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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 415 records · Page 23
All sourcesNASA NTRSDOE OSTI
DOE OSTI2020

Metal-free photocatalysts for hydrogen evolution

This review focuses on the discussion of the latest progress and remaining challenges in selected metal-free photocatalysts for hydrogen production. The scope of this review is limited to the metal-free elemental photocatalysts (i.e. B, C, P, S, Si, Se etc.), binary photocatalysts (i.e. BC 3 , B 4 C, C x N y , h-BN etc.) and their heterojunction, ternary photocatalysts (i.e. BCN) and their heterojunction, and different types of organic photocatalysts (i.e. linear, covalent organic frameworks, microporous polymer, covalent triazine frameworks etc.) and their heterostructures. Following a succinct depiction of the latest progress in hydrogen evolution on these photocatalysts, discussion has been extended to the potential strategies that are deemed necessary to attain high quantum efficiency and high solar-to-hydrogen (STH) conversion efficiency. Issues with reproducibility and the disputes in reporting the hydrogen evolution rate have been also discussed with recommendations to overcome them. A few key factors are highlighted that may facilitate the scalability of the photocatalyst from microscale to macroscale production in meeting the targeted 10% STH. This review is concluded with additional perspectives regarding future research in fundamental materials aspects of high efficiency photocatalysts followed by six open questions that may need to be resolved by forming a global hydrogen taskforce in order to translate bench-top research into large-scale production of hydrogen.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2020

A new platform for development of photosystem I based thin films with superior photocurrent: TCNQ charge transfer salts derived from ZIF-8

The transmembrane photosynthetic protein complex Photosystem I (PSI) is highly sought after for incorporation into biohybrid photovoltaic devices due to its remarkable photoactive electrochemical properties, chiefly driving charge separation with ~1 V potential and ~100% quantum efficiency. In pursuit of these integrated technologies, three factors must be simultaneously tuned, namely, direct redox transfer steps, three-dimensional coordination and stabilization of PSI aggregates, and interfacial connectivity with conductive pathways. Building on our recent successful encapsulation of PSI in the metal–organic framework ZIF-8, herein we use the zinc and imidazole cations from this precursor to form charge transfer complexes with an extremely strong organic electron acceptor, TCNQ. Specifically, the PSI-Zn-H 2 mim-TCNQ charge transfer salt complex was drop cast on ITO to form dense films. Subsequent voltammetric cycling induced cation exchange and electrochemical annealing of the film was used to enhance electron conductivity giving rise to a photocurrent in the order of 15 μA cm -2 . This study paves the way for a myriad of future opportunities for successful integration of this unique class of charge transfer salt complexes with biological catalysts and light harvesters.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2020

Foldable semi-ladder polymers: novel aggregation behavior and high-performance solution-processed organic light-emitting transistors

A critical issue in developing high-performance organic light-emitting transistors (OLETs) is to balance the trade-off between charge transport and light emission in a semiconducting material. Although traditional materials for organic light-emitting diodes (OLEDs) or organic field-effect transistors (OFETs) have shown modest performance in OLET devices, design strategies towards high-performance OLET materials and the crucial structure–performance relationship remain unclear. Our research effort in developing cross-conjugated weak acceptor-weak donor copolymers for luminescent properties lead us to an unintentional discovery that these copolymers form coiled foldamers with intramolecular H-aggregation, leading to their exceptional OLET properties. An impressive external quantum efficiency (EQE) of 6.9% in solution-processed multi-layer OLET devices was achieved.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2020

Diazirine-based photo-crosslinkers for defect free fabrication of solution processed organic light-emitting diodes

