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At least 793 records · Page 44

Introducing Nonstructural Ligands to Zirconia-like Metal–Organic Framework Nodes To Tune the Activity of Node-Supported Nickel Catalysts for Ethylene Hydrogenation [Introducing Nonstructural Ligands to Zirconia-like MOF Nodes To Tune the Activity of Node-Supported Nickel Catalysts for Ethylene Hydrogenation]

Previous work has shown that introduction of hexafluoroacetylacetone (Facac) units as nonstructural ligands for the zirconia-like nodes of the eight-connected metal-organic framework (MOF), NU-1000, greatly alters the selectivity of node-supported oxy-nickel clusters for ethylene dimerization vs oligomerization. Here we i explore a related concept: tuning of support/catalyst interactions, and therefore, catalyst activity, via parallel installation of organic modifiers on the support itself. As modifiers we focused on para-substituted benzoates (R-BA – ; R = -NH 2 , -OCH 3 , -CH 3 , -H, -F, and -NO 2 ) where the substituents were chosen to present similar steric demand, but varying electron-donating or electron-withdrawing properties. R-benzoate-engendered shifts in the node-based aqua O-H stretching frequency for NU-1000, as measured by DRIFTS (diffuse-reflectance infrared Fourier-transform spectroscopy), together with systematic shifts in Ni 2p peak energies, as measured by X-ray photoelectron spectroscopy, show that the electronic properties of the support can be modulated. The vibrational and electronic peak shifts correlate with the putative electron-withdrawing vs electron-donating strength of the para-substituted benzoate modifiers. Subsequent installation of node-supported, oxy-Ni(II) clusters for ethylene hydrogenation yield a compelling correlation between log (catalyst turnover frequency) and the electron donating or withdrawing character of the substituent of the benzoate units. Single crystal X-ray diffraction measurements reveal that each organic modifier makes use of only one of two available carboxylate oxygens to accomplish grafting. The remaining oxygen atom is, in principle, well positioned to coordinate directly to an installed Ni(II) ion. We postulate that the unanticipated direct coordination of the catalyst by the node-modifier (rather than indirect modifier-based tuning of support(node)/catalyst electronic interactions) is the primary source of the observed systematic tuning of hydrogenation activity. Here we suggest, however, that regardless of mechanism for communication with active-sites of MOF-supported catalysts, intentional elaboration of nodes via grafted, nonstructural organic species could prove to be a valuable general strategy for fine-tuning supported-catalyst activity and/or selectivity.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Compact magnetograph

A compact magnetograph system based on solid Fabry-Perot interferometers as the spectral isolation elements was studied. The theory of operation of several Fabry-Perot systems, the suitability of various magnetic lines, signal levels expected for different modes of operation, and the optimal detector systems were investigated. The requirements that the lack of a polarization modulator placed upon the electronic signal chain was emphasized. The PLZT modulator was chosen as a satisfactory component with both high reliability and elatively low voltage requirements. Thermal control, line centering and velocity offset problems were solved by a Fabry-Perot configuration.

Title, A. M.↗

Experimental Study of Synchro-Betatron Coupling Induced By Dipole Modulation

Synchro-betatron coupling in a proton storage ring with electron cooling was studied experimentally by modulating a transverse dipole field close to the synchrotron frequency. The combination of the electron cooling and transverse field modulation on the synchrotron oscillation is equivalent to a dissipative parametric resonant system. The proton bunch was observed to split longitudinally into two pieces, or beamlets, converging toward attractors of the dissipative system. These phenomena might be important in understanding the effect of ground vibration on the Superconducting Super Collider beam, and the effect of power supply ripple on the Relativistic Heavy-Ion Collider beam.

43 PARTICLE ACCELERATORS↗

Giant Undulations Driven by Pitch‐Angle Scattering of Time Domain Structures Modulated by Plasmapause Surface Wave

Abstract Plasmapause surface waves (PSWs) near the plasmapause boundary are regarded to be the magnetospheric source of ionospheric auroral giant undulations (GUs) located at the equatorward boundary of diffuse aurora. However, the observational evidence of wave‐particle interaction connecting PSWs and GUs is absent. In this letter, we demonstrate GUs are driven by pitch‐angle scattering of time domain structures modulated by the PSWs, based on the conjugated ionospheric and magnetospheric observations. Specifically, ionospheric GUs are lighted by the pitch‐angle scattering of <1 keV thermal electron and ions and energetic ions with energy up to dozens of keV near the plasmapause. Further, the total fluxes during one PSW period and energy of scattered electron and ions determine the size and luminosity of GUs. Our research provides observational evidence that PSWs cause periodic electron precipitation via modulating the time domain structures rather than the previously predicted chorus or electron cyclotron harmonic waves.

