Capturing the non-equilibrium state in light–matter–free-electron interactions through ultrafast transmission electron microscopy

Ultrafast transmission electron microscope(UTEM) with the multimodality of time-resolved diffraction, imaging,and spectroscopy provides a unique platform to reveal the fundamental features associated with the interaction between free electrons and matter. In this review, we summarize the principles, instrumentation, and recent developments of the UTEM and its applications in capturing dynamic processes and non-equilibrium transient states. The combination of the transmission electron microscope with a femtosecond laser via the pump–probe method guarantees the high spatiotemporal resolution, allowing the investigation of the transient process in real, reciprocal and energy spaces. Ultrafast structural dynamics can be studied by diffraction and imaging methods, revealing the coherent acoustic phonon generation and photoinduced phase transition process. In the energy dimension, time-resolved electron energy-loss spectroscopy enables the examination of the intrinsic electronic dynamics of materials, while the photon-induced near-field electron microscopy extends the application of the UTEM to the imaging of optical near fields with high real-space resolution. It is noted that light–free-electron interactions have the ability to shape electron wave packets in both longitudinal and transverse directions, showing the potential application in the generation of attosecond electron pulses and vortex electron beams.

Strong metal–support interaction boosts the electrocatalytic hydrogen evolution capability of Ru nanoparticles supported on titanium nitride

Ruthenium(Ru)has been regarded as one of the most promising alternatives to substitute Pt for catalyzing alkaline hydrogen evolution reaction(HER),owing to its inherent high activity and being the cheapest platinum-group metal.Herein,based on the idea of strong metal–support interaction(SMSI)regulation,Ru/TiN catalysts with different degrees of TiN overlayer over Ru nanoparticles were fabricated,which were applied to the alkaline electrolytic water.Characterizations reveal that the TiN overlayer would gradually encapsulate the Ru nanoparticles and induce more electron transfer from Ru nanoparticles to TiN support by the Ru–N–Ti bond as the SMSI degree increased.Further study shows that the exposed Ru–TiN interfaces greatly promote the H_(2) desorption capacity.Thus,the Ru/TiN-300 with a moderate SMSI degree exhibits excellent HER performance,with an overpotential of 38 mV at 10 mA cm^(−2).Also,due to the encapsulation role of TiN overlayer on Ru nanoparticles,it displays super long-term stability with a very slight potential change after 24 h.This study provides a deep insight into the influence of the SMSI effect between Ru and TiN on HER and offers a novel approach for preparing efficient and stable HER electrocatalysts through SMSI engineering.

Skin‑Inspired Ultra‑Tough Supramolecular Multifunctional Hydrogel Electronic Skin for Human–Machine Interaction

Multifunctional supramolecular ultra-tough bionic e-skin with unique durability for human–machine interaction in complex scenarios still remains challenging.Herein,we develop a skininspired ultra-tough e-skin with tunable mechanical properties by a physical cross-linking salting-freezing-thawing method.The gelling agent(β-Glycerophosphate sodium:Gp)induces the aggregation and binding of PVA molecular chains and thereby toughens them(stress up to 5.79 MPa,toughness up to 13.96 MJ m^(−3)).Notably,due to molecular self-assembly,hydrogels can be fully recycled and reprocessed by direct heating(100°C for a few seconds),and the tensile strength can still be maintained at about 100%after six recoveries.The hydrogel integrates transparency(>60%),super toughness(up to 13.96 MJ m^(−3),bearing 1500 times of its own tensile weight),good antibacterial properties(E.coli and S.aureus),UV protection(Filtration:80%–90%),high electrical conductivity(4.72 S m^(−1)),anti-swelling and recyclability.The hydrogel can not only monitor daily physiological activities,but also be used for complex activities underwater and message encryption/decryption.We also used it to create a complete finger joint rehabilitation system with an interactive interface that dynamically presents the user’s health status.Our multifunctional electronic skin will have a profound impact on the future of new rehabilitation medical,human–machine interaction,VR/AR and the metaverse fields.

