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Search indexed NASA NTRS and DOE OSTI research on propulsion, heat transfer, battery materials and energy systems. Follow report and document links to the original sources.

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At least 163 records · Page 9

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↗

Structured ionized winds shooting out from a quasar at relativistic speeds

Evidence indicates that supermassive black holes (SMBHs) exist at the centres of most galaxies. Their mass correlates with the galactic bulge mass, suggesting a coevolution with their host galaxies, most likely through powerful winds. X-ray observations have detected highly ionized winds outflowing at sub-relativistic speeds from the accretion disks around SMBHs. However, the limited spectral resolution of present X-ray instruments has left the physical structure and location of the winds poorly understood, hindering accurate estimates of their kinetic power. Here, in this study, the first X-Ray Imaging and Spectroscopy Mission (XRISM) observation of the luminous quasar PDS 456 is reported. The high-resolution spectrometer Resolve aboard XRISM enabled the discovery of five discrete velocity components outflowing at 20–30% of the speed of light. This demonstrates that the wind structure is highly inhomogeneous, which probably consists of up to a million clumps. The mass outflow rate is estimated to be 60–300 solar masses per year, with the wind kinetic power exceeding the Eddington luminosity limit. Compared with the galaxy-scale outflows, the kinetic power is more than three orders of magnitude larger, whereas the momentum flux is ten times larger. These estimates disfavour both energy-driven and momentum-driven outflow models. This suggests that such wind activity occurs in less than 10% of the quasar phase and/or that its energy/momentum is not efficiently transferred to the galaxy-scale outflows owing to the clumpiness of the wind and the interstellar medium.

Audard, Marc [Univ. of Geneva, Versoix (Switzerlan↗

Disentangling multiple gas kinematic drivers in the Perseus galaxy cluster

Galaxy clusters, the Universe’s largest halo structures, are filled with an X-ray-emitting gas with a temperature between 10 million and 100 million degrees. Their evolution is shaped by energetic processes such as feedback from supermassive black holes (SMBHs) and mergers with other cosmic structures. The imprints of these processes on gas kinematics remain largely unknown, restricting our understanding of energy conversion within clusters4. High-resolution spectral mapping with the X-Ray Imaging and Spectroscopy Mission (XRISM) observatory offers a way forward. Here we present XRISM kinematic measurements of the Perseus cluster, radially covering the extent of its cool core. We find direct evidence for at least two dominant drivers of gas motions operating on distinct physical scales: a small-scale driver in the inner approximately 60 kpc, probably associated with the SMBH feedback; and a large-scale driver in the outer core, powered by mergers. This finding suggests that, during the active phase, SMBH feedback drives gas motions, which, if fully dissipated into heat, could have a substantial role in offsetting radiative cooling losses in the Perseus core. Furthermore, our study underscores the necessity of kinematic mapping observations of extended sources to robustly characterize the velocity fields and their role in the evolution of massive halos. It further offers a kinematic diagnostic for SMBH feedback models.

Astronomy and AstroPhysics↗

Multi-campaign ship and aircraft observations of marine cloud condensation nuclei and droplet concentrations

In situ marine cloud droplet number concentrations (CDNCs), cloud condensation nuclei (CCN), and CCN proxies, based on particle sizes and optical properties, are accumulated from seven field campaigns: ACTIVATE; NAAMES; CAMP 2 EX; ORACLES; SOCRATES; MARCUS; and CAPRICORN2. Each campaign involves aircraft measurements, ship-based measurements, or both. Measurements collected over the North and Central Atlantic, Indo-Pacific, and Southern Oceans, represent a range of clean to polluted conditions in various climate regimes. With the extensive range of environmental conditions sampled, this data collection is ideal for testing satellite remote detection methods of CDNC and CCN in marine environments. Remote measurement methods are vital to expanding the available data in these difficult-to-reach regions of the Earth and improving our understanding of aerosol-cloud interactions. The data collection includes particle composition and continental tracers to identify potential contributing CCN sources. Several of these campaigns include High Spectral Resolution Lidar (HSRL) and polarimetric imaging measurements and retrievals that will be the basis for the next generation of space-based remote sensors and, thus, can be utilized as satellite surrogates.