The fabrication of solution deposited OLEDs is fraught with difficulties, largely due to the interlayer mixing and surface erosion during sequential deposition of the layers. We demonstrate that these problems can be circumvented by using photopolymerizable diazirine-based cross-linker capable of converting soluble organic materials into highly cross-linked insoluble networks. 3-Trifluoromethyl(aryl)diazirines photolyze readily upon the 10–15 min exposure of 365 nm UV irradiation to generate carbenes, which react with polymers or small molecules via C–H bond insertion producing highly cross-linked materials. This photo-generated cross-linking does not require any catalyst, initiator or short-wavelength UV light and is performed at room temperature, releasing molecular nitrogen as the only byproduct. To show the cross-linked polymer layers do not display inter-layer mixing, we deposited red-emitting regioregular poly(3-hexylthiophene-2,5-diyl) (P3HT) over cross-linked (10% cross-linker) blue emitting dioctyl polyfluorene (PFO) layer. The overlaid layers showed clear and well-defined boundary with no interlayer mixing. The surface morphology of the solution deposited layers was investigated by AFM to show that the cross-linked layers exhibited significant decrease in surface roughness. This is also shown on the example of the hole transporting material 4,4'-bis[N-(1-naphthyl)-N-phenylamino]-biphenyl (NPB) which displayed roughness average to decrease from 6.4 nm to 1.0 nm. The effect of decreased surface roughness on the performance of phosphorescent OLEDs was investigated by fabricating devices with configuration of ITO/PEDOT:PSS/NPB:(0%/5%/10%) cross-linker/MCP:6% Ir(mppy) 3 /TPBI/CsF/Al. Furthermore, following the diazirine-mediated cross-linking, the OLEDs displayed a decrease in turn-on voltage from 3.8 V to 3.0 V along with a six-fold enhancement of external quantum efficiency (EQE max ) from 1.1% to 6.8% and maximum luminous efficiency increase from 3.8 cd A -1 to 22.9 cd A -1 . These results demonstrate that the simple diazirine mediated photo-cross-linking using mild conditions compatible with organic layers is a promising strategy for improving the performance of the solution-processed OLEDs.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Photogating-driven enhanced responsivity in a few-layered ReSe 2 phototransistor

A wide variety of two-dimensional (2D) metal dichalcogenide compounds have recently attracted much research interest due to their very high photoresponsivities (R) making them excellent candidates for optoelectronic applications. High R in 2D photoconductors is associated with trap state dynamics leading to a photogating effect, which is often manifested by a fractional power dependence (γ) of the photocurrent (I ph ) at an effective illumination intensity (P eff ). Furthermore, we present photoconductivity studies as a function of gate voltages, over a wide temperature range (20 K to 300 K) of field-effect transistors fabricated using thin layers of mechanically exfoliated Rhenium Diselenide (ReSe 2 ). We obtain very high responsivities R ~ 16500 A/W and external quantum efficiency (EQE) ~ 3.2 × 106% (at 140 K, V g = 60 V and P eff = 0.2 nW). A strong correlation between R and γ was established by investigating the dependence of these two quantities at various gate voltages and over a wide range of temperatures. Such correlations indicate the importance of trap state mediated photogating and its role in promoting high photo-responsivities in these materials. We believe such correlations can offer valuable insights for the design and development of high-performance photoactive devices using 2D materials.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2022

Angle-resolved polarimetry of hybrid perovskite emission for photonic technologies

Coupling between light and matter strongly depends on the polarization of the electromagnetic field and the nature of excitations in a material. As hybrid perovskites emerge as a promising class of materials for light-based technologies such as LEDs, LASERs, and photodetectors, it is critical to understand how their microstructure changes the intrinsic properties of the photon emission process. While the majority of optical studies have focused on the spectral content, quantum efficiency and lifetimes of emission in various hybrid perovskite thin films and nanostructures, few studies have investigated other properties of the emitted photons such as polarization and emission angle. Here, we use angle-resolved cathodoluminescence microscopy to access the full polarization state of photons emitted from large-grain hybrid perovskite films with spatial resolution well below the optical diffraction limit. In this work, mapping these Stokes parameters as a function of the angle at which the photons are emitted from the thin film surface, we reveal the effect of a grain boundary on the degree of polarization and angle at which the photons are emitted. Such studies of angle- and polarization-resolved emission at the single grain level are necessary for future development of perovskite-based flat optics, where effects of grain boundaries and interfaces need to be mitigated.

