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DOE OSTI2025

Dynamic Behavior of Bound Interlayer Excitons in Interlayer-Doped Cs 3 Bi 2 Br 9 Vacancy-Ordered Perovskite

Interlayer doping of the vacancy-ordered 2D perovskite Cs 3 Bi 2 Br 9 (CBB) enables the formation of bound interlayer excitons (BIEs), a unique charge-transfer excited state within the layered solid. BIEs previously reported with silver (Ag + ) as an interlayer dopant exhibited bright broadband photoluminescence (PL) with prolonged lifetime at room temperature, offering potential applications in efficient white light emission, photocatalysis, and optoelectronics. However, the dynamic behavior of radiation and excited carriers remains poorly understood due to the limitations of ensemble spectroscopic measurements. Here, we investigate the temperature-dependent dynamics of Ag-doped Cs 3 Bi 2 Br 9 (Ag-CBB) using single-particle time-resolved PL spectroscopy and ultrafast transient absorption imaging. Single-particle PL measurements reveal three distinct emission regimes across temperature: (i) BIE-dominant emission at high temperatures, (ii) a mixture of radiation from BIEs and self-trapped excitons (STEs) at intermediate temperatures, and (iii) STE-dominant emission below 100 K. Rapid transient absorption mapping using Parallel Rapid Imaging with Spectroscopic Mapping (PRISM) reveals subpicosecond STE formation in pristine CBB and long-lived photoinduced absorption by BIEs, consistent with electron–hole separation and suppressed STE transfer. The spatial uniformity of these signals confirms homogeneous Ag doping across single crystals. These findings highlight the role of Ag interlayer dopants in governing the BIE dynamics.

bound interlayer exciton↗

DOE OSTI2023

The dynamics, mixing, and thermonuclear burn of compressed foams with varied gas fills

Inertial confinement fusion (ICF) implosions involve highly coupled physics and complex hydrodynamics that are challenging to model computationally. Due to the sensitivity of such implosions to small features, detailed simulations require accurate accounting of the geometry and dimensionality of the initial conditions, including capsule defects and engineering features such as fill tubes used to insert gas into the capsule, yet this is computationally prohibitive. It is therefore difficult to evaluate whether discrepancies between the simulation and experiment arise from inadequate fidelity to the capsule geometry and drive conditions, uncertainties in physical data used by simulations, or inadequate physics. We present results from detailed high-resolution three-dimensional simulations of ICF implosions performed as part of the MARBLE campaign on the National Ignition Facility [Albright et al., Phys. Plasmas 29, 022702 (2022)]. These experiments are foam-filled separated-reactant experiments, where deuterons reside in the foam and tritons reside in the capsule gas fill and deuterium–tritium (DT) fusion reactions only occur in the presence of mixing between these materials. Material mixing in these experiments is primarily seeded by shock interaction with the complex geometry of the foam and gas fill, which induces the Richtmyer–Meshkov instability. We compare results for experiments with two different gas fills (ArT and HT), which lead to significant differences in the hydrodynamic and thermodynamic developments of the materials in the implosion. Our simulation results show generally good agreement with experiments and demonstrate a substantial impact of hydrodynamic flows on measured ion temperatures. The results suggest that viscosity, which was not included in our simulations, is the most important unmodeled physics and qualitatively explains the few discrepancies between the simulation and experiment. The results also suggest that the hydrodynamic treatment of shocks is inadequate to predict the heating and yield produced during shock flash, when the shock converges at the center of the implosion. Alternatively, underestimation of the level of radiative preheat from the shock front could explain many of the differences between the experiment and simulation. Nevertheless, simulations are able to reproduce many experimental observables within the level of experimental reproducibility, including most yields, time-resolved X-ray self-emission images, and an increase in burn-weighted ion temperature and neutron down-scattered ratio in the line of sight that includes a jet seeded by the glue spot that joins capsule hemispheres.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

DOE OSTI2023

Real-time observation of multi-electron processes in atoms and diatomic molecules

We report on the implementation of a reliable experimental approach to observe, in real-time, electron dynamics in atoms and molecules at the attosecond time scale. The experimental approach combines a source of shape-controlled attosecond pulses, a stabilized XUV/IR interferometer for time-resolved measurements, and a multi-particle imaging system (Coltrims). In addition, we report new capabilities to control electron dynamics in quantum systems.

