Research in the development effort of an improved multiplier phototube Seventh quarterly report
Test data on effective photocathode size, response uniformity, and pulse amplitude distribution of multiplier phototubes
PHOTOMULTIPLIER↗
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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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Two Artificial Leaf Architectures for Solar Formate Production From CO 2 and H 2 O
Sunlight-powered artificial leaves for the production of formate from CO 2 are an attractive route to solar fuels, yet existing solar formate devices remain low in performance, and their architecture and material choices are underexplored. Herein, we report the fabrication of two distinct fully integrated, self-standing solar formate device architectures and elucidate the underlying design principles and material selection strategies. The first architecture integrates a Si photocathode with a BiVO 4 photoanode and utilizes a highly active Pd catalyst for CO 2 reduction. It represents the first artificial leaf device comprising two photoelectrodes (excluding photovoltaic [PV]-biased electrodes) for effective formate production under single-beam illumination. The second architecture employs a dark cathode and a dark anode driven by a 4-junction perovskite solar cell and uses a highly stable Bi catalyst for CO 2 reduction. This device delivers a record-high formate production rate of 174 µmol h −1 with a remarkable solar-to-formate energy efficiency of 2% among all artificial leaf devices reported to date. Finally, these results demonstrate the feasibility and outline the design principles of both PV-free and PV-assisted device architectures in solar fuel production.
electrocatalysis↗
Formation of tunable diamond micro- and nanopillars for field effect enhancement applications
Here, we developed a process for the fabrication of tunable single crystal diamond micro- and nanopillars, with tip widths ranging from 40 to 460 nm, densities ranging from 0.5 to 53.5 pillars/μm 2 , and heights greater than 4.5 μm. A self-assembled Au nanodot ensemble etch mask was formed from an annealed Au thin film. The nanodot diameter and density can be tuned using the initial film thickness. The pillars were etched from the nanodot mask using an RIE O 2 plasma, which has infinite selectivity for the diamond when applied at low RF powers (50 W). Finally, the pillars can be sharpened to ~40 nm tip widths by annealing in air at 650 °C. These pillars can be used for applications such as field effect enhancement of diamond photocathode devices, enhancement of optical emission from N-V centers, and antireflective coatings.
36 MATERIALS SCIENCE↗
Single channel PICOSEC Micromegas detector with improved time resolution
This paper presents design guidelines and the experimental verification of a single-channel PICOSEC Micromegas (MM) detector with an improved time resolution. The design encompasses the detector board, vessel, auxiliary mechanical parts, and electrical connectivity for high voltage (HV) and signals, focusing on improving the stability, reducing noise, and ensuring signal integrity to optimize timing performance. A notable feature is the simple and fast reassembly procedure, facilitating quick replacement of the detector internal components that allows for an efficient measurement strategy involving different detector components. The paper also examines the influence of parasitic capacitance and inductance on the output signal integrity. To validate the design, a prototype assembly and three interchangeable detector boards with varying readout pad diameters were manufactured. Detectors were initially tested in the laboratory. Finally, the timing performance of the detectors with different pad sizes was verified using 150 GeV muons. Notably, a record time resolution for a PICOSEC Micromegas detector technology with a CsI photocathode of 12.5 ± 0.8 ps was achieved for a detector with 10 mm diameter readout pad size.