77 NANOSCIENCE AND NANOTECHNOLOGY↗
DOE OSTI2024

Photosynthetic biohybrid systems for solar fuels catalysis

Photosynthetic reaction center (RC) proteins are finely tuned molecular systems optimized for solar energy conversion. RCs effectively capture and convert sunlight with near unity quantum efficiency utilizing light-induced directional electron transfer through a series of molecular cofactors embedded within the protein core to generate a long-lived charge separated state with a useable electrochemical potential. Of current interest are new strategies that couple RC chemistry to the direct synthesis of energy-rich compounds. This Feature Article highlights recent work from our lab on RC and RC-inspired hybrid systems that capture the Sun's energy and convert it to chemical energy in the form of H2, a carbon-neutral energy source derived from water. Further, biohybrids made from the Photosystem I (PSI) RC are among the best photocatalytic H2-producing protein hybrids to date. Targeted self-assembly strategies that couple abiotic catalysts to PSI translate to catalyst incorporation at intrinsic PSI sites within thylakoid membranes to achieve complete solar water-splitting systems. RC-inspired biohybrids interface synthetic photosensitizers and molecular catalysts with small proteins to create photocatalytic systems and enable the spectroscopic discernment of the structural features and electron transfer processes that underpin solar-driven proton reduction. In total, these studies showcase the incredible scientific opportunities photosynthetic biohybrid research provides for harnessing the optimal qualities of both artificial and natural photosynthetic systems and developing materials that capture, convert, and store solar energy as a fuel.

14 SOLAR ENERGY↗
DOE OSTI2022

The throughput calibration of the VERITAS telescopes

Context. The response of imaging atmospheric Cherenkov telescopes to incident γ -ray-initiated showers in the atmosphere changes as the telescopes age due to exposure to light and weather. These aging processes affect the reconstructed energies of the events and γ -ray fluxes. Aims. This work discusses the implementation of signal calibration methods for the Very Energetic Radiation Imaging Telescope Array System (VERITAS) to account for changes in the optical throughput and detector performance over time. Methods. The total throughput of a Cherenkov telescope is the product of camera-dependent factors, such as the photomultiplier tube gains and their quantum efficiencies, and the mirror reflectivity and Winston cone response to incoming radiation. This document summarizes different methods to determine how the camera gains and mirror reflectivity have evolved over time and how we can calibrate this changing throughput in reconstruction pipelines for imaging atmospheric Cherenkov telescopes. The implementation is validated against seven years of observations with the VERITAS telescopes of the Crab Nebula, which is a reference object in very-high-energy astronomy. Results. Regular optical throughput monitoring and the corresponding signal calibrations are found to be critical for the reconstruction of extensive air shower images. The proposed implementation is applied as a correction to the signals of the photomultiplier tubes in the telescope simulation to produce fine-tuned instrument response functions. This method is shown to be effective for calibrating the acquired γ -ray data and for recovering the correct energy of the events and photon fluxes. At the same time, it keeps the computational effort of generating Monte Carlo simulations for instrument response functions affordably low.

79 ASTRONOMY AND ASTROPHYSICS↗
DOE OSTI2020

Graphene as reusable substrate for bialkali photocathodes

Bialkali photocathodes, such as cesium potassium antimonide (CsK 2 Sb), can generate a high-brightness electron beam using a high-power green laser. These photocathode materials have potential applications in advanced accelerators and electron microscopes. It is known that the quantum efficiency (QE) of these photocathodes is affected severely by their substrates; however, reusability of the substrates is not well known. Here, we use graphene, silicon (Si), and molybdenum (Mo) substrates to evaluate the effects of substrates on the QE of redeposited CsK 2 Sb photocathodes after thermal cleanings. We found the QE of CsK 2 Sb photocathodes redeposited on a graphene substrate after a thermal cleaning at 500 °C remained largely unchanged. On the other hand, the QE of redeposited photocathodes on Si and Mo substrates after thermal cleaning at the same temperature decreased drastically. We used X-ray photoelectron spectroscopy (XPS) to quantitatively evaluate the residues of photocathodes after thermal cleaning at 400 °C and 500 °C. We found that the Sb, K, and Cs are removed by thermal cleaning at 500 °C for the graphene substrate, but all or the majority of these elements remained on the Si and Mo substrates. The results were consistent with our density functional theory (DFT) calculations for the case of Si, which we investigated. Furthermore, our angle-resolved photoemission spectroscopy (ARPES) on graphene indicated that its intrinsic electronic structure is preserved after photocathode deposition and thermal cleaning at 500 °C. Hence, we attributed the difference in amount of photocathode residue to the unique dangling-bond- free surface of inert graphene. Our results provide a foundation for graphene-based reusable substrates for high-QE semiconductor photocathodes.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗
DOE OSTI2020

