In Situ X-ray Absorption Spectroscopy of Metal/Nitrogen-doped Carbons in Oxygen Electrocatalysis

Metal/nitrogen-doped carbons (M−N−C) are promising candidates as oxygen electrocatalysts due to their low cost, tunable catalytic activity and selectivity, and well-dispersed morphologies. To improve the electrocatalytic performance of such systems, it is critical to gain a detailed understanding of their structure and properties through advanced characterization. In situ X-ray absorption spectroscopy (XAS) serves as a powerful tool to probe both the active sites and structural evolution of catalytic materials under reaction conditions. In this review, we firstly provide an overview of the fundamental concepts of XAS and then comprehensively review the setup and application of in situ XAS, introducing electrochemical XAS cells, experimental methods, as well as primary functions on catalytic applications. The active sites and the structural evolution of M−N−C catalysts caused by the interplay with electric fields, electrolytes and reactants/intermediates during the oxygen evolution reaction and the oxygen reduction reaction are subsequently discussed in detail. Finally, major challenges and future opportunities in this exciting field are highlighted.</p

A new method to measure true two-photoncorrelation of soft X-ray synchrotronradiation

Two-photon correlation measurement provides a promising way to experimentally demonstrate the statistical nature of a light source, which is very significant for the deep understanding of the photon-generating process and the diagnosing of the coherence property. Quantitatively two- photon correlation is described by second-order coherence. Usually the behavior of the second-order coherence against any of the parameters defining the phase volume is different for different photon statistics. The Poisson photon statistics for coherent light gives its second-order coherence as a flat response; The Bose-Einstein photon statistics for chaotic light gives its second-order coherence as a bunching effect; While the Sub-Poisson photon statistics for non-classical light gives its second-order coherence as an anti-bunching effect. Therefore the measurement of two-photon correlation is proved to be a good finger print to check whether light is in coherent state or incoherent state such as thermal state or non-classical state.Historically the measurement of two-photon correlation was first performed by Hanbury-Brown and Twiss (HBT) in 1956. They used a linear mixer to realize the correlation of the two currents from the photoelectric detectors illuminated by a stationary thermal light souece, a mercury arc, and the photo-bunching effect was first successfully observed in the visible region of 435.8 nm.HBT method is no doubt a good way to extract the small excess two-photon correlation for a stationary light because the background, that is the DC components, has been cut off automatically by the broad band amplifiers, which is in fact the key of the success of HBT experiment. However there exists a general problem, to which no attention has ever been paid, in measuring the two-photon correlation of non-stationary light such as synchrotron radiation (SR) by the HBT method. Here the "non-stationary" means a sense of classical mechanics that the observed intensity has some deterministic time structure. The systematic time structure of SR decided by the bunch distribution of the electric current in a storage ring will give rise to a large amount of unexpected accidental correlation, which in fact has nothing to do with the inherent photon statistics of light source and usually l000～l0000 times larger than the true two-photon correlation due to the short bunch separation length (2ns) and the short coherence time (～0.1ps) which is not comparable to the time resolution (1ns) of the measuring system. The existence of the accidental correlation would severely prevent us from observing the bunching effect of the true two-photon correlation.Therefore to suppress the much larger accidental correlation and to extract the small true two-photon correlation, a novel intensity interferometer has been developed for soft X-ray synchrotron radiation. This intensity interferometer consists of an optical vacuum chamber and an electric correlator. All the essential optical elements which includes a wire scanner, a precise diffraction slit, a grating monochromator with a coherence time modulator, a beam divider and two fast-response photon detectors (microchannel plates) are mounted in this high vacuum chamber. The electric correlator completes the multiplication of the two broad band electric currents coming from the photoelectric detectors. The basic idea to suppress the much larger accidental correlation is to modulate the coherence time by modulating the entrance slit width of the monochromator by a piezoclectric translator. The two sets of light intensity are simultaneously modulated too. When the frequency of modulation is f, the third harmonics 3f is detected with a loch-in amplifier because the 3f components include only the true two-photon correlation. Practically it is difficult to modulate with frequency f without any higher order harmonics distortion which might add some false 3f components. To overcome this difficulty we have used a sharp bandpass filter of l00～350 MHz in each branch of the correlator, which is lower than the RF frequency 500 MHz and much higher than 1.6 MHz, the revolution frequency of the stored beam of the 2.5 GeV storage ring.This new apparatus has been operated successfully in the measurement of the horizontal two-photon correlation for the first harmonic of undulator radiation with photon energy of 70 eV at the Photon Factory, KEK. By narrowing the precise slit width which correspondingly changes the spatial coherence of the incident SR, a bunching effect of the normalized excess two-photon correlation has been clearly observed. This explicit bunching effect implies that synchrotron radiation is chaotic radiation.Further investigation shows that although second-order coherence is completely determined by the first-order coherence for the case of chaotic light, the measured information from the light source is essentially different. The two-photon correlation of synchrotron radiation does not depend on the response time of the detectors but gives the information of instantaneous emittance of the stored beam with the time scale of coherence time τC. By fitting the experimental data, the horizontal instantaneous emittance of the stored beam is estimated to be 40nmrad.This intensity interferometer can be utilized to characterize the coherence properties of incomplete FELs, such as SASE, because if they are fully coherent light sources the normalized excess two-photon correlation would have a flat response, but not showing a photon-bunching effect

