Si photocathode with Ag-supported dendritic Cu catalyst for CO2 reduction

Si photocathodes integrated with Ag-supported dendritic Cu catalysts are used to perform light-driven reduction of CO2 to C2 and C3 products in aqueous solution. A back illumination geometry with an n-type Si absorber was used to permit the use of absorbing metallic catalysts. Selective carrier collection was accomplished by a p+ implantation on the illumination side and an n+ implantation followed by atomic layer deposition of TiO2 on the electrolyte site. The Ag-supported dendritic Cu CO2 reduction catalyst was formed by evaporation of Ag followed by high-rate electrodeposition of Cu to form a high surface area structure. Under simulated 1 sun illumination in 0.1 M CsHCO3 saturated with CO2, the photovoltage generated by the Si (∼600 mV) enables C2 and C3 products to be produced at -0.4 vs. RHE. Texturing of both sides of the Si increases the light-limited current density, due to reduced reflection on the illumination side, and also deceases the onset potential. Under simulated diurnal illumination conditions photocathodes maintain over 60% faradaic efficiency to hydrocarbon and oxygenate products (mainly ethylene, ethanol, propanol) for several days. After 10 days of testing, contamination from the counter electrode is observed, which causes an increase in hydrogen production. This effect is mitigated by a regeneration procedure which restores the original catalyst selectivity. A tandem, self-powered CO2 reduction device was formed by coupling a Si photocathode with two series-connected semitransparent CH3NH3PbI3 perovskite solar cells, achieving an efficiency for the conversion of sunlight to hydrocarbons and oxygenates of 1.5% (3.5% for all products)

Deterministic Assembly of Arrays of Lithographically Defined WS2 and MoS2 Monolayer Features Directly from Multilayer Sources into Van der Waals Heterostructures

One of the major challenges in the van der Waals (vdW) integration of two-dimensional (2D) materials is achieving high-yield and high-throughput assembly of predefined sequences of monolayers into heterostructure arrays. Mechanical exfoliation has recently been studied as a promising technique to transfer monolayers from a multilayer source synthesized by other techniques, allowing the deposition of a wide variety of 2D materials without exposing the target substrate to harsh synthesis conditions. Although a variety of processes have been developed to exfoliate the 2D materials mechanically from the source and place them deterministically onto a target substrate, they can typically transfer only either a wafer-scale blanket or one small flake at a time with uncontrolled size and shape. Here, we present a method to assemble arrays of lithographically defined monolayer WS2 and MoS2 features from multilayer sources and directly transfer them in a deterministic manner onto target substrates. This exfoliate-align-release process - without the need of an intermediate carrier substrate - is enabled by combining a patterned, gold-mediated exfoliation technique with a new optically transparent, heat-releasable adhesive. WS2/MoS2 vdW heterostructure arrays produced by this method show the expected interlayer exciton between the monolayers. Light-emitting devices using WS2 monolayers were also demonstrated, proving the functionality of the fabricated materials. Our work demonstrates a significant step toward developing mechanical exfoliation as a scalable dry transfer technique for the manufacturing of functional, atomically thin materials

Formation of diluted III–V nitride thin films by N ion implantation

iluted III–Nₓ–V₁ˍₓ alloys were successfully synthesized by nitrogen implantation into GaAs,InP, and AlyGa1−yAs. In all three cases the fundamental band-gap energy for the ion beam synthesized III–Nₓ–V₁ˍₓ alloys was found to decrease with increasing N implantation dose in a manner similar to that observed in epitaxially grownGaNₓAs1−x and InNₓP₁ˍₓalloys. In GaNₓAs₁ˍₓ the highest value of x (fraction of “active” substitutional N on As sublattice) achieved was 0.006. It was observed that NAs is thermally unstable at temperatures higher than 850 °C. The highest value of x achieved in InNₓP₁ˍₓ was higher, 0.012, and the NP was found to be stable to at least 850 °C. In addition, the N activation efficiency in implantedInNₓP₁ˍₓ was at least a factor of 2 higher than that in GaNₓAs₁ˍₓ under similar processing conditions. AlyGa1−yNₓAs₁ˍₓ had not been made previously by epitaxial techniques. N implantation was successful in producing AlyGa1−yNₓAs₁ˍₓalloys. Notably, the band gap of these alloys remains direct, even above the value of y (y>0.44) where the band gap of the host material is indirect.This work was supported by the ‘‘Photovoltaic Materials Focus Area’’ in the DOE Center of Excellence for the Synthesis and Processing of Advanced Materials, Office of Science, Office of Basic Energy Sciences, Division of Materials Sciences under U.S. Department of Energy Contract No. DE-ACO3-76SF00098. The work at UCSD was partially supported by Midwest Research Institute under subcontractor No. AAD-9-18668-7 from NREL

