Visualizing lattice dynamic behavior by acquiring a single time-resolved MeV diffraction image
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99 GENERAL AND MISCELLANEOUS↗
SEARCH · Engineering Papers
Results for “photocathode”
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Enhancement of Photoemission on p-Type GaAs Using Surface Acoustic Waves
We demonstrate that photoemission properties of p-type GaAs can be altered by surface acoustic waves (SAWs) generated on the GaAs surface due to dynamical piezoelectric fields of SAWs. Multiphysics simulations indicate that charge-carrier recombination is greatly reduced, and electron effective lifetime in p-doped GaAs may increase by a factor of 10× to 20×. It implies a significant increase, by a factor of 2× to 3×, of quantum efficiency (QE) for GaAs photoemission applications, like GaAs photocathodes. Conditions of different SAW wavelengths, swept SAW intensities, and varied incident photon energies were investigated. Essential steps in SAW device fabrication on a GaAs substrate are demonstrated, including deposition of an additional layer of ZnO for piezoelectric effect enhancement, measurements of current–voltage (I–V) characteristics of the SAW device, and ability to survive high-temperature annealing. Results obtained and reported in this study provide the potential and basis for future studies on building SAW-enhanced photocathodes, as well as other GaAs photoelectric applications.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
Integrated Solar-Driven Device with a Front Surface Semitransparent Catalysts for Unassisted CO 2 Reduction
Monolithic integrated photovoltaic-driven electrochemical (PV-EC) artificial photosynthesis is reported for unassisted CO 2 reduction. The PV-EC structures employ triple junction photoelectrodes with a front mounted semitransparent catalyst layer as a photocathode. The catalyst layer is comprised of an array of microscale triangular metallic prisms that redirect incoming light toward open areas of the photoelectrode to reduce shadow losses. Full wave electromagnetic simulations of the prism array (PA) structure guide optimization of geometries and length scales. An integrated device is constructed with Ag catalyst prisms covering 35% of the surface area. The experimental device has close to 80% of the transmittance with a catalytic surface area equivalent 144% of the glass substrate area. Experimentally this photocathode demonstrates a direct solar-to-CO conversion efficiency of 5.9% with 50 h stability. Selective electrodeposition of Cu catalysts onto the surface of the Ag triangular prisms allows CO2 conversion to higher value products enabling demonstration of a solar-to-C 2+ product efficiency of 3.1%. This design featuring structures that have a semitransparent catalyst layer on a PV-EC cell is a general solution to light loss by shadowing for front surface mounted metal catalysts, and opens a route for the development of artificial photosynthesis based on this scalable design approach.
14 SOLAR ENERGY↗
Copper Tantalate by a Sodium-Driven Flux-Mediated Synthesis for Photoelectrochemical CO 2 Reduction
Copper-tantalate, Cu 2 Ta 4 O 11 (CTO), shows significant promise as an efficient photocathode for multi-carbon compounds (C 2+ ) production through photoelectrochemical (PEC) CO 2 reduction, owing to its suitable energy bands and catalytic surface. However, synthesizing CTO poses a significant challenge due to its metastable nature and thermal instability. In this study, this challenge is addressed by employing a flux-mediated synthesis technique using a sodium-based flux to create sodium-doped CTO (Na-CTO) thin films, providing enhanced nucleation and stabilization for the CTO phase. To evaluate the PEC performance and catalytic properties of the films, copper(II) oxide (CuO) at the Na-CTO surface is selectively etched. The etched Na-CTO shows a lower dark current, with decreased contribution from photocorrosion, unlike the non-etched Na-CTO which has remaining CuO on the surface. Furthermore, Na-CTO exhibits 7.3-fold ethylene selectivity over hydrogen, thus highlighting its promising potential as a photocathode for C 2+ production through PEC CO 2 reduction.
