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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 19 records

Let There Be Neutrons! Hadronic Photoproduction from a Large Flux of High-energy Photons

We propose that neutrons may be generated in high-energy, high-flux photon environments via photo-induced reactions on pre-existing baryons. These photohadronic interactions are expected to occur in astrophysical jets and surrounding material. Historically, these reactions have been attributed to the production of high-energy cosmic rays and neutrinos. We estimate the photoproduction off of protons in the context of gamma-ray bursts, where it is expected there will be sufficient baryonic material that may be encompassing or entrained in the jet. We show that typical stellar baryonic material, even material completely devoid of neutrons, can become inundated with neutrons in situ via hadronic photoproduction. Consequently, this mechanism provides a means for collapsars and other astrophysical sites containing substantial flux of high-energy photons to be favorable for neutron-capture nucleosynthesis.

79 ASTRONOMY AND ASTROPHYSICS↗

Perovskite CsPbBr 3 Single-Crystal Detector Operating at 10 10 Photons s -1 mm -2 for Ultra-High Flux X-ray Detection

Semiconductors for detecting hard radiation are confronted with considerable problems when operating at high photon fluxes. A perovskite CsPbBr 3 single-crystal detector capable of operating at X-ray fluxes of up to 10 10 photons s -1 mm -2 with beam area ≤ 0.25 mm 2 at 58.61 keV for current-mode X-ray detection is reported. The spectrometer-grade melt-grown CsPbBr 3 detectors show a gamma-ray energy resolution of ~7.5% at 122 keV for 57 Co and dark current as low as 4.3 nA (0.5 nA mm -2 ) at a reverse bias voltage of 200 V (118 V mm -1 ). The detector is tested at X-ray energies of 8.2, 10, and 58.61 keV at a synchrotron light source under a reverse bias voltage of up to 1000 V (588 V mm -1 ). Under a sufficiently high bias voltage and within several hundreds of seconds X-ray exposure, good photocurrent linearity (goodness of fit R 2 > 0.99) and reproducibility are obtained up to a flux of ≈10 10 photons s -1 mm -2 at beam area 0.25 mm 2 with Lower Limit of Detection of ≈10 5 photons s -1 mm -2 and Charge Collection Efficiency of ≈100% for 58.61 keV X-rays. Therefore, wide application of CsPbBr 3 detectors in high-flux X-ray detection is anticipated.

36 MATERIALS SCIENCE↗

Multi-Dimensional Spectroscopy with Intense Entangled Beams: Entanglement-Enabled Phase Matching in a Collinear Beam Geometry

The experimental realization of quantum molecular spectroscopy with entangled photons remains challenging owing to the low signal-to-noise ratio resulting from the use of low-flux entangled photons. High-flux entangled photons via intense entangled beams can be used to improve the signal-to-noise ratio, but the presence of unentangled photons contaminates the quantum signal stemming from entangled photons. Here, we demonstrate how intense entangled beams can be used in multi-dimensional spectroscopy while retaining the advantage of photon entanglement. Our approach is broadly applicable to odd-ordered nonlinear spectroscopies, and it generates purely quantum spectroscopic signals. The proposed approach allows the recording of desired phase-matched signals even in a collinear beam geometry, which lifts the requirement of complicated beam geometry setups for phase matching in multi-dimensional spectroscopies.

Absorption spectroscopy↗

Low Catalyst Loading Enhances Charge Accumulation for Photoelectrochemical Water Splitting

Abstract Solar water oxidation is a critical step in artificial photosynthesis. Successful completion of the process requires four holes and releases four protons. It depends on the consecutive accumulation of charges at the active site. While recent research has shown an obvious dependence of the reaction kinetics on the hole concentrations on the surface of heterogeneous (photo)electrodes, little is known about how the catalyst density impacts the reaction rate. Using atomically dispersed Ir catalysts on hematite, we report a study on how the interplay between the catalyst density and the surface hole concentration influences the reaction kinetics. At low photon flux, where surface hole concentrations are low, faster charge transfer was observed on photoelectrodes with low catalyst density compared to high catalyst density; at high photon flux and high applied potentials, where surface hole concentrations are moderate or high, slower surface charge recombination was afforded by low‐density catalysts. The results support that charge transfer between the light absorber and the catalyst is reversible; they reveal the unexpected benefits of low‐density catalyst loading in facilitating forward charge transfer for desired chemical reactions. It is implied that for practical solar water splitting devices, a suitable catalyst loading is important for maximized performance.