74 ATOMIC AND MOLECULAR PHYSICS↗

DOE OSTI2020

Experimental investigation of internal two-phase flow structures and dynamics of quasi-stable sheet cavitation by fast synchrotron x-ray imaging

The quasi-stable sheet cavitation produced in a small Venturi channel is investigated using a fast synchrotron X-ray imaging technique aided with conventional high speed photography. The use of X-rays instead of visible light solves cavitation opacity related issues, and X-ray phase contrast-based edge enhancement enables high-definition visualization of the internal two-phase morphology. The simultaneous acquisition of time-resolved velocity and void fraction fields through post-processing the recorded X-ray images reveals, for the first time, the complex diphasic flow structures inside the sheet cavity, which is essentially divided into 6 characteristic parts. Distinct from the current mainstream view, the globallysteady sheet cavitation is found to be characterized by a weak but constantly-existing re-entrant flow that can penetrate the entire cavity. The turbulent velocity fluctuations inside the sheet cavity are also investigated. The turbulence level in the reverse flow region is observed to be as low as in the outer main flow demonstrating the relatively steady status of the reentrant flow. Unlike the streamwise and cross-stream fluctuations, the shear stress appears to be weakly correlated with the velocity gradient. The collapse of vapor phase and the vaporization at the upstream cavity interface are found to be the primary causes of shear stress intensification.

42 ENGINEERING↗

DOE OSTI2022

Ghost-imaging-enhanced noninvasive spectral characterization of stochastic x-ray free-electron-laser pulses

Abstract High-intensity ultrashort X-ray free-electron laser (XFEL) pulses are revolutionizing the study of fundamental nonlinear x-ray matter interactions and coupled electronic and nuclear dynamics. To fully exploit the potential of this powerful tool for advanced x-ray spectroscopies, a noninvasive spectral characterization of incident stochastic XFEL pulses with high resolution is a key requirement. Here we present a methodology that combines high-acceptance angle-resolved photoelectron time-of-flight spectroscopy and ghost imaging to enhance the quality of spectral characterization of x-ray free-electron laser pulses. Implementation of this noninvasive high-resolution x-ray diagnostic can greatly benefit the ultrafast x-ray spectroscopy community by functioning as a transparent beamsplitter for applications such as transient absorption spectroscopy in averaging mode as well as covariance-based x-ray nonlinear spectroscopies in single-shot mode where the shot-to-shot fluctuations inherent to a self-amplified spontaneous emission (SASE) XFEL pulse are a powerful asset.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

DOE OSTI2026

A Natural ≳100× Telescope: Discovery of the Strongly Lensed Type II SN 2025mkn at z = 1.37

We present the discovery of SN 2025mkn, a gravitationally lensed Type II supernova. First detected as a blue transient in Zwicky Transient Facility (ZTF), 0. "83 from a z = 0.42 elliptical galaxy, the follow-up SNIFS/UH2.2 m and LRIS/Keck spectra revealed absorption lines at z = 1.371. Later JWST NIRCam imaging shows that the bright transient is a close pair of point sources separated by 0. "07, and a 30 times fainter counterimage opposite the lens, for which NIRSpec reveals strong Hα emission also at z = 1.371. The lightcurves and spectra are consistent with the Type II supernova source being magnified ≳100 times, with ∼250 required to reconcile its luminosity with that of nearby events such as SN 2023ixf. Lens models are consistent with such high magnifications, and always show that the faint image arrived first (undetected in earlier ZTF imaging), consistent with the later spectral phase of this fainter image. A fourth image is also predicted and possibly detected in the NIRSpec data. Lightcurve-based time-delay measurements are not possible due to the first image being the faintest; however, the resolved NIRSpec spectra offer a future opportunity for time-delay cosmography through supernova phase measurements.