Effects of electron–optical phonon interactions on the polaron energy in a wurtzite ZnO/Mg_xZn_(1-x)O quantum well

We investigated the properties of polarons in a wurtzite ZnO/MgxZn1-xO quantum well by adopting a modified Lee–Low–Pines variational method, giving the ground state energy, transition energy, and phonon contributions from various optical-phonon modes to the ground state energy as functions of the well width and Mg composition. In our calculations, we considered the effects of confined optical phonon modes, interface-optical phonon modes, and half-space phonon modes, as well as the anisotropy of the electron effective band mass, phonon frequency, and dielectric constant. Our numerical results indicate that the electron–optical phonon interactions importantly affect the polaronic energies in the ZnO/MgxZn1-xO quantum well. The electron–optical phonon interactions decrease the polaron energies. For quantum wells with narrower wells, the interface optical phonon and half-space phonon modes contribute more to the polaronic energies than the confined phonon modes. However, for wider quantum wells, the total contribution to the polaronic energy mainly comes from the confined modes. The contributions of the various phonon modes to the transition energy change differently with increasing well width. The contribution of the half-space phonons decreases slowly as the QW width increases, whereas the contributions of the confined and interface phonons reach a maximum at d ≈ 5.0 nm and then decrease slowly. However,the total contribution of phonon modes to the transition energy is negative and increases gradually with the QW width of d.As the composition x increases, the total contribution of phonons to the ground state energies increases slowly, but the total contributions of phonons to the transition energies decrease gradually. We analyze the physical reasons for these behaviors in detail.

Storm-Time Evolution of Energetic Electron Pitch Angle Distributions by Wave-Particle Interaction

The quasi-pure pitch-angle scattering of energetic electrons driven by field-aligned propagating whistler mode waves during the 9～15 October 1990 magnetic storm at L≈ 3 ～ 4 is studied, and numerical calculations for energetic electrons in gyroresonance with a band of frequency of whistler mode waves distributed over a standard Gaussian spectrum is performed. It is found that the whistler mode waves can efficiently drive energetic electrons from the larger pitchangles into the loss cone, and lead to a flat-top distribution during the main phase of geomagnetic storms. This result perhaps presents a feasible interpretation for observation of time evolution of the quasi-isotropic pitch-angle distribution by Combined Release and Radiation Effects Satellite （CRRES） spacecraft at L ≈ 3 ～ 4.

Superthermal Electron Produced in Relativistic Laser-Plasma Interaction

The dynamics of a relativistic electron submitted to an intense, plane wave, linearly polarized laser field is reviewed. Based on the dynamics, the temperature of the electron in the laser field is delined and calculated. It is found that the calculated temperature fits the first temperature observed in the experiment by Malka et al. A model to evaluate the electron temperature by taking the electron-ion scattering into account is proposed. It is found that when I ≥ 4.0 × 101s W/cm2 the electron temperature by considering the scattering, T hs, is evidently larger than the electron temperature without considering the scattering, Th. This result is in favor of explaining the two-temperature distribution of the electron energy observed in the experiment by Malka et al.

Polaronic Electron-Phonon Interactions on the Third-Harmonic Generation in a Square Quantum Well

在方形的量的第三泛音的产生上的电子声子相互作用的影响很好被调查。第一泛音、第三泛音的产生系数被使用 compact-density-matrix 途径和反复的方法获得，并且数字结果为 GaAs 方形的量被介绍很好。结果证明第三泛音的产生系数显然在考虑电子声子相互作用的影响以后被提高。

Influence of Characteristics of Substance on Parameters of Interaction of Photons High Energy with Free Electrons

Various variants of interaction of photons high energy with free electrons in substance are investigated. It is shown, that among these variants, in substance can be observed: absorption of a photon by electron, coherent and not coherent scattering of photons, a stop electron after interaction with a photon. Dependence of change of length of a wave of a photon after interaction with electron from parameters of substance and speed of movement electron is found.

Valence electronic engineering of superhydrophilic Dy-evoked Ni-MOF outperforming RuO_(2) for highly efficient electrocatalytic oxygen evolution