Impact of dopant-induced optoelectronic tails on open-circuit voltage in arsenic-doped Cd(Se)Te solar cells

Fluctuations refer to inhomogeneity in the distribution of donors and acceptors at the nanometer scale and occur in many compound solar cell materials such as Cu(In,Ga)Se 2 , Cu 2 ZnSn(S,Se) 4 , and CdSe x Te 1-x . In this work, numerical simulations show that these fluctuations produce not only electrostatic potential variation, but also, local changes in the carrier density and effective bandgap. For a CdSe x Te 1-x absorber doped with arsenic, simulations and cathodoluminescence data within single grains demonstrate how donor and acceptor densities—consistent with capacitance-voltage and secondary-ion mass-spectrometry data—produce tails in photoluminescence, quantum efficiency, and absorption measurements. Using multiple theoretical approaches, we demonstrate that the fluctuations can hinder expected performance gains from increased carrier density, and we describe the significant open-circuit voltage deficit observed in the CdSe x Te 1-x :As solar technology. Our results demonstrate that it is critical to characterize and reduce carrier compensation to realize a higher efficiency.

14 SOLAR ENERGY↗
DOE OSTI2020

Demonstration of nitrogen-incorporated ultrananocrystalline diamond photocathodes in a RF gun environment

Quantum efficiency (QE), intrinsic emittance, and robustness are the three most important figures of merit for photocathodes, the first two determine the ultimate achievable brightness of an electron beam, and the third one directly correlates with the complications of a beamline design. Nitrogen-incorporated ultrananocrystalline diamond [(N)UNCD] materials are promising candidates for photocathode applications due to their remarkable electron emission performance as well as the moderate vacuum requirement. Two (N)UNCD photocathodes have been characterized in a realistic RF gun environment with the nicely balanced performance of all three figures of merit. In this work, the QE of the first (N)UNCD cathode (stored in air for two years before the test) was found to be 3.8 x 10 –4 using a 262 nm UV laser and a cathode surface field of 30MV/m. It was found that the QE of the second (N)UNCD sample (grown days before the test) was nearly the same and, therefore, demonstrates the exceptional environmental tolerance of the material. The intrinsic emittance of (N)UNCD was measured to be 1.00 μm/mm.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Incoherent Thomson scattering system for PHAse space MApping (PHASMA) experiment

A new incoherent Thomson scattering system measures the evolution of electron velocity distribution functions perpendicular and parallel to the ambient magnetic field during kinking of a single flux rope and merging of two flux ropes through magnetic reconnection. The Thom-son scattering system provides sub-millimeter spatial resolution, sufficient to diagnose the several millimeters sized magnetic reconnection electron diffusion region in the PHAse Space MAppgin experiment. Due to the relatively modest plasma density ~ 10 19 m -3 and electron tem-perature ~1 eV, stray light suppression is critical for these measurements. Two volume Bragg gratings are used in series as a notch filter with a spectral bandwidth <0.1 nm in the collection branch. A CCD with a Gen III intensifier with peak quantum efficiency >47% is used as the detector in a 1.3 m spectrometer. Preliminary results of gun plasma electron temperature will be reported and compared with measurements obtained from a triple Langmuir probe.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2021

Recombination rate analysis in long minority carrier lifetime mid-wave infrared InGaAs/InAsSb superlattices

