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At least 55 records · Page 3

III-V photocathode with nitrogen doping for increased quantum efficiency

An increase in the quantum efficiency of a 3-5 photocathode is achieved by doping its semiconductor material with an acceptor and nitrogen, a column-5 isoelectronic element, that introduces a spatially localized energy level just below the conduction band similar to a donor level to which optical transitions can occur. This increases the absorption coefficient, alpha without compensation of the acceptor dopant. A layer of a suitable 1-5, 1-6 or 1-7 compound is included as an activation layer on the electron emission side to lower the work function of the photocathode.

James, L. W.

Ultraviolet response of semitransparent multialkali photocathodes

The UV spectral sensitivity of two semitransparent visible sensitive photocathodes for spaceborne applications, a trialkali, Cs-Na2KSB, and a bialkali, K2CsSb, both on MgF2 substrates. Results show that for extended wavelength coverage, the bialkali photocathode affords increased quantum yield as compared with the trialkali type, and that the latter has a more variable responsivity with wavelength.

Sobieski, S.

Ultraviolet response of InGaAsP photocathodes

Three type VPM 164 photomultiplier tubes with III-IV compound InGaAsP reflective photocathodes were developed for use in ground-based and space-borne astronomical detectors. Although the achieved response of about 0.02% quantum efficiency at 1.083 microns fell short of the goal of 1% quantum efficiency, the broadband characteristics are still considerably better than those of the S-1 photocathode.

Feibelman, W. A.

Quantum efficiency of opaque CsI photocathodes with channel electron multiplier arrays in the extreme and far ultraviolet

The arrays are overcoated with a CsI photocathode in the VUV. The measurements are part of the development program for the Extreme Ultraviolet Explorer. Monochromatic light from a hollow cathode discharge source passing through a McPherson grazing incidence monochromator is used to illuminate the CsI photocathode. The beam diameter is kept small (approximately 2 mm) to confine it within the individual thickness strips. A bias grid is used to produce a 50-V/mm electric field to guarantee collection of all photoelectrons emitted by the CEMA (channel electron multiplier array) webbing. The CEMAs are operated with a gain of 2-3 x 10 to the 6th and are moderately saturated. A channeltron secondary transfer standard is used to determine the absolute QE in the EUV, whereas an NBS calibrated windowed photodiode is used to measure the FUV absolute QE. It is noted that the CsI gives a factor of 3 increase in the QE in the EUV and a factor of 50-5000 in the FUV.

Martin, C.

Ultraviolet quantum detection efficiency of potassium bromide as an opaque photocathode applied to microchannel plates

The quantum detection efficiency (QDE) of potassium bromide as a photocathode applied directly to the surface of a microchannel plate over the 250-1600 A wavelength range has been measured. The contributions of the photocathode material in the channels and on the interchannel web to the QDE have been determined. Two broad peaks in the QDE centered at about 450 and about 1050 A are apparent, the former with about 50 percent peak QDE and the latter with about 40 percent peak QDE. The photoelectric threshold is observed at about 1600 A, and there is a narrow QDE minimum at about 750 A which correlates with 2X the band gap energy for KBr. The angular variation of the QDE from 0 to 40 deg to the channnel axis has also been examined. The stability of Kbr with time is shown to be good with no significant degradation of QDE at wavelengths below 1216 A over a 15-day period in air.

Siegmund, Oswald H. W.

Extreme ultraviolet quantum detection efficiency of rubidium bromide opaque photocathodes

Measurements are presented of the quantum detection efficiency (QDE) of three samples of RbBr photocathode layers over the 44-150-A wavelength range. The QDE of RbBr-coated microchannel plate (MCP) was measured using a back-to-back Z-stack MCP configuration in a detector with a wedge and strip position-sensitive anode, of the type described by Siegmund et al. (1984). To assess the stability of RbBr layer, the RbBr photocathode was exposed to air at about 30 percent humidity for 20 hr. It was found that the QDE values for the aged cathode were within the QDE measurement errors of the original values. A simple QDE model was developed, and it was found that its predictions are in accord with the QDE measurements.

Siegmund, Oswald H. W.

Photoelectron energy spectra of opaque photocathodes in the extreme and far ultraviolet

Measurements of the EUV quantum detection efficiency (QDE) of opaque RbBr, CsBr, and KBr photocathodes are described and investigations of their photoemission characteristics over the 44-1560 A wavelength range are reported. The results show that high QDEs can be obtained in the EUV. Narrow QDE peaks at soft X-ray wavelengths occur at slightly different wavelengths for each of the materials studied. The long-wavelength thresholds vary according to the material band gap. Data on the photoemission from the photocathode layer on the microchannel plate interchannel web area are used to determine the number and energy distribution of the emitted photoelelectrons as a function of wavelength.

Siegmund, Oswald H. W.

