Intense Electron Research Articles

Supramolecular Interface Buffer Layer for Stable Zinc Anode.

The aqueous zinc ion batteries (AZIBs) are chronically plagued by the inevitable side-reaction and uneven Zn planets stack. Through regulating the water activity and Zn2+ crystal dynamics could effectively relieve those anode/electrolyte interface problems. The (2-hydroxypropyl)-β-cyclodextrin (HBCD), characterized by the excluded-volume and mitigating zinc-flux aggregation effect, is chosen as the electrolyte additive to tail the anode/electrolyte interface. In this work, the supermolecule interface buffer layer is conducted to screen active water and modulate Zn crystallography. Capitalized on the intense electron density of exterior cavity, the HBCD molecules are proven to chemically adsorb onto anode, which sterically repulse the active waters and disrupt H-bonds among waters. Concurrently, the (002)-preferred texture is achieved through inducing Zn2+ ions transport and nucleation. The assembled symmetric Zn//Zn batteries show ameliorated lifespan at various current density (350h for 10mA cm-2/10mAhcm-2 and 100h for 20mA cm-2/20mAhcm-2) and steady operation at 73.26% high Depth of Discharge (DOD). The Zn//NVO batteries deliver 380.4mAhg-1 high discharge capacity at 1Ag-1. To prove the feasibility, the full battery with a low N/P ratio (2.16) is assembled, it shows ≈260mAhg-1 discharge capacity and runs stably during 500 cycles.

Amplification of O-D stimulated Raman scattering in DMSO-D2O solution via intense laser-driven electron transfer.

In this study, we investigated in detail the regulation mechanism of electron transfer under laser-induced breakdown (LIB) on weak O-D stimulated Raman scattering (SRS) in DMSO-D2O solutions. Significantly, the Raman activity of O-D vibrations was greatly enhanced by two orders of magnitude due to electron transfer in DMSO molecules. Density functional theory (DFT) calculations showed that the O-D Raman activity was significantly enhanced in the DMSO-D2O dimer compared to the D2O dimer. Additionally, the high-order (third-order) SRS peaks originating from the O-D vibration and the characteristic peaks representing the ice-like structure were detected, which were due to the Raman-enhanced four-wave mixing (FWM) process induced by the hydrated electron and intramolecular electron transfer. It was hoped that our results could provide a meaningful reference for the development of multi-wavelength and significant frequency-shifted Raman lasers.

Simulation investigation of a Ka-band phase-locked klystron-type coaxial relativistic Cherenkov generator

To achieve coherent power combination of Ka-band high-power microwave (HPM), a phase-locked klystron-type coaxial relativistic Cherenkov generator (PKC-RCG), which combines the advantageous characteristics of weak dimensional sensitivity of RCG and low input power ratio of relativistic triaxial klystron amplifier (TKA), is proposed and investigated in this paper. The PKC-RCG is composed of two parts: a pre-modulation region adapted from TKA and an energy exchange region adapted from RCG. The pre-modulation region is used for initial speed modulation of intense relativistic electron beams (IREB), ensuring that the output frequency is consistent with the input frequency. The energy exchange region is used for deep clustering of the IREB and achieving efficient beam–wave energy conversion. Phase locking of the output HPM is accomplished through phase delivery of the modulated IREB. Specially designed reflectors and cascaded single-gap bunching cavities with active suppression of asymmetric TM mode are employed in the pre-modulation region to suppress energy coupling and achieve a lower input power ratio. Disk-loaded slow-wave structure with smooth inner conductor is employed in the energy exchange region to further decrease the dimensional sensitivity of RCG. By the proposed Ka-band PKC-RCG, an HPM with a power of 550 MW and a frequency of 29.0 GHz is obtained with ohmic loss being taken into account. Moreover, the input power ratio and phase-locking bandwidth of the proposed Ka-band PKC-RCG are −51.4 dB and 30 MHz, respectively.

