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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 613 records · Page 34

Optical tuning of the diamond Fermi level measured by correlated scanning probe microscopy and quantum defect spectroscopy

Quantum technologies based on quantum point defects in crystals require control over the defect charge state. Here we tune the charge state of shallow nitrogen-vacancy and silicon-vacancy centers by locally oxidizing a hydrogenated surface with moderate optical excitation and simultaneous spectral monitoring. The loss of conductivity and change in work function due to oxidation are measured in atmosphere using conductive atomic force microscopy and Kelvin probe force microscopy (KPFM). We correlate these scanning probe measurements with optical spectroscopy of the nitrogen-vacancy and silicon-vacancy centers created via implantation 15–25 nm beneath the diamond surface and annealing. The observed charge state of the defects as a function of optical exposure demonstrates that laser oxidation provides a way to precisely tune the Fermi level over a range of at least 2.00 eV. We also observe a significantly larger oxidation rate for implanted surfaces compared to unimplanted surfaces under ambient conditions. Here, combined with knowledge of the electron affinity of a surface, these results suggest KPFM is a powerful, high-spatial-resolution technique to advance surface Fermi level engineering for charge stabilization of quantum defects.

36 MATERIALS SCIENCE↗

Final report: Mapping Interactions in Hybrid Systems with Active Scanning Probes

This project aimed to study and map interactions between components of hybrid nanodevices using a novel scanning probe approach. To enable this work, we initially constructed a flexible experimental apparatus allowing for simultaneous scanning probe and confocal optical microscopy measurements. This setup was first used for all-optical measurements of nanostructures, with the focus then shifting to hybrid devices in which single coherent electron spins are coupled to micron-scale ferromagnetic elements, which may prove useful for addressing single spins, enhanced sensing, or spin-wave-mediated coupling of spins for quantum information applications. A significant breakthrough was the realization that it is not necessary to fabricate a magnetic structure on a scanning probe – instead a ferromagnetic vortex core can act as an integrated, solid state, scanning probe. The core of the vortex produces a very strong, localized fringe field which can be used analogously to an MFM tip. Unlike a traditional MFM tip, however, the vortex core is scanned within an integrated device (eliminating drift), and can be moved on vastly faster timescales. This approach allows the detailed investigation of interactions between single spins and complex driven ferromagnetic dynamics.

77 NANOSCIENCE AND NANOTECHNOLOGY↗

X-ray Transient Absorption Studies of Exciton Self-Trapping

Here, we present optical pump/X-ray absorption probe studies to probe changes in electronic distribution and local structure upon formation of a self-trapped exciton. The experiments were carried out on the mixed-valence halide-bridged transition metal linear chain charge density wave material [Pt(en 2 )][Pt(en 2 )Cl 2 ]·(ClO 4 ) 4 . Photoinduced changes in the Pt L III XANES spectrum were measured on a picosecond time scale following generation of excitons via optical excitation of the intervalence charge transfer transition. Ab initio FEFF9 modeling of the spectra and the associated angular momentum projected density of states was used to interpret the response. We find photoinduced changes reflecting electronic redistribution and local lattice distortions that correspond to strong localization of the self-trapped state.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Excitation correlation photoluminescence in the presence of Shockley-Read-Hall recombination

Excitation correlation photoluminescence (ECPL) measurements are often analyzed in the approximation of a cross correlation of charge carrier populations generated by the two delayed pulses. In semiconductors, this approach is valid for a linear non-radiative recombination path, but not for a non-linear recombination rate as in the general Shockley-Read-Hall recombination scenario. Here, the evolution of the ECPL signal was studied for deep trap recombination following Shockley-Read-Hall statistics. Analytic solutions can be obtained for a fast minority trapping regime and steady state recombination. For the steady state case, our results show that the quadratic radiative term plays only a minor role, and that the shape of the measured signal is mostly determined by the non-linearity of the recombination itself. We find that measurements with unbalanced intense pump and probe pulses can directly provide information about the dominant non-radiative recombination mechanism. The signal traces follow the charge carrier concentrations, despite the complex origins of the signal, thus showing that ECPL can be applied to study charge carrier dynamics in semiconductors without requiring elaborate calculations. The model is compared with measurements on a reference sample with alternating layers of InGaAs/InAlAs that were additionally cross-checked with time resolved optical pump terahertz probe measurements and found to be in excellent agreement.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

