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At least 613 records · Page 34
All sourcesNASA NTRSDOE OSTI
DOE OSTI2023

Probing Boron Vacancy Complexes in h-BN Semi-Bulk Crystals Synthesized by Hydride Vapor Phase Epitaxy

Hexagonal BN (h-BN) has emerged as an important ultrawide bandgap (UWBG) semiconductor (Eg~6 eV). The crystal growth technologies for producing semi-bulk crystals/epilayers in large wafer sizes and understanding of defect properties lag decades behind conventional III-nitride wide bandgap (WBG) semiconductors. Here we report probing of boron vacancy (VB)-related defects in freestanding h-BN semi-bulk wafers synthesized by hydride vapor phase epitaxy (HVPE). A photocurrent excitation spectroscopy (PES) was designed to monitor the transport of photoexcited holes from deep-level acceptors. A dominant transition line at 1.66 eV with a side band near 1.62 eV has been directly observed, which matches well with the calculated energy levels of 1.65 for the VB-H deep acceptor in h-BN. The identification of VB complexes via PES measurement was further corroborated by the temperature-dependent dark resistivity and secondary ion mass spectrometry measurements. The results presented here suggested that it is necessary to focus on the optimization of V/III ratio during HVPE growth to minimize the generation of VB-related defects and to improve the overall material quality of h-BN semi-bulk crystals. The work also provided a better understanding of how VB complexes behave and affect the electronic and optical properties of h-BN.

36 MATERIALS SCIENCE↗
DOE OSTI2024

Light-Induced Charge Separation in Photosystem I from Different Biological Species Characterized by Multifrequency Electron Paramagnetic Resonance Spectroscopy

Photosystem I (PSI) serves as a model system for studying fundamental processes such as electron transfer (ET) and energy conversion, which are not only central to photosynthesis but also have broader implications for bioenergy production and biomimetic device design. In this study, we employed electron paramagnetic resonance (EPR) spectroscopy to investigate key light-induced charge separation steps in PSI isolated from several green algal and cyanobacterial species. Following photoexcitation, rapid sequential ET occurs through either of two quasi-symmetric branches of donor/acceptor cofactors embedded within the protein core, termed the A and B branches. Using high-frequency (130 GHz) time-resolved EPR (TR-EPR) and deuteration techniques to enhance spectral resolution, we observed that at low temperatures prokaryotic PSI exhibits reversible ET in the A branch and irreversible ET in the B branch, while PSI from eukaryotic counterparts displays either reversible ET in both branches or exclusively in the B branch. Furthermore, we observed a notable correlation between low-temperature charge separation to the terminal [4Fe-4S] clusters of PSI, termed F A and F B , as reflected in the measured F A /F B ratio. These findings enhance our understanding of the mechanistic diversity of PSI’s ET across different species and underscore the importance of experimental design in resolving these differences. Though further research is necessary to elucidate the underlying mechanisms and the evolutionary significance of these variations in PSI charge separation, this study sets the stage for future investigations into the complex interplay between protein structure, ET pathways, and the environmental adaptations of photosynthetic organisms.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2024

Carbon Dioxide Pressure and Catalyst Quantity Dependencies in Artificial Photosynthesis of Hydrocarbon Chains on Nanostructured Co/CoO Surfaces

In this study, we investigated the influence of pressure and the quantity of Co/CoO catalyst on an artificial photosynthesis process that converts CO 2 and H 2 O into hydrocarbons (C n H 2n+2 , where n ≤ 18). The adsorption of CO 2 and H 2 O on Co/CoO surfaces proved to be pivotal in this photo-catalytic reaction. Photoexcited carbon dioxide and water molecules ((CO 2 )* and (H 2 O)*) generated by illuminating the catalyst surface led to the formation of alkene hydrocarbon molecules with carbon numbers following an approximate Poisson distribution. The optimal pressure was found to be 0.40 MPa. Pressure less than 0.40 MPa resulted in low CO 2 adsorption, impeding excitation for photosynthesis. At greater pressure, oil/wax accumulation on Co/CoO surfaces hindered CO 2 adsorption, limiting further photosynthesis reactions. The average number of carbon atoms in the hydrocarbons and hydrocarbon yield were correlated. The amount of Co/CoO was also found to affect the hydrocarbon yield. Our study contributes to the understanding of Co/CoO-catalyzed photosynthesis and suggests that an open-flow system could potentially enhance the productivity of long-chain hydrocarbons.