Tackling the problem of poor conductivity and catalytic stability of pristine metal-organic frameworks(MOFs) is crucial to improve their oxygen evolution reaction(OER) performance.Herein,we introduce a novel strategy of dysprosium(Dy) doping,using the unique 4f orbitals of this rare earth element to enhance electrocatalytic activity of MOFs.Our method involves constructing Dy-doped Ni-MOF(Dy@Ni-MOF) nanoneedles on carbon cloth via a Dy-induced valence electronic perturbation approach.Experiments and density functional theory(DFT) calculations reveal that Dy doping can effectively modify the electronic structure of the Ni active centers and foster a strong electronic interaction between Ni and Dy.The resulting benefits include a reduced work function and a closer proximity of the d-band center to the Fermi level,which is conducive to improving electrical conductivity and promoting the adsorption of oxygen-containing intermediates.Furthermore,the Dy@Ni-MOF achieves superhydrophilicity,ensuring effective electrolyte contact and thus accelerating reaction kinetics,Ex-situ and in-situ analysis results manifest Dy_(2)O_(3)/NiOOH as the actual active species.Therefore,Dy@Ni-MOF shows impressive OER performance,significantly surpassing Ni-MOF.Besides,the overall water splitting device with Dy@NiMOF as an anode delivers a low cell voltage of 1.51 V at 10 mA cm^(-2) and demonstrates long-term stability for 100 h,positioning it as a promising substitute for precious metal catalysts.

Generation and regulation of electromagnetic pulses generated by femtosecond lasers interacting with multitargets

Ultrashort and powerful laser interactions with a target generate intense wideband electromagnetic pulses(EMPs).In this study,we report EMPs generated by the interactions between petawatt(30 fs,1.4×10^(20) W/cm^(2))femtosecond(fs)lasers with metal flat,plastic flat,and plastic nanowire-array(NWA)targets.Detailed analyses are conducted on the EMPs in terms of their spatial distribution,time and frequency domains,radiation energy,and protection.The results indicate that EMPs from metal targets exhibit larger amplitudes at varying angles than those generated by other types of targets and are enhanced significantly for NWA targets.Using a plastic target holder and increasing the laser focal spot can significantly decrease the radiation energy of the EMPs.Moreover,the composite shielding materials indicate an effective shielding effect against EMPs.The simulation results show that the NWA targets exert a collimating effect on thermal electrons,which directly affects the distribution of EMPs.This study provides guidance for regulating EMPs by controlling the laser focal spot,target parameters,and target rod material and is beneficial for electromagnetic-shielding design.

Interfacial Electronic Modulation of Dual-Monodispersed Pt–Ni_(3)S_(2) as Efficacious Bi-Functional Electrocatalysts for Concurrent H_(2) Evolution and Methanol Selective Oxidation

Constructing the efficacious and applicable bifunctional electrocatalysts and establishing out the mechanisms of organic electro-oxidation by replacing anodic oxygen evolution reaction(OER) are critical to the development of electrochemicallydriven technologies for efficient hydrogen production and avoid CO_(2) emission. Herein, the hetero-nanocrystals between monodispersed Pt(~ 2 nm) and Ni_(3)S_(2)(~ 9.6 nm) are constructed as active electrocatalysts through interfacial electronic modulation, which exhibit superior bi-functional activities for methanol selective oxidation and H_(2) generation. The experimental and theoretical studies reveal that the asymmetrical charge distribution at Pt–Ni_(3)S_(2) could be modulated by the electronic interaction at the interface of dual-monodispersed heterojunctions, which thus promote the adsorption/desorption of the chemical intermediates at the interface. As a result, the selective conversion from CH_(3)OH to formate is accomplished at very low potentials(1.45 V) to attain 100 m A cm^(-2) with high electronic utilization rate(~ 98%) and without CO_(2) emission. Meanwhile, the Pt–Ni_(3)S_(2) can simultaneously exhibit a broad potential window with outstanding stability and large current densities for hydrogen evolution reaction(HER) at the cathode. Further, the excellent bi-functional performance is also indicated in the coupled methanol oxidation reaction(MOR)//HER reactor by only requiring a cell voltage of 1.60 V to achieve a current density of 50 m A cm^(-2) with good reusability.

Effects of Electron-Phonon Interaction on Linear and Nonlinear Optical Absorption in Cylindrical Quantum Wires

对在有一个无限的限制潜力的圆柱的量电线(CQW ) 中的线性、非线性的光吸收的电子声子相互作用影响被调查。光吸收系数被使用 compact-density-matrix 途径和反复的方法获得，并且数字结果为 GaAs CQW 被介绍。结果证明电子声子相互作用在 CQW 在光吸收上做不同影响。电子的波浪功能上的电子声子相互作用统治吸收系数的价值，电子的精力上的电子声子效果的修正让吸收山峰蓝色变并且变得更