54 ENVIRONMENTAL SCIENCES↗

Stereogenic-at-silicon hybrid conjugated polymers

Stereoregularity in carbon-based polymers impacts critical physical properties such as crystallinity, but achieving comparable precision in polysilanes remains challenging. Herein, we report the synthesis of hybrid σ,π-conjugated polysilanes with defined stereoregularity, derived from cis- and trans-cyclosilane building blocks. Using Kumada polycondensation, we accessed a series of atactic, trans-enriched, and cis-enriched polysilanes, enabling a systematic investigation of how tacticity influences thermal and optical properties. Differential scanning calorimetry revealed distinct glass transition behaviors for stereoregular polymers compared to their atactic counterpart, and UV-vis spectroscopy demonstrated enhanced spectral resolution upon annealing of stereoregular films. A linear silane-based analog further underscored the structural impact of cyclic stereogenic units. These findings highlight how stereochemical precision in silicon-containing backbones can modulate macromolecular properties, opening avenues for the rational design of stereoregular polysilanes.

36 MATERIALS SCIENCE↗

JWST’s PEARLS: A z ≃ 6 quasar in a train-wreck galaxy merger system

We present JWST NIRSpec integral field spectroscopy observations of the z = 5.89 quasar NDWFS J1425+3254 from 0.6–5.3 μm, covering the rest-frame ultraviolet and optical at a spectral resolution of R ∼ 100. The quasar has a black hole mass of M BH = (1.4 +3.1 −1.0 ) × 10 9 M ⊙ and an Eddington ratio of L Bol /L Edd = 0.3 +0.6 −0.2 , as implied from the broad Balmer Hα and Hβ lines. The quasar host has significant ongoing obscured star formation, as well as a quasar-driven outflow with velocity 6050 +460 −630 km s −1 and ionised outflow rate of 1650 +130 −1230 M ⊙ yr −1 . This is possibly one of the most extreme outflows in the early Universe. The data also reveal that two companion galaxies are merging with the quasar host. The north-eastern companion galaxy is relatively old and very massive, with a luminosity-weighted stellar age of 65 +9 −4 Myr, stellar mass of (3.6 +0.6 −0.3 #x00D7; 10 11 M ⊙ , and star-formation rate (SFR) of ∼15–30 M ⊙ yr −1 . A bridge of gas connects this companion galaxy and the host, confirming their ongoing interaction. A second merger is occurring between the quasar host and a much younger companion galaxy to the south, with a stellar age of 6.7 ± 1.8 Myr, stellar mass of (1.9 ± 0.4)×10 10 M ⊙ , and SFR of ∼40–65 M ⊙ yr −1 . There is also another galaxy in the field, likely in the foreground at z = 1.135, which could be gravitationally lensing the quasar with a magnification of 1 < μ < 2 and, thus, < 0.75 mag. Overall, the system is a ‘train-wreck’ merger of three galaxies, with star formation and extreme quasar activity that were likely triggered by these ongoing interactions.

79 ASTRONOMY AND ASTROPHYSICS↗

Measurements of ion velocity distributions in a large scale laser-produced plasma

Laser-produced plasma velocity distributions are an important, but difficult quantity to measure. In this work, we present a noninvasive technique for measuring individual charge state velocity distributions of laser-produced plasmas using a high temporal and spectral resolution monochromator. The novel application of this technique is its ability to detect particles up to seven meters from their inception (significantly larger than most laboratory plasma astrophysics experiments, which take place at or below the millimeter scale). The design and assembly of this diagnostic is discussed in terms of maximizing the signal to noise ratio, maximizing the spatial and temporal resolution, and other potential use cases. The analysis and results of this diagnostic are demonstrated by directly measuring the time-of-flight velocity of all ion charge states in a laser produced carbon plasma.

