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Accelerated Cu2O Reduction by Single Pt Atoms at the Metal-Oxide Interface§
The reducibility of metal oxides, when serving as the catalyst support or the active sites themselves, plays an important role in heterogeneous catalytic reactions. Here we present an integrated experimental and theoretical study that reveals how the addition of small amounts of atomically dispersed Pt at the metal/oxide interface dramatically enhances the reducibility of a Cu2O thin film by H2. X-ray photoelectron spectroscopy (XPS) and temperature-programmed desorption (TPD) results reveal that upon oxidation, a PtCu single-atom alloy (SAA) surface is covered by a thin Cu2O film and is therefore unable to dissociate H2. Despite this, in situ studies using ambient pressure (AP) XPS reveal that the presence of a small amount of Pt under the oxide layer can, at the single-atom limit, promote the reduction of Cu2O by H2 at room temperature. We build two density functional theory based surface models to better understand these experimental findings: A Cu2O/Cu(111)-like surface oxide layer, known as the ‘29’ oxide, in which Pt is alloyed into the Cu(111) surface as well as a PtCu SAA. Our calculations suggest that the increased activity is due to the presence of atomically dispersed Pt under the surface oxide layer, which weakens the Cu-O bonds in its immediate vicinity, thus making the interface between subsurface Pt and the surface oxide a nucleation site for the formation of metallic Cu. This initial step in the reduction process results in the presence of surface Pt atoms surrounded by metallic Cu patches, and the Pt atoms become active in H2 dissociation, which consequently accelerates the reduction of the oxide layer. This work demonstrates how isolated Pt atoms at the metal/oxide interface of a Cu-based catalyst accelerate the reduction of the oxide and, therefore, helps maintain the active, reduced state of the catalyst under reaction conditions, as is required for the synthesis of methanol from CO2 hydrogenation.
Non-adiabatic molecular dynamics by accelerated semiclassical Monte Carlo
Non-adiabatic dynamics, where systems non-radiatively transition between electronic states, plays a crucial role in many photo-physical processes, such as fluorescence, phosphorescence, and photoisomerization. Methods for the simulation of non-adiabatic dynamics are typically either numerically impractical, highly complex, or based on approximations which can result in failure for even simple systems. Recently, the Semiclassical Monte Carlo (SCMC) approach was developed in an attempt to combine the accuracy of rigorous semiclassical methods with the efficiency and simplicity of widely used surface hopping methods. However, while SCMC was found to be more efficient than other semiclassical methods, it is not yet as efficient as is needed to be used for large molecular systems. Here, we have developed two new methods: the accelerated-SCMC and the accelerated-SCMC with re-Gaussianization, which reduce the cost of the SCMC algorithm up to two orders of magnitude for certain systems. In most cases shown here, the new procedures are nearly as efficient as the commonly used surface hopping schemes, with little to no loss of accuracy. This implies that these modified SCMC algorithms will be of practical numerical solutions for simulating non-adiabatic dynamics in realistic molecular systems.
Electron Bulk Acceleration and Thermalization at Earth’s Quasiperpendicular Bow Shock [Electron Acceleration and Thermalization at Earth's Quasi-Perpendicular Bow Shock]
Electron heating at Earth’s quasiperpendicular bow shock has been surmised to be due to the combined effects of a quasistatic electric potential and scattering through wave-particle interaction. Here we report the observation of electron distribution functions indicating a new electron heating process occurring at the leading edge of the shock front. Incident solar wind electrons are accelerated parallel to the magnetic field toward downstream, reaching an electron-ion relative drift speed exceeding the electron thermal speed. The bulk acceleration is associated with an electric field pulse embedded in a whistler-mode wave. The high electron-ion relative drift is relaxed primarily through a nonlinear current-driven instability. Here, the relaxed distributions contain a beam traveling toward the shock as a remnant of the accelerated electrons. Similar distribution functions prevail throughout the shock transition layer, suggesting that the observed acceleration and thermalization is essential to the cross-shock electron heating.
Overall Performance Losses and Activated Mechanisms in Double Glass and Glass-backsheet Photovoltaic Modules with Monofacial and Bifacial PERC Cells, under Accelerated Exposures
Commercial PV modules have various packaging choices nowadays, which influence their long-term reliability. This study compared the degradation behaviors of sixteen module variants from two brands with varying encapsulant materials (EVA or POE), encapsulant types, module architectures (GB or DG), and cell types (monofacial or bifacial) using null hypothesis testing to determine statistical significant findings. The modules were exposed for 2,520 hours under two accelerated exposures: modified damp heat (mDH) and modified damp heat with full-spectrum light (mDH+FSL). For both brands, two DG module variants with UV-Cutoff rear encapsulant are found to have significantly lower average power loss than the module variants of EVA+GB with opaque rear encapsulant after each accelerated exposure. Metallization interconnect corrosion is identified as the primary degradation mechanism. Furthermore, unsupervised hierarchical clustering finds that the degradation behaviors of modules from one brand with a more strict manufacturing quality control depends on module architectures only.