Observation and Reconstruction of Electron Vortex in Reconnection Outflow

AbstractOn 27 January 2017, Magnetospheric Multi‐Scale observed a series of electron vortexes, which are driven by the electron Kelvin‐Helmholtz (K‐H) instability in the reconnection outflow at terrestrial magnetopause. We find the electron vorticity can reach above 200 s−1 inside the vortexes, which is comparable to the strong vorticity events in the electron diffusion region. Using the First‐Order Taylor Expansion for Velocity field method, we further reconstruct the 3D topology of two electron vortexes and find one vortex is converging while another vortex is diverging. Interestingly, enhancement of electron temperature was observed in the diverging vortex but not in the converging vortex, indicating electron dynamics is related to the vortex topology. Our study suggests that electron K‐H vortexes formed by the intense electron shear flow in the reconnection outflow have different types of topologies and will help us better understand the reconnection picture at the terrestrial magnetopause.

Influence of electron irradiation on self‐healing and thermal oxidation of SiC dispersed yttrium silicate composites

AbstractElectron irradiation‐induced acceleration of self‐healing and high‐temperature oxidation has been discovered in SiC/Y2Si2O7–Y2SiO5 composites. Bulk samples were produced by pulsed electric current sintering. These samples were exposed to an electron beam from the pulsed intense relativistic electron beam accelerator with a beam energy of 2 MeV at irradiation doses of 10–40 kGy. The self‐healing and high‐temperature oxidation experiments were carried out at 1100–1300°C for 1–24 h in laboratory air. Electron irradiation significantly improved the self‐healing effectiveness. The closure of surface cracks was caused by the volume expansion of SiC via transformation to SiO2 and the outward diffusion of Y3+ ions. Electron irradiation also increased the thickness of the internally oxidized zone, formed by the inward diffusion of O2− ions. Enhanced self‐healing and oxidation behavior were associated with defect formation induced by electron beam exposure, which facilitated the diffusion of ions within the crystal lattice.

Acceleration of Energetic Electrons in Jovian Middle Magnetosphere by Whistler‐Mode Waves

AbstractAn abundant multi‐MeV electron population beyond the orbit of Io is required to explain the intense inner radiation belt (electrons MeV) at Jupiter and its synchrotron radiation. In order to better understand the synergistic effect of radial transport and local wave‐particle interactions driven by whistler‐mode waves on the formation of Jupiter's radiation belt, we perform 3‐D Fokker‐Planck simulations for Jovian energetic electrons with the Versatile Electron Radiation Belt code. An empirical model of Jovian whistler‐mode waves updated with measurements from the Juno extended mission is used to quantify the local acceleration and pitch angle scattering. Resonant cyclotron acceleration by whistler‐mode waves leads to significant enhancement in the intensity of electrons above 1 MeV in the middle magnetosphere. Radial diffusion is capable of transporting MeV electrons accelerated by outer‐belt whistler‐mode waves into the region, where they are further accelerated adiabatically to energies of about 10 MeV.

The evolution of coronal shock wave properties and their relation with solar energetic particles

Context. Shock waves driven by fast and wide coronal mass ejections (CMEs) are considered to be very efficient particle accelerators and are involved in the production of solar energetic particle (SEP) events. These events cause space weather phenomena by disturbing the near-Earth radiation environment. In past studies, we analysed statistically the relation between the maximum intensity of energetic electrons and protons and the properties of coronal shocks inferred at the point of magnetic connectivity. The present study focuses on a gradual SEP event measured by STEREO-A and -B on 11 October 2013. This event had the interesting properties that it (1) occurred in isolation with very low background particle intensities measured before the event, (2) was associated with a clear onset of SEPs measured in situ allowing detailed timing analyses, and (3) was associated with a fast CME event that was magnetically connected with STEREO-A and -B. These three properties allowed us to investigate at a high cadence the temporal connection between the rapidly evolving shock properties and the SEPs measured in situ. Aims. The aim of the present study is to investigate the relative roles of fundamental shock parameters such as the compression ratio, Mach number and geometry, in the intensity and composition of the associated SEP event measured in situ. Methods. We used shock reconstruction techniques and multi-viewpoint imaging data obtained by the STEREO-A and -B, SOHO, and SDO spacecraft to determine the kinematic evolution of the expanding shock wave. We then exploited 3D magneto-hydrodynamic modelling to model the geometry and Mach number of the shock wave along an ensemble of magnetic field lines connected to STEREO-A and -B, also estimating the uncertainties of the shock parameters. Using a velocity dispersion analysis of the available SEP data we time-shifted the SEP time series and analysed the relations between observed SEP properties and the modelled shock properties. We also studied the energy dependence of these relations. Results. We find a very good temporal agreement between the formation of the modelled shock wave and the estimated release times for both electrons and protons. The simultaneous release of protons and electrons suggests a common acceleration process. This early phase is marked at both STEREOs by elevated electron-to-proton ratios that coincide with the highly quasi-perpendicular phase of the shock. These findings suggest that the rapid evolution of the shock as it transits from the low to the high corona modifies the conditions under which particles are accelerated. We discuss these findings in terms of basic geometry and acceleration processes.