47 OTHER INSTRUMENTATION↗

Measurement of L-shell emission from mid-Z targets under non-LTE conditions using Transmission Grating Spectrometer and DANTE power diagnostics

In this work, we present the measurement of L-band emission from buried Sc/V targets in experiments performed at the OMEGA laser facility. The goal of these experiments was to study non-local thermodynamic equilibrium plasmas and benchmark atomic physics codes. The L-band emission was measured simultaneously by the time resolved DANTE power diagnostic and the recently fielded time integrated Soreq-Transmission Grating Spectrometer (TGS) diagnostic. The TGS measurement was used to support the spectral reconstruction process needed for the unfolding of the DANTE data. The Soreq-TGS diagnostic allows for broadband spectral measurement in the 120 eV–2000 eV spectral band, covering L- and M-shell emission of mid- and high-Z elements, with spectral resolution λ/Δλ = 8–30 and accuracy better than 25%. The Soreq-TGS diagnostic is compatible with ten-inch-manipulator platforms and can be used for a wide variety of high energy density physics, laboratory astrophysics, and inertial confinement fusion experiments.

Fraenkel, M. (ORCID:0000000291939544)↗

A dual high-energy radiography platform with 15 μ m resolution at the National Ignition Facility

To study matter at extreme densities and pressures, we need mega laser facilities such as the National Ignition Facility as well as creative methods to make observations during timescales of a billionth of a second. To facilitate this, we developed a platform and diagnostic to characterize a new point-projection radiography configuration using two micro-wires irradiated by a short pulse laser system that provides a large field of view with up to 3.6 ns separation between images. In this work, we used tungsten-carbide solid spheres as reference objects and inferred characteristics of the back-lighter source using a forward-fitting algorithm. The resolution of the system is inferred to be 15 μm (using 12.5 μm diameter wires). The bremsstrahlung temperature of the source is 70–300 keV, depending on laser energy and coupling efficiency. By adding the images recorded on multiple stacked image plates, the signal-to-noise of the system is nearly doubled. The imaging characterization technique described here can be adapted to most point-projection platforms where the resolution, spectral contrast, and signal-to-noise are important.

47 OTHER INSTRUMENTATION↗

Demonstration of an x-ray Raman spectroscopy setup to study warm dense carbon at the high energy density instrument of European XFEL

We present a proof-of-principle study demonstrating x-ray Raman Spectroscopy (XRS) from carbon samples at ambient conditions in conjunction with other common diagnostics to study warm dense matter, performed at the high energy density scientific instrument of the European x-ray Free Electron Laser (European XFEL). We obtain sufficient spectral resolution to identify the local structure and chemical bonding of diamond and graphite samples, using highly annealed pyrolytic graphite spectrometers. Due to the high crystal reflectivity and XFEL brightness, we obtain signal strengths that will enable accurate XRS measurements in upcoming pump–probe experiments with a high repetition-rate, where the samples will be pumped with high-power lasers. Molecular dynamics simulations based on density functional theory together with XRS simulations demonstrate the potential of this technique and show predictions for high-energy-density conditions. Our setup allows simultaneous implementation of several different diagnostic methods to reduce ambiguities in the analysis of the experimental results, which, for warm dense matter, often relies on simplifying model assumptions. The promising capabilities demonstrated here provide unprecedented insights into chemical and structural dynamics in warm dense matter states of light elements, including conditions similar to the interiors of planets, low-mass stars, and other celestial bodies.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Two-dimensional electronic–vibrational spectroscopy: Exploring the interplay of electrons and nuclei in excited state molecular dynamics

