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At least 235 records · Page 13

Structure–Activity Relationships for Ethanol Dehydrogenation to Acetaldehyde by Silica-Supported Zinc Oxide Catalysts

Silica-supported ZnO efficiently catalyzes the nonoxidative dehydrogenation of ethanol to acetaldehyde, which is relevant for production of 1,3-butadiene from bioethanol. Characterization with in situ spectroscopies under dehydrated conditions (high sensitivity-low energy ion scattering (HS-LEIS), diffuse reflectance (DR) UV–vis, X-ray absorption spectroscopy (XAS), diffuse reflectance Fourier transform infrared spectroscopy (DRIFTS), inelastic neutron scattering (INS), and UV Raman), and ammonia adsorption probed by temperature-programmed desorption followed by DRIFTS and mass spectrometry (DRIFTS-MS NH 3 -TPD), and DFT calculations revealed that the supported ZnO x phase was present as isolated surface ZnO x sites on SiO 2 , with the vast majority coordinated by two siloxane bonds and one silicon atom with two nonbridging oxygens ((≡SiO) 2 Zn 2+ O 2 Si=), anchored at 4-, 5-, and 6-membered siloxane rings. A minor fraction of surface ZnO x sites possessed Lewis acidity, and even fewer sites possessed a Bro̷nsted acidic Zn(OH) + Si moiety. Ethanol temperature-programmed surface reaction-mass spectrometry (TPSR-MS) with various oxidative or ethanol reaction pretreatments indicated that only sites with Lewis and Bro̷nsted acidic character (Zn(OH) + Si) were active for ethanol dehydrogenation, while the majority surface (≡SiO) 2 Zn 2+ O 2 Si= sites were inactive. Greater heterogeneity among all surface ZnO x sites, as assessed by in situ DR UV–vis spectroscopy, was associated with a greater number of ZnO x sites that were active for ethanol dehydrogenation as well as lower enthalpic barriers for acetaldehyde production among the most active surface ZnO x sites. Turnover frequencies and the apparent activation energy for ethanol dehydrogenation were determined from steady-state kinetics. Together, these findings suggested that anchoring inactive surface (≡SiO) 2 Zn 2+ O 2 Si= sites on the silica support caused a greater number of active surface ZnO x sites to adopt a more strained configuration, promoting ethanol dehydrogenation catalysis. Pretreatments and catalysts that promoted desorption of ethanol during TPSR, taken as a marker of surface dehydroxylation, were associated with an increased number of the most active surface (Zn(OH) + Si) sites. Such findings suggested that inactive surface ZnO x sites were activated for ethanol dehydrogenation by dehydroxylation of the support and/or decreased coordination to hemilabile siloxane ligands.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Solid state NMR Investigation of Structural Differences in Pelletized DEB Samples

Upon hydrogenation of DEB pellets, which are composed of 75% virgin DEB and 25% of nanometer scale Pd catalysts on activated carbon, the uptake rate is strong, and the hydrogenation process is fast. However, the last batch of DEB pellets from KCNSC uptakes 10 times slower than traditional DEB pellets after ~ 50% consumption. In addition, the last batch of DEB getter pellets also became partially molten/wet during the hydrogenation process. This molten/wet phase during hydrogenation has only been observed with DPB and never with DEB formulation. DRIFT (diffuse reflection infrared Fourier transform) and XRD (x-ray diffraction) confirm that the questionable batch of DEB pellets from KCNSC are truly 100% DEB and not a mixture of DEB and DPB. So, there must be something different in the composition (like concentration and distribution of Pd) or interaction between the DEB molecules with the surrounding environment (activated carbon spreading medium). The possibility of some chemical contamination in the processing of this batch of questionable DEB getter pellets also comes to mind. Due to the ability of NMR to detect intermolecular interaction and sensitivity to small chemical concentration, NMR investigation was requested for this questionable batch of DEB getter pellets from KCNSC.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Applying Linear Optics from Closed Orbits Modulation for finding beam-based alignment of harmonic sextupoles