46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗
WO 3 /CuWO 4 Ratio Controls Open-Circuit Photovoltage and Photocurrent in Type II Heterojunction Solar Fuel Photoelectrodes
WO 3 /CuWO 4 photoelectrodes for the oxygen evolution reaction benefit from a type II heterojunction for charge separation. However, the impact of the WO 3 /CuWO 4 ratio on the photocurrent and the photovoltage is not clear. To probe the effect of composition, Cu x W 1-x O y thin films with variable W:Cu ratio were prepared on FTO by reactive magnetron co-sputtering of W and Cu, followed by air annealing at 500ºC. EDS, XRD, Rietveld refinement, and Raman spectroscopy confirm the presence of crystalline WO 3 and CuWO 4 in the W rich films and increasing amounts of amorphous copper oxides in the Cu rich films. Bandgaps were determined by optical absorption spectroscopy, surface photovoltage spectroscopy (SPS), and photoaction spectra and are found to decrease from 2.7 eV to 1.2 eV with increasing copper oxide content. SPS reveals n-type semiconductor photoanode behavior for WO 3 /CuWO 4 samples and p-type photocathode behavior for CuO x rich films. Photoelectrochemical experiments confirm stable water oxidation with Faraday efficiency near unity for all W rich films and photocurrents that are increasing with CuWO 4 content. Optimal performance is seen for WO 3 /CuWO 4 mixed phases containing 47-75 mass% CuWO 4 . These compositions maximize charge separation at the type II heterojunction interface between the two materials. Additionally, according to incident photon to current efficiency (IPCE) data, the WO 3 improves photon conversion below 350 nm, while CuWO 4 improves conversion at 450-525 nm. Overall, this work shows for the first time how the WO 3 /CuWO 4 ratio controls the photovoltage and the photocurrent in type II heterojunction solar fuel photoelectrodes, and how copper oxides in the copper rich films severely degrade the performance. Furthermore, these results are useful in the context of bulk-heterojunction electrodes for the conversion of solar energy into fuels.
CuWO4↗
A Vibrational Probe of Electrical Doping in N2200 and Fermi-Level Alignment at Polymer Cathode/Metal Cocatalyst/Electrolyte Junctions
Hybrid (photo)cathodes consisting of conjugated polymer and hydrogen evolution reaction (HER) cocatalysts are an emerging platform for low-cost solar fuel generation. Poly{[N,N′-bis(2-octyldodecyl)-naphthalene-1,4,5,8-bis(dicarboximide)-2,6-diyl]-alt-5,5′-(2,2′-bithiophene)}, known as P(NDI2OD-T2) or N2200, is a promising electron accepting material for bulk heterojunction photocathodes. Unlike inorganic (photo)electrodes, much less is known about the energetic alignment of conjugated polymer electrode/metal/electrolyte junctions. Here, in this work, we investigate the electrical doping behavior in an N2200 cathode and its Fermi-level alignment with gold nanoparticles, which is used here as a model for the hydrogen evolution metal cocatalyst. Through UV/visible, Raman, and attenuated total-reflectance infrared spectroelectrochemistry, we observe the impact of electrical doping on the vibrational frequencies of neutral, anion, and dianion species in N2200, which suggests that electron density changes within the corresponding naphthalene-diimide (NDI) units. Upon one-electron reduction, the $C=O$ stretching frequency of the NDI anion unit (polaron) shows a red shift by ∼ 68 cm –1 . Additionally, the $C=O$ stretching frequency of neutral units in the doped N2200 shows a minor red shift of ∼ 5 cm –1 , suggesting charge transfer from neighboring polaron units. Surface-enhanced Raman spectroscopy measurements of a gold nanoparticle-functionalized N2200 electrode revealed that the Au Fermi level only shifts with that of N2200 upon polaron formation; thus, the formal potential of polymer polaron formation determines the behavior of the catalyst Fermi level, which we posit will modulate reaction capability. This mechanistic study provides a new approach for understanding the nanometer-scale energetics at the conjugated polymer/cocatalyst junction and provides critical insights for the future design of HER (photo)cathodes.