Unexpected Scaling of Peak Acceleration for a Yielding Mass-Spring System Subjected to a Triangular Base Acceleration Pulse
The use of bounding scenarios is a common practice that greatly simplifies the design and qualification of structures. However, this approach implicitly assumes that the quantities of interest increase monotonically with the input to the structure, which is not necessarily true for nonlinear structures. This paper surveys the literature for observations of nonmonotonic behavior of nonlinear systems and finds such observations in both the earthquake engineering and applied mechanics literature. Numerical simulations of a single degree-of-freedom mass-spring system with an elastic–plastic spring subjected to a triangular base acceleration pulse are then presented, and it is shown that the relative acceleration of this system scales nonmonotonically with the input magnitude in some cases. The equation of motion for this system is solved symbolically and an approximate expression for the relative acceleration is developed, which qualitatively agrees with the nonmonotonic behavior seen in the numerical results. The nonmonotonicity is investigated and found to be a result of dynamics excited by the discontinuous derivative of the base acceleration pulse, the magnitude of which scales nonmonotonically with the input magnitude due to the fact that the first yield of the spring occurs earlier as the input magnitude is increased. The relevance of this finding within the context of defining bounding scenarios is discussed, and it is recommended that modeling be used to perform a survey of the full range of possible inputs prior to defining bounding scenarios.
Accelerated Springtime Melt of Snow on Tundra Downwind from Northern Alaska River Systems Resulting from Niveo-aeolian Deposition Events
It is well known that light-absorbing particulate matter (PM) enhances absorption of sunlight when deposited on ice and snow. Such increased absorption is due to a reduction in surface albedo, resulting in accelerated melt of frozen surfaces. In isolation, earlier melt enhances Arctic warming since dark surfaces underlying snow and ice are exposed and absorb additional solar energy. Here, we combine various observational tools to demonstrate that aeolian deposition of PM along fluvial features on the North Slope of Alaska resulted in a notable reduction of surface albedo in the spring of 2016, from values typical for snow (~0.8) to around 0.35 on average. This reduction resulted in accelerated snow and ice melt by up to three weeks compared to unaffected areas. This phenomenon was observed to some degree in 12 other years dating back to 2003. Deposition generally was found to occur near particular sections of the rivers, with several areas affected by events in multiple years. In all years, the deposition is attributed to high wind events. The extreme case in 2016 is linked to unusually strong and extraordinarily persistent winds during April. The deposited material is thought to be the natural sediment carried by the rivers, resulting in a seasonally replenished source of PM. These findings indicate a previously unreported impact of both fluvial and atmospheric processes on the seasonal melt of northern Alaska rivers.
Evaluate data lake design for the accelerator control system
Increasing precision in automation for modern particle accelerators not only creates a requirement to gather data from all devices but also demands scalable and high-performance data infrastructure with the capability of handling vast incoming device data. A well architected data lake is suitable for such a system which integrates real-time data acquisition, transient data caching, and long-term storage. This paper evaluates data lake architecture for an Accelerator Control System (ACS), focusing on two critical components of a data lake, data cache and long-term storage.
APOLLO: a facility-scale differentiable virtual accelerator at Fermilab FAST/IOTA
As the design complexity of modern accelerators grows, there is more interest in using advanced simulations that have fast execution time or yield additional insights like gradients. The FAST/IOTA facility has been working on implementing and experimentally validating an end-to-end digital twin that is both fast and gradient-aware, allowing for rapid prototyping of new software and experiments with minimal beam time costs. Our framework integrates physics and ML codes for linac and ring simulation through a set of generic interfaces between surrogate and physics-based sections. To reproduce device inputs and outputs, system state is exposed as a deterministic event loop in a specialized discrete event simulator architecture. Because Fermilab is undergoing control system transition, several APIs were implemented as final user interfaces - a fully asynchronous EPICS soft IOC, a gRPC-based Data Pool Manager (DPM), and legacy ACNET protocols. We discuss implementation details as well as challenges handling live data assimilation and future plans to extend modelling to main complex proton accelerators like PIPII and Booster.
Implementation of a 1550-nm laser system for beam characterization at the Argonne Wakefield Accelerator
Accurately recording an electron bunch’s longitudinal profile is an important diagnostic for wakefield accelerators employing shaped bunches to increase transformer ratios. Electro-optic sampling of terahertz radiation from the bunch is an attractive approach due to its non-destructive nature. In preparation for future characterization experiments, the Argonne Wakefield Accelerator test facility has recently installed a 1550 nm laser system, including the necessary support systems to synchronize with the photoinjector laser system at 81.25 MHz. We report here on the initial installation and synchronization demonstrations.
Cosmic-ray acceleration by stellar winds. II - The spectrum of accelerated particles
Consideration is given to the spectrum of particles accelerated at a stellar wind terminal shock and, at the same time, modulated by convection and diffusion in the stellar wind and decelerated by adiabatic expansion of the unshocked wind. It is noted that a proper study of this problem combines the whole of the cosmic-ray modulation problem with first-order Fermi acceleration at the shock due to repeated diffusive scattering across the shock. The modulation aspect of the model described here is much simpler than modern models of modulation alone; this makes it possible to derive illustrative analytical expressions for the accelerated spectra. Particular cases of monoenergetic and truncated power laws are computed. Energy losses and convective modulation compete with acceleration at the shock so effectively in this model that enhancement of the background cosmic-ray flux by a factor of more than 2 is extremely unlikely.