Strong gravitational lensing↗

DOE OSTI2025

Imaging Valence Electron Rearrangement in a Chemical Reaction Using Hard X-Ray Scattering

We have observed the signatures of valence electron rearrangement in photoexcited ammonia using ultrafast hard x-ray scattering. Time-resolved x-ray scattering is a powerful tool for imaging structural dynamics in molecules because of the strong scattering from the core electrons localized near each nucleus. Such core-electron contributions generally dominate the differential scattering signal, masking any signatures of rearrangement in the chemically important valence electrons. Ammonia represents an exception to the typically high core-to-valence electron ratio. Here, we measured 9.8 keV x-ray scattering from gas-phase deuterated ammonia following photoexcitation via a 200 nm pump pulse to the 3s Rydberg state. We observed changes in the recorded scattering patterns due to the initial photoexcitation and subsequent deuterium dissociation. Ab initio calculations confirm that the observed signal is sensitive to the rearrangement of the single photoexcited valence electron as well as the interplay between adiabatic and nonadiabatic dissociation channels. The use of ultrafast hard x-ray scattering to image the structural rearrangement of single valence electrons constitutes an important advance in tracking valence electronic structure in photoexcited atoms and molecules.

Gabalski, Ian [SLAC National Accelerator Laborator↗

DOE OSTI2024

Time-resolved cryogenic electron tomography for the study of transient cellular processes

Cryogenic electron tomography (cryo-ET) is the highest resolution imaging technique applicable to the life sciences, enabling sub-nanometer visualization of specimens preserved in their near native states. The rapid plunge freezing process used to prepare samples lends itself to time-resolved studies, which researchers have pursued for in vitro samples for decades. Here, we focus on developing a freezing apparatus for time-resolved studies in situ. The device mixes cellular samples with solution-phase stimulants before spraying them directly onto an electron microscopy grid that is transiting into cryogenic liquid ethane. By varying the flow rates of cell and stimulant solutions within the device, we can control the reaction time from tens of milliseconds to over a second prior to freezing. In a proof-of-principle demonstration, the freezing method is applied to a model bacterium, Caulobacter crescentus, mixed with an acidic buffer. Through cryo-ET we resolved structural changes throughout the cell, including surface-layer protein dissolution, outer membrane deformation, and cytosolic rearrangement, all within 1.5 seconds of reaction time. This new approach, Time-Resolved cryo-ET (TR-cryo-ET), enhances the capabilities of cryo-ET by incorporating a sub-second temporal axis and enables the visualization of induced structural changes at the molecular, organelle, or cellular level.

59 BASIC BIOLOGICAL SCIENCES↗

DOE OSTI2020

Wave-by-Wave Forecasting via Assimilation of Marine Radar Data

Abstract This work describes a phase-resolving wave-forecasting algorithm that is based on the assimilation of marine radar image time series. The algorithm is tested against synthetic data and field observations. The algorithm couples X-band marine radar observations with a phase-resolving wave model that uses the linear mild slope equations for reconstruction of water surface elevations over a large domain of O (km) and a prescribed time window of O (min). The reconstruction also enables wave-by-wave forecasting through forward propagation in space and time. Marine radar image time series provide the input wave observations through a previously given relationship between backscatter intensity and the radial component of the sea surface slope. The algorithm assimilates the wave slope information into the model via a best-fit wave source function at the boundary that minimizes the slope reconstruction error over an annular region at the outer ranges of the radar images. The wave model is then able to propagate the waves across a polar domain to a location of interest at nearer ranges. The constraints on the method for achieving real-time forecasting are identified, and the algorithm is verified against synthetic data and tested using field observations.

