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At least 235 records · Page 13

Novel Chalcopyrites for Advanced Photoelectrochemical Water Splitting

With the support of DoE’s EERE office, our team has established a unique tool-chest of capabilities, including theoretical modeling (Lawrence Livermore National Laboratory: LLNL), state-of-the-art synthesis (Hawaii Natural Energy Institute: HNEI, Stanford, and the National Renewable Energy Laboratory: NREL) and advanced materials and interfaces characterization (University of Nevada, Las Vegas: UNLV, and Lawrence Berkeley National Laboratory: LBNL), to accelerate the development of high efficiency and durable chalcopyrite materials for advanced photoelectrochemical (PEC) water splitting. Using this synergistic approach, we have successfully created new wide bandgap chalcopyrite photocathodes generating over 10 mA/cm 2 , developed innovative strategies to protect them from corrosion, and engineered novel integration methods to circumvent thin film materials mechanical, chemical and thermal incompatibility. In Task 1 “Modeling and synthesis of chalcopyrite photocathodes”, we expanded our library of wide bandgap chalcopyrites for PEC water splitting. With support from LLNL’s “Computational Materials Diagnostics and Optimization of PEC Devices”, LBNL’s “photophysical” and NREL’s “I-III-VI Compound Semiconductors for Water-Splitting” nodes, we investigated two new chalcopyrite candidates for PEC water splitting: Cu(In,Al)Se 2 and Cu(In,B)Se 2 . We also further developed ordered vacancy compounds, such as CuGa 3 Se 5 , with unprecedented durability during PEC waters splitting in acidic solutions. In Task 2 “Interfaces engineering for enhanced efficiency and durability”, we addressed both the non-ideal band-edge positions of chalcopyrites with respect to water redox potentials, as well as their chemical instability under PEC water splitting, with a buried-junctions approach. With help from NREL’s “High-Throughput Experimental Thin Film Combinatorial Capabilities” and “Corrosion Analysis of Materials” nodes, we engineered environmentally friendly n-type buffers, including Mn x Zn 1-x O, to adjust the chalcopyrite band-edge positions and achieved photovoltages as high as 925 mV. Also, we integrated non-precious catalytic-protecting layers, such as WO 3 , to enhance the water splitting long-term stability of chalcopyrite absorbers. Finally, in Task 3 “Hybrid photoelectrode device integration”, we proposed an innovative method to bond wide bandgap photocathodes onto narrow bandgap PV drivers at room temperature using conductive polymers. Our semi-monolithic approach addressed fundamental processing incompatibility issues, as both the photocathode and the PV driver are processed separately. Proof-of-concept whole-chalcopyrite tandems were obtained by consecutive exfoliation and transfer of fully integrated 1.85 eV CuGa 3 Se 5 and 1.13 eV CuInGaSe 2 stacks from their Mo/SLG substrates onto a new single FTO host substrate.

08 HYDROGEN↗

Image tube

An optical image is projected onto a planar surface of a photocathode that derives an electron beam replica of the image. A target electrode displaced relative to the photocathode so that it does not obstruct the optical image includes a planar surface for receiving and deriving an accurate replica of the electron beam image. The two planar surfaces are parallel. The electron beam image is focused on the target electrode by providing throughout a region that extends between the planar surfaces of the photocathode and receiving electrode, constant homogeneous dc electric and magnetic fields. The electric field extends in a direction perpendicular to the planar surfaces while the magnetic field extends along a straight line that intersects the photocathode and target electrode at an acute angle.

Hallam, K. L.↗

Refractive field correctors for the Starlab ultraviolet telescope

Field correctors for a one-meter, f/15 cassegrainian telescope were designed as part of a NASA-funded study of an astronomical obervatory on board of the Space Shuttle. By means of a Gasgoigne corrector and a biconcave field flattener, astigmatism and field curvature are corrected in a 0.6 deg field. Applicable wavelength ranges are limited by chromatic aberrations. The upper wavelength is selected to match a photocathode response limit. The lower wavelength limit is defined by a filter. Examples of usable wavelength ranges are: 210 nm - 1100 nm (multialkali photocathode, fused-silica corrector elements), 177 nm - 320 nm (cesium telluride photocathode, calcium fluoride correctors); and possibly 134 nm - 190 nm (cesium iodide photocathode, lithium fluoride correctors). Residual rms lateral color is smaller than 0.02 arc sec, and axial color is smaller than 0.25 arc sec (blur diameter at the ends of the wavelength range). The correctors introduce a small amount of coma. This is compensated by adjustment of the conic constants of the telescope mirrors.

