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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 37 records · Page 2
All sourcesNASA NTRSDOE OSTI
DOE OSTI2025

Emission properties of a hybrid metallized diamond(001) photocathode

The spectral emission characteristics of a proof-of-concept hybrid metallized diamond(001) photocathode are presented. The quantum efficiency (QE) is shown to be determined by the photoinjection efficiency across the ohmic contact at the back metallized face, whereas the mean transverse energy (MTE) of the photoemitted electrons is consistent with an (optical)phonon-assisted and momentum-resonant Franck-Condon mechanism [Franck-Condon electron emission from polar semiconductor photocathodes, Phys. Rev. Appl. 23, 054065 (2025)] following electron drift transport to the untreated diamond(001) front emission face. Emission is observed from both the lower and upper conduction bands of diamond with positive and negative electron affinity, respectively. A potential route to the realization of a red-visible photocathode based on this concept with a sub-50 meV MTE and a QE greater than 0.1% is discussed.

Density of states↗
DOE OSTI2026

Buried Interfaces in Organic Photocathodes for H 2 Evolution: Fermi-Level Pinning and Recombination

Herein, we demonstrate how Fermi-level pinning at buried contacts impacts solar fuel generation in all-polymer photocathodes by systematically comparing the effects of work function, hydroxyl coverage, and hydrogen evolution using chemically modified indium tin oxide (ITO) supports. Photovoltages and net photocathode performance are improved when the ITO is passivated using phosphonic acids, independent of work function, suggesting that the passivation reduces Fermi-level pinning at the buried interface arising from blended heterojunction interactions with surface metal hydroxyls. Transient photovoltage decay reveals differences in recombination mechanisms, supported by light intensity-dependent measurements. Briefly, nonpassivated, hydrophilic contacts exhibit trap-assisted recombination, while passivated, hydrophobic contacts follow bimolecular recombination. We then investigate changes in electroactivity of hole-transfer processes as a function of scan rate and repetitive cycling using a diffusion-controlled molecular redox probe, analogous to a hole-only device achieved via the electrolyte. The nonpassivated buried contacts exhibit higher overpotentials for oxidation, indicative of hole injection/extraction barriers. We observe irreversible electron transfer via the hole-transport level of the blended heterojunction and a strong cycle dependence, consistent with changes in the hole trap state density. Passivation results in more reversible redox behaviors, consistent with more Ohmic-like contacts. Collectively, these results provide context toward the realization of durable organic photoelectrodes with optimized photovoltages and net solar-to-hydrogen conversion efficiencies via fundamental understanding of the rates of carrier generation, recombination, and transport in high-dielectric aqueous environments and opportunities to characterize buried interfaces under device-relevant electric fields.

buried interfaces↗
DOE OSTI2024

High-intensity polarized electron gun featuring distributed Bragg reflector GaAs photocathode

The polarized electron source is a critical component in accelerator facilities such as the electron–ion collider, which requires a polarized electron gun with higher voltage and higher bunch charge than existing sources. One challenge we faced was the surface charge limit of the distributed Bragg reflector GaAs/GaAsP superlattice (DBR-SL-GaAs) photocathode. We suppressed this effect by optimizing the surface doping and heat cleaning procedures. We achieved up to 11.6 nC bunch charge of polarized electron beam. In this report, we discuss the performance of tests of a DBR-SL-GaAs photocathode in the high voltage direct current gun. Possible reasons for the observed peak quantum efficiency wavelength shift are analyzed, and we addressed it by using a wavelength tunable laser. In addition, the impact of the DBR layer and laser on the lifetime is investigated in this paper. The optimal DBR-SL-GaAs operating zone has been proposed, which gave us a long lifetime and high polarization at 30 μA operation. Finally, the success of this polarized gun will be key to the future of the nuclear sciences.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2025

Characterization of Cs 3 Sb photocathodes at cryogenic temperatures

Here, we report measurements of quantum efficiency (QE) and mean transverse energy (MTE) from Cs 3 Sb photocathodes in a wide range of photon energies at both room and cryogenic temperatures. Our measurements show a strong temperature dependence of MTE even at photon energies well above threshold, indicating the presence of strong inelastic scattering of excited electrons during transport before emission into vacuum. We also demonstrate a cathode cooling method that largely preserves the QE while reducing MTE, allowing us to achieve MTEs as low as 58 meV with 3% QE in green light from Cs 3 Sb photocathodes. Our results are crucial for producing brighter electron beams for various photoinjector applications like ultrafast electron diffraction and microscopy, x-ray free-electron lasers, and particle colliders.