Engineering↗

DOE OSTI2026

Characterizing core and edge turbulence regimes with fluctuation imaging diagnostics in Wendelstein 7-X

Two density fluctuation imaging systems, phase contrast imaging (PCI) and gas puff imaging (GPI) measure spatially resolved density fluctuations with high time resolution throughout the core plasma (PCI) and in the scrape-off layer (GPI) of the Wendelstein 7-X (W7-X) stellarator. Both systems combined give a comprehensive overview of overall fluctuation levels, spectral properties such as their distribution in frequency and wavenumber space as well as their spatial distribution. These tools are used to assess changes in density turbulence in three representative discharges that transition into stable divertor detachment by different strategies (impurity seeding, density ramping and power starvation). Several general trends are identified when the radiated power fraction is systematically increased: In the plasma edge, the line emission observed by GPI shifts radially inward with a drop in electron temperature, and normalized intensity fluctuation profiles follow this inward shift. Skewness and kurtosis of these edge fluctuations are reduced, indicating a reduction of large intermittent transport events, and poloidal phase velocities decrease in magnitude. These observations are consistent with a reduced power input into the plasma edge and a general reduction of turbulent activity. Core density fluctuation levels remain nearly constant in the impurity seeding scenario, indicating that detachment does not significantly impact turbulence there. However, a strong reduction in the dominant outboard fluctuation phase velocity is observed that deviates from the previous interpretation of neoclassical radial electric field changes, showing that the core plasma is not completely unaffected. In the density ramp and power starvation scenarios, undesirable and irregular large-scale events arise clearly in both diagnostic systems as the radiative fraction is increased. Impurity seeding therefore seems to be a promising strategy on W7-X to achieve detachment without significantly altering core turbulence, especially when targeting a specific operating point in core density and heating power.

Wendelstein 7-X↗

DOE OSTI2020

Megahertz-rate shock-wave distortion cancellation via phase conjugate digital in-line holography

Abstract Holography is a powerful tool for three-dimensional imaging. However, in explosive, supersonic, hypersonic, cavitating, or ionizing environments, shock-waves and density gradients impart phase distortions that obscure objects in the field-of-view. Capturing time-resolved information in these environments also requires ultra-high-speed acquisition. To reduce phase distortions and increase imaging rates, we introduce an ultra-high-speed phase conjugate digital in-line holography (PCDIH) technique. In this concept, a coherent beam passes through the shock-wave distortion, reflects off a phase conjugate mirror, and propagates back through the shock-wave, thereby minimizing imaging distortions from phase delays. By implementing the method using a pulse-burst laser setup at up to 5 million-frames-per-second, time-resolved holograms of ultra-fast events are now possible. This technique is applied for holographic imaging through laser-spark plasma-generated shock-waves and to enable three-dimensional tracking of explosively generated hypersonic fragments. Simulations further advance our understanding of physical processes and experiments demonstrate ultra-high-speed PCDIH techniques for capturing dynamics.

Science & Technology - Other Topics↗

DOE OSTI2020

Temperature distributions and gradients in laser-heated plasmas relevant to magnetized liner inertial fusion

We present two-dimensional temperature measurements of magnetized and unmagnetized plasma experiments performed at Z relevant to the preheat stage in magnetized liner inertial fusion. The deuterium gas fill was doped with a trace amount of argon for spectroscopy purposes, and time-integrated spatially resolved spectra and narrow-band images were collected in both experiments. The spectrum and image data were included in two separate multiobjective analysis methods to extract the electron temperature spatial distribution T e ( r , z ) . The results indicate that the magnetic field increases T e , the axial extent of the laser heating, and the magnitude of the radial temperature gradients. Comparisons with simulations reveal that the simulations overpredict the extent of the laser heating and underpredict the temperature. Temperature gradient scale lengths extracted from the measurements also permit an assessment of the importance of nonlocal heat transport.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