Two-dimensional electronic-vibrational spectroscopy (2DEVS) is an emerging spectroscopic technique which exploits two different frequency ranges for the excitation (visible) and detection (infrared) axes of a 2D spectrum. In contrast to degenerate 2D techniques, such as 2D electronic or 2D infrared spectroscopy, the spectral features of a 2DEV spectrum report cross correlations between fluctuating electronic and vibrational energy gaps rather than autocorrelations as in the degenerate spectroscopies. The center line slope of the spectral features reports on this cross correlation function directly and can reveal specific electronic-vibrational couplings and rapid changes in the electronic structure, for example. The involvement of the two types of transition moments, visible and infrared, makes 2DEVS very sensitive to electronic and vibronic mixing. 2DEV spectra also feature improved spectral resolution, making the method valuable for unraveling the highly congested spectra of molecular complexes. The unique features of 2DEVS are illustrated in this paper with specific examples and their origin described at an intuitive level with references to formal derivations provided. Although early in its development and far from fully explored, 2DEVS has already proven to be a valuable addition to the tool box of ultrafast nonlinear optical spectroscopy and is of promising potential in future efforts to explore the intricate connection between electronic and vibrational nuclear degrees of freedom in energy and charge transport applications.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Ultra-compact x-ray spectrometer for high-repetition-rate laser–plasma experiments

Here, we present in this work the development of an ultra-compact, multi-channel x-ray spectrometer (UCXS). This diagnostic has been specially built and adapted to perform at high-repetition-rate (>1 Hz) for high-intensity, short-pulse laser plasma experiments. X-ray filters of varying materials and thicknesses are chosen to provide spectral resolution up to ΔE ≈ 1 keV over the x-ray energy range of 1–30 keV. These filters are distributed over a total of 25 channels, where each x-ray filter is coupled to a single scintillator. The UCXS is designed to detect and resolve a large variety of laser-driven x-ray sources such as low energy bremsstrahlung emission, fluorescence, and betatron radiation (up to 30 keV). Preliminary results from commissioning experiments at the ABL laser facility at Colorado State University are provided.

47 OTHER INSTRUMENTATION↗

Calibration of the sub-aperture backscatter system on OMEGA EP

The sub-aperture backscatter (SABS) diagnostic on the OMEGA EP Laser System is a diagnostic that is used to measure the backscattered and sidescattered light during laser–plasma interaction experiments that are relevant to high-energy-density physics and inertial confinement fusion. The diagnostic collects stimulated Brillouin scattering (SBS) UV light at around 351 nm and stimulated Raman scattering (SRS) in the visible-light regime in the 420–720-nm-wavelength range and provides spectrally and temporally resolved information. Five 1-in. light collectors, composed of a lens, ground glass diffuser, and coupling into a 300-μm fiber, are positioned behind the last steering mirror on one of the four beamlines to catch a portion of the beam cross section (~1.5%) of the emission that is scattered into the beamline. The SRS light is collected in two light collectors, combined, and transported via graded index fibers to a streaked spectrometer. The SABS-SRS streak spectrometer has a temporal and spectral resolution of 100 ps and 1 nm, respectively. Three other light collectors collect, combine, and transport the SBS signal to a Hamamatsu high-voltage photodiode, where an oscilloscope digitizes the data, providing a time resolution of better than 1 ns. To obtain an absolute energy calibration of SRS measurements, light signals of known energy and wavelength were injected into the light collectors one at a time. The resulting counts on the streak camera charge-coupled device for SRS are then correlated with the incident fluence of scattered light at the light collector in order to allow a quantitative assessment of streak camera sensitivity to determine the energy of the scattered light during experiments. The measurements were performed in situ from the light collectors to the detectors. Other offline measurements provided the transmission of the optics between the target chamber center and the light collectors.

47 OTHER INSTRUMENTATION↗

Improvements to the characterization of Agfa x-ray film for use on opacity spectroscopy diagnostics

The National Ignition Facility uses a soft x-ray opacity spectrometer for x-ray spectral imaging in high-energy-density experiments. The increased demand for a better spectral resolution prompted the investigation into the Agfa D4 film. Characterization is already under way for the film. A Manson x-ray source using six different anodes was used to expose film to the linear optical density (OD) region. This is a continuation of the previous work, and the updated analysis process is communicated here. The identified uncertainties have been reduced with the updated steps that improve the results of the characterization process. In conclusion, when the Stanford Synchrotron Radiation Lightsource Beamline 16-2 was operational, the film was characterized at that source. Its beam offered a higher fluency with a lower exposure time needed to reach saturation. Results for both sources are compared in this paper.