36 MATERIALS SCIENCE↗
DOE OSTI2026

Impact of superlattice size on quantum efficiency and polarization in MOCVD-grown strained GaAs/GaAsP photocathodes

Strained superlattice GaAs photocathodes are crucial for providing high photocurrent beams of spin-polarized electrons at several accelerator facilities including the Continuous Electron Beam Accelerator Facility at Thomas Jefferson National Accelerator Facility and the future Electron–Ion Collider at Brookhaven National Laboratory. Here, in this work, we study the effects of varying the number of superlattice pairs on the polarization and photocurrent of the photocathodes. We observe a saturation in quantum efficiency beyond 30 pairs, with additional layers yielding minimal photocurrent improvement while noticeably reducing the polarization of the beam.

Chemical vapor deposition↗
DOE OSTI2025

Mild-Annealed Molecular Layer Deposition (MLD) Tincone Thin Film as Photoelectrochemically Stable and Efficient Electron Transport Layer for Si Photocathodes

Metalcone thin films, composed of inorganic–organic hybrids, are synthesized using molecular layer deposition (MLD) through reactions between organometallic precursors (e.g., Sn, Al, and Ti) and organic reactants (e.g., ethylene glycol and glycerol). Despite their unique properties, metalcones exhibit significant vulnerability to water due to their organic components, limiting their potential in electrochemical applications. This study focuses on enhancing the photoelectrochemical stability of tincone thin films in aqueous electrolyte while preserving their hybrid characteristics through mild annealing in air at 250 °C. As-deposited and vacuum-annealed tincone thin films exhibited significant degradation under these conditions, while high-temperature-annealed (500 °C) tincone thin films offered improved stability with a significant decline in charge transfer efficiency. In contrast, mild annealing in air maintained the C–O bond at half level and improved the stability and charge transport without compromising the unique characteristics of tincone. This was confirmed by ellipsometry, X-ray photoelectron spectroscopy (XPS), and Fourier transform infrared spectroscopy (FTIR). Mild-annealed tincone deposited on a lightly doped p-type silicon (p-Si) photocathode produced a 20-fold increase in CO volume compared to high-temperature annealed tincone in a CO 2 -saturated potassium bicarbonate (KHCO 3 ) electrolyte with dispersed graphene oxide–cobalt phthalocyanine (GO-CoPc) under 1 sun illumination at 0.9 V vs reversible hydrogen electrode (RHE), while maintaining the faradaic efficiency for CO and H 2 . These results suggest that mild-annealed tincone thin films hold significant potential as protective charge transport layers on silicon photocathodes for the aqueous CO 2 reduction reaction (CO 2 RR).

Annealing (metallurgy)↗
DOE OSTI2026

Front-Surface Potential of Platinized p -InP Photocathodes Probed by Dual-Working-Electrode Measurements

The front-surface potential (E fr ) of p-InP/Pt photocathodes performing the hydrogen-evolution reaction has been probed under operating conditions using a dual-workingelectrode (DWE) method. The DWE data are consistent with expectations for proposed stability mechanisms for p-InP photocathodes. Specifically, E fr for Pt-modified p-InP adopts a value near the reversible hydrogen electrode (RHE) potential, consistent with kinetic suppression of metallic In 0 formation. The data provide a rapid, operando metric of interfacial catalyst activity, and indicate that E fr for the p-InP/Pt junction is governed by surface catalytic kinetics rather than by the applied back-contact potential (E b ).

Catalysts↗
DOE OSTI2025

Pulsed laser deposition of delafossite oxide thin films on YSZ (001) substrates as solar water splitting photocathodes

Development of solar energy converters with earth-abundant and environmentally friendly materials is one of the key routes explored towards a sustainable future. In this work, crystalline delafossite-phase CuAlO 2 and CuFeO 2 thin film solar water splitting photocathodes were fabricated using pulsed laser deposition. It was found that the desired delafossite phase was formed only after high temperature annealing in an oxygen-free atmosphere. Further, the homogeneous delafossite bulk structure of the films was determined by correlating simulation results from first-principles calculations with synchrotron-based X-ray absorption near edge structure (XANES) spectroscopy. Both CuAlO 2 and CuFeO 2 photocathodes are active for solar water splitting, with the latter more efficient due to its narrower band gap and improved light absorption.

