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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↗

NASA NTRS1982

Speckle spectroscopy; an application for the multi-anode microchannel array detector system

Plans to combine the High Angular Resolution Imager/Spectrometer on the 4-meter Mayall telescope at the Kitt Peak National Observatory and the (256 x 1024)-pixel Multi-Anode Microchannel Array detector system to produce a unique instrument for speckle spectroscopy are described. The pulse-counting detector system will provide distortion-free imaging and will time tag each spatially-resolved photon event with an accuracy of 100 ns. The Imager/Spectrometer will provide a spatial resolution of 0.07 arcsec orthogonal to the plane of dispersion and 0.18 arcsec in the plane of dispersion.

Butcher, H. R.↗

NASA NTRS2012

Probable Rotation States of Rocket Bodies in Low Earth Orbit

In order for Active Debris Removal to be accomplished, it is critically important to understand the probable rotation states of orbiting, spent rocket bodies. As compared to the question of characterizing small unresolved debris, in this problem there are several advantages: (1) objects are of known size, mass, shape and color, (2) they have typically been in orbit for a known period of time, (3) they are large enough that resolved images may be obtainable for verification of predicted orientation, and (4) the dynamical problem is simplified to first order by largely cylindrical symmetry. It is also nearly certain for realistic rocket bodies that internal friction is appreciable in the case where residual liquid or, to a lesser degree, unconsolidated solid fuels exist. Equations of motion have been developed for this problem in which internal friction as well as torques due to solar radiation, magnetic induction, and gravitational gradient are included. In the case of pure cylindrical symmetry, the results are compared to analytical predictions patterned after the standard approach for analysis of symmetrical tops. This is possible because solar radiation and gravitational torques may be treated as conservative. Agreement between results of both methods ensures their mutual validity. For monotone symmetric cylinders, solar radiation torque vanishes if the center of mass resides at the geometric center of the object. Results indicate that in the absence of solar radiation effects, rotation states tend toward an equilibrium configuration in which rotation is about the axis of maximum inertia, with the axis of minimum inertia directed toward the center of the earth. Solar radiation torque introduces a modification to this orientation. The equilibrium state is asymptotically approached within a characteristic timescale given by a simple ratio of relevant characterizing parameters for the body in question. Light curves are simulated for the expected asymptotic final rotation states of model objects, and these are compared to data derived from physical models of the same objects, tested in the Optical Measurements Center at JSC. Comparison to relevant light curves from actual orbiting rocket bodies are also performed, and diagnostic features of such curves are examined.

Ojakangas, Gregory W.↗

NASA NTRSDate not supplied

Thermal Band Observations of the May 2022 Total Lunar Eclipse by the Landsat Thermal Infrared Sensors

The Thermal Infrared Sensor (TIRS) instruments on board Landsat 8 and Landsat 9 provide routine thermal band image measurements of the Earth for the Landsat program. Although these observatories are specifically designed for mapping the Earth’s surface from their 705-km altitude orbits, they were recently utilized to image the Moon during the total lunar eclipse of May 2022. The full Moon is frequently used as a calibration target for Landsat. However, the imaging of the lunar eclipse provided a unique opportunity to gather accurate temporal thermal band data over the full lunar disc as solar illumination is removed. This campaign required a large effort by the Landsat Flight Operations teams to coordinate acquisitions and technical constraints on both observatories to capture the long temporal extent of the eclipse. The result of this effort was a series of resolved thermal images of the Moon at discrete times as the Earth’s shadow swept across the lunar surface through the start, partial, and total phases of the eclipse. This sequence of images showed an overall drop in surface temperature from approximately 370 K to 180 K in about 300 minutes as solar insolation was removed. Furthermore, the spatial distribution of cooling rates from this unique event provided information about different material properties (density and thermal inertia) across the lunar surface and showed a clear distinction among mare, highlands, and impact craters.