Zhou, Yi‐Jia [Weihai Institute for Interdisciplina↗

Electrostatically transparent graphene quantum-dot trap layers for efficient nonvolatile memory

In this study, we have demonstrated nonvolatile memory devices using graphene quantum-dots (GQDs) trap layers with indium zinc oxide (IZO) semiconductor channel. The Fermi-level of GQD was effectively modulated by tunneling electrons near the Dirac point because of limited density of states and weak electrostatic screening in monolayer graphene. As a result, large gate modulation was driven in IZO channel to achieve a subthreshold swing of 5.21 V/dec (300 nm SiO{sub 2} gate insulator), while Au quantum-dots memory shows 15.52 V/dec because of strong electrostatic screening in metal quantum-dots. Together, discrete charge traps of GQDs enable stable performance in the endurance test beyond 800 cycles of programming and erasing. Our study suggests the exciting potential of GQD trap layers to be used for a highly promising material in non-volatile memory devices.

77 NANOSCIENCE AND NANOTECHNOLOGY↗

Well‐Dispersed Nickel‐ and Zinc‐Tailored Electronic Structure of a Transition Metal Oxide for Highly Active Alkaline Hydrogen Evolution Reaction

Abstract The practical scale‐up of renewable energy technologies will require catalysts that are more efficient and durable than present ones. This is, however, a formidable challenge that will demand a new capability to tailor the electronic structure. Here, an original electronic structure tailoring of CoO by Ni and Zn dual doping is reported. This changes it from an inert material into one that is highly active for the hydrogen evolution reaction (HER). Based on combined density functional theory calculations and cutting‐edge characterizations, it is shown that dual Ni and Zn doping is responsible for a highly significant increase in HER activity of the host oxide. That is, the Ni dopants cluster around surface oxygen vacancy of the host oxide and provide an ideal electronic surface structure for hydrogen intermediate binding, while the Zn dopants distribute inside the host oxide and modulate the bulk electronic structure to boost electrical conduction. As a result, the dual‐doped Ni, Zn CoO nanorods achieve current densities of 10 and 20 mA cm −2 at overpotentials of, respectively, 53 and 79 mV. This outperforms reported state‐of‐the‐art metal oxide, metal oxide/metal, metal sulfide, and metal phosphide catalysts.

Ling, Tao↗

Reducing Radiation Damage in Soft Matter with Femtosecond-Timed Single-Electron Packets

In spite of the development of a myriad of mitigation methods, radiation damage continues to be a major limiting factor in transmission electron microscopy. Intriguing results have been reported using pulsed-laser driven and chopped electron beams for modulated dose delivery, but the underlying relationships and effects remain unclear. Indeed, delivering precisely timed single-electron packets to the specimen has yet to be systematically explored, and no direct comparisons to conventional methods within a common parameter space have been made. Here, using a model linear saturated hydrocarbon (n-hexatriacontane, C 36 H 74 ), we show that precisely timed delivery of each electron to the specimen, with a well-defined and uniform time between arrival, leads to a repeatable reduction in damage compared to conventional ultralow-dose methods for the same dose rate and the same accumulated dose. Using a femtosecond pulsed laser to confine the probability of electron emission to a 300 fs temporal window, we find damage to be sensitively dependent on the time between electron arrival (controlled with the laser repetition rate) and on the number of electrons per packet (controlled with the laser-pulse energy). Relative arrival times of 5, 20, and 100 μs were tested for electron packets comprised of, on average, 1, 5, and 20 electrons. In general, damage increased with decreasing time between electrons and, more substantially, with increasing electron number. Further, we find that improvements relative to conventional methods vanish once a threshold number of electrons per packet is reached. The results indicate that precise electron-by-electron dose delivery leads to a repeatable reduction in irreversible structural damage, and the systematic studies indicate this arises from control of the time between sequential electrons arriving within the same damage radius, all else being equal.

36 MATERIALS SCIENCE↗

High-mobility capacitively-induced two-dimensional electrons in a lateral superlattice potential