36 MATERIALS SCIENCE↗
DOE OSTI2026

Recent developments and operation of polarized photocathodes at Jefferson Lab

Spin-polarized electron sources are critical to a wide range of accelerator-based applications for nuclear and particle physics. At Thomas Jefferson National Accelerator Facility, they play a central role in delivering high-quality polarized beams for precision nuclear physics experiments and next-generation parity-violation measurements, where stringent control of systematic uncertainties is essential. These sources are also expected to be key components of other initiatives, including the Electron-Ion Collider and the potential future positron capabilities at Jefferson Lab. In this talk, I will present ongoing research and development efforts at Jefferson Lab focused on the design, fabrication and optimization of spin-polarized photocathodes. This includes growth using molecular beam epitaxy (MBE) or metal-organic chemical vapor deposition (MOCVD), along with detailed characterization of their performance metrics, such as quantum efficiency (QE), electron spin polarization and QE anisotropy, all of which are increasingly important metrics for polarized electron sources at Jefferson Lab and the Electron-Ion Collider. Strategies to mitigate QE anisotropy, which is critical for reducing helicity-correlated beam asymmetries in precision experiments such as MOLLER will be highlighted. Finally, I will present recent efforts aimed at improving the operational lifetime of spin-polarized photocathodes in injector environments, particularly under high-voltage conditions in DC electron guns. These developments are essential for enabling reliable, high-performance operation of polarized sources for current and future accelerator programs.

Kachwala, Alimohammed [Thomas Jefferson National A↗
DOE OSTI2025

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↗
DOE OSTI2025

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↗
DOE OSTI2026

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↗
DOE OSTI2025

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↗
DOE OSTI2026

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↗
DOE OSTI2026

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↗
DOE OSTI2026

Intrinsic emittance properties of an Fe-doped β-Ga 2 O 3 (010) photocathode: Ultracold electron emission at 300 K and the polaron self-energy

Measurements of the spectral emission properties of an iron-doped a β-Ga 2 O 3 (010) photocathode at 300 K reveal the presence of an ultracold contribution to the total electron beam emission with a 6 meV mean transverse energy (MTE) in the 3.5–4.4 eV photon energy range (282–354 nm). This extreme sub-thermal photoemission signal is consistent with direct emission of electrons photoexcited from the Fe dopant states into the low effective mass and positive electron affinity primary conduction band, and it is superimposed on a stronger signal with a larger MTE associated with an (optical)phonon-mediated momentum-resonant Franck–Condon (FC) emission process from a thermally populated and negative electron affinity upper conduction band. For photon energies above 4.5 eV, a transition from a long to a short transport regime is forced by an absorption depth reduction to below 100 nm and both MTE signals exhibit spectral trends consistent with phonon-mediated FC emission if the polaron formation self-energy is included in the temperature of the initial thermalized photoexcited electron distribution.

Angeloni, Louis A. [University of Illinois, Chicag↗
DOE OSTI2026

Enhanced quantum efficiency from optical interference in alkali antimonide photocathodes: Modeling and experimental results

We present measurements of enhanced quantum efficiency (QE) in thin film alkali antimonide photocathodes from optical interference in the cathode-substrate multilayer. Modulations in the spectral response are observed over a range of visible wavelengths and are shown to increase the QE by more than a factor of two at specific wavelengths. We present a model describing the QE modulations based on the three step photoemission process incorporating cases of both constant density of states and density functional theory-derived density of states and show that the calculated results are in good agreement with the measurements. Model predictions demonstrate that QE can be enhanced by more than a factor of 5 by optimization of cathode and substrate layer thicknesses. Additionally, these calculations reveal that optical interference can yield higher quantum efficiencies in thin films compared to thick, optically dense films. We model the QE vs excitation wavelength of multiple alkali antimonide compounds at different thicknesses. We then discuss the advantages of this interference effect for electron accelerators.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