copper tantalate↗
Sub-25 ps timing measurements with 10 × 10 cm 2 PICOSEC Micromegas detectors
The PICOSEC Micromegas detector is a precise timing gaseous detector based on a Cherenkov radiator coupled to a semi-transparent photocathode and a Micromegas amplifying structure. First single-pad prototypes demonstrated a time resolution below σ = 25 ps, however, to make the concept appropriate to physics applications, several developments are required. The objective of this work was to achieve an equivalent time resolution for a 10 × 10 cm 2 area PICOSEC Micromegas detector. The prototype was designed, produced and tested in the laboratory and successfully operated with a 80 GeV/c muon beam. Preliminary results for this device equipped with a CsI photocathode demonstrated a time resolution below σ = 25 ps for all measured pads. The time resolution was reduced to be below σ = 18 ps by decreasing the drift gap to 180 μm and using dedicated RF amplifier cards as new electronics. The excellent timing performance of the single-channel proof of concept was not only transferred to the 100-channel prototype, but even improved, making the PICOSEC Micromegas detector more suitable for large-area experiments in need of detectors with high time resolutions.
46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗
PICOSEC-Micromegas Detector, an innovative solution for Lepton Time Tagging
The PICOSEC-Micromegas (PICOSEC-MM) detector is a novel gaseous detector designed for precise timing resolution in experimental measurements. It eliminates time jitter from charged particles in ionization gaps by using extreme UV Cherenkov light emitted in a crystal, detected by a Micromegas photodetector with an appropriate photocathode. The first single-channel prototype tested in 150 GeV/c muon beams achieved a timing resolution below 25 ps, a significant improvement compared to standard Micropattern Gaseous Detectors (MPGDs). This work explores the specifications for applying these detectors in monitored neutrino beams for the ENUBET Project. Key aspects include exploring resistive technologies, resilient photocathodes, and scalable electronics. New 7-pad resistive detectors are designed to handle the particle flux. In this paper, two potential scenarios are briefly considered: tagging electromagnetic showers with a timing resolution below 30ps in an electromagnetic calorimeter as well as individual particles (mainly muons) with about 20ps respectively.
46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗
Influence of Surface and Structural Variations in Donor–Acceptor–Donor Sensitizers on Photoelectrocatalytic Water Splitting
Conjugated organic chromophores composed of linked donor (D) and acceptor (A) moieties have attracted considerable attention for photoelectrochemical applications. In this work, we compare the optoelectronic properties and photoelectrochemical performance of two D–A–D structural isomers with thiophene-X-carboxylic acid (X denotes 3 and 2 positions) derivatives and 2,1,3-benzothiadiazole as the D and A moieties, respectively. 5,5′-(Benzo[c][1,2,5]thiadiazole-4,7-diyl)bis(thiophene-3-carboxylic acid), BTD1, and 5,5′-(benzo[c][1,2,5]thiadiazole-4,7-diyl)bis(thiophene-2-carboxylic acid), BTD2, were employed in the study to understand how structural isomers affect surface attachments within chromophore–catalyst assemblies and their influence on charge-transfer dynamics. Crystal structures revealed that varying the position of the −COOH anchoring group causes the molecules to either contort out of a plane (BTD1) or adopt a near-perfect planar conformation (BTD2). BTD1 and BTD2 were co-loaded with either a water oxidation catalyst, [Ru(2,6-bis(1-methylbenzimidazol-2-yl)pyridine)-(4,4′-((HO) 2 OPCH 2 )2-2,2′-bipyridine)(OH 2 )] 2 , RuCt 2+ , or proton reduction catalyst [Ni(P 2 Ph N 2 C 6 H 4 CH 2 PO 3 H 2 ) 2 ] 2+ , NiCt 2+ , on oxide electrodes to facilitate photodriven water splitting reactions. Emission quenching measurements indicate that both BTD1 and BTD2 inject electrons into n-type SnO 2 |TiO 2 electrodes and holes into p-type NiO semiconductors from their respective excited states at high efficiencies >60%. Photocurrent densities of chromophore–catalyst assemblies obtained using linear sweep voltammetry (LSV) show that BTD2-sensitized photoanodes generate significantly more photocurrent than BTD1-sensitized electrodes; however, both exhibit similar performances at the photocathode. Photoelectrocatyltic measurements demonstrate that both BTD1 and BTD2 performed similarly, generating Faradaic efficiencies of 39 and 38% at the anode or 61 and 79% at the cathode. Transient absorption measurements suggest that the differences between the LSV and photoelectrocatalytic measurements result from the differences in quantum yields of the photogenerated redox equivalents, which is also a reflection of the varying metal oxide surface conformation. Our findings suggest that BTD2 should be investigated further in photocathodic studies since it has the structural advantage of being incorporated into diverse types of chromophore–catalyst assemblies.