47 OTHER INSTRUMENTATION↗

A platform for non-local thermodynamic equilibrium atomic physics research using the buried layer target approach at a kJ level laser facility

Here we present a design and first use of a kJ level laser facility for research of non-local thermodynamic equilibrium atomic physics using the buried layer target method. The target design included a metal layer buried inside a plastic tamper with thicknesses tailored to the expected laser intensities. The target was illuminated from each side by two laser beams with intensities of 0.5–5 × 10 14 W/cm 2 . The advanced diagnostic suite included static and time-resolved imagers and spectrometers with various spectral resolutions. A 3D printed dual elliptically curved spectrometer is presented, and its results are compared to a traditional crystal spectrometer. Experimental results and radiation hydrodynamic simulations demonstrate that the target achieved the desired thermodynamic conditions of n e ≈ 10 21 –10 22 cm -3 and T e ≈ 1–2 keV.

3D printing↗

Population inversion X-ray laser oscillator

Oscillators are at the heart of optical lasers, providing stable, transform-limited pulses. Until now, laser oscillators have been available only in the infrared to visible and near-ultraviolet (UV) spectral region. In this paper, we present a study of an oscillator operating in the 5- to 12-keV photon-energy range. We show that, using the Kα 1 line of transition metal compounds as the gain medium, an X-ray free-electron laser as a periodic pump, and a Bragg crystal optical cavity, it is possible to build X-ray oscillators producing intense, fully coherent, transform-limited pulses. As an example, we consider the case of a copper nitrate gain medium generating ~ 5 × 10 10 photons per pulse with 37-fs pulse length and 48-meV spectral resolution at 8-keV photon energy. Our theoretical study and simulation of this system show that, because of the very large gain per pass, the oscillator saturates and reaches full coherence in four to six optical-cavity transits. We discuss the feasibility and design of the X-ray optical cavity and other parts of the oscillator needed for its realization, opening the way to extend X-ray–based research beyond current capabilities.

47 OTHER INSTRUMENTATION↗

Visualizing conical intersection passages via vibronic coherence maps generated by stimulated ultrafast X-ray Raman signals

Significance The capabilities of modern X-ray sources have substantially increased the temporal and spectral resolutions for the observation of elementary molecular events. Theoretically, it has been shown that these unique features can be exploited to probe vibronic coherences that emerge when molecules pass through conical intersections. Here, we demonstrate this technique for the photorelaxation of the RNA-nucleobase uracil after UV excitation. The generated coherence maps reveal the path of the nuclear wavepacket on the excited-state surface in the vicinity of the conical intersection. This information is directly accessible from the spectroscopically recorded signal. Being transferrable to other molecules, these coherence maps will provide detailed visualizations of other nonadiabatic passages in the future.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

From antenna to reaction center: Pathways of ultrafast energy and charge transfer in photosystem II

The photosystem II core complex (PSII-CC) is the smallest subunit of the oxygenic photosynthetic apparatus that contains core antennas and a reaction center, which together allow for rapid energy transfer and charge separation, ultimately leading to efficient solar energy conversion. However, there is a lack of consensus on the interplay between the energy transfer and charge separation dynamics of the core complex. Here, we report the application of two-dimensional electronic-vibrational (2DEV) spectroscopy to the spinach PSII-CC at 77 K. The simultaneous temporal and spectral resolution afforded by 2DEV spectroscopy facilitates the separation and direct assignment of coexisting dynamical processes. Our results show that the dominant dynamics of the PSII-CC are distinct in different excitation energy regions. By separating the excitation regions, we are able to distinguish the intraprotein dynamics and interprotein energy transfer. Additionally, with the improved resolution, we are able to identify the key pigments involved in the pathways, allowing for a direct connection between dynamical and structural information. Specifically, we show that C505 in CP43 and the peripheral chlorophyll Chlz D1 in the reaction center are most likely responsible for energy transfer from CP43 to the reaction center.

59 BASIC BIOLOGICAL SCIENCES↗