59 BASIC BIOLOGICAL SCIENCES↗
DOE OSTI2025

Driving Electron Transfer in Photosystem I Using Far-Red Light: Overall Perspectives

Photosystem I (PSI) is a photosynthetic protein–pigment complex that, upon photoexcitation, transfers electrons to ferredoxin, facilitating the production of NADPH. Isolated PSI reaction centers (RCs) have also been used in hybrid systems to reduce protons and produce ‘biohydrogen’. This review article examines how various cyanobacteria with similar photosynthetic machinery utilize different wavelengths of light to execute photosynthetic electron transport through PSI. Key factors, such as, the structure of the electron transfer cofactors, the protein environment surrounding the primary donor pigments and hydrogen-bonding interactions with the surrounding protein matrix are analyzed to understand their roles in maintaining efficient electron transfer when it is driven using photons of different energies. We compare PSI complexes with known atomic structures from four species of cyanobacteria, Thermosynechococcus elongatus, Acaryochloris marina, Halomicronema hongdechloris, and Fischerella thermalis. T. elongatus is typical of most oxygenic photosynthetic organisms in that it requires visible light and uses only chlorophyll a (Chl a ) in PSI. In contrast, H. hongdechloris and F. thermalis are photoacclimating species capable of producing Chl f and Chl d that use red light when little visible light is available. A. marina , on the other hand, is adapted to red light conditions and consistently utilizes Chl d as its primary photosynthetic pigment, maintaining a stable pigment composition. Here, we explore the structural and functional differences between the PSI RCs of these organisms and the impact of these differences on electron transport. The structural differences in the cofactors influence both the absorption wavelengths of the cofactors and the energy levels of the intermediate states of electron transfer. An analysis of the surrounding protein shows how it has been adapted and underscores the interplay between the pigment structure, protein environment, and hydrogen bonding networks in tuning the efficiency and adaptability of photosynthetic mechanisms across different species of cyanobacteria.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2023

Beyond n-dopants for organic semiconductors: use of bibenzo[ d ]imidazoles in UV-promoted dehalogenation reactions of organic halides

2,2’-Bis(4-dimethylaminophenyl)- and 2,2'-dicyclohexyl-1,1',3,3'-tetramethyl-2,2',3,3'-tetrahydro-2,2'-bibenzo[ d ]imidazole ((N-DMBI) 2 and (Cyc-DMBI) 2 ) are quite strong reductants with effective potentials of ca. −2 V vs ferrocenium/ferrocene, yet are relatively stable to air due to the coupling of redox and bond-breaking processes. Here, we examine their use in accomplishing electron transfer-induced bond-cleavage reactions, specifically dehalogenations. The dimers reduce halides that have reduction potentials less cathodic than ca. −2 V vs ferrocenium/ferrocene, especially under UV photoexcitation (using a 365 nm LED). In the case of benzyl halides, the products are bibenzyl derivatives, whereas aryl halides are reduced to the corresponding arenes. The potentials of the halides that can be reduced in this way, quantum-chemical calculations, and steady-state and transient absorption spectroscopy suggest that UV irradiation accelerates the reactions via cleavage of the dimers to the corresponding radical monomers.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
NASA NTRS1972

Photocapacitance effects at a Cu2S-CdS heterojunction.

The influence of trapped charge on the photovoltaic properties of an efficient Cu2S-CdS single-crystal heterojunction has been studied by a photocapacitance technique. For the nonheat-treated cell, a persistent increment in capacitance as high as 70% of the dark capacitance remained after illumination of the junction by band-gap light at 100 K. The additional capacitance is due to holes trapped in deep levels in the CdS depletion region near the interface. The trapped holes enhanced the 100 K photocurrent spectrum uniformly by a factor of 3 before heat treatment. After a 200 C heat treatment in air, the maximum trapped charge at 100 K enhanced the photocurrent by two orders of magnitude. The results are interpreted in terms of the tunneling through a conduction band spike of electrons photoexcited in the Cu2S.

Lindquist, P. F.↗
NASA NTRS1973

Laser scanner for testing semiconductor chips

Individual ''fingerprint'' signals are produced when system photoexcites chips. ''Fingerprints'' are analyzed for characteristics associated with defects, including many not visible to the naked eye. Electromagnetic radiation photogenerates free electrons and holes in semiconductor chip. These carriers produce electrical signals at terminals. Signals vary depending on what defects are present.

Hall, T. C.↗
NASA NTRS1974

Development of ultraviolet lasers

The pulsed electron accelerator selected for use in the development of ultraviolet laser capability suitable for use in photoexcitation and photoionization studies of the upper atmosphere is reported. Performance figures, installation specifications, and total cost of the equipment are briefly shown, and plans for further studies are outlined.

Walters, G. K.↗
NASA NTRS1974

Heat treatment effects in Cu2S-CdS heterojunction photovoltaic cells

The dependence of the short-circuit current on photon energy, temperature, and the state of optical degradation (or enhancement) is determined in a study of the photovoltaic properties of Cu2S-CdS single-crystal heterojunctions. A coherent formulation is proposed for the relationship between enhancement and optical degradation and for their effects on the transport of a short-circuit photoexcited current and dark forward-bias current in a photovoltaic cell. Optical degradation in a Cu2S-CdS cell is shown to be identical to the optical degradation of lifetime in a homogeneous CdS:Cd:Cu crystal.