Liu, Tianying↗

Low Catalyst Loading Enhances Charge Accumulation for Photoelectrochemical Water Splitting

Abstract Solar water oxidation is a critical step in artificial photosynthesis. Successful completion of the process requires four holes and releases four protons. It depends on the consecutive accumulation of charges at the active site. While recent research has shown an obvious dependence of the reaction kinetics on the hole concentrations on the surface of heterogeneous (photo)electrodes, little is known about how the catalyst density impacts the reaction rate. Using atomically dispersed Ir catalysts on hematite, we report a study on how the interplay between the catalyst density and the surface hole concentration influences the reaction kinetics. At low photon flux, where surface hole concentrations are low, faster charge transfer was observed on photoelectrodes with low catalyst density compared to high catalyst density; at high photon flux and high applied potentials, where surface hole concentrations are moderate or high, slower surface charge recombination was afforded by low‐density catalysts. The results support that charge transfer between the light absorber and the catalyst is reversible; they reveal the unexpected benefits of low‐density catalyst loading in facilitating forward charge transfer for desired chemical reactions. It is implied that for practical solar water splitting devices, a suitable catalyst loading is important for maximized performance.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Magnetic‐Field‐Switchable Laser via Optical Pumping of Rubrene

Abstract Volumetric optical imaging of magnetic fields is challenging with existing magneto‐optical materials, motivating the search for dyes with strong magnetic field interactions, distinct emission spectra, and an ability to withstand high photon flux and incorporation within samples. Here, the magnetic field effect on singlet‐exciton fission is exploited to demonstrate spatial imaging of magnetic fields in a thin film of rubrene. Doping rubrene with the high‐quantum yield dye dibenzotetraphenylperiflanthene (DBP) is shown to enable optically pumped, slab waveguide lasing. This laser is magnetic‐field‐switchable: when operated just below the lasing threshold, application of a 0.4 T magnetic field switches the device between nonlasing and lasing modes, accompanied by an intensity modulation of +360%. This is thought to be the first demonstration of a magnetically switchable laser, as well as the largest magnetically induced change in emission brightness in a singlet‐fission material to date. These results demonstrate that singlet‐fission materials are promising materials for magnetic sensing applications and could inspire a new class of magneto‐optical modulators.

36 MATERIALS SCIENCE↗

Double diffraction imaging of x-ray induced structural dynamics in single free nanoparticles

Abstract Because of their high photon flux, x-ray free-electron lasers (FEL) allow to resolve the structure of individual nanoparticles via coherent diffractive imaging (CDI) within a single x-ray pulse. Since the inevitable rapid destruction of the sample limits the achievable resolution, a thorough understanding of the spatiotemporal evolution of matter on the nanoscale following the irradiation is crucial. We present a technique to track x-ray induced structural changes in time and space by recording two consecutive diffraction patterns of the same single, free-flying nanoparticle, acquired separately on two large-area detectors opposite to each other, thus examining both the initial and evolved particle structure. We demonstrate the method at the extreme ultraviolet (XUV) and soft x-ray Free-electron LASer in Hamburg (FLASH), investigating xenon clusters as model systems. By splitting a single XUV pulse, two diffraction patterns from the same particle can be obtained. For focus intensities of about 2 × 10 12 W cm −2 we observe still largely intact clusters even at the longest delays of up to 650 picoseconds of the second pulse, indicating that in the highly absorbing systems the damage remains confined to one side of the cluster. Instead, in case of five times higher flux, the diffraction patterns show clear signatures of disintegration, namely increased diameters and density fluctuations in the fragmenting clusters. Future improvements to the accessible range of dynamics and time resolution of the approach are discussed.

Sauppe, M. (ORCID:0000000163123102)↗

Photoinduced correlations in stochastic dynamics of a solid-state ionic conductor

Photoexcitation by ultrashort laser pulses plays a crucial role in controlling reaction pathways, creating nonequilibrium material properties, and probing complex molecular dynamics. The photoresponse following a laser pulse is generally nonidentical between exposures due to spatiotemporal fluctuations or the stochastic nature of dynamical pathways. However, most ultrafast pump-probe experiments struggle to distinguish intrinsic sample fluctuations from extrinsic apparatus noise, often missing deviations from the averaged response. Leveraging the stability and high photon flux of time-resolved X-ray micro-diffraction at a synchrotron, we characterized stochastic photoinduced dynamics in a solid-state ionic conductor. By analyzing temporal evolutions of the lattice parameter of a single grain, we found that shot-to-shot fluctuations are not independent. Instead, correlations exist between nonequilibrium lattice trajectories following adjacent shots, with a characteristic correlation length of approximately 1500 shots, corresponding to an energy barrier of 0.4 ± 0.1 eV, close to the activation energy of lithium-ion diffusion.