A fast and accurate beam-based alignment (BBA) method for harmonic sextupoles has been devel oped at NSLS-II using Linear Optics from Closed Orbit Modulation (LOCOM). The approach excites the beam with simultaneous sine-wave signals at two fast correctors, chosen with an appropriate phase advance to span the full betatron phase space. This strategy suppresses systematic errors from hysteresis, while additional errors from orbit drift and power-supply calibration are minimized by the short measurement time (a few minutes) and reliance solely on beam-based current-to-field conver sion of the sextupoles, with hysteresis explicitly included. Simulations indicate that Linear Optics from Closed Orbits (LOCO) combined with 0.5 mm local orbit bumps can resolve relative sextupole field offsets (∆k₂) with precision better than 10% of k₂, reflecting to beam-based alignment (BBA) accuracy finer than 50 µm. Moreover, employing machine-learning-optimized local orbit bumps en hances sextupole-induced quadrupole signals in a deterministic manner and maintains orbit stability under large sextupole strength variations (±40%). The proposed method is experimentally validated through proof-of-principle measurements at NSLS-II, demonstrating its potential as a fast, precise, and robust tool for harmonic sextupole alignment.

43 PARTICLE ACCELERATORS↗

Relativistic electron precipitation during magnetic storm main phase

Relativistic electrons can have cyclotron resonances with electromagnetic cyclotron waves. The resonant energy is generally well above 1 MeV throughout the magnetosphere, but it can fall to 1 MeV just within the plasmapause. This also corresponds to the region where ring current (10 to 50 keV) protons are expected to be strongly unstable. The resulting ion cyclotron wave amplitudes necessary to precipitate ring current protons leads to electron lifetimes near the strong diffusion limit ( 100 sec). Thus, 1 MeV electrons whose drift orbits intersect the stormtime plasmapause should rapidly be precipitated in the region 3 L 5 during the initial phase of a magnetic storm.

Thorne, R. M.↗

Cross-tail ion drift in a realistic model magnetotail

By integrating the exact equations of motion, particle orbits have been followed in a good model magnetospheric field consisting of a planetary dipole, forward magnetosphere, and magnetotail current system. Proton energies from 2 eV to 20 keV were used for the full range of equatorial pitch angles and phase. Despite considerable pitch angle scattering in the equatorial plane crossings, it is found, first, that the bounce-averaged cross-tail drift velocity is approximately independent of pitch angle. Second, it is found that, averaged over initial gyrophase, the drift velocity (due to field curvature and gradient) is proportional to proton energy and is given to good approximation by adiabatic approximations, even up to 20 keV, despite the extreme lack of meeting the adiabatic criteria.

Propp, K.↗

Satellite measurements through the center of a substorm surge

Measurements have been made of electric and magnetic fields, plasma drifts, and electron precipatation within a surge at the westward, leading edge of the auroral 'bulge' at the peak of the substorm expansion phase. The trajectroy of the Dynamics Explorer 2 (DE 2) satellite over the auroral emissions is determined from nearly simultaneous observations with the imager on the DE 1 satellite at a higher altitude. The electric field and plasma drift measurements have enabled us to deduce the basic configuration of the ionospheric electric potential, or plasma convection, around the surge. The electric potential shows that the bulge is associated with a protrusion of the dawn convection cell into the dusk cell, poleward of the 'Harang discontinity.' This protrusion conains a westward electric field that strongly enhances the westard electrojet current by the creation of a "Cowling channel.' This westward electric field, and the associated Cowling current, appear to terminate within the surge, which contains an intense, upward field-aligned current. The magneitc field measurements show that the region containing this field-aligned current is shaped more like a cylinger rather than a long sheet. The total is found to exceed one-half million amperes.