G-Value of Hydrogen Peroxide Generated by Water Radiolysis with Irradiation of Pulsed Intense Relativistic Electron Beam

G-Value of Hydrogen Peroxide Generated by Water Radiolysis with Irradiation of Pulsed Intense Relativistic Electron Beam

Intensive electron transfer of a single-atom Fe-based catalytic ceramic membrane for municipal wastewater treatment: The synergistic effects of nitrogen vacancy defect and ultrathin nanostructure.

The integration of membrane separation with heterogeneous advanced oxidation processes is a prospective strategy for the elimination of contaminants during wastewater treatment. Fe-based catalysts and the green oxidant peracetic acid (PAA) are desirable candidates for the development of catalytic membranes because they are environmentally friendly. However, the construction of catalytic ceramic membranes (CMs) modified with efficient Fe-based catalysts that generate increased amounts of high-valent Fe-O species during PAA activation for the degradation of specific pollutants, especially during instantaneous membrane filtration, remains challenging. Herein, a single-atom Fe-based catalytic CM was fabricated and further optimized via the "electron enrichment + electron-transfer enhancement" method, which specifically refers to the simultaneous introduction of nitrogen vacancy (Nv) defects and the construction of ultrathin nanostructures. The CM-UCNv-Fe/PAA system exhibited outstanding bisphenol A (BPA) removal performance, with a first-order rate constant of 0.078 ms-1 (4680 min-1), which was 37 times greater than that of CM-BCN-Fe/PAA system (126 min-1). In addition, the remarkable environmental adaptability, stability and low Fe leakage underscored its practical application potential. Mechanistic investigations revealed that Fe(V)=O was the predominant reactive oxygen species. Multi-scaled characterization and theoretical calculations confirmed that engineered Nv defects facilitated the construction of electron-rich single-atom Fe sites, which had the potential to supply more electrons. Porous ultrathin nanosheets exposed more Fe active sites, and many microinterfaces within the catalytic layers of the CM increased the possibility of contact between the Fe sites and PAA. The synergy of them enabled intensive electron transfer from Fe sites to PAA, which was the driving force for Fe(V)=O conversion during transient membrane filtration. In addition, the efficacy of the catalytic CM in municipal wastewater treatment and membrane fouling control were investigated. This work expands the research on the intensive electron transfer of a single-atom Fe-based catalytic CM for increased Fe(V)=O conversion via Nv defect introduction and ultrathin nanostructure construction.

The anomalous state of Uranus’s magnetosphere during the Voyager 2 flyby

The Voyager 2 flyby of Uranus in 1986 revealed an unusually oblique and off-centred magnetic field. This single in situ measurement has been the basis of our interpretation of Uranus’s magnetosphere as the canonical extreme magnetosphere of the solar system; with inexplicably intense electron radiation belts and a severely plasma-depleted magnetosphere. However, the role of external forcing by the solar wind has rarely been considered in explaining these observations. Here we revisit the Voyager 2 dataset to show that Voyager 2 observed Uranus’s magnetosphere in an anomalous, compressed state that we estimate to be present less than 5% of the time. If the spacecraft had arrived only a few days earlier, the upstream solar wind dynamic pressure would have been ~20 times lower, resulting in a dramatically different magnetospheric configuration. We postulate that such a compression of the magnetosphere could increase energetic electron fluxes within the radiation belts and empty the magnetosphere of its plasma temporarily. Therefore, the interpretation of Uranus’s magnetosphere as being extreme may simply be a product of a flyby that occurred under extreme upstream solar wind conditions.