Fahrenbruch, A. L.↗
NASA NTRS1974

Separation of surface and bulk minority-carrier lifetimes in silicon

A photoexcitation technique is suggested which is direct and convenient, requiring little special equipment. No change in the dimensions of the crystal sample is necessary. Although related to the technique of interposing a filter between the light source and the sample, it differs in that the filter is part of the crystal itself. Basically, one of the electrodes is split into two electrodes, one collecting charge from carriers excited in the bulk. This phenomenon in which the carriers follow very closely the electric field lines has been used in position-sensitive semiconductor radiation detectors (Norbeck and Carlson, 1963) but has not been applied to lifetime measurements. In a sense, the split electrode creates a sample without a surface.

Carroll, K. A.↗
NASA NTRS1974

Possible H2/+/ ultraviolet spectrum of Jupiter

An ultraviolet spectral probe for a hydrogen-rich planetary atmosphere, such as that of Jupiter, is suggested, utilizing discrete lines in the H2(+) 2p pi u - /s sigma g electronic transition. For the Jovian atmosphere, the dominant mechanism for exciting H2(+) to its 2p pi u state appears to be photoexcitation, principally through absorption of the solar Lyman-alpha line. The critical role of corrections to the Born-Oppenheimer approximation in the use of an H2(+) probe is discussed.

Wu, F.-M.↗
NASA NTRS1975

OSO-7 results on coronal emission near 304 A

The spectral composition and spatial distribution of equatorial coronal emission near 304 A is examined. Spectral scans indicate that the predominant line is from Si XI. Comparisons of observations with calculations of intensity changes with altitude indicate that collisional excitation is important near the sun but that photoexcitation becomes dominant beyond about 1.3 solar radii from the solar center. Observed and calculated intensities are in approximate agreement for abundances and electron densities that are within the range of observed values.

Nakada, M. P.↗
NASA NTRS1976

Post sunset behavior of the 6300 A atomic oxygen airglow emission

A theoretical model of the 6300 A OI airglow emission was developed based on the assumptions that both the charged and neutral portions of the Earth's upper atmosphere are in steady state conditions of diffusive equilibrium. Intensities of 6300 A OI emission line were calculated using electron density true height profiles from a standard C-4 ionosonde and exospheric temperatures derived from Fabry-Perot interferometer measurements of the Doppler broadened 6300 A emission line shape as inputs to the model. Reaction rate coefficient values, production mechanism efficiencies, solar radiation fluxes, absorption cross sections, and models of the neutral atmosphere were varied parametrically to establish a set of acceptable inputs which will consistently predict 6300 A emission intensities that closely agree with intensities observed during the post-sunset twilight period by an airglow observatory consisting of a Fabry-Perot interferometer and a turret photometer. Emission intensities that can only result from the dissociative recombination of molecular oxygen ions were observed during the latter portion of the observational period. Theoretical calculations indicate that contamination of the 6300 A OI emission should be on the order of or less than 3 percent; however, these results are very sensitive to the wavelengths of the individual lines and their intensities relative to the 6300 A OI intensity. This combination of a model atmosphere, production mechanism efficiencies, and quenching coefficient values was used when the dissociative photoexcitation and direct impact excitation processes were contributing to the intensity to establish best estimates of solar radiation fluxes in the Schumann--Runge continuum and associated absorption cross sections. Results show that the Jacchia 1971 model of the upper atmosphere combined with the Ackerman recommended solar radiation fluxes and associated absorption cross sections produces theoretically calculated intensities that more closely agree with the observed intensities than all the other combinations.

Smith, R. E.↗
NASA NTRS1976

Coronal temperatures and temperature gradients from OSO-7 spectroheliograms

Temperatures and temperature gradients for the outer corona are obtained from brightness gradients of EUV lines that were measured with the spectroheliograph on OSO-7. Brightness gradients show considerable deviations from isothermal model calculations that include collisional excitation and photoexcitation. A negative temperature gradient that gives both positive and negative ion-abundance gradients appears to be able to account for the discrepancy. For the 284-A of Fe XV, perhaps the strongest line from the outer corona, measurements during 1972 appear to be consistent with a temperature near 2.3 million K near the equator at about 1.3 solar radii from the solar center and with temperature-gradient values near -0.7 that extend from as low as 1.2 to about 1.8 solar radii. Temperatures from strong lines of Fe XIV and Fe XVI indicate that variations of about 200,000 K exist along lines of sight where emission is appreciable. There appears to be some agreement between these results and temperature measurements from ion abundances in the solar wind and the Doppler width of the 5303-A line.

Nakada, M. P.↗
NASA NTRS1978

Solar photolysis of water

A cyclic process is described for the solar photolysis of water, including a first stage in which water is reduced in the presence of a Eu(+2) photooxidizable reagent producing hydrogen and spent oxidized Eu(+3) reagent. The spent reagent Eu(+3) is reduced by means of a transition metal ligand complex reductant, RuL(+3) in a photoexcited state, such as a ruthenium pyridyl complex. Due to competing reactions between the photolysis and regeneration products, the photooxidation reaction must be separated from the regeneration in space and time by supporting the reagent and/or the reductant on solid supports and utilizing pH, wavelength and flow control to maximize hydrogen and oxygen production.

Ryason, P. R.↗