Weimer, D. R.↗

Optimizing 4d Emittance Measurements Using the Pinhole Scan Technique

Accurate measurement of electron beam emittance is essential for optimizing high-brightness electron sources. The Pinhole Scan Technique measures the 4D phase space and hence the emittance by measuring the beam profile after clipping the beam using a pinhole followed by a drift section and then scanning the beam over the pinhole. This technique has been implemented in low energy (< 200 keV) beamlines at both Cornell University and Arizona State University. However, the technique poses several practical challenges. In this work, we analyze and address key issues affecting the 4D phase space and emittance measurements using this technique. We identify and investigate sources of inaccuracies like the pinhole aspect ratio, beam divergence, position-momentum correlations in the phase space, and the point-spread-function of the detector and suggest techniques to minimize them. Our findings offer a pathway to more accurate 4D phase space characterization in advanced electron beam systems.

42 ENGINEERING↗

A Kinetic Monte Carlo Approach for Simulating Cascading Transmission Line Failure

In this work, cascading transmission line failures are studied through a dynamical model of the power system operating under fixed conditions. The power grid is modeled as a stochastic dynamical system where first-principles electromechanical dynamics are excited by small Gaussian disturbances in demand and generation around a specified operating point. In this context, a single line failure is interpreted in a large deviation context as a first escape event across a surface in phase space defined by line security constraints. The resulting system of stochastic differential equations admits a transverse decomposition of the drift, which leads to considerable simplification in evaluating the quasipotential (rate function) and, consequently, computation of exit rates. Tractable expressions for the rate of transmission line failure in a restricted network are derived from large deviation theory arguments and validated against numerical simulations. Extensions to realistic settings are considered, and individual line failure models are aggregated into a Markov model of cascading failure inspired by chemical kinetics. Cascades are generated by traversing a graph composed of weighted edges representing transitions to degraded network topologies. Numerical results indicate that the Markov model can produce cascades with qualitative power-law properties similar to those observed in empirical cascades.

Kinetic Monte Carlo, rare events, Cascading Failur↗

Injection Locking of Gigahertz‐Frequency Surface Acoustic Wave Phononic Crystal Oscillator

Low-noise gigahertz (GHz) frequency sources are essential for applications in signal processing, sensing, and telecommunications. Surface acoustic wave (SAW) resonator-based oscillators offer compact form factors and low-phase noise due to their short mechanical wavelengths and high-quality (Q) factors. However, their small footprint makes them vulnerable to environmental variation, resulting in their poor long-term frequency stability. Injection locking is widely used to suppress frequency drift of lasers and oscillators by synchronizing to an ultra-stable reference. Here, injection locking of a 1-GHz SAW phononic-crystal oscillator is demonstrated, achieving 40-dB phase noise reduction at low offset frequencies and unperturbed low noise at large offset frequencies. Compared to a free-running SAW oscillator, which typically exhibits frequency drifts of several hundred hertz over minutes, the injection-locked oscillator reduces the frequency deviation to below 0.35 Hz. The locking range and oscillator dynamics is also investigated in the injection pulling region. The demonstrated injection-locked SAW oscillator could find applications in high-performance portable telecommunications and sensing systems.

injection locking↗

Quantifying the Contribution of Microbursts to Global Electron Loss in the Radiation Belts

We use the Solar, Anomalous, and Magnetospheric Particle Explorer to explore the relationship between microbursts and global flux decay of electrons from the outer Van Allen belt during the recovery phase of geomagnetic storms. We investigate the correlation between microbursts and global electron loss in each of the quasi‐trapped (drift loss cone), stably trapped, and untrapped electron (bounce loss cone) populations. For the quasi‐trapped electrons, we separately classify the storms as driven by coronal mass ejections or corotating interaction regions and explore their connection to microburst loss. We find that the decay lifetime of electron fluxes, that is, e‐folding times of macroscopic fluxes in the recovery phase is correlated with strong microburst activity. That is, when the microburst activity is high, global flux decay times are short, and vice versa, suggesting a cross‐scale coupling between microloss and macroloss phenomena. Furthermore, we find that the microburst to global loss coupling is predominant in the quasi‐trapped population of radiation belt electrons while having negligible influence on the untrapped and stably trapped populations. We find that microburst activity during storms driven by coronal mass ejections is coupled more strongly with global flux decay as compared with corotating interaction regions. In addition, we find that distance from the plasmapause is likely a better indicator of microburst location than L‐shell, with most microbursts occurring ~0.5–2.0 L from the model plasmapause location.