Planar Field Emitters and High Efficiency Photocathodes Based on Ultrananocrystalline Diamond

A method of forming a field emitter comprises disposing a first layer on a substrate. The first layer is seeded with nanodiamond particles. The substrate with the first layer disposed thereon is maintained at a first temperature and a first pressure in a mixture of gases which includes nitrogen. The first layer is exposed to a microwave plasma to form a nitrogen doped ultrananocrystalline diamond film on the first layer, which has a percentage of nitrogen in the range of about 0.05 atom % to about 0.5 atom %. The field emitter has about 10.sup.12 to about 10.sup.14 emitting sites per cm.sup.2. A photocathode can also be formed similarly by forming a nitrogen doped ultrananocrystalline diamond film on a substrate similar to the field emitter, and then hydrogen terminating the film. The photocathode is responsive to near ultraviolet light as well as to visible light.

Sumant, Anirudha V.

ZnTiN 2 as an Electron-Selective, Protective Layer on Si Photocathodes

Photoelectrochemical production of fuels requires photoelectrodes that efficiently convert sunlight to electrochemical energy by producing photovoltage and photocurrent and maintain this ability over time under a variety of pH, illumination, and applied bias conditions. Work in the photovoltaic community has demonstrated that interfaces with high charge carrier selectivity provide high photovoltages. This offers a co-design opportunity to create semiconductor photoelectrodes with contact layers that are both carrier-selective and offer protection from degradation in aqueous solutions. In this work, we explored the ternary nitride ZnTiN 2 as an electronselective, protective layer for Si-based photocathodes. We demonstrated that ZnTiN 2 formed a heterojunction with p-type Si that facilitated electron movement toward the ZnTiN 2 surface for light-driven reduction reactions. Across a variety of electrolyte conditions, ZnTiN 2 /Si produced an open circuit voltage of ca. 400 mV vs the solution potential, while bare Si produced 220−480 mV vs the solution potential depending on conditions. ZnTiN 2 was also shown to protect Si over 72 h at open circuit in the dark in 0.1 M KHCO 3 aqueous solution at pH 10.5, with a 2.4% loss in open circuit voltage compared to a 17% loss for unprotected Si. A protective effect was also observed under illumination during methyl viologen reduction at pH 3.5 for 21 h, with a 2.5% loss in open circuit voltage observed for ZnTiN 2 /Si compared to a 25% loss in open circuit voltage for unprotected Si under the same conditions. Elemental characterization revealed the presence of oxides on the surface of ZnTiN 2 that are consistent with the Pourbaix diagram after photoelectrochemical operation; these oxides appeared to support durability without hindering charge carrier extraction to drive electrochemical work. This work highlights the promise of ZnTiN 2 for durable photoelectrochemical applications.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH

Electrolyte Immersion Increases Photoconductivity in a Model Polymer Photocathode

Immersing polymer solar cells in aqueous electrolyte for photoelectrochemical (PEC) hydrogen production is likely to cause photophysical changes that could present both challenges and opportunities for engineering functional and durable devices. Herein we study the bulk heterojunction blend poly(4,8-bis(5-(2-ethylhexyl)thiophen-2-yl)benzo[1,2-b:4,5-b']dithiophene-2,6-diyl)-alt-(2-(((2-ethylhexyl)oxy)carbonyl)-3-fluorothieno[3,4-b]thiophene-4,6-diyl):poly(N,N'-di(2-octyldodecyl)naphthalene-1,8:4,5-bis(dicarboximide)-2,6-diyl)-alt-(2,2-bithiophene-5,5'-diyl) (PTB7-Th:N2200) excited-state dynamics in electrolyte from femtosecond to millisecond time scales using pump-probe microwave conductivity and absorption spectroscopy. While the blend swells very little, electrolyte exposure increases the microwave-frequency mobility and possibly the yield of photogenerated charges while also decreasing crystallinity. These results indicate an enhancement in key performance metrics, implying that any limitations on the performance of PEC test devices do not arise from active layer-electrolyte interactions. For the PTB7-Th:N2200 blend or similar photocathode systems, our results indicate that improving the interfacial kinetics and/or the carrier lifetime should be prioritized, not protecting the active layer from the electrolyte. Since this observation may not be universal to all polymer systems, future research should focus on identifying their limiting photophysical processes. electrolyte.

