors, the early-stage nucleation pathways are insufficiently understood. Here, in this study, the chemical and structural transformation of ion disordered rocksalt (DRX) Li 1.2 Mn 0.4 Ti 0.4 O 2 (LMTO), a promising cathode material for lithium batteries, is studied by multiscale characterizations. In situ heating transmission electron microscopy (TEM) using a liquid cell visualizes and identifies crystallization pathways at the nanoscale. While some regions follow a classical multi-step transition through thermodynamically stable intermediates, others exhibit a kinetic shortcut via a localized amorphous matrix to directly form the DRX structure. Macroscale Fourier transform infrared spectroscopy corroborates the findings and reveals that transition metal ions are more strongly incorporated into the acetate-coordinated network than lithium. Although in situ heating TEM captures diverse local transformation pathways, in situ synchrotron X-ray diffraction indicates that the macroscopic transformation proceeds predominantly through spinel LMTO and lithium titanates toward DRX-LMTO. The findings uncover the spatiotemporal chemical and structural transformations in sol–gel derived DRX-LMTO materials, and call for fine-tuning of such sol–gel chemistries to manipulate the crystallization pathways and achieve target material homogeneity more efficiently.

cathode material↗

DOE OSTI2026

Probing and Tuning Spatiotemporal pH Evolution in Aqueous Zinc Ion Batteries

Aqueous zinc-ion batteries (AZIBs) offer a combination of safety and low cost, but they suffer from dynamic pH fluctuations that drive parasitic reactions and capacity fading. In this review, we report the current mechanistic understanding of the dynamic pH evolution across the electrolyte-electrode interface and its role in triggering interphase instability. We summarize advanced strategies to regulate pH, including electrolyte engineering, electrode surface modification, and interphase construction. We further discuss current methods for probing pH dynamics and outline potential future approaches for gaining deeper mechanistic and design insights.

Zheng, Xueli [SLAC]↗