Ultra-Compact Digital Metasurface Polarization Beam Splitter via Physics-Constrained Inverse Design

Inverse design effectively promotes the miniaturization of integrated photonic devices through the modulation of subwavelength structures. Utilizing a theoretical prior based inverse design, we propose an ultra-compact integrated polarizing beam splitter consisting of a standard silicon-on-insulator (SOI) substrate and a tunable air–silicon column two-dimensional code metasurface, with a footprint of 5 × 2.7 μm2. The effective refractive index of the waveguide is modulated by adjusting the two-dimensional code morphology in the additional layer to achieve efficient polarization beam splitting. The simulation results demonstrate high performance, with a low insertion loss (10.76 dB) in a bandwidth of 80 nm covering the C-band. The device can withstand manufacturing errors up to ±20 nm and is robust to process defects, such as the outer proximity effect, and thus is suitable for ultra-compact on-chip optical interconnects

Cloud–Edge Hybrid Computing Architecture for Large-Scale Scientific Facilities Augmented with an Intelligent Scheduling System

Synchrotron radiation sources are widely used in interdisciplinary research, generating an enormous amount of data while posing serious challenges to the storage, processing, and analysis capabilities of the large-scale scientific facilities worldwide. A flexible and scalable computing architecture, suitable for complex application scenarios, combined with efficient and intelligent scheduling strategies, plays a key role in addressing these issues. In this work, we present a novel cloud–edge hybrid intelligent system (CEHIS), which was architected, developed, and deployed by the Big Data Science Center (BDSC) at the Shanghai Synchrotron Radiation Facility (SSRF) and meets the computational needs of the large-scale scientific facilities. Our methodical simulations demonstrate that the CEHIS is more efficient and performs better than the cloud-based model. Here, we have applied a deep reinforcement learning approach to the task scheduling system, finding that it effectively reduces the total time required for the task completion. Our findings prove that the cloud–edge hybrid intelligent architectures are a viable solution to address the requirements and conditions of the modern synchrotron radiation facilities, further enhancing their data processing and analysis capabilities

Mutual optical intensity propagation through non-ideal two-dimensional mirrors

The mutual optical intensity (MOI) model is a partially coherent radiation propagation tool that can sequentially simulate beamline optics and provide beam intensity, local degree of coherence and phase distribution at any location along a beamline. This paper extends the MOI model to non-ideal two-dimensional (2D) optical systems, such as ellipsoidal and toroidal mirrors with 2D figure errors. Simulation results show that one can tune the trade-off between calculation efficiency and accuracy by varying the number of wavefront elements. The focal spot size of an ellipsoidal mirror calculated with 100 × 100 elements gives less than 0.4% deviation from that with 250 × 250 elements, and the computation speed is nearly two orders of magnitude faster. Effects of figure errors on 2D focusing are also demonstrated for a non-ideal ellipsoidal mirror and by comparing the toroidal and ellipsoidal mirrors. Finally, the MOI model is benchmarked against the multi-electron Synchrotron Radiation Workshop (SRW) code showing the model's high accuracy

Pressure-induced phase transition in cubic Yb2O3 and phase transition enthalpies

The high pressure structural evolution of cubic Yb2O3 has been studied using in situ synchrotron angle dispersive x-ray diffraction in combination with diamond anvil cell techniques up to 44.1 GPa. The XRD measurements revealed an irreversible reconstructive phase transition from cubic to monoclinic Yb2O3 at 11.2 GPa and extending up to 28.1 GPa with ∼8.1% volume collapse and a subsequent reversible displacive transition from monoclinic to hexagonal phase starting at 22.7 GPa. The monoclinic phase coexists with the hexagonal phase up to 44.1 GPa. After pressure releases, the hexagonal Yb2O3 reverts to the monoclinic structure. The second-order Birch–Murnaghan equation of state fit to the pressure–volume data yields a bulk modulus of 201 (4), 187 (6), and 200 (4) GPa for the cubic, monoclinic, and hexagonal phases, respectively. Furthermore, the effects of the hydrostatic pressure state on the diffraction patterns, bulk modulus, and onset transition pressure of Yb2O3 under high pressure have been discussed. It is concluded that the bulk modulus of the cubic Ln2O3 phase increases with decreasing cation radius due to lanthanide contraction. Another important work in this study is the determination of the enthalpies of the cubic to monoclinic and monoclinic to hexagonal phase transitions of Yb2O3 of 37.0 and 17.4 kJ/mol, respectively, based on the basic thermodynamic equations and using the onset transition pressures and corresponding volume changes obtained from high pressure XRD experiments

Monte Carlo simulation on a new artificial spin ice lattice consisting of hexagons and three-moment vertices

A new artificial spin ice lattice called vortex lattice is proposed based on the Kagome lattice. Monte Carlo simulations were performed to investigate the magnetization reversal process of the new artificial spin ice lattice at external magnetic field and different lattice parameters. The results demonstrate some interesting phenomena which are different from Kagome lattice. There are four typical sub-structures emerged in the vortex lattice, which are clockwise and counter-clockwise hexagons, and frustrated +3q and -3q vertices. The occurrence frequency of the four sub-structures change dramatically at different lattice parameter. The new lattice can be partially frustrated at different lattice parameter