36 MATERIALS SCIENCE↗

In situ X-ray area detector flat-field correction at an operating photon energy without flat illumination

Flat-field calibration of X-ray area detectors is a challenge due to the inability to generate an X-ray flat-field at the selected photon energy the beamline operates at, which has a strong influence on the measurement behavior of the detector. A method is presented in which a simulated flat-field correction is calculated without flat-field measurements. Instead, a series of quick scattering measurements from an amorphous scatterer is used to calculate a flat-field response. The ability to rapidly obtain a flat-field response allows for recalibration of an X-ray detector as needed without significant expenditure of either time or effort. Area detectors on the beamlines used, such as the Pilatus 2M CdTe, PE XRD1621 and Varex XRD 4343CT, were found to have detector responses that drift slightly over timescales of several weeks or after exposure to high photon flux, suggesting the need to more frequently recalibrate with a new flat-field correction map.

47 OTHER INSTRUMENTATION↗

Simple steps to enable reproducibility: culture conditions affecting Chlamydomonas growth and elemental composition

Even subtle modifications in growth conditions elicit acclimation responses affecting the molecular and elemental makeup of organisms, both in the laboratory and in natural habitats. Here, we systematically explored the effect of temperature, pH, nutrient availability, culture density, and access to CO 2 and O 2 in laboratory-grown algal cultures on growth rate, the ionome, and the ability to accumulate Fe. We found algal cells accumulate Fe in alkaline conditions, even more so when excess Fe is present, coinciding with a reduced growth rate. Using a combination of Fe-specific dyes, X-ray fluorescence microscopy, and NanoSIMS, we show that the alkaline-accumulated Fe was intracellularly sequestered into acidocalcisomes, which are localized towards the periphery of the cells. At high photon flux densities, Zn and Ca specifically over-accumulate, while Zn alone accumulates at low temperatures. The impact of aeration was probed by reducing shaking speeds and changing vessel fill levels; the former increased the Cu quota of cultures, the latter resulted in a reduction in P, Ca, and Mn at low fill levels. Trace element quotas were also affected in the stationary phase, where specifically Fe, Cu, and Zn accumulate. Cu accumulation here depends inversely on the Fe concentration of the medium. Individual laboratory strains accumulate Ca, P, and Cu to different levels. All together, we identified a set of specific changes to growth rate, elemental composition, and the capacity to store Fe in response to subtle differences in culturing conditions of Chlamydomonas, affecting experimental reproducibility. Accordingly, we recommend that these variables be recorded and reported as associated metadata.

59 BASIC BIOLOGICAL SCIENCES↗

Short pulsewidth high repetition rate nanosecond transient absorption spectrometer

A high-sensitivity nanosecond to millisecond transient absorption spectrometer for measurements of miniscule signals under low excitation intensities includes an excitation source generating a >100 Hz, <5 ns pulsewidth excitation pulse for exciting a light absorbing sample, a probe light source for generating a high photon flux probe light beam producing an average irradiance greater than 1 μW m-2 nm-1 for measuring the transient absorption spectrum of the sample before and after excitation by the excitation source, a DC-coupled detector capable of measuring light for enabling synchronous measurement of both the transmission of the probe light beam and the change in transmission of the probe light beam between a signal with the excitation pulse present and a signal in the absence of the excitation pulse, and a digital oscilloscope with a trigger rearm time capable of collecting every trigger event at frequencies including 1MHz, for enabling sequential noise subtraction protocols.