Greeley, A. D.↗

Effect of parallel flow on resonant layer responses in high beta plasmas

Abstract Resonant layers in a tokamak respond to non-axisymmetric magnetic perturbations by amplifying the mode amplitude and balancing the plasma rotation through magnetic reconnection and force balance, respectively. This resonant response can be characterized by local layer parameters and especially by a single quantity in the linear regime, the so-called inner-layer Δ. The computation of Δ under two-fluid drift-MHD formalism has been progressed by reducing the order of the system in the phase space, where the shielding current is approximated as being only carried by electrons, a posteriori . In this study, we relax the approximation and compute Δ accounted for by the parallel flow associated with the ion shielding current. The posteriori is numerically verified in great agreement with the original SLAYER developed in a previous paper (J.-K. Park 2022 Phys. Plasmas 29 072506). Extending the resonant layer response theory to high β plasmas, our research findings answer two important questions: how the parallel flow influences the resonant layer response and why the parallel flow effect appears in high β plasmas. The complicated plasma compression in high β regime allows the parallel flow response to give rise to the ion shielding current, which not only shifts the zero-crossing condition of the ExB flow but also enhances the field penetration threshold. Technically, the Riccati matrix transformation method is adapted to handle the numerical stiffness due to the increased order of the system. The high fidelity of this numerical method makes use of further extension of the model to higher-order systems to take other physical phenomena into account. This work is envisaged to predict the resonant layer response under high β fusion reactor conditions.

Lee, Yeongsun (ORCID:000000034474416X)↗

Super-Resolution Ptychography with Small Segmented Detectors

To overcome the spatial resolution limit set by aperture-limited diffraction in traditional scanning transmission electron microscopy, microscopists have developed ptychography enabled by iterative phase retrieval algorithms and high-dynamic-range pixel array detectors. Current detector designs are limited by the data rate off chip, so a high-pixel-count detector has a proportionally lower frame rate than the few-segment detectors used for differential phase contrast (DPC) imaging. This slower acquisition speed leads to heightened vulnerability to scan noise, drift, and potential sample damage. This creates opportunities for repurposing fast segmented detectors for ptychography by trading a reduction in reciprocal space pixels for an increase in real space pixels. Here, we explore a strategy of oversampling in real space and instead apply detector pixel upsampling during the reconstruction process. Further, we demonstrate the viability of achieving super-resolution ptychography on thin objects using only 2 × 2 detector pixels, surpassing the resolution of integrated DPC (iDPC) imaging. With optimization using simulated datasets and experiments on MoTe 2 /WSe 2 bilayer moiré superlattices, we achieved super-resolution ptychography reconstructions under rapid acquisition conditions (37.5 pA, 1 μs dwell time), yielding over 50% improvements in contrast and information limit compared to annular dark field and iDPC imaging on the same detectors.

2D materials↗

Quantum nonlocal modulation cancelation with distributed clocks

We demonstrate nonlocal modulation of entangled photons with truly distributed radio frequency (RF) clocks. Leveraging a custom radio-over-fiber (RFoF) system characterized via classical spectral interference, we validate its effectiveness for quantum networking by multiplexing the RFoF clock with one photon from a frequency-bin-entangled pair and distributing the coexisting quantum-classical signals over fiber. Phase modulation of the two photons reveals nonlocal correlations in excellent agreement with theory: in-phase modulation produces additional sidebands in the joint spectral intensity, while out-of-phase modulation is nonlocally canceled. Our simple, feedback-free design attains subpicosecond synchronization—namely, drift less than ~0.5 ps in a 5.5 km fiber over 30 min (fractionally only ~2×10 -8 of the total fiber delay)—and should facilitate frequency-encoded quantum networking protocols such as high-dimensional quantum key distribution and entanglement swapping, unlocking frequency-bin qubits for practical quantum communications in deployed metropolitan-scale networks.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Drift and observations in cosmic-ray modulation, 1