Chromophores↗
Covalent Functionalization of Silicon with Plasma-Grown “Fuzzy” Graphene: Robust Aqueous Photoelectrodes for CO 2 Reduction by Molecular Catalysts
Carbon electrodes are ideal for electrochemistry with molecular catalysts, exhibiting facile charge transfer and good stability. Yet for solar-driven catalysis with semiconductor light absorbers, stable semiconductor/carbon interfaces can be difficult to achieve, and carbon’s high optical extinction means it can only be used in ultrathin layers. Here, we demonstrate a plasma-enhanced chemical vapor deposition process that achieves well-controlled deposition of out-of-plane “fuzzy” graphene (FG) on thermally oxidized Si substrates. The resulting Si|FG interfaces possess a silicon oxycarbide (SiOC) interfacial layer, implying covalent bonding between Si and the FG film that is consistent with the mechanical robustness observed from the films. The FG layer is uniform and tunable in thickness and optical transparency by deposition time. Using p-type Si|FG substrates, noncovalent immobilization of cobalt phthalocyanine (CoPc) molecular catalysts was employed for the photoelectrochemical reduction of CO 2 in aqueous solution. The Si|FG|CoPc photocathodes exhibited good catalytic activity, yielding a current density of ∼1 mA/cm 2 , Faradaic efficiency for CO of ∼70% (balance H 2 ), and stable photocurrent for at least 30 h at −1.5 V vs Ag/AgCl under 1-sun illumination. Furthermore, the results suggest that plasma-deposited FG is a robust carbon electrode for molecular catalysts and suitable for further development of aqueous-stable Si photocathodes for CO 2 reduction.
CO2 reduction↗
All-Perovskite Tandem Photoelectrodes for Unassisted Solar Hydrogen Production
Unassisted solar water splitting by multi-junction tandem photoelectrodes is a sustainable approach to generating green hydrogen fuels. Here, we report on the fabrication of monolithically integrated all-perovskite tandem photocathodes for efficient unassisted solar water splitting. All-perovskite tandem photocathodes wired to an iridium oxide anode deliver a high photovoltage of more than 2 V with an operating photocurrent density of 12.5 mA cm -2 at zero applied bias under simulated AM1.5G one sun illumination, yielding a solar-to-hydrogen (STH) conversion efficiency of 15%. The tandem photoelectrode demonstrates continuous operation for more than 120 hours in water under simulated one-sun illumination with less than 5% efficiency loss. A technoeconomic analysis shows the projected production cost of all-perovskite tandem photoelectrodes is $\$30$ m -2 , promising a levelized cost of hydrogen of less than $\$1$/kg if sufficient device longevity is realized. Finally, this work provides a path toward achieving cost-effective unassisted solar hydrogen fuel production.