The effect of dilution on the energy dissipation in water interstellar ice analogues

Context. Interstellar ices and their energetic processing play an important role in advancing the chemical complexity in space. Interstellar ices covering dust grains are intrinsically mixed, and it is assumed that physicochemical changes induced by energetic processing – triggered by photons, electrons, and ions – strongly depend on the content of the ice. Yet, the modelling of these complex mixed systems in experiments and theory is complicated. Aims. In this paper, we investigate the effect of infrared irradiation on a series of different molecules mixed with porous amorphous solid water (pASW) to study the release of vibrational energy in the hydrogen-bonding network of water as a function of mixing ratio and ice content. Particularly, we select mixtures of 20:1 H2O:X and 5:1 H2O:X with X=CO2, NH3, or CH4. Methods. Infrared radiation was supplied by the intense and tunable free electron laser (FEL) 2 at the HFML-FELIX facility. We monitored the structural changes in the interstellar ice analogue after resonant infrared excitation using Fourier-transform reflection absorption infrared (FT-RAIR) spectroscopy. Results. We observed that on-resonance irradiation at the OH-stretching vibration of pASW results in quantitatively identical changes compared to pure pASW for all investigated mixtures. The structural changes we observed closely resemble the previously reported local reordering. The 5:1 mixtures show weaker changes compared to pure pASW, with a decrease in strength from NH3 to CO2. Conclusions. Since the hydrogen-bonding network of pASW restructures similarly upon FEL irradiation, regardless of the mixing component, treating ice layers in models that simulate energy dissipation in the hydrogen-bonding network as pure H2O ice layers can be a justified approximation. Hence, complex systems might not always be necessary to describe the infrared energetic processing of ices.

Catalytic behavior, electronic structure and spectroscopic (FT-IR, Raman, UV–vis) properties for the new ionic liquid imidazolium hydrogen sulfate

Catalytic performance, chemical reactivity, vibrational modes and electronic transitions of the ion pair [H–Im]+[HSO4]– were investigated in the current paper. Hence, a combined experimental (Hammett acidity function, infrared, Raman and ultraviolet-visible spectroscopies) and theoretical (molecular electrostatic potential surface, reduced density gradient, frontier molecular orbital analysis, quantum theory of atoms in molecules, net atomic charges, global and local reactivity descriptors) study was conducted. In terms of the catalytic performance, the acetic acid esterification with butanol was evaluated. Important kinetic (rate constant, activation energy, pre-exponential factor) and thermodynamic (enthalpy, entropy, Gibbs free energy barrier) factors for ester production as a function of the temperature and catalyst loading have been determined. Results revealed intensive electron density distribution in [H–Im]+[HSO4]– due to chemical interactions between the cationic and anionic moieties. These bonds were established as electrostatic in nature. The pronounced charge transfers within [H–Im]+[HSO4]– managed the title compound acidity (H0) and its catalytic behavior towards butyl acetate synthesis. Using the thermodynamic and kinetic measurements, a mechanism for acetic acid esterification with butanol in the presence of imidazolium hydrogen sulfate ionic liquid was offered.

Local Time Distribution and Activity Dependence of Extreme Electron Densities in the Auroral D‐Region as an Image of Energy‐Dependent Energetic Electron Precipitation

AbstractStudying the episodes with the most elevated electron density (Ne) values provides valuable information about spatial distribution and drivers of intense energetic electron (EE) precipitation, which has important space weather implications. By combining EISCAT‐Tromso UHF observations in different modes made in 2001–2021, we survey Ne occurrences and study statistical properties of EE precipitation, producing the highest 10% and 1% of Ne values at the altitudes between 100 and 75 km (corresponding to EE energies of ∼20–∼200 keV). We found that the highest Ne values occur in the nightside‐morning local time sector at the altitudes 90–100 km and in the morning‐noon sector at low altitudes (75–85 km). Although this bimodal pattern could partly be contributed by the suppressed Ne in the dark ionosphere, by analyzing measurements in the twilight conditions at all MLTs together with published patterns of EE precipitation, we argue that a dominance of pre‐noon maximum at low altitudes reflects the enhanced precipitation of >100 keV electrons in this local time sector. At all altitudes (especially below 90 km), the appearance of the highest Ne values favors enhanced auroral activity and shows a strong correlation with fast solar wind (V > 550 km/s) events. These properties mimic the well‐known driving characteristics of energetic electrons. From the correlation of Ne with integral magnetic activity indexes we found that the memory of preceding magnetic activity increases with decreasing altitude, reaching roughly one day at H = 75 km. We discuss the advantages of exploring Ne data at specific altitudes (compared to direct measurements of EE precipitation) to investigate statistically the effects of specific precipitated energy components and the evolution of EE energy spectra.