Bottema, M.↗

High efficiency photon counting detectors for the FAUST Spacelab far ultraviolet astronomy payload

The performances of sealed tube microchannel-plate position sensitive detectors having transmission CsI photocathodes or opaque CsI photocathodes are compared. These devices were developed for the FAUST Spacelab payload to accomplish imaging surveys in the band between 1300 A and 1800 A. It is demonstrated that photocathode quantum efficiencies in excess of 40 percent at 1216 A have been achieved with the transmission and the opaque CsI photocathodes. The effect of the photoelectron trajectory on the spatial resolution is assessed. Spatial resolution of less than 70 microns FWHM has been obtained and is maintained up to event rates of 50,000/sec. Background rates of 0.55 events sq cm per sec have been achieved and low distortion (less than 1 percent) imaging has been demonstrated.

Siegmund, O. H. W.↗

Near-Infrared Photon-Counting Camera for High-Sensitivity Observations

The dark current of a transferred-electron photocathode with an InGaAs absorber, responsive over the 0.9-to-1.7- micron range, must be reduced to an ultralow level suitable for low signal spectral astrophysical measurements by lowering the temperature of the sensor incorporating the cathode. However, photocathode quantum efficiency (QE) is known to reduce to zero at such low temperatures. Moreover, it has not been demonstrated that the target dark current can be reached at any temperature using existing photocathodes. Changes in the transferred-electron photocathode epistructure (with an In- GaAs absorber lattice-matched to InP and exhibiting responsivity over the 0.9- to-1.7- m range) and fabrication processes were developed and implemented that resulted in a demonstrated >13x reduction in dark current at -40 C while retaining >95% of the approximately equal to 25% saturated room-temperature QE. Further testing at lower temperature is needed to confirm a >25 C predicted reduction in cooling required to achieve an ultralow dark-current target suitable for faint spectral astronomical observations that are not otherwise possible. This reduction in dark current makes it possible to increase the integration time of the imaging sensor, thus enabling a much higher near-infrared (NIR) sensitivity than is possible with current technology. As a result, extremely faint phenomena and NIR signals emitted from distant celestial objects can be now observed and imaged (such as the dynamics of redshifting galaxies, and spectral measurements on extra-solar planets in search of water and bio-markers) that were not previously possible. In addition, the enhanced NIR sensitivity also directly benefits other NIR imaging applications, including drug and bomb detection, stand-off detection of improvised explosive devices (IED's), Raman spectroscopy and microscopy for life/physical science applications, and semiconductor product defect detection.

Jurkovic, Michael↗

Operation of Cs–Sb–O activated GaAs in a high voltage DC electron gun at high average current

Negative Electron Affinity (NEA) activated GaAs photocathodes are the most popular option for generating a high current (>1 mA) spin-polarized electron beam. Despite its popularity, a short operational lifetime is the main drawback of this material. Recent works have shown that the lifetime can be improved by using a robust Cs–Sb–O NEA layer with minimal adverse effects. In this work, we operate GaAs photocathodes with this new activation method in a high voltage environment to extract a high current. We demonstrate that improved chemical resistance of Cs–Sb–O activated GaAs photocathodes allowed them to survive a day-long transport process from a separate vacuum system using a vacuum suitcase. During beam running, we observed spectral dependence on lifetime improvement. In particular, we saw a 45% increase in the lifetime at 780 nm on average for Cs–Sb–O activated GaAs compared to Cs–O activated GaAs.

47 OTHER INSTRUMENTATION↗

High figure of merit spin polarized electron sources grown via MOCVD

Spin polarized photocathodes are key to the future operation of electron accelerators such as the ones at Thomas Jefferson National Accelerator Facility and Brookhaven National Laboratory. Currently, these photocathodes come in short supply due to limited production by molecular beam epitaxy. By developing a process to implement similar structures using metal organic chemical vapor deposition, the availability of these devices can be increased. Here, in this paper, we detail the implementation of recent photocathode advancements via metal organic chemical vapor deposition process and show an improvement in both polarization and quantum efficiency of our devices compared to those fabricated via molecular beam epitaxy, with devices reaching 82% polarization and 2.9% quantum efficiency.

43 PARTICLE ACCELERATORS↗

Generation and characterization of magnetized electron beam from a DC high voltage photogun for electron beam cooling application

One of the most challenging requirements for the proposed Electron-Ion Collider is the strong cooling of the proton beam, which is key to achieving the collider’s desired luminosity of order 10 33 -10 34 cm -2 s -1 . Magnetized bunched-beam electron cooling could be a means to achieve the required high luminosity, where strong cooling is accomplished inside a cooling solenoid where the ions co-propagate with an electron beam generated from a source immersed in a magnetic field. To increase the cooling efficiency, a bunched electron beam with high bunch charge and high repetition rate is required. This work describes the production and characterization of magnetized electron beam using a compact 300 kV DC high voltage photogun and bi-alkali antimonide photocathode. Beam magnetization was studied using a diagnostic beamline that includes viewer screens for measuring the shearing angle of the electron beamlet passing through a narrow upstream slit. Simulations and corresponding measurements of beam magnetization are presented as a function of laser spot size and magnetic field strength. Correlated beam emittance with magnetic field (0–0.15 T) at the photocathode was measured for various laser spot sizes. Measurements of photocathode lifetime were carried out at different magnetized electron beam currents up to 28 mA, and bunch charge up to 0.7 nC (not simultaneously).