VLA Imaging of Protoplanetary Environments

We summarize the major accomplishments of our program to use high angular resolution observations at millimeter wavelengths to probe the structure of protoplanetary disks in nearby regions of star formation. The primary facilities used in this work were the Very Large Array (VLA) of the National Radio Astronomy Observatories (NRAO) located in New Mexico, and the recently upgraded Australia Telescope Compact Array (ATCA), located in Australia (to access sources in the far southern sky). We used these facilities to image thermal emission from dust particles in disks at long millimeter wavelengths, where the emission is optically thin and probes the full disk volume, including the inner regions of planet formation that remain opaque at shorter wavelengths. The best resolution obtained with the VLA is comparable to the size scales of the orbits of giant planets in our Solar System (< 10 AU).

Wilner, David J.↗

Parallel Plate Capacitor Aluminum KIDs for Future Far-Infrared Space-Based Observatories

Future space-based far-infrared astrophysical observatories will require exquisitely sensitive detectors consistent with the low optical backgrounds. The PRobe far-Infrared Mission for Astrophysics (PRIMA) will deploy arrays of thousands of superconducting kinetic inductance detectors (KIDs) sensitive to radiation between 25 and 265 μm. Here, we present laboratory characterization of prototype, 25 – 80 μm wavelength, low-volume, aluminum KIDs designed for the low-background environment expected with PRIMA. A compact parallel plate capacitor is used to minimize the detector footprint and suppress TLS noise. A novel resonant absorber is designed to enhance response in the band of interest. We present noise and optical efficiency measurements of these detectors taken with a low background cryostat and a cryogenic blackbody. A microlens-hybridized KID array is found to be photon noise limited down to about 50 aW with a limiting detector NEP of about 6.5×10 −19 W/Hz 1/2 . A fit to an NEP model shows that our optical system is well characterized and understood down to 50 aW. We discuss future plans for low-volume aluminum KID array development as well as the testbeds used for these measurements.

Far-Infrared↗

An Infrared Database of n/k Optical Constants for Calculating Aerosol Spectra for the PICARD Program

The objective of the PICARD Program is to develop fieldable sensing platforms for the rapid chemical identification of aerosol particles in plumes. Standoff detection involves interrogating the aerosol cloud from a distance using optical methods and probing the signal returned from direct backscattering from the aerosol particles or transmitted through the plume after reflection from a retroreflector or surface of opportunity (SOO). The identification of chemical species, however, in aerosols is complicated by their complex compositions and morphologies, chemical interferants, and non-uniform particle sizes. To advance standoff detection of aerosols, modelling the infrared transmittance, reflectance and scattering spectra of aerosolized liquid and solid chemical compounds is required, and then testing that model experimentally via laboratory and field experiments. To perform accurate modeling, the infrared optical constants (n/k), i.e., the complex refractive index, of the compounds of interest are required. Thus, PNNL was tasked to provide the optical constants for a set of analytes relevant to the PICARD program. This report describes the experimental techniques used to derive the optical constants of both liquid and solid compounds using established “gold-standard” protocols, how the experimental data are processed to produce the wavenumber dependent optical constant vectors, and how the data are used in the aerosol absorption spectra modeling.