In the presence of a lateral periodic potential modulation, two-dimensional electrons may exhibit interesting phenomena, such as a graphene-like energy-momentum dispersion, Bloch oscillations, or the Hofstadter butterfly band structure. To create a sufficiently strong potential modulation using conventional semiconductor heterostructures, aggressive device processing is often required, unfortunately resulting in strong disorder that masks the sought-after effects. Here, we report a novel fabrication process flow for imposing a strong lateral potential modulation onto a capacitively induced two-dimensional electron system, while preserving the host material quality. Using this process flow, the electron density in a patterned Si/SiGe heterostructure can be tuned over a wide range, from 4.4 × 10 10 cm –2 to 1.8 × 10 11 cm –2 , with a peak mobility of 6.4 × 10 5 cm 2 /V·s. The wide density tunability and high electron mobility allow us to observe sequential emergence of commensurability oscillations as the density, the mobility, and in turn the mean free path, increase. Magnetic-field-periodic quantum oscillations associated with various closed orbits also emerge sequentially with increasing density. We show that, from the density dependence of the quantum oscillations, one can directly extract the steepness of the imposed superlattice potential. Lastly, this result is then compared to a conventional lateral superlattice model potential.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Controlling resonant tunneling in graphene via Fermi velocity engineering

We investigate the resonant tunneling in a single layer graphene superlattice with modulated energy gap and Fermi velocity via an effective Dirac-like Hamiltonian. We calculate the transmission coefficient with the transfer matrix method and analyze the effect of a Fermi velocity modulation on the electronic transmission, in the case of normal and oblique incidence. We find it is possible to manipulate the electronic transmission in graphene by Fermi velocity engineering, and show that it is possible to tune the transmitivity from 0 to 1. We also analyze how a Fermi velocity modulation influences the total conductance and the Fano factor. Our results are relevant for the development of novel graphene-based electronic devices.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Electronics Systems for the Gamma Ray Energy Tracking Nuclear Array (GRETA)

The Gamma Ray Energy Tracking Nuclear Array (GRETA), a 4-π germanium detector system capable of measuring energy and position (within better than 2mm rms) of gamma-ray interaction points and tracking multiple gamma-ray interactions, is being designed. GRETA is composed of 30 detector modules, each with four high purity germanium crystals. Four electronics modules will support the operation of the detectors: the Digitizer Module, the Signal Filter Board and the Trigger and Timing Modules. The Digitizer Module converts the analog information with analog to digital converters operating at 100 MS/s and sends the conversions through fiber optics to the Signal Filter Board. The Signal Filter Board digitally processes the data to determine the energy and timing information of the gamma interactions within a crystal. The Digitizer and Signal Filter Board send trigger information to the Trigger System. Different trigger algorithms for trigger decision are planned for the Trigger System. The Timing System provides the clock for the electronics systems and auxiliary detectors. In this paper we review the details of the planned GRETA Electronics System.

data acquisition↗

Squeezing the periodicity of Néel-type magnetic modulations by enhanced Dzyaloshinskii-Moriya interaction of 4d electrons

In polar magnets, such as GaV 4 S 8 , GaV 4 Se 8 and VOSe 2 O 5 , modulated magnetic phases namely the cycloidal and the Néel-type skyrmion lattice states were identified over extended temperature ranges, even down to zero Kelvin. Our combined small-angle neutron scattering and magnetization study shows the robustness of the Néel-type magnetic modulations also against magnetic fields up to 2 T in the polar GaMo 4 S 8 . In addition to the large upper critical field, enhanced spin-orbit coupling stabilize cycloidal, Néel skyrmion lattice phases with sub-10 nm periodicity and a peculiar distribution of the magnetic modulation vectors. Moreover, we detected an additional single-q state not observed in any other polar magnets. Thus, our work demonstrates that non-centrosymmetric magnets with 4d and 5d electron systems may give rise to various highly compressed modulated states.

36 MATERIALS SCIENCE↗

A non-uniform three-gap buncher cavity with suppression of transverse-electromagnetic mode leakage in the triaxial klystron amplifier

The triaxial klystron amplifier is an efficient high power relativistic klystron amplifier operating at high frequencies due to its coaxial structure with large radius. However, the coaxial structures result in coupling problems among the cavities as the TEM mode is not cut-off in the coaxial tube. Therefore, the suppression of the TEM mode leakage, especially the leakage from the buncher cavity to the input cavity, is crucial in the design of a triaxial klystron amplifier. In this paper, a non-uniform three-gap buncher cavity is proposed to suppress the TEM mode leakage. The cold cavity analysis shows that the non-uniform three-gap buncher cavity can significantly suppress the TEM mode generation compared to a uniform three-gap buncher cavity. Particle-in-cell simulation shows that the power leakage to the input cavity is less than 1.5‰ of the negative power in the buncher cavity and the buncher cavity can efficiently modulate an intense relativistic electron beam free of self-oscillations. A fundamental current modulation depth of 117% is achieved by employing the proposed non-uniform buncher cavity into an X-band triaxial amplifier, which results in the high efficiency generation of high power microwave.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

All-Optical Photochromic Spatial Light Modulators

Photochemical transfer of electrons enables fast reading and writing. New concept based on transfer of electrons between donor and acceptor molecules randomly distributed or covalently linked and dispersed in glassy-polymer host material. Transfer causes significant changes in optical-transmission characteristics of material and used to modulate transmission of reading beam of light impinging on material.