08 HYDROGEN↗
A Monolithic Artificial Leaf for Solar Methanol Production from CO 2 and H 2 O
Methanol, an important liquid fuel and chemical feedstock, has yet to be produced using solar energy, H 2 O, and CO 2 as sole inputs in a standalone device. Here, this study directly addresses this longstanding challenge through presenting the first demonstration of unbiased solar methanol production from CO 2 and H 2 O with a monolithic artificial leaf design, surpassing the previous best energy efficiency in solar alcohol production by at least 1 order of magnitude. We first develop a new generation of photocathodes based on Si micropillar arrays and a cobalt tetraaminophthalocyanine molecular catalyst. By integrating a C 60 interlayer that facilitates unidirectional electron transfer through the semiconductor/catalyst interface, we realize a photovoltage of 500 mV, one of the highest recorded for single-junction Si-based photoelectrodes in aqueous CO 2 reduction, as well as unprecedented methanol formation with a Faradaic efficiency of 30% and a partial current density of 6.3 mA cm –2 . We further integrate the photocathode with a multijunction perovskite photovoltaic minimodule to afford a standalone solar fuel system, which demonstrates a light-to-methanol conversion efficiency of 0.8%, 32 times higher than the present record in light-to-alcohol conversion with an artificial leaf.
alcohols↗
Oxynitrides enabled photoelectrochemical water splitting with over 3,000 hrs stable operation in practical two-electrode configuration
Solar photoelectrochemical reactions have been considered one of the most promising paths for sustainable energy production. To date, however, there has been no demonstration of semiconductor photoelectrodes with long-term stable operation in a two-electrode configuration, which is required for any practical application. Herein, we demonstrate the stable operation of a photocathode comprising Si and GaN, the two most produced semiconductors in the world, for 3,000 hrs without any performance degradation in two-electrode configurations. Measurements in both three- and two-electrode configurations suggest that surfaces of the GaN nanowires on Si photocathode transform in situ into Ga-O-N that drastically enhances hydrogen evolution and remains stable for 3,000 hrs. First principles calculations further revealed that the in-situ Ga-O-N species exhibit atomic-scale surface metallization. This study overcomes the conventional dilemma between efficiency and stability imposed by extrinsic cocatalysts, offering a path for practical application of photoelectrochemical devices and systems for clean energy.
14 SOLAR ENERGY↗
Towards advanced polarized electron sources
Polarized electrons play an important role in high-energy and nuclear physics, and their properties have also been exploited in ultrafast electron microscopy. Currently, gallium arsenide crystals illuminated by circular polarized infrared laser light are commonly used for generating polarized electrons. However, the achievable accelerating voltage and the gradient of these electrostatic sources limit the beam quality and quantity. A solution could be to combine gallium arsenide photocathodes with radio-frequency electron guns, which are capable of accelerating beams with significantly higher gradients and voltage. Here we report the successful operation of a gallium arsenide photocathode in a superconducting radio-frequency gun. Our findings are relevant for future sources of polarized electrons.
73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
A red-light-powered silicon nanowire biophotochemical diode for simultaneous CO 2 reduction and glycerol valorization
A bias-free photochemical diode, in which a p-type photocathode is connected to an n-type photoanode to harness light for driving photoelectrochemical reduction and oxidation pairs, serves as a platform for realizing light-driven fuel generation from CO 2 . However, the conventional design, in which cathodic CO 2 reduction is coupled with the anodic oxygen evolution reaction (OER), requires substantial energy input. Here we present a photochemical diode device that harnesses red light (740 nm) to simultaneously drive biophotocathodic CO 2 -to-multicarbon conversion and photoanodic glycerol oxidation as an alternative to the OER to overcome the above thermodynamic limitation. The device consists of an efficient CO 2 -fixing microorganism, Sporomusa ovata, interfaced with a silicon nanowire photocathode and a Pt–Au-loaded silicon nanowire photoanode. This photochemical diode operates bias-free under low-intensity (20 mW cm –2 ) red light irradiation with ~80% Faradaic efficiency for both the cathodic and anodic products. Finally, this work provides an alternative photosynthetic route to mitigate excessive CO 2 emissions and efficiently generate value-added chemicals from CO 2 and glycerol.