complex refractive index↗

Photocurrent Nanoscopy of Quantum Hall Bulk

Understanding nanoscale electronic and thermal transport of two-dimensional (2D) electron systems in the quantum Hall regime, particularly in the bulk insulating state, poses considerable challenges. One of the primary difficulties arises from the presence of chiral edge channels, whose transport behavior obscures the investigation of the insulating bulk. Using near-field optical and photocurrent nanoscopy, we probe real-space variations of the optical and thermal dynamics of graphene in the quantum Hall regime without relying on complex sample or electrode geometries. Near the charge-neutrality point, we detect strong optical and photothermal signals from resonant inter-Landau-level (LL) magnetoexciton excitations between the zeroth and ± 1 st LLs, which gradually weaken with increasing doping due to Pauli blocking. Interestingly, at higher doping levels and full-integer LL fillings, photothermal signals reappear across the entire sample over an approximately 10 − μ m scale, indicating unexpectedly long cooling lengths and nonlocal photothermal heating through the insulating bulk. This observation suggests that thermal conductivity persists for the localized states even as electronic transport is suppressed—a clear violation of the Wiedemann-Franz law. Our experiments provide novel insights into nanoscale thermal and electronic transport in incompressible 2D gases, highlighting the roles of magnetoexcitons and chiral edge states in the thermo-optoelectric dynamics of the Dirac quantum Hall state. Published by the American Physical Society 2025

36 MATERIALS SCIENCE↗

Lyα Profile, Dust, and Prediction of Lyα Escape Fraction in Green Pea Galaxies

We studied Lyman-α (Lyα) escape in a statistical sample of 43 Green Peas with HST/COS Lyα spectra. Green Peas are nearby star-forming galaxies with strong [O iii]λ5007 emission lines. Our sample is four times larger than the previous sample and covers a much more complete range of Green Pea properties. We found that about two-thirds of Green Peas are strong Lyα line emitters with rest-frame Lyα equivalent width >20 A-ring . The Lyα profiles of Green Peas are diverse. The Lyα escape fraction, defined as the ratio of observed Lyα flux to intrinsic Lyα flux, shows anti-correlations with a few Lyα kinematic features—both the blue peak and red peak velocities, the peak separations, and the FWHM of the red portion of the Lyα profile. Using properties measured from Sloan Digital Sky Survey optical spectra, we found many correlations—the Lyα escape fraction generally increases at lower dust reddening, lower metallicity, lower stellar mass, and higher [O iii]/[O ii] ratio. We fit their Lyα profiles with the H i shell radiative transfer model and found that the Lyα escape fraction is anti-correlated with the best-fit N {sub H i}. Finally, we fit an empirical linear relation to predict f{sub esc}{sup Lyα} from the dust extinction and Lyα red peak velocity. The standard deviation of this relation is about 0.3 dex. This relation can be used to isolate the effect of intergalactic medium (IGM) scatterings from Lyα escape and to probe the IGM optical depth along the line of sight of each z>7 Lyα emission-line galaxy in the James Webb Space Telescope era.

79 ASTRONOMY AND ASTROPHYSICS↗

The birth and evolution of solvated electrons in the water

The photo-induced radiolysis of water is an elementary reaction in biology and chemistry, forming solvated electrons, OH radicals, and hydronium cations on fast time scales. Here, we use an optical-pump terahertz-probe spectroscopy setup to trigger the photoionization of water molecules with optical laser pulses at ~400 nm and then time-resolve the transient solvent response with broadband terahertz (THz) fields with a ~90 fs time resolution. We observe three distinct spectral responses. The first is a positive broadband mode that can be attributed to an initial diffuse, delocalized electron with a radius of (22 ± 1) Å, which is short lived (<200 fs) because the absorption is blue-shifting outside of the THz range. The second emerging spectroscopic signature with a lifetime of about 150 ps is attributed to an intermolecular mode associated with a mass rearrangement of solvent molecules due to charge separation of radicals and hydronium cations. After 0.2 ps, we observe a long-lasting THz signature with depleted intensity at 110 cm -1 that is well reproduced by ab initio molecular dynamics. We interpret this negative band at 110 cm -1 as the solvent cage characterized by a weakening of the hydrogen bond network in the first and second hydration shells of the cavity occupied by the localized electron.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Equation of State and Thermometry of the 2D SU ( N ) Fermi-Hubbard Model