Gallium is incorporated into the strain-balanced In(Ga)As/InAsSb superlattice system to achieve the same mid-wave infrared cutoff tunability as conventional Ga-free InAs/InAsSb type-II superlattices, but with an additional degree of design freedom to enable optimization of absorption and transport properties. Time-resolved photoluminescence measurements of InGaAs/InAsSb superlattice characterization- and doped device structures are reported from 77 to 300 K and compared to InAs/InAsSb. The low-injection photoluminescence decay yields the minority carrier lifetime, which is analyzed with a recombination rate model, enabling the determination of the temperature-dependent Shockley–Read–Hall, radiative, and Auger recombination lifetimes and extraction of defect energy levels and capture cross section defect concentration products. The Shockley–Read–Hall-limited lifetime of undoped InGaAs/InAsSb is marginally reduced from 2.3 to 1.4 μs due to the inclusion of Ga; however, given that Ga improves the vertical hole mobility by a factor of >10×, a diffusion-limited InGaAs/InAsSb superlattice nBn could expect a lower bound of 2.5× improvement in diffusion length with significant impact on photodetector quantum efficiency and radiation hardness. At temperatures below 120 K, the doped device structures are Shockley–Read–Hall limited at 0.5 μs, which shows promise for detector applications.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗
DOE OSTI2022

Photoemission characterization of N-polar III-nitride photocathodes as candidate bright electron beam sources for accelerator applications

We report on the growth and characterization of a new class of photocathode structures for use as electron sources to produce high brightness electron beams for accelerator applications. The sources are realized using III-nitride materials and are designed to leverage the strong polarization field, which is characteristic of this class of materials when grown in their wurtzite crystal structure, to produce a negative electron affinity condition without the use of Cs, possibly allowing these materials to be operated in radio frequency guns. A Quantum Efficiency (QE) of about 1×10−3 and an emitted electrons’ Mean Transverse Energy (MTE) of about 100 meV are measured at a wavelength of 265 nm. In a vacuum level of 3×10−10 Torr, the QE does not decrease after more than 24 h of continuous operation. The lowest MTE of about 50 meV is measured at 300 nm along with a QE of 1.5×10−5. Surface characterizations reveal a possible contribution to the MTE from surface morphology, calling for more detailed studies.

Cultrera, L. (ORCID:0000000235606059)↗
DOE OSTI2022

Cesium intercalation of graphene: A 2D protective layer on alkali antimonide photocathode

Alkali antimonide photocathodes have wide applications in free-electron lasers and electron cooling. The short lifetime of alkali antimonide photocathodes necessitates frequent replacement of the photocathodes during a beam operation. Furthermore, exposure to mediocre vacuum causes loss of photocathode quantum efficiency due to the chemical reaction with residual gas molecules. Theoretical analyses have shown that covering an alkali antimonide photocathode with a monolayer graphene or hexagonal boron nitride protects it in a coarse vacuum environment due to the inhibition of chemical reactions with residual gas molecules. Alkali antimonide photocathodes require an ultra-high vacuum environment, and depositing a monolayer 2D material on it poses a serious challenge. In the present work, we have incorporated a novel method known as intercalation, in which alkali atoms pass through the defects of a graphene thin film to create a photocathode material underneath. Initially, Sb was deposited on a Si substrate, and a monolayer graphene was transferred on top of the Sb film. Heat cleaning around 550–600 °C effectively removed the Sb oxides, leaving metallic Sb underneath the graphene layer. Depositing Cs on top of a monolayer graphene enabled the intercalation process. Atomic force microscopy, Raman spectroscopy, x-ray photoelectron spectroscopy, low energy electron microscopy, and x-ray diffraction measurements were performed to evaluate photocathode formation underneath the monolayer graphene. Our analysis shows that Cs penetrated the graphene and reacted with Sb and formed Cs 3 Sb.

2D materials↗
DOE OSTI2023

All-epitaxial resonant cavity enhanced long-wave infrared detectors for focal plane arrays

Here, we demonstrate a monolithic all-epitaxial resonant-cavity architecture for long-wave infrared photodetectors with substrate-side illumination. An nBn detector with an ultra-thin (t ≈ 350 nm) absorber layer is integrated into a leaky resonant cavity, formed using semitransparent highly doped (n⁺⁺) epitaxial layers, and aligned to the anti-node of the cavity’s standing wave. The devices are characterized electrically and optically and demonstrate an external quantum efficiency of 25% at T ¼ 180 K in an architecture compatible with focal plane array configurations.

42 ENGINEERING↗