charge transfer↗
Solar-driven selective conversion of millimolar dissolved carbon to fuels with molecular flux generation
Abstract The direct utilization of dissolved inorganic carbon in seawater for CO 2 conversion promises chemical production on-demand and with zero carbon footprint. Photoelectrochemical (PEC) CO 2 reduction (CO 2 R) devices promise the sustainable conversion of dissolved carbon in seawater to carbon products using sunlight as the only energy input. However, the diffusion-dominant transport mechanism and the near-zero concentration of CO 2 (aq) (CO 2 dissolved in aqueous solution) in static seawater has made it extremely challenging to achieve high solar-to-fuel (STF) efficiency and high carbon-product selectivity. Here, where CO 2 (aq) as a reactant generated in situ by acidification of HCO 3 - flows continuously from BiVO 4 photoanodes to Si photocathodes, enabling a single-step conversion of dissolved carbon into products. Our PEC device significantly increases the CO selectivity from 3% to 21%, which approaches the 30% theoretical limit according to multi-physics modeling. Meanwhile, the Si/BiVO 4 PEC CO 2 R device achieved a STF efficiency of 0.71%. Such flow engineering achieves flow-dependent selectivity, rate, and stability in simulated seawater, thus promising practical solar fuel production at scale.
Liu, Bin↗
Atomic doping to enhance the p-type behavior of BiFeO 3 photoelectrodes for solar H 2 O 2 production
Na-doped BiFeO 3 demonstrates an enhanced p-type behavior compared to p-type BiFeO 3 prepared without extrinsic dopants, and Na-doped BiFeO 3 can serve as a photocathode for solar O 2 reduction to H 2 O 2 when coupled with Ag nanoparticle catalysts.
Seo, Daye↗
Photosynthesis of CO from CO 2 with an iron polypyridyl catalyst at a passivated silicon photoelectrode
A first-row transition metal catalyst, [Fe(tpy)(Mebim-py)(NCCH 3 )] 2+ (tpy = 2,2′:6′,2′′-terpyridine, Mebim-py = 1-methylbenzimidazol-2-ylidene-3-(2′-pyridine)) mediates CO 2 reduction to CO at passivated p-Si photoelectrodes with applied potentials 240 mV positive of the standard CO 2 /CO reduction potential. The molecular catalyst's selectivity for CO was retained under photoelectrochemical conditions, with negligible direct proton reduction promoted by the photoelectrode. The faradaic efficiency for CO (44 ± 6%) was slightly enhanced relative to the catalyst performance in the dark (33%). A photosynthetic cell based on this photocathode system, coupled with ferrocene oxidation at the anode, successfully operated at a cell voltage of −1.2 V. The photovoltage generated by illumination of p-Si–CH 3 met and surpassed the potential required for CO 2 reduction when coupled with ferrocene oxidation. By leveraging a low-overpotential CO 2 reduction electrocatalyst, a photo-assisted electrochemical efficiency of 0.15% and applied bias photon-to-current efficiency of 0.05% was achieved for this single-junction cell, ultimately storing 46 kJ mol −1 (11 kcal mol −1 ) of photon energy.
Carbon Dioxide Reduction↗
First operation of a multi-channel Q-Pix prototype: measuring transverse electron diffusion in a gas time projection chamber
We report measurements of the transverse diffusion of electrons in P-10 gas (90% Ar, 10% CH 4 ) in a laboratory-scale time projection chamber (TPC) utilizing a novel pixelated signal capture and digitization technique known as Q-Pix. The Q-Pix method incorporates a precision switched integrating transimpedance amplifier whose output is compared to a threshold voltage. Upon reaching the threshold, a comparator sends a 'reset' signal, initiating a discharge of the integrating capacitor. The time difference between successive resets is inversely proportional to the average current at the pixel in that time interval, and the number of resets is directly proportional to the total collected charge. We developed a 16-channel Q-Pix prototype fabricated from commercial off-the-shelf components and coupled them to 16 concentric annular anode electrodes to measure the spatial extent of the electron swarm that reaches the anode after drifting through the uniform field of the TPC. The swarm is produced at a gold photocathode using pulsed UV light. The measured transverse diffusion agrees with simulations in PyBoltz across a range of operating pressures (200–1500 Torr). These results demonstrate that a Q-Pix readout can successfully reconstruct the ionization topology in a TPC.