Rimshaw, Adam↗

Characterization of lateral amorphous selenium photodetectors for low-photon and VUV detection at cryogenic temperatures

The performance of amorphous selenium (a-Se) as a cryogenic photodetector material is evaluated through a series of experiments using laterally structured devices operated in a custom optical test stand. These studies investigate the response of a-Se detectors to low-photon fluxes at high electric fields near avalanche conditions, the linearity of the photoconductive response over a wide dynamic range and the direct detection of narrowband 130 nm vacuum ultraviolet (VUV) illumination. At 87 K, matched-filter analysis shows reliable single-shot detection with efficiencies ≥80% and area under the curve (AUC) ≥ 0.85 using as few as ∼ 6800 incident 401 nm photons, corresponding to ∼ 3400 photons within field-active regions after accounting for geometric constraints. Measurements are performed at cryogenic temperatures using calibrated photon fluxes derived from a silicon photomultiplier reference and a characterized optical filter stack. Additional experiments using a tellurium-doped a-Se (a-SeTe) device explore the material's behavior under identical test conditions and demonstrate that avalanche is achievable in a-SeTe at cryogenic temperatures. The results demonstrate reproducible low-noise operation, VUV sensitivity and field-dependent gain behavior in a lateral a-Se architecture, representing the first reported observation of avalanche multiplication in laterally structured a-Se and a-SeTe devices at cryogenic temperatures. These findings support the potential integration of laterally structured a-Se devices into next-generation pixelated liquid-argon time projection chambers (TPCs) requiring scalable, high-field-compatible photon detection systems.

Amorphous selenium↗

Characterization of Lateral Amorphous Selenium Photodetectors for Low-Photon and VUV Detection at Cryogenic Temperatures

The performance of amorphous selenium (a-Se) as a cryogenic photodetector material is evaluated through a series of experiments using laterally structured devices operated in a custom optical test stand. These studies investigate the response of a-Se detectors to low-photon fluxes at high electric fields near avalanche conditions, the linearity of the photoconductive response over a wide dynamic range and the direct detection of narrowband 130 nm vacuum ultraviolet (VUV) illumination. At 87 K, matched-filter analysis shows reliable single-shot detection with efficiencies greater than or equal to 80 percent and area under the curve (AUC) greater than or equal to 0.85 using as few as approximately 6800 incident 401 nm photons, corresponding to approximately 3400 photons within field-active regions after accounting for geometric constraints. Measurements are performed at cryogenic temperatures using calibrated photon fluxes derived from a silicon photomultiplier reference and a characterized optical filter stack. Additional experiments using a tellurium-doped a-Se (a-SeTe) device explore the material's behavior under identical test conditions and demonstrate that avalanche is achievable in a-SeTe at cryogenic temperatures. The results demonstrate reproducible low-noise operation, VUV sensitivity and field-dependent gain behavior in a lateral a-Se architecture, representing the first reported observation of avalanche multiplication in laterally structured a-Se and a-SeTe devices at cryogenic temperatures. These findings support the potential integration of laterally structured a-Se devices into next-generation pixelated liquid-argon time projection chambers (TPCs) requiring scalable, high-field-compatible photon detection systems.

FOS: Physical sciences↗

An Artificial Neural Network System for Photon-Based Active Interrogation Applications

Active interrogation (AI) is a promising technique to detect shielded special nuclear materials (SNMs). At the University of Michigan, we are developing a photon-based AI system that uses bremsstrahlung radiation from an electron linear accelerator (linac) as an ionizing source and stilbene organic scintillating detectors for neutron detection. Stilbene scintillators are sensitive to fast neutrons and photons and have excellent pulse shape discrimination (PSD) capabilities. The traditional charge integration (CI) method commonly used for PSD analysis eliminates piled-up pulses and relies on a particle discrimination line to separate neutrons and photons. The presence of the intense photon flux during AI creates a significant number of piled-up events in the stilbene scintillator, thereby posing a great challenge to the traditional CI method. Identifying true single neutron pulses becomes challenging due to the presence of a pile-up cloud and overlapping neutron, photon and pile-up clouds in the PSD analysis. To mitigate the effect of pulse pile up and identify true single neutron pulses from stilbene scintillators, an artificial neural network (ANN) system is developed. The developed ANN system identifies single neutron pulses and neutron-photon combinations from piled-up events. The results obtained from a 252Cf measurement in the presence of the intense photon flux show that the developed ANN system outperforms the traditional CI method. Since many piled-up events lie above the particle discrimination line, they get misclassified as neutrons by the traditional CI method resulting in 25% overestimation of the net neutron count rate during the linac pulse. The overall net neutron count rate (single and restored neutrons) during the linac pulse, estimated by the ANN system is 60% of the ground truth. Energy spectroscopy of the ANN attributed single neutron pulses further provides evidence on the detection of prompt fission neutrons from the 252Cf fission source.