Non-radiative recombination centres in InGaN/GaN nanowires revealed by statistical analysis of cathodoluminescence intensity maps and electron microscopy

The methodology of statistical analysis of cathodoluminescence (CL) intensity mappings on ensembles of several hundreds of InGaN/GaN nanowires (NWs) used to quantify non-radiative recombination centres (NRCs) was validated on InGaN/GaN NWs exhibiting spatially homogeneous cathodoluminescence at the scale of single NWs. Cathodoluminescence intensity variations obeying Poisson's statistics were assigned to the presence of randomly incorporated point defects acting as NRCs. Additionally, another type of NRCs, namely extended defects leading to spatially inhomogeneous cathodoluminescence intensity at the scale of single InGaN/GaN NWs are revealed by high resolution scanning transmission electron microscopy, geometrical phase analysis and two-beam diffraction conditions techniques. Such defects are responsible for deviations from Poisson's statistics, allowing one to achieve a rapid evaluation of the crystallographic and optical properties of several hundreds of NWs in a single cathodoluminescence intensity mapping experiment.

Outer Zone Relativistic Electron Response to Mesoscale Periodic Density Structures in the Solar Wind: Van Allen Probes Measurements

AbstractWe investigate the relativistic and the ultra‐relativistic outer radiation belt electron response to the Periodic Density Structures (PDS) in the solar wind. We have studied four intervals between 0000 UT and 1500 UT during 17 January 2013 interplanetary coronal mass ejection (ICME) sheath event following the passage of an interplanetary shock (IP) on 16 January, at 2240 UT. Earlier studies limited to geosynchronous orbit have shown that PDS induce Ultra‐Low‐Frequency (ULF) oscillations in the magnetosphere and modulate energetic electron intensities. Our study shows for the first time, using pitch angle resolved electron intensity measurements, that PDS modulate relativistic and ultra‐relativistic electron intensities in the heart of the radiation belts (L ≈ 4). We find that the modulation of electron intensities occur at frequencies close to those of interplanetary PDS. Furthermore, electron intensity modulations occur over a wide range of energy (≈200 keV to 4 MeV) and pitch angles (≈20–120°). This event study suggests that relativistic and ultra‐relativistic electron intensity modulations driven by PDS may be largely energy and pitch angle independent.

Electron Acceleration via Secondary Reconnection in the Separatrix Region of Magnetopause Reconnection

AbstractMagnetic reconnection is a fundamental process known to play a crucial role in electron acceleration and heating, however, the mechanism of electron energization during reconnection is still not fully understood. This study introduces a novel electron acceleration mechanism in which electrons can be accelerated by secondary reconnection in the separatrix region. The secondary reconnection occurs in a thin current sheet resulted from the shear of the out‐of‐plane Hall magnetic fields of the primary magnetopause reconnection. It results in the intense electron energy fluxes toward the primary X‐line. This mechanism will likely be an important piece in the puzzle of particle acceleration by reconnection.

Complex electron-ion-plasma surface modification of high-alloy stainless steel

The work is devoted to identification and analysis of patterns of change in the elemental and phase composition, defective substructure, mecha­nical (microhardness) and tribological (wear resistance and friction coefficient) properties of stainless high-chromium steel subjected to complex processing, combining vacuum irradiation of the samples surface layer with an intense pulsed electron beam of submillisecond exposure duration and subsequent nitriding under electron-ionic heating conditions. High-chromium steel AISI 310S, which in the initial state is a polycrystalline aggregate based on γ-iron, was used as the research material. Pulsed electron beam treatment of steel was carried out on a “SOLO” installation equipped with an electron source with a plasma cathode based on a low-pressure pulsed arc discharge with grid stabilization of the cathode plasma boundary and an open anode plasma boundary. Steel nitriding was carried out on a “TRIO” installation with a chamber size of 600×600×600 mm, equipped with a switching unit to implement the electron-ionic processing mode. Nitriding was carried out at 723, 793, and 873 K temperatures for 1, 3 and 5 h. It was found that electron-ionic nitriding of the samples pre-irradiated with an electron beam (10 J/cm2, 200 μs, 3 pulses at 723 and 793 K for 3 h) is accompanied by the formation of a ceramic layer containing only iron and chromium nitrides. The highest values of steel wear resistance after electron-ionic nitriding, exceeding the wear resistance of the initial steel by more than 700 times, are observed at nitriding parameters of 793 K, 3 h.