47 OTHER INSTRUMENTATION↗
Advances in the Large Area Picosecond Photo-Detector (LAPPD TM ): 8" × 8" MCP-PMT with Capacitively Coupled Readout
Abstract We present advances made in the Large Area Picosecond Photodetector (LAPPD), an 8" × 8" microchannel plate photomultiplier tube (MCP-PMT), since pilot production was initiated at Incom, Inc. in 2018. The Gen-I LAPPD utilizes a stripline anode for direct charge readout. The novel Gen-II LAPPD employs an internal resistive thin-film which capacitively couples to a customizable external signal readout board, streamlining production and increasing customer flexibility. The Gen-II LAPPD, with an active area of 373 cm 2 , is capable of high single photoelectron (PE) gain of ∼10 7 , low dark rates (∼1 kHz/cm 2 ), single PE (SPE) timing resolution of ∼65 ps, and 𝒪(mm) position resolution. Coupled with a UV-grade fused silica window, the LAPPD features a high quantum efficiency (QE) bialkali photocathode of >30% at 365 nm with spectral response down to ∼165 nm. The LAPPD is an excellent candidate for electromagnetic calorimeter (ECAL) timing layers, photon-based neutrino detectors, high energy collider experiments, medical imaging systems, and nuclear non-proliferation applications.
Instruments & Instrumentation↗
Measurement of the liquid argon scintillation pulse shape using differentiable simulation in the coherent CAPTAIN-Mills experiment
The coherent CAPTAIN-Mills (CCM) experiment is a liquid argon (LAr) light collection detector searching for MeV-scale neutrino and beyond Standard Model physics signatures. Two hundred eight-inch photomultiplier tubes instrument the seven-ton fiducial volume with 50% photocathode coverage to detect light produced by charged particles. CCM’s light-based approach reduces requirements of LAr purity, compared to other detection technologies, such that sub-MeV particles can be reliably detected without additional LAr filtration and with 𝒪(1) parts per million of common contaminants. We present a measurement of LAr light production and propagation parameters, with uncertainties, obtained from a sample of MeV-scale electromagnetic events. The optimization of this high-dimensional parameter space was facilitated by a differentiable optical photon Monte Carlo simulation and detailed photomultiplier tube response characterization. This result accurately predicts the timing and spatial distribution of light due to scintillation and Cherenkov emission in the detector. This is the first description of photon propagation in LAr to include several effects, including anomalous dispersion of the index of refraction near the ultraviolet resonance, Mie scattering from impurities, and Cherenkov light production.
Cherenkov detectors↗
Tomography of longitudinal phase space linearization for the generation of attosecond electron bunches
The generation of electron bunches on the attosecond timescale is important for a multitude of accelerator-based applications. Here, we report on a tomographic measurement of the (pre)linearized longitudinal phase space of a low charge 3 MeV electron bunch generated with the 1.6 cell Pegasus photoinjector for the generation of attosecond bunches. The nonlinear correlations in the longitudinal phase space induced by space charge at the photocathode, radiofrequency field curvature of the gun, and vacuum dispersion are compensated using a compact X-band linearizer. Then, the initial and compensated phase of the picosecond electron bunch is precisely reconstructed by neural network assisted tomographic reconstruction from momentum spectra at varying buncher linac phase. Finally, we combine the measured phase space shape with particle tracking simulations to show that electron bunches as short as 941 as develop downstream the beamline.
Beam control↗
Modeling betatron radiation using particle-in-cell codes for plasma wakefield accelerator diagnostics
The analysis of plasma wakefield acceleration experimental measurements, particularly in the characterization of photons emitted through the betatron radiation mechanism, requires the development of accurate numerical models. These computational models are crucial for supporting modern instrumentation designed to measure the single-shot, double-differential angular-energy radiation spectra resulting from interactions between beams and plasmas. Motivated by the needs of such applications, this paper presents detailed numerical models of betatron radiation generated in beam-plasma acceleration experiments. These models are based on the integration of the Liénard-Wiechert (LW) potentials, applied to computed particle trajectories. The particle trajectories are generated using three distinct methods: first, by tracking particles through idealized fields in the blowout regime of PWFA; second, by obtaining trajectories using the fast quasistatic particle-in-cell (PIC) code quickpic; and third, obtaining trajectories from the fully self-consistent PIC code osiris. To ensure the accuracy and reliability of these models, the paper includes various benchmark tests using analytical expressions, as well as employing the PIC code epoch, which takes an alternative approach by using a Monte Carlo quantum electrodynamics (QED)-based radiation model. Additionally, the paper presents simulations of the expected experimental betatron radiation spectra, taking into account parameters relevant to PWFA and plasma photocathode experiments at the SLAC FACET-II facility.