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Perovskite-driven solar C 2 hydrocarbon synthesis from CO 2

Photoelectrochemistry (PEC) presents a direct pathway to solar fuel synthesis by integrating light absorption and catalysis into compact electrodes. Yet, PEC hydrocarbon production remains elusive due to high catalytic overpotentials and insufficient semiconductor photovoltage. Here we demonstrate ethane and ethylene synthesis by interfacing lead halide perovskite photoabsorbers with suitable copper nanoflower electrocatalysts. The resulting perovskite photocathodes attain a 9.8% Faradaic yield towards C 2 hydrocarbon production at 0 V against the reversible hydrogen electrode. The catalyst and perovskite geometric surface areas strongly influence C 2 photocathode selectivity, which indicates a role of local current density in product distribution. The thermodynamic limitations of water oxidation are overcome by coupling the photocathodes to Si nanowire photoanodes for glycerol oxidation. These unassisted perovskite–silicon PEC devices attain partial C 2 hydrocarbon photocurrent densities of 155 µA cm -2 , 200-fold higher than conventional perovskite–BiVO 4 artificial leaves for water and CO 2 splitting. These insights establish perovskite semiconductors as a versatile platform towards PEC multicarbon synthesis.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Charge lifetime improvement of the Continuous Electron Beam Accelerator Facility photogun with a biased anode

GaAs photocathodes in dc high-voltage photoguns are highly susceptible to ion back-bombardment, which reduces the photocathode quantum efficiency and limits the useful operating lifetime for producing polarized electron beams. This paper demonstrates that applying a small positive bias to the photogun anode can significantly suppress ion back-bombardment and increase charge lifetime. This technique was studied extensively using the Continuous Electron Beam Accelerator Facility photogun, where highly polarized electron beams created using a strained-superlattice GaAs / GaAsP photocathode were used and charge lifetimes improved by almost a factor of 2. A new simulation code was developed to model ion production and tracking in order to better understand and explain the factors that led to the performance improvement. Results of the experiments and simulations are discussed in detail. Published by the American Physical Society 2024

43 PARTICLE ACCELERATORS↗

Near-Threshold Photoemission from Graphene-Coated Cu(110)

In this article, the brightness of electron beams emitted from photocathode sources plays a critical role in determining the performance of x-ray free-electron lasers and ultrafast electron-diffraction applications. In order to achieve the maximum brightness, the electrons need to be emitted from a photocathode with the lowest-possible mean transverse energy (MTE). Recent investigations have shown that capping a Cu(110) photocathode with a monolayer of graphene can protect the quantum efficiency (QE) from long-term exposure to varying vacuum conditions. However, there have been no studies that investigate the effects that a monolayer of graphene has on the MTE. Here, we report on measurements of a graphene-coated Cu(110) single crystal near the photoemission threshold for room and liquid-nitrogen temperatures. At room temperature, a minimum MTE of 25 meV is measured at 295 nm. At liquid-nitrogen temperatures, a minimum MTE of 9 meV is measured at the photoemission threshold of 290 nm.

36 MATERIALS SCIENCE↗

Development of High-QE GaN Photodectors for Liquid Noble Particle Detectors

Detection of the handful of photons generated when a dark matter particle interacts in a liquid Xenon detector requires a new type of photodetector with very high detection efficiency at ultraviolet wavelengths, very low radioactive backgrounds, and essentially no measureable readout noise (achieved with devices with high intrisic gain). Such devices would find wide applicability to not only high energy physics experiments, but to a number of commercial applications including, e.g., biomedical imaging of fluorescent tags. We developed photodetectors based on amorphous GaN thin film structures (photocathodes) grown by molecular beam epitaxy on quartz windows. We also developed approaches to integrate these photocathode device structures with vacuum electron multipliers. All materials and fabrication techniques were developed to minimize radioactive backgrounds in materials, so these detectors could be used for very low count rate experiments, such as the future liquid-Xenon dark matter detectors, and future liquid-Argon neutrino detectors. We demonstrated growth of very high quantum efficiency amorphous GaN cathodes grown on a number of different substrates (Stainless steel, p-Silicon) reaching detection efficiencies of 80% at 220nm. The key to this growth was to use nitrogen plasma-assistend MBEs and very low growth temperatures. We also discovered that thinner structures (e.g.,40nm a-GaN thin films) had the best performance. We successfully demonstrated techniques for the vacuum transfer of these photocathode structures to a novel chamber that used hydraulics and bellow to form a cold indium bond needed to integrate these cathodes into sealed-tube devices. A complete, stand-along, device could not be completed during this proposal period due to difficulties in growing structures on the thick quartz window. Subsequent work is aimed at addressing this difficulty, by growing a buffer layer on the quartz substrate.