We characterize the equation of state (EoS) of the SU ( N > 2 ) Fermi-Hubbard Model (FHM) in a two-dimensional single-layer square optical lattice. We probe the density and the site occupation probabilities as functions of interaction strength and temperature for N = 3 , 4, and 6. Our measurements are used as a benchmark for state-of-the-art numerical methods including determinantal quantum Monte Carlo and numerical linked cluster expansion. By probing the density fluctuations, we compare temperatures determined in a model-independent way by fitting measurements to numerically calculated EoS results, making this a particularly interesting new step in the exploration and characterization of the SU ( N ) FHM. Published by the American Physical Society 2024

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Photonic Doppler velocimetry probe used to measure grain boundaries of dynamic shocked materials

Material scientists have developed computational modeling to predict the dynamic response of materials undergoing stress, but there is still a need to make precision measurements of surfaces undergoing shock compression. Miniature photonic Doppler velocimetry (PDV) probes have been developed to measure the velocity distribution from a moving surface traveling tens of kilometers per second. These probes use hundreds of optical fibers imaged by optical relays onto different regions of this moving surface. While previous work examined large surface areas, we have now developed a PDV microscope that can interrogate 37 different spots within a field of view of <1 mm, with a standoff distance of 17 mm, to analyze the motion differences across grain boundaries of the material undergoing dynamic stress. Each PDV fiber interrogates a 10 μm spot size on the moving surface. A separate imaging system using a coherent bundle records the location of the PDV spots relative to the grain boundaries prior to the dynamic event. Designing the mounting structures for the lenses, fibers, and coherent bundle was a challenge. To minimize back reflections, the fibers are index matched onto the first relay lens, which is made of fused silica. The PDV fibers are aligned normal to the moving surface. The imaging probe views the surface at an 18° angle. The coherent bundle is tilted 11° to its optical relay. All components are assembled into a single probe head assembly. The coherent bundle is removed from the probe head to be used for the next dynamic event. Alignment issues will also be discussed.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

SU-F-J-176: Development of a Patient-Specific 3D Couplant Pad for Ultrasound IGRT

Purpose: to overcome the several issues of ultrasound image-guided radiation therapy (US IGRT) such as probe pressure and optical tracking disability by using a patient-specific three-dimensional couplant pad (CP) fabricated by a patient’s skin mold using a 3D printing technique. Methods: A CP was then fabricated by pouring gelatin solution into a fixed-shape container accommodating the patient skin mold fabricated by a 3D printer. A breast phantom was fabricated with the compound of gelatin and agarose and a phantom study was carried out. From four patients who underwent US IGRT, total 486 ultrasound images with and without a CP were acquired before treatment. Effectiveness of the use of the CP was evaluated. Results: The positioning accuracies in the phantom study were 0.9 ± 0.3 mm and 1.3 ± 0.4 mm with and without the CP in 3D vector amplitude, respectively. In the patient study, the use of CP reduced the mean target shift from 4.7 mm to 3.7 mm in 3D vector amplitude and the one standard deviation from 2.2 mm to 1.7 mm. It also improved the image contrast around the treatment target by 10 %. The centroid offset of the target volume affected from the US scanning coverage and the target deformation due to the excessive probe pressure was decreased from 4.4 mm to 2.9 mm due to the use of CP. Its difference among three different users was statistically significant (p=0.020) without the use of CP but not significantly different (p=0.133) with the use of CP. Conclusion: Our patient-specific 3D CP using a mold by 3D printing technique is a promising strategy for improving tracking accuracy, image quality, and inter-observer variation for ultrasound-based image guided radiotherapy. In addition to its conventional advantage of non-invasiveness, US can be more facilitated in radiotherapy by the developed CP.

60 APPLIED LIFE SCIENCES↗

Ultrafast time-resolved 2D imaging of laser-driven fast electron transport in solid density matter using an x-ray free electron laser