Host isotope mass effects on the hyperfine interaction of group-V donors in silicon

The effects of host isotope mass on the hyperfine interaction of group-V donors in silicon are revealed by pulsed electron nuclear double resonance (ENDOR) spectroscopy of isotopically engineered Si single crystals. Each of the hyperfine-split P-31, As-75, Sb-121, Sb-123, and Bi-209 ENDOR lines splits further into multiple components, whose relative intensities accurately match the statistical likelihood of the nine possible average Si masses in the four nearest-neighbor sites due to random occupation by the three stable isotopes Si-28, Si-29, and Si-30. Further investigation with P-31 donors shows that the resolved ENDOR components shift linearly with the bulk-averaged Si mass.Comment: 5 pages, 4 figures, 1 tabl

Electron-phonon renormalization of electronic band gaps of semiconductors: Isotopically enriched silicon

Photoluminescence and wavelength-modulated transmission spectra displaying phonon-assisted indirect excitonic transitions in isotopically enriched Si-28, Si-29, Si-30, as well as in natural Si, have yielded the isotopic mass (M) dependence of the indirect excitonic gap (E-gx) and the relevant phonon frequencies. Interpreting these measurements on the basis of a phenomenological theory for (partial derivativeE(gx)/partial derivativeM), we deduce E-gx(M=infinity)=(1213.8+/-1.2) meV, the purely electronic value in the absence of electron-phonon interaction and volume changes associated with anharmonicity

Band offset determination of the GaAs/GaAsN interface using the DFT method

The GaAs/GaAsN interface band offset is calculated from first principles. The electrostatic potential at the core regions of the atoms is used to estimate the interface potential and align the band structures obtained from respective bulk calculations. First, it is shown that the present method performs well on the well-known conventional/conventional AlAs/GaAs (001) superlattice system. Then the method is applied to a more challenging nonconventional/conventional GaAsN/GaAs (001) system, and consequently type I band lineup and valence-band offset of about 35 meV is obtained for nitrogen concentration of about 3 %, in agreement with the recent experiments. We also investigate the effect of strain on the band lineup. For the GaAsN layer longitudinally strained to the GaAs lattice constant, the type II lineup with a nearly vanishing band offset is found, suggesting that the anisotropic strain along the interface is the principal cause for the often observed type I lineup

Aperiodic dynamical decoupling sequences in presence of pulse errors

Dynamical decoupling (DD) is a promising tool for preserving the quantum states of qubits. However, small imperfections in the control pulses can seriously affect the fidelity of decoupling, and qualitatively change the evolution of the controlled system at long times. Using both analytical and numerical tools, we theoretically investigate the effect of the pulse errors accumulation for two aperiodic DD sequences, the Uhrig's DD UDD) protocol [G. S. Uhrig, Phys. Rev. Lett. {\bf 98}, 100504 (2007)], and the Quadratic DD (QDD) protocol [J. R. West, B. H. Fong and D. A. Lidar, Phys. Rev. Lett {\bf 104}, 130501 (2010)]. We consider the implementation of these sequences using the electron spins of phosphorus donors in silicon, where DD sequences are applied to suppress dephasing of the donor spins. The dependence of the decoupling fidelity on different initial states of the spins is the focus of our study. We investigate in detail the initial drop in the DD fidelity, and its long-term saturation. We also demonstrate that by applying the control pulses along different directions, the performance of QDD protocols can be noticeably improved, and explain the reason of such an improvement. Our results can be useful for future implementations of the aperiodic decoupling protocols, and for better understanding of the impact of errors on quantum control of spins.Comment: updated reference

Evolution of Testing Algorithms at a University Hospital for Detection of Clostridium difficile Infections

We present the evolution of testing algorithms at our institution in which the C. Diff Quik Chek Complete immunochromatographic cartridge assay determines the presence of both glutamate dehydrogenase and Clostridium difficile toxins A and B as a primary screen for C. difficile infection and indeterminate results (glutamate dehydrogenase positive, toxin A and B negative) are confirmed by the GeneXpert C. difficile PCR assay. This two-step algorithm is a cost-effective method for highly sensitive detection of toxigenic C. difficile

Phosphoramidite-controlled asymmetric hydrogenation with rhodium catalysts

Phosphoramidites, and in particular those derived from BINOL, the MonoPhos family of ligands, have proven extremely useful for the asymmetric hydrogenation of carbon-carbon unsaturation using a rhodium catalyst. Many classes of alkenes can be reduced by these catalyst systems. The use of high-throughput experimentation can be applied to the synthesis of MonoPhos ligands and their subsequent screening, in order to find an appropriate candidate for a specific transformation. Suitable mixtures of ligands can also be found by these high-throughput methods