14 SOLAR ENERGY

The Cascade Effectiveness of 3-Terminal Tandem Photocathode Architectures as Applied to CO 2 Reduction

Cascade catalysis for photoelectrochemical CO 2 reduction (CO 2 R) decouples the overall reaction into sequential steps occurring on separately optimized catalysts (for example, Ag and Cu) between which an intermediate species such as CO is transferred. A 3-terminal tandem (3TT) photovoltaic architecture advantageously holds two different catalytic regions at different potentials under a single illumination source, but its overall efficiency is low. Using a stochastic reaction-diffusion model, we have examined 3TT photocathode design principles, focusing on the coupling of surface chemistry and transport of CO both inside the boundary layer and outward, into the bulk electrolyte. We find that ensuring that the lateral diffusion distance within the boundary layer is short compared to the boundary layer thickness and controlling bulk flow are key, with interdigitated designs showing an overall conversion efficiency improvement by 2 orders of magnitude compared to the side-by-side case without flow. These findings can be adapted for other cascaded architectures.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH

Pulsed laser deposition assisted epitaxial growth of cesium telluride photocathodes for high brightness electron sources

The development of high-brightness electron sources is critical to state-of-the-art electron accelerator applications like X-ray free electron laser (XFEL) and ultra-fast electron microscopy. Cesium telluride is chosen as the electron source material for multiple cutting-edge XFEL facilities worldwide. This manuscript presents the first demonstration of the growth of highly crystalized and epitaxial cesium telluride thin films on 4H-SiC and graphene/4H-SiC substrates with ultrasmooth film surfaces. The ordering of the film was characterized by in situ reflection high energy electron diffraction and multiple X-ray diagnostics. The results of the quantum efficiency performance for epitaxial cesium telluride photocathodes are also reported.

43 PARTICLE ACCELERATORS

Power conversion in SnS photocathodes made by electrochemical growth is limited by recombination at (002) buried facets

Herzenbergite α-SnS is a promising p-type semiconductor for photovoltaic and solar fuel applications, but current devices are plagued by substantial photovoltage losses. Here we use vibrating Kelvin probe surface photovoltage for the first time to study the recombination losses in microcrystalline SnS photoelectrodes. α-SnS films of varied crystal orientation, size, and shape are obtained by electrochemical growth from aqueous tin( II ) chloride and sodium thiosulfate solutions near room temperature. After application of a CdS passivation layer, the films function as photocathodes for the methylviologen reduction reaction. Photoelectrochemical and surface photovoltage measurements reveal that the performance of these devices is sensitively controlled by mainly the SnS crystal orientation and to a lesser extent by the grain size. For example, the highest charge recombination rates of 8.97 × 10 14 s −1 cm −2 and lowest photocurrent (0.73 mA cm −2 ) and lowest photovoltage (0.12 V) occur for SnS films containing 500 nm crystals with irregular shapes and SnS lattices tilted away from the (001) orientation. On the other hand, the best performance (1.62 mA cm −2 , 0.16 V, 3.32 × 10 12 s −1 cm −2 ) is seen for 1100 nm fully (001) oriented SnS nanoplates. Furthermore, these findings agree with improved charge carrier mobility in the 001 direction and they also show that charge recombination in SnS films occurs mainly at dangling Sn–S bonds at buried (002) facets. Such buried interfaces need to be suppressed for optimized solar energy conversion with SnS.

Najaf, Zainab [University of California, Davis, CA

Photovoltage behaviour of p-Sb 2 S 3 photocathodes for hydrogen evolution: effect of n-In 2 S 3 passivation layers

The 1.76 eV band gap of antimony(iii) sulphide (Sb 2 S 3 ) makes this semiconductor material a promising light absorber for photoelectrochemical water splitting, but scalable fabrication approaches to efficient devices are still lacking. Here we show that compact Sb 2 S 3 films on FTO can be obtained by electrochemical growth from aqueous colloidal sulphur and antimony trichloride solutions, followed by mild annealing. These films can be converted into hydrogen evolution photocathodes after coating with In 2 S 3 passivation layers and the addition of Pt proton reduction co-catalysts. For the first time, vibrating Kelvin probe surface photovoltage (VKP-SPV) spectroscopy is used to observe the carrier dynamics in such photoelectrodes. While the bare Sb 2 S 3 films suffer from high surface recombination rates and poor electron extraction, the In 2 S 3 overlayer is found to raise the photovoltage and cathodic photocurrent density, due to passivation of surface defects and formation of a p–n heterojunction. In thick In 2 S 3 films, these benefits are offset by shading and slow electron transfer. Also, we find that O 2 strongly affects the band bending in the Sb 2 S 3 –air and In 2 S 3 –air junctions and their photovoltage. The optimised devices evolve H 2 at 77.5% Faradaic efficiency and with 0.084% applied bias photon-to-current efficiency (ABPE) at 0.12 V vs. RHE. The low ABPE value is attributed to Sb 2 S 3 sub-bandgap defects visible in SPV spectra, the random orientation of Sb 2 S 3 crystallites in the films, which inhibits charge transport, the absence of crystal facets of Sb 2 S 3 , and a detrimental Schottky junction at the FTO|Sb 2 S 3 interface.

de Araújo, Moisés A. [University of California, Da