DOE OSTI2022

Standoff Infrared Measurements of Chemical Plume Dynamics in Complex Terrain Using a Combination of Active Swept-ECQCL Laser Spectroscopy with Passive Hyperspectral Imaging

Chemical plume detection and modeling in complex terrain present numerous challenges. We present experimental results from outdoor releases of two chemical tracers (sulfur hexafluoride and Freon-152a) from different locations in mountainous terrain. Chemical plumes were detected using two standoff instruments collocated at a distance of 1.5 km from the plume releases. A passive long-wave infrared hyperspectral imaging system was used to show time- and space-resolved plume transport in regions near the source. An active infrared swept-wavelength external cavity quantum cascade laser system was used in a standoff configuration to measure quantitative chemical column densities with high time resolution and high sensitivity along a single measurement path. Both instruments provided chemical-specific detection of the plumes and provided complementary information over different temporal and spatial scales. The results show highly variable plume propagation dynamics near the release points, strongly dependent on the local topography and winds. Effects of plume stagnation, plume splitting, and plume mixing were all observed and are explained based on local topographic and wind conditions. Measured plume column densities at distances ~100 m from the release point show temporal fluctuations over ~1 s time scales and spatial variations over ~1 m length scales. The results highlight the need for high-speed and spatially resolved measurement techniques to provide validation data at the relevant spatial and temporal scales required for high-fidelity terrain-aware microscale plume propagation models.

47 OTHER INSTRUMENTATION↗

DOE OSTI2026

Spatially resolved polarization swings in the supermassive binary black hole candidate OJ 287 with first Event Horizon Telescope observations

We present the first Event Horizon Telescope 1.3 mm observations of the supermassive binary black hole candidate OJ 287. The observations achieved an unprecedented angular resolution of 18 μas and reveal significant structural and polarization variability over just five days, marking the shortest timescale on which such changes have been directly imaged in this source. The inner jet exhibits a twisted ridgeline structure, with features displaying apparent superluminal motions up to about 22 c. The linear polarization maps reveal three main polarized features whose electric-vector position angles (EVPAs) change substantially over the time span of our observations, including a component with a radial polarization consistent with being produced by a recollimation shock. Most notably, we directly resolved two innermost jet components whose EVPAs rotate in opposite directions. The faster component, moving at 2.4 ± 0.9 μas/day (17.4 ± 6.5 c), exhibits counterclockwise EVPA swings of roughly 3.7° per day, while the slower component, with a proper motion of 1.4 ± 0.3 μas/day (10.2 ± 2.2 c), rotates clockwise at approximately 2.5° per day. Previous studies inferred helical magnetic fields in AGN jets from time-resolved or integrated polarization variability but lacked the angular resolution to directly image this effect. Our results provide spatially resolved evidence that a helical magnetic field threads the jet’s collimation and acceleration zone, ruling out models based on the superposition of unresolved components. Our analysis suggests that propagating shocks interact with a Kelvin–Helmholtz plasma instability, illuminating different phases of the helical magnetic field and producing the observed polarization spatial and temporal variability. Moreover, our model naturally accounts for the more rapid polarization rotation observed in the faster moving component. Our model predicts even more rapid swings in polarization, which could be tested with future observations featuring a more densely sampled time coverage.

OJ 287↗

DOE OSTI2021

Probing atom dynamics of excited Co-Mo-S nanocrystals in 3D

Advances in electron microscopy have enabled visualizations of the three-dimensional (3D) atom arrangements in nano-scale objects. The observations are, however, prone to electron-beam-induced object alterations, so tracking of single atoms in space and time becomes key to unravel inherent structures and properties. Here, we introduce an analytical approach to quantitatively account for atom dynamics in 3D atomic-resolution imaging. The approach is showcased for a Co-Mo-S nanocrystal by analysis of time-resolved in-line holograms achieving ~1.5 Å resolution in 3D. The analysis reveals a decay of phase image contrast towards the nanocrystal edges and meta-stable edge motifs with crystallographic dependence. These findings are explained by beam-stimulated vibrations that exceed Debye-Waller factors and cause chemical transformations at catalytically relevant edges. This ability to simultaneously probe atom vibrations and displacements enables a recovery of the pristine Co-Mo-S structure and establishes, in turn, a foundation to understand heterogeneous chemical functionality of nanostructures, surfaces and molecules.