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
Investigations of the stability of GaAs for photoelectrochemical H 2 evolution in acidic or alkaline aqueous electrolytes
The long-term stability of p-GaAs photocathodes has been investigated for the hydrogen-evolution reaction (HER) in contact with either 1.0 M H 2 SO 4 (aq) or 1.0 M KOH(aq). Stability for the HER was evaluated using p-GaAs electrodes that were either etched or coated with active HER catalysts (Pt and CoP). Changes in surface characteristics of GaAs after exposure to electrochemical conditions were monitored by X-ray photoelectron spectroscopy (XPS), and electrode dissolution processes were evaluated by inductively coupled plasma mass spectrometry (ICP-MS). Consistent with thermodynamic predictions, after operation of the HER at pH 0 or pH 14, illuminated etched p-GaAs electrodes exhibited minimal dissolution while preserving a nearly stoichiometric surface. Electrodeposition or sputtering of Pt on the p-GaAs surface promoted the formation of excess As 0 via an interfacial reaction during the HER. The resulting non-stoichiometric As 0 -rich surface of p-GaAs/Pt electrodes caused a loss in photoactivity as well as substantial cathodic dark current. In contrast, p-GaAs electrodes coated with thin-film CoP catalysts did not display an increase in surficial As 0 after operation of the HER in acidic electrolytes. Minimization of deleterious interfacial reactions is thus critical to obtain extended stability in conjunction with high performance from p-GaAs photocathodes.
32 ENERGY CONSERVATION, CONSUMPTION, AND UTILIZATI↗
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↗
Air-transfer production method for large-area picosecond photodetectors
We have designed and prototyped the process steps for the batch production of large-area micro-channel-plate photomultipliers (MCPPMT) using the “air-transfer” assembly process developed with single LAPPD TM modules. Results are presented addressing the challenges of designing a robust package that can transmit large numbers of electrical signals for pad or strip readout from inside the vacuum tube and of hermetically sealing the large-perimeter window–body interface. We have also synthesized a photocathode in a large-area low-aspect-ratio volume and have shown that the micro-channel plates recover their functionality after cathode synthesis. These steps inform a design for a multi-module batch facility employing dual nested low-vacuum and ultra-high-vacuum systems in a small-footprint. The facility design provides full access to multiple MCP-PMT modules prior to hermetic pinch-off for leak-checking and real-time photocathode optimization.
47 OTHER INSTRUMENTATION↗
A Monte Carlo technique to model performance of streak camera-based time-resolving x-ray spectrometers
A Monte Carlo technique has been developed to simulate the expected signal and the statistical noise of x-ray spectrometers that use streak cameras to achieve the time resolution required for ultrafast diagnostics of laser-generated plasmas. The technique accounts for statistics from both the photons incident on the streak camera’s photocathode and the electrons emitted by the photocathode travelling through the camera’s electron optics to the sensor. We use the technique to optimize the design of a spectrometer, which deduces the temporal history of electron temperature of the hotspot in an inertial confinement fusion implosion from its hard x-ray continuum emission spectra. The technique is general enough to be applied to any instrument using an x-ray streak camera.
Stoupin, S. (ORCID:0000000226225270)↗
A large area 100-channel PICOSEC Micromegas detector with time resolution at the 20 ps level
Abstract The PICOSEC Micromegas precise timing detector is based on a Cherenkov radiator coupled to a photocathode operating in a semi-transparent mode and a Micromegas amplification structure. The first proof of concept single-channel prototype was able to achieve a time resolution below 25 ps. One of the crucial aspects in the development of precise timing gaseous detectors applicable in high-energy physics experiments is a modular design that enables large area coverage. The first 19-channel multi-pad prototype with an active area of approximately 10 cm 2 suffered from degraded timing resolution due to the non-uniformity of the preamplification gap thickness. A new 100 cm 2 detector module with 100 channels based on a rigid hybrid ceramic/FR4 Micromegas board for improved drift gap uniformity was developed. Initial measurements with 80 GeV/c muons showed improvements in timing response over the measured pads and a time resolution below 25 ps. More recent measurements with a thinner drift gap detector module and newly developed RF pulse amplifiers show that the pad centre resolution can be enhanced to the level of 17 ps. This work will present the development of the detector from structural simulations, design, and beam test commissioning with a focus on the timing performance of a thinner drift gap detector module in combination with new electronics using an automated timing scan method.
Utrobicic, A.↗