07 ISOTOPE AND RADIATION SOURCES↗

The oblique electron lens.

An oblique electron lens is described that is especially applicable to image converters and camera tubes employing flat opaque photocathodes. The use of optical lenses, corrector plates, and/or mirrors (often employed in other electron lenses designed for use with opaque photocathodes) are eliminated. The oblique electron lens is well suited to ultraviolet and vacuum ultraviolet image converters, and to image converters employing opaque negative electron affinity photocathodes. It is also possible to use this oblique electron lens for electronography. Measurements on an experimental tube show that a limiting resolution of 50 line pairs/mm is possible, but the intrinsic lens quality is believed to approach that of a conventional electromagnetic lens having uniform and colinear electric and magnetic fields.

Johnson, C. B.↗

SEC vidicon testing

Results obtained from several basic measurements of the performance of an SEC vidicon camera head are presented. The measurements or tests are patterned around the sensor requirements which exist for a rapid response coronagraph. Following a brief description of the SEC vidicon camera head, test set-up, and operating procedures, results are presented for five basic tests. These tests include: (1) Input-output, or transfer, characteristics; (2) modulation transfer function; (3) signal-to-noise ratio; (4) photocathode sensitivity; and (5) target gain. The input-output characteristics and photocathode sensitivity measurements were obtained for three bandpasses centered about 4000, 5250, and 6200 A. Results are also given for the variation of photocathode sensitivity with position on the cathode surface.

Johnson, D. S., Jr.↗

Evaluation of the amperex 56 TVP photomultiplier

Characteristics were measured for the Amperex 56 TVP 42 mm-diameter photomultiplier. Some typical photomultiplier characteristics-such as gain, dark current, transit and rise times-are compared with data provided. Photomultiplier characteristics generally not available such as the single photoelectron time spread, the relative collection efficiency, the relative anode pulse amplitude as a function of the voltage between the photocathode and focusing electrode, and the position of the photocathode sensing area were measured and are discussed for two 56 TVP's. The single photoelectron time spread, the relative collection efficiency, and the transit time difference as a function of the voltage between photocathode and focusing electrode were also measured and are discussed, particularly with respect to the optimization of photomultiplier operating conditions for timing applications.

Lo, C. C.↗

State-of-the-art Space Telescope Digicon performance data

The Digicon has been chosen as the detector for the High Resolution Spectrograph and the Faint Object Spectrograph of the Space Telescope. Both tubes are 512 channel, parallel-output devices and feature CsTe photocathodes on MgF2 faceplates. Using a computer-assisted test facility, the tubes have been characterized with respect to diode array performance, photocathode response (1100-9000 A), and imaging capability. Data are presented on diode dark current and capacitance distributions, pulse height resolution, photocathode quantum efficiency, uniformity and blemishes, dark count rate, distortion, resolution, and crosstalk.

Ginaven, R. O.↗

Multi-anode microchannel arrays - New detectors for imaging and spectroscopy in space

Consideration is given to the construction and operation of multi-anode microchannel array detector systems having formats as large as 256 x 1024 pixels. Such arrays are being developed for imaging and spectroscopy at soft X-ray, ultraviolet and visible wavelengths from balloons, sounding rockets and space probes. Both discrete-anode and coincidence-anode arrays are described. Two types of photocathode structures are evaluated: an opaque photocathode deposited directly on the curved-channel MCP and an activated cathode deposited on a proximity-focused mesh. Future work will include sensitivity optimization in the different wavelength regions and the development of detector tubes with semitransparent proximity-focused photocathodes.

Timothy, J. G.↗

Calculation of resolution for a windowless charge coupled device (CCD)-Digicon

A new version of an intensified charge-coupled device (ICCD) system, which is based on the incorporation of a CsI mesh photocathode and a thinned backside-illuminated CCD into a Space Telescope design Digicon tube, is being developed for future use in space-based observations in the Extreme Ultraviolet waveband. In this paper, a report is presented of the results of computer simulations involving the effects of the non-uniform electrostatic field near the mesh photocathode on imaging properties (especially, the spread function and modulation transfer function) of the detector system. The results are of importance in the design of the front end of the tube and the selection of optimum tube operating conditions. The overall resolution characteristics of the tube, including the effects of the mesh, the electron optics of the region between the mesh photocathode and the CCD target, and the structure of the CCD itself, are estimated.

Jia, X. Z.↗