It is illustrated that a relative simple drift model can, in contrast with no drift models, simultaneously fit proton and electron spectra observed in 1965-66 and 1977, using a single set of modulation parameters except for a change in the IMF polarity. This result is interpreted together with the observation of Evenson and Meyer that electrons are recovering more rapidly than protons after 1980, in contrast with what Burger and Swanenburg observed in 1968-72, as a charge sign dependent effect due to the occurrence of drift in cosmic ray modulation. The same set of parameters produces a shift in the phase and amplitude of the diurnal anisotropy vector, consistent with observations in 1969-71 and 1980-81.

Potgieter, M. S.↗

Three-wave coupling coefficient in a drifting bi-Maxwellian plasma

A general electrostatic coupling coefficient which satisfies the Manley-Rowe relations is used to derive an explicit expression for the resonant three-wave coupling coefficient between electrostatic normal modes of a uniformly magnetized, infinite, homogeneous plasma with species described by drifting bi-Maxwellian distribution functions. The limit of this expression is taken when the phase velocities of the three waves are much larger than a species thermal speed, and also when the phase velocities are much smaller than the thermal speed. These are fluid limits and are applicable to the three-wave interaction between some low-frequency electrostatic waves, such as ion acoustic and ion cyclotron modes, in a plasma where T(e) is much greater than T(i).

Bergmann, Rachelle↗

Pd/Cr Strain Gauges For High Temperatures

Temperature-compensated Pd/Cr electrical-resistance strain gauges measure static strains in combustors, blades, and vanes of gas turbine engines. Made of alloy of 87 weight percent Pd and 13 weight percent Cr. Microstructure highly stable; undergoes no transformation of phase between ambient temperature and 1,000 degrees C. Gives highly repeatable readings with low drift at temperatures from ambient to 600 degrees C.

Lei, Jih-Fen↗

Recurrent structures of the interplanetary magnetic field observed by Ulysses

Since its launch in October 1990, Ulysses has provided good quality magnetic field data, practically covering the whole time interval until now. We have studied the very long time scale evolution of the interplanetary magnetic field, in particlular, we have search for recurrent disturbances in the magnetic field. The magnetic field vectors have been mapped back to the Sun along Parker spirals, in order to determine the Heliographic longitude of the source regions in the corona. It was found that the position of many high field sources drifts systematically relative to the corona assumed to rotate with the equatorial rotation period of the Sun. The results are compared to similar observations on the eastward drift of magnetic sectors observed after about June 1992. Changes associated with both the declining phase of the solar cycle and the latitudinal excursion of Ulysses are also discussed.

Erdos, G.↗

Investigation of Arctic Cloud Properties and Surface Radiation Based on MOSAiC Shipborne Observations

The Arctic is rapidly changing due to changes of the Earth system. This study investigates cloud fraction, phase partition, cloud type, and their relationships with surface radiation based on yearlong shipborne observations in the Arctic regions. The Multidisciplinary drifting Observatory for the Study of Arctic Climate (MOSAiC) campaign provided lidar and radar observations of cloud microphysical properties and surface shortwave (SW) and longwave (LW) radiation. Cloud and radiative properties were examined at daily and monthly resolutions in four seasons. Low clouds were found to be most prevalent throughout the year, followed by deep clouds. The ice phase is the dominant phase except for summer (June–August). Liquid and mixed phases show more significant monthly and annual mean radiative effects in SW and LW than the ice phase. The clouds show net warming effects due to LW heating in most months, while the SW cooling effects of clouds become more dominant for July and August. The cloud and radiation observations from MOSAiC were used to evaluate simulations of the atmospheric component of the Energy Exascale Earth System Model version 2. The simulations show large overestimations of the liquid and mixed phases in the Arctic regions from February to September. The simulations also underestimate the percentages of low clouds and overestimate the percentages of deep clouds throughout the year. Altogether, this work provides a unique analysis of cloud and radiation properties based on high-resolution shipborne observations, which can be used to assist future model evaluation and development.

58 GEOSCIENCES↗