42 ENGINEERING↗

Attosecond intra-valence band dynamics and resonant-photoemission delays in W(110)

Time-resolved photoelectron spectroscopy with attosecond precision provides new insights into the photoelectric effect and gives information about the timing of photoemission from different electronic states within the electronic band structure of solids. Electron transport, scattering phenomena and electron-electron correlation effects can be observed on attosecond time scales by timing photoemission from valence band states against that from core states. However, accessing intraband effects was so far particularly challenging due to the simultaneous requirements on energy, momentum and time resolution. Here we report on an experiment utilizing intracavity generated attosecond pulse trains to meet these demands at high flux and high photon energies to measure intraband delays between sp- and d- band states in the valence band photoemission from tungsten and investigate final-state effects in resonant photoemission.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Integration of physiologically relevant photosynthetic energy flows into whole genome models of light‐driven metabolism

SUMMARY Characterizing photosynthetic productivity is necessary to understand the ecological contributions and biotechnology potential of plants, algae, and cyanobacteria. Light capture efficiency and photophysiology have long been characterized by measurements of chlorophyll fluorescence dynamics. However, these investigations typically do not consider the metabolic network downstream of light harvesting. By contrast, genome‐scale metabolic models capture species‐specific metabolic capabilities but have yet to incorporate the rapid regulation of the light harvesting apparatus. Here, we combine chlorophyll fluorescence parameters defining photosynthetic and non‐photosynthetic yield of absorbed light energy with a metabolic model of the pennate diatom Phaeodactylum tricornutum. This integration increases the model predictive accuracy regarding growth rate, intracellular oxygen production and consumption, and metabolic pathway usage. Through the quantification of excess electron transport, we uncover the sequential activation of non‐radiative energy dissipation processes, cross‐compartment electron shuttling, and non‐photochemical quenching as the rapid photoacclimation strategy in P. tricornutum. Interestingly, the photon absorption thresholds that trigger the transition between these mechanisms were consistent at low and high incident photon fluxes. We use this understanding to explore engineering strategies for rerouting cellular resources and excess light energy towards bioproducts in silico . Overall, we present a methodology for incorporating a common, informative data type into computational models of light‐driven metabolism and show its utilization within the design–build–test–learn cycle for engineering of photosynthetic organisms.

59 BASIC BIOLOGICAL SCIENCES↗

Characterization of a Small-Scale Prototype Detector With Wide Dynamic Range for Time-Resolved High-Energy X-Ray Applications

We present characterization measurements of a fast-framing, wide-dynamic-range x-ray area detector intended for high-energy applications (≥20 keV photons). The MM-PAD-2.1 combines an integrating pixel front-end with a charge-removal mechanism to extend the maximum measurable signal to > 107 20-keV ph/pixel/frame. The charge-removal mechanism is dead-time-less (i.e., incoming signal continues to be integrated by the front-end while charge removal is taking place) up to an incoming photon rate of > 109 20-keV ph/pix/s. A 16×16 pixel prototype was fabricated and characterized using both laboratory and synchrotron x-ray sources, allowing for measurements from single-photon to high-flux conditions. High-flux measurements show linear performance up to ~1010 ph/s in a spot spanning approximately 2×1.5 pixels (FWHM). The onset of temporary radiation damage in the detector was observed during these measurements, manifesting as failure of the digital readout from the detector. These effects were seen to reverse after annealing at 30° C for several hours.

47 OTHER INSTRUMENTATION↗

New constraints on the dark matter-neutrino and dark matter-photon scattering cross sections from TXS 0506+056

The flux of high energy neutrinos and photons produced in a blazar could get attenuated when they propagate through the dark matter spike around the central black hole and the halo of the host galaxy. Using the observation by IceCube of a few high-energy neutrino events from TXS 0506+056, and their coincident gamma ray events, we obtain new constraints on the dark matter-neutrino and dark matter-photon scattering cross sections. Our constraints are orders of magnitude more stringent than those derived from considering the attenuation through the intergalactic medium and the Milky Way dark matter halo. When the cross-section increases with energy, our constraints are also stronger than those derived from the CMB and large-scale structure.

79 ASTRONOMY AND ASTROPHYSICS↗