Regulating Aggregation-Induced Emission Luminogen for Multimodal Imaging-Navigated Synergistic Therapy Involving Anti-Angiogenesis.

As a new avenue for cancer research, phototheranostics has shown inexhaustible and vigorous vitality as it permits real-time diagnosis and concurrent in situ therapy upon non-invasive light-initiation. However, construction of an advanced material, allowing prominent phototheranostic outputs and synchronously surmounting the inherent deficiency of phototheranostics, would be an appealing yet significantly challenging task. Herein, an aggregation-induced emission (AIE)-active luminogen (namely DBD-TM) featured by intensive electron donor-acceptor strength and twisted architecture with finely modulated intramolecular motion, is tactfully designed and prepared. DBD-TM simultaneously possessed fluorescence emission in the second near-infrared (NIR-II) region and high-efficiency photothermal conversion. By integrating DBD-TM with anti-angiogenic agent sorafenib, a versatile nanomaterial is smoothly fabricated and utilized for trimodal imaging-navigated synergistic therapy involving photothermal therapy and anti-angiogenesis toward cancer. This advanced approach is capable of affording accurate tumor diagnosis, complete tumor elimination, and largely restrained tumor recurrence, evidently denoting a prominent theranostic formula beyond phototheranostics. This study will offer a blueprint for exploiting a new generation of cancer theranostics.

Electronic interaction between sub-nanometric Ru entity and TiO2 support regulates the hydrogenation chemistry for selective C-O bond cleavage

Selective C-O bond cleavage without ring saturation is the pillar pursuit in the hydrotreating process for lignin valorization/depolymerization since it avoids the consumption of excessive hydrogen. In this work, the sub-nanometric cluster and nanometric particle of Ru were supported on TiO2 for the hydrogenolysis of C-O bond in aromatic ether. The experimental and theoretical results reveal that, in the catalyst of larger Ru nanoparticles, less electron transfer occurs from individual Ru atom to TiO2, making the Ru-related domains retain the nature of bulky Ru for deep hydrogenation. Sub-nanometric Ru cluster shows more intense electron transfer for individual Ru atom, leading to a stronger modification to Ru domain by TiO2. Such electronic hybridization makes Ru gain the catalytic property of TiO2 to attenuate the activation of aromatic ring, inhibiting ring saturation with maintained C-O cleavage activity. This work implies that further decrease of Ru entity size to single-atom level may achieve the complete inhibition of ring saturation.

Quantifying Covalency and Environmental Effects in RASSCF-Simulated O K-Edge XANES of Uranyl.

A RASSCF approach to simulate the O K-edge XANES spectra of uranyl is employed, utilizing three models that progressively improve the representation of the local crystal environment. Simulations successfully reproduce the observed three-peak profile of the experimental spectrum and confirm peak assignments made by Denning. The [UO2Cl4]2- model offers the best agreement with experiment, with peak positions (to within 1 eV) and relative peak separations accurately reproduced. Establishing a direct link between a specific electronic transition and peak intensity is complicated, as a large number of possible transitions can contribute to the overall peak profile. Furthermore, a relationship between oxygen character in the antibonding orbital and the strength of the transition breaks down when using a variety of orbital composition approaches at larger excitation energy. Covalency analysis of the U-O bond in both the ground- and excited-state reveals a dependence on the crystal environment. Orbital composition analysis reveals an underestimation of the uranium contribution to ground-state bonding orbitals when probing O K-edge core-excited states, regardless of the uranyl model employed. However, improving the environmental model provides core-excited state electronic structures that are better representative of that of the ground-state, validating their use in the determination of covalency and bonding.