Beratan, David N.↗

Aperiodic graphene ribbons in MOSFET topology for multi-wavelength terahertz generation

This paper proposes and simulates multi-wavelength terahertz wave generation using MOSFET with aperiodic gate structure. This emitter works at room temperature and spans the whole terahertz spectra. Structure of the emitter is like a MOSFET for which the channel and gate respectively consist of periodic and aperiodic graphene ribbons. By applying a DC voltage to the source and drain contacts, a DC current flows through the periodic channel. Then by applying a gate voltage to aperiodic graphene ribbons, the current is modulated with aperiodic graphene potential of the gate. The gate voltage applies aperiodic potential U(x) to channel’s electrons that subsequently modulates current of the periodic channel. The modulated current radiates coherent electromagnetic waves. By tuning parameters of the emitter, the radiated coherent electromagnetic wave is in THz range.

77 NANOSCIENCE AND NANOTECHNOLOGY↗

An X-band phase-locked relativistic backward wave oscillator

For the purpose of coherent high power microwave combining at high frequency band, an X-band phase-locked relativistic backward wave oscillator is presented and investigated. The phase-locking of the oscillator is accomplished by modulation of the electron beam before it reaches the oscillator. To produce a bunched beam with an acceptable injected RF power requirement, an overmoded input cavity is employed to provide initial density modulation. And a buncher cavity is introduced to further increase the modulation depth. When the beam enters the oscillator, the modulation depth is enough to lock the frequency and phase of the output microwave generated by the oscillator. Particle-in-cell simulation shows that an input power of 90 kW is sufficient to lock the frequency and phase of 1.5 GW output microwave with locking bandwidth of 60 MHz.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Electrically controlled spin polarization and selection in a topological insulator sandwiched between ferromagnetic electrodes

We theoretically investigate the electrically controllable spin polarization and selective efficiency of the edge state Dirac electron in a two-dimensional topological insulator (TI) sandwiched between ferromagnetic (FM) electrodes by using the method of Keldysh nonequilibrium Green's function. A nearly full spin polarization of the topological edge state with giant inversion of ∼80% is observed, which is much higher than the value previously reported. Moreover, the selective efficiency for spin-up electrons under the modulation of the parallel configuration of FM electrodes has been demonstrated to be larger than 95% for the first time, while that for spin-down electrons in the antiparallel case is higher than 90% in a wide energy range, owing to the inter-edge spin tunneling induced backscattering and spin dephasing effect. The obtained results may provide a deeper understanding of the TI edge states and a valuable guidance to design spin switch and filter with high on-off speed and selective efficiency based on TIs.

36 MATERIALS SCIENCE↗

Dual AC Dipole Excitation for the Measurement of Magnetic Multipole Strength from Beam Position Monitor Data

An experiment was conducted at Jefferson Lab's Continuous Electron Beam Accelerator Facility to develop a technique for characterizing the nonlinear fields of the beam transport system. Two air-core dipole magnets were simultaneously driven at two different frequencies to provide a time-dependent transverse modulation of the electron beam. Fourier decomposition of beam position monitor data was then used to measure the amplitude of these frequencies at different positions along the beamline. For a purely linear transport system one expects to find solely the frequencies that were applied to the dipoles with amplitudes that depend on the phase advance of the lattice. In the presence of nonlinear fields one expects to also find harmonics of the driving frequencies that depend on the order of the nonlinearity. The technique was calibrated using one of the sextupole magnets in a CEBAF beamline and then applied to a dipole to measure the sextupole and octupole strength of the magnet. A comparison is made between the beam-based measurements, results from TOSCA and data from our Magnet Measurement Facility.

43 PARTICLE ACCELERATORS↗

Strain-Modulated Slater-Mott Crossover of Pseudospin-Half Square-Lattice in ( SrIrO 3 ) 1 / ( SrTiO 3 ) 1 Superlattices

Here, we report on the epitaxial strain-driven electronic and antiferromagnetic modulations of a pseudospin-half square lattice realized in superlattices of (SrIrO 3 ) 1 /(SrTiO 3 )1. With increasing compressive strain, we find the low-temperature insulating behavior to be strongly suppressed with a corresponding systematic reduction of both the Néel temperature and the staggered moment. However, despite such a suppression, the system remains weakly insulating above the Néel transition. The emergence of metallicity is observed under large compressive strain but only at temperature far above the Néel transition. These behaviors are characteristics of the Slater-Mott crossover regime, providing a unique experimental model system of the spin-half Hubbard Hamiltonian with a tunable intermediate coupling strength.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