Yadav, M. [University of California, Los Angeles, ↗
Deep learning-assisted modeling for χ (2) nonlinear optics
Modeling second-order (χ(2)) nonlinear optical processes remains computationally expensive due to the need to resolve fast field oscillations and simulate wave propagation using methods such as the split-step Fourier method (SSFM). This can become a bottleneck in real-time applications, such as high-repetition-rate laser systems requiring rapid feedback and control. We present a long short-term memory-based surrogate model trained on SSFM simulations generated from a start-to-end model of the photocathode drive laser at SLAC National Accelerator Laboratory’s Linac Coherent Light Source II. The model achieves over 250× speedup while maintaining high fidelity, enabling future real-time optimization and laying the foundation for data-integrated modeling frameworks and digital twins of laser systems.
Accelerator Physics (physics.acc-ph)↗
Time-resolved detectors for quantum ghost imaging
Quantum ghost imaging is a method that utilizes the correlated detection of two photons to generate an image. One photon is detected by an imaging sensor and the other by a single-element bucket detector. The selection of the imaging sensor and its capabilities relative to the bucket detector impact the quality of the ghost images. This work examines a SPAD array and a photocathode detector as imaging sensors for quantum ghost imaging. We discuss how to achieve optimal images using these two technologies. We also demonstrate that these devices are able to generate ghost images at 1Hz frame rates, expanding the technique to biologically relevant time scales.
36 MATERIALS SCIENCE↗
New Materials for Photoelectrochemical Energy Conversion
This review concerns light-to-chemical energy conversion, focusing on approaches that could be driven by terrestrial sunlight to produce hydrogen and/or reduce carbon dioxide. Recent advances in photocatalytic (PC) and photoelectrocatalytic (PEC) materials are covered. In both approaches, the electron-hole pairs that are created by photon absorption must travel in specific directions to the sites that mediate multielectron bond making/breaking redox reactions. Thermodynamic requirements for materials stability are described, although some recently discovered materials appear to be exceptions. For PC materials, the importance of rate matching between reduction and oxidation processes and the mass transfer of intermediates and products is emphasized. Surprisingly, metal sulfides appear to be promising for PC carbon dioxide reduction. For PEC materials, recent work elucidating the elementary step mechanism for oxygen evolution on metal oxides and the discovery of chalcogen-based photocathode materials capable of sustained light-driven CO 2 reduction are discussed.
energy conversion↗
Optically Stimulated Luminescence Data Storage (Abstract)
We will develop a tunable pulsed electron source capable of generating variable intensity highly-focused electron pulses at high repetition rates. Specifically, we need to demonstrate a high-speed variable electron gun capable of generating a variable intensity electron pulse containing between 102 and 105 electrons with an accelerating voltage of 1kV focused into a spot size <100nm in diameter at with a pulse rate >10MHz (with path to 300MHz). This combined performance cannot be achieved by commercially available electron sources. The primary technology path selected for this work will be to use a photocathode approach, where an easily modulated UV laser is used to stimulate electron emission. The approach utilizes the advances made in the development of the Dynamic TEM (DTEM), though this project will be simpler in that the pulse intensity is lower and there is no requirement for coherency. Alternate paths, including using a traditional electron beam modulated using a v-shaped slit and electrostatically deflecting the beam to adjust intensity; will also be considered for future capabilities. The electron source will then be used generate optically stimulated luminescence (OSL) in lithium fluoride (LiF) substrates to demonstrate the potential for OSL to serve as a basis technology for next generation data storage systems.
42 ENGINEERING↗