Second-phase acceleration versus second-step acceleration in solar flares
Solar hard-X-ray and gamma-ray observations are reviewed that make it possible to distinguish two phases and two steps of energetic electron and ion acceleration in solar flares. A distinction is made between second-phase and second-step acceleration of electrons, protons, and heavy nuclei in flares, and the impulsive acceleration of flare protons is discussed. Hard-X-ray and gamma-ray time profiles of a solar flare are examined in detail. It is proposed that in flares producing impulsive gamma rays, energetic protons and heavy nuclei are accelerated by the second-step mechanism.
Shock acceleration of diffuse ions at the earth's bow shock Acceleration efficiency and A/Z enhancement
Observations of particle spectra, intensity, and enhancement of alpha particles over protons at diffuse ion events at the quasi-parallel earth bow shock are compared to a Monte Carlo simulation of diffusive shock acceleration. The simulation includes the back reaction of accelerated particles on the shock structure, particle escape at an upstream free escape boundary, and a low energy per nucleon threshold for thermal leakage of downstream, shock-heated particles into the upstream region. The simulation assumes that the same scattering operator that gives rise to shock acceleration can also describe a viscous shock governed by hydrodynamic turbulence. This implies that accelerated ions can be drawn directly from the thermal solar wind with no separate superthermal seed population. Good agreement between the simulation and observations made during nearly radial magnetic field configurations lends support to thermal leakage of downstream, shock-heated ions as the mode of injection for diffusion ion events.
Modeling of Particle Acceleration at Multiple Shocks Via Diffusive Shock Acceleration: Preliminary Results
We present preliminary results from a model that diffusively accelerates particles at multiple shocks. Our basic approach is related to box models (Protheroe and Stanev, 1998; Moraal and Axford, 1983; Ball and Kirk, 1992; Drury et al., 1999) in which a distribution of particles is diffusively accelerated inside the box while simultaneously experiencing decompression through adiabatic expansion and losses from the convection and diffusion of particles outside the box (Melrose and Pope, 1993; Zank et al., 2000). We adiabatically decompress the accelerated particle distribution between each shock by either the method explored in Melrose and Pope (1993) and Pope and Melrose (1994) or by the approach set forth in Zank et al. (2000) where we solve the transport equation by a method analogous to operator splitting. The second method incorporates the additional loss terms of convection and diffusion and allows for the use of a variable time between shocks. We use a maximum injection energy (Emax) appropriate for quasi-parallel and quasi-perpendicular shocks (Zank et al., 2000, 2006; Dosch and Shalchi, 2010) and provide a preliminary application of the diffusive acceleration of particles by multiple shocks with frequencies appropriate for solar maximum (i.e., a non-Markovian process).
Numerical Modeling of Ion-Optical Systems for Extraction of a Beam of Negative Hydrogen Ions and Its Acceleration and Matching with a Radio-Frequency Quadrupole Accelerator
A source of negative hydrogen ions is constructed at the Institute for High Energy Physics in order to raise the intensity of the U-70 accelerator complex using multiturn charge-exchange injection. The 3D ion-optical IBSimu simulation package was used to model and optimize the system for extraction of an ion beam from plasma, its acceleration to 100 keV, and matching with a radio-frequency quadrupole (RFQ) accelerator. The system of extraction of an ion beam with a current of 50 mA and electron-flow suppression was modeled. The magnetic transport channels with two solenoids and six quadrupole lenses were compared. The end goals of analysis of the matching channel were to obtain the needed Twiss parameters and to minimize the emittance growth at the RFQ input.
Accelerated Electron-Beam Formation with a High Capture Coefficient in a Parallel Coupled Accelerating Structure
An electron beam with a high (close to 100%) coefficient of electron capture into the regime of acceleration has been obtained in a linear electron accelerator based on a parallel coupled slow-wave structure, electron gun with microwave-controlled injection current, and permanent-magnet beam-focusing system. The high capture coefficient was due to the properties of the accelerating structure, beam-focusing system, and electron-injection system. Main characteristics of the proposed systems are presented.
Advanced surface treatments for medium-velocity superconducting cavities for high-accelerating gradient continuous-wave operation
Not Available
Near monochromatic 20 Me V proton acceleration using fs laser irradiating Au foils in target normal sheath acceleration regime
A 200 mJ laser pulse energy, 39 fs-pulse duration, 10 μm focal spot, p-polarized radiation has been employed to irradiate thin Au foils to produce proton acceleration in the forward direction. Gold foils were employed to produce high density relativistic electrons emission in the forward direction to generate a high electric field driving the ion acceleration. Measurements were performed by changing the focal position in respect of the target surface. Proton acceleration was monitored using fast SiC detectors in time-of-flight configuration. A high proton energy, up to about 20 Me V, with a narrow energy distribution, was obtained in particular conditions depending on the laser parameters, the irradiation conditions, and a target optimization.