36 MATERIALS SCIENCE↗

DOE OSTI2025

Carbon Fiber Oxidation in 4D

The oxidation of carbon fibers at high temperatures is the primary degradation process in the thermal protection system of many hypersonic flight vehicles. Predicting the rate and the extent of oxidation is critical to ensure a safe and effective design. An oversized thermal protection system adds unnecessary mass, while an under-designed one risks system failure and mission loss. Resolving high-temperature material degradation due to oxidation has been a long-standing challenge in designing for re-entry flight environments. Using time-resolved in situ X-ray microtomography, the oxidation of carbon fibers at high temperatures is directly imaged, resolving the two limiting degradation regimes: diffusion- and reaction-limited. The ability to resolve material degradation in time at the sub-micron scale sheds light on the ablation phenomenon and enables predictions of material constitutive properties evolving in time, with profound implications on the ability to model the aerothermal response of heat shield materials in hostile environments.

ablation↗

DOE OSTI2021

Commissioning of a Cask Enabling Characterization of Irradiated Nuclear Fuels with Pulsed Neutrons

Irradiation tests are a key component of nuclear fuel development and identifying typical and atypical regions in the irradiated fuel volume relies on very few characterization techniques. The goal of the effort reported here is to provide complementary measurements adding to the available parameter space for post irradiation examination as well as to inform subsequent hot cell PIE examinations by identifying typical and atypical regions with respect to microstructure, tomographic data, or isotope densities. Pulsed neutrons, enabling diffraction as well as energy-resolved neutron imaging and neutron absorption resonance spectroscopy, offer unique capabilities for this purpose. Time-of-flight neutron diffraction has the potential to offer efficient, non-destructive and non-contact microstructural characterization of irradiated fuel pins with spatial resolution of 1 mm 3 to 1 cm 3 while for energy-resolved neutron imaging (and by extension tomography) a resolution of 100 μm was demonstrated. The potential results include crystallinity vs. amorphous volumes and microstructural information such as phase compositions, lattice strains (indicative of residual stresses or chemistry variations) and textures from the diffraction data as well as distances (e.g. pellet to cladding), cracks, and isotopic distributions of minor actinides, fission products as well as fission gas partial pressures e.g. in the plenum from energy resolved neutron imaging.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

DOE OSTI2022

Progress Report on Mockup Irradiation Capsule Fuel Measurements at LANSCE

Irradiation tests are a key component of nuclear fuel development and identifying typical and atypical regions in the irradiated fuel volume relies on very few characterization techniques. The goal of the effort reported here is to provide complementary measurements adding to the available parameter space for post irradiation examination as well as to inform subsequent hot cell PIE examinations by identifying typical and atypical regions with respect to microstructure, tomographic data, or isotope densities. Pulsed neutrons, enabling diffraction as well as energy-resolved neutron imaging and neutron absorption resonance spectroscopy, offer unique capabilities for this purpose. Time-of-flight neutron diffraction has the potential to offer efficient, non-destructive and non-contact microstructural characterization of irradiated fuel specimen with spatial resolution of 1 mm 3 to 1 cm 3 while for energy-resolved neutron imaging (and by extension tomography) a resolution of 100 μm 3 was demonstrated. The potential results include crystallinity vs. amorphous volumes and microstructural information such as phase compositions, lattice strains (indicative of residual stresses or chemistry variations) and textures from the diffraction data as well as distances (e.g. pellet to cladding), cracks, and isotope densities of minor actinides, fission products as well as fission gas partial pressures e.g. in the plenum from energy resolved neutron imaging.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