High-power, short-pulse laser-driven fast electrons can rapidly heat and ionize a high-density target before it hydrodynamically expands. The transport of such electrons within a solid target has been studied using two-dimensional (2D) imaging of electron-induced Kα radiation. However, it is currently limited to no or picosecond scale temporal resolutions. Here, we demonstrate femtosecond time-resolved 2D imaging of fast electron transport in a solid copper foil using the SACLA x-ray free electron laser (XFEL). An unfocused collimated x-ray beam produced transmission images with sub-micron and ~10 fs resolutions. The XFEL beam, tuned to its photon energy slightly above the Cu K-edge, enabled 2D imaging of transmission changes induced by electron isochoric heating. Time-resolved measurements obtained by varying the time delay between the x-ray probe and the optical laser show that the signature of the electron-heated region expands at ~25% of the speed of light in a picosecond duration. Time-integrated Cu Kα images support the electron energy and propagation distance observed with the transmission imaging. The x-ray near-edge transmission imaging with a tunable XFEL beam could be broadly applicable for imaging isochorically heated targets by laser-driven relativistic electrons, energetic protons, or an intense x-ray beam.

47 OTHER INSTRUMENTATION↗

Ultrafast carrier dynamics in the large-magnetoresistance material WTe 2

In this study, ultrafast optical pump-probe spectroscopy is used to track carrier dynamics in the large-magnetoresistance material WTe 2 . Our experiments reveal a fast relaxation process occurring on a subpicosecond time scale that is caused by electron-phonon thermalization, allowing us to extract the electron-phonon coupling constant. An additional slower relaxation process, occurring on a time scale of ~5–15 ps, is attributed to phonon-assisted electron-hole recombination. As the temperature decreases from 300 K, the time scale governing this process increases due to the reduction of the phonon population. However, below ~50 K, an unusual decrease of the recombination time sets in, most likely due to a change in the electronic structure that has been linked to the large magnetoresistance observed in this material.

36 MATERIALS SCIENCE↗

Thermal transport across nanoscale damage profile in sapphire irradiated by swift heavy ions

In this work, we studied the degradation of thermal conductivity in single crystal sapphire (α-Al 2 O 3 ) irradiated by 167 MeV Xe swift heavy ions (SHIs) over the multiple fluences in the range of 10 12 –10 14 ions/cm 2 . Thermal conductivity was measured primarily in the cross-plane direction using a noncontact ultrafast optical pump-probe technique called picosecond time domain thermoreflectance (TDTR). Multiple samples with variable ion fluences allowed us to probe distinct regions resulting from different regimes of microstructure evolution caused by electronic energy loss. By tuning the penetration depth of the thermal waves using different modulation frequencies, two regions with distinct conductivities were identified and the values of which were found to be consistent with phonon-mediated thermal transport models while the microstructure was confirmed by electron microscopy characterization. These damaged regions were determined to be a several micrometer thick ion track region and several tens of nanometer-thick amorphous layer present only above 5.0 × 10 13 ions/cm 2 . These results demonstrate the applicability of TDTR to resolve thermal transport behavior in SHI irradiated oxides having nonhomogeneous damage profile on a nanometer scale. The presented approach facilitates future studies aiming at resolving the impact of distinct damage resulting from electronic and nuclear stopping regimes under irradiation.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

The influence of laser power modulation on melt pool dynamics in laser powder bed fusion

While the majority of laser powder bed fusion (LPBF) metal additive manufacturing uses a continuous wave (CW) laser heat source, some commercial applications of LPBF additive manufacturing instead involve the modulation of the laser power on tens-of-microsecond timescales as an adjustable process variable. This article reports the use of in situ, high speed x-ray and optical imaging to probe melt pool fluid flow, defect formation, and nearby powder motion during LPBF with both modulated and CW laser heat sources. We observe melt pool dynamics unique to modulated laser melting even at very high duty cycles that are related to fluctuations in vapor depression depth, complex pore formation mechanisms, and changes to denudation physics when compared to CW melting. These behaviors are present in Ti–6Al–4V, 316L stainless steel, and AL1100 alloys but vary slightly as a function of material, indicating a substantial dependence on the viscosity and surface tension of the liquid metal. While high duty cycles produce weld tracks of comparable quality to CW melting, lower duty cycles introduce substantial defect concentrations. At intermediate duty cycles, careful control of modulation parameters can repeatably and precisely yield one pore per laser pulse, suggesting a method for intentionally inserting engineered porosity at specific sites during an LPBF build.

3D printing↗