Matthew Montanaro↗

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↗

NASA NTRS2024

orbitize! v3: Orbit fitting for the High-contrast Imaging Community

orbitize! is a package for Bayesian modeling of the orbital parameters of resolved binary objects from time series measurements. It was developed with the needs of the high-contrast imaging community in mind, and has since also become widely used in the binary star community. A generic orbitize! use case involves translating relative astrometric time series, optionally combined with radial velocity or astrometric time series, into a set of derived orbital posteriors. This paper is published alongside the release of orbitize! version 3.0, which has seen significant enhancements in functionality and accessibility since the release of version 1.0 (Blunt et al., 2020).

Sarah Blunt↗

NASA NTRS2020

100-kHz Interferometric Rayleigh Scattering Flow Diagnostics at 266 nm

Interferometric Rayleigh scattering (IRS) is a laser-based technique capable of spatially and temporally resolved measurement of gas velocity and temperature in unseeded gaseous flows. In the present embodiment of the technique, IRS is performed at 266 nm for the first time. IRS at 266 nm is potentially much less susceptible to interferences from particles and other stray light sources. A pulse-burst laser and high-speed camera provided image rates of 100 kHz, allowing simultaneous space- and time-resolved measurement in high speed flow at multiple points along a line. The use of 266 nm excitation and detection is compared with prior work that used 532 nm. New experimental interferogram modelling and fitting techniques for single and multi-velocity-component IRS were demonstrated in a study of the spatial and temporal variation of the flow along a line through a supersonic jet. Single component velocity and temperature measurements using 266 nm were successfully made and compared with prior 532 nm results. Two-component velocity measurements at 266 nm, using the reflected image method, were compared to single-component measurements.

Andrew D Cutler↗

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↗

NASA NTRSDate not supplied

Experimental and Theoretical Needs for the JWST Early Release Science Program on Radiative Feedback from Massive Stars (PDRs4ALL): III. A Quantum Chemistry Perspective

Massive stars disrupt their natal molecular cloud material by dissociating molecules, ionizing atoms and molecules, and heating the gas and dust. These processes drive the evolution of interstellar matter in our Galaxy and throughout the Universe from the era of vigorous star formation at z=1-3 to the present day. Much of this interaction occurs in Photo- Dissociation Regions (PDRs) where far-ultraviolet photons of these stars create a largely neutral, but warm region of gas and dust. PDR emission dominates the IR spectra of starforming galaxies and provides a unique tool to study the physical and chemical processes that are relevant for inter- and circumstellar media including diffuse clouds, molecular cloud and protoplanetary disk surfaces, and starburst galaxies. The ERS program ID1288 is dedicated to provide template data as well as data processing and analysis tools for PDRs. To this end, it will observe the Orion Bar, the proto-typical PDR situated in the nearby Orion Nebula, using NIRSpec IFU, MIRI IFU, and NIRCAM and MIRI imaging. These observations will, for the first time, spatially resolve and perform a tomography of the PDR, revealing the individual IR spectral signatures from the key zones and sub-regions within the ionized gas, the PDR, and the molecular cloud. Quantum chemistry can be used to determine molecular data such as ionization potentials, chemical reaction rates, electronic spectra, dissociation energies, channels, and branching ratios, etc. These are often used in synergy with experiment to take advantage of the strengths of each approach. An area of active research is modeling the infrared (IR) emission spectra produced by PAH molecules, including the effects of anharmonicity. This will be important in the interpretation of JWST data which will yield higher-resolution spectral data compared to Spitzer or ISO. Quantum chemistry methods can compute accurate anharmonic IR absorption spectra of PAH molecules up to about 25 C atoms, and the results have been benchmarked against high-resolution experimental spectra. These feed into a quantum Monte Carlo (QMC) approach to generate temperature-dependent anharmonic IR emission spectra and then used to generate fully anharmonic cascade emission IR spectra of PAH molecules -- the very type of spectra that JWST will observe. Work continues to extend these methods to larger PAH molecules. We will discuss the current state of this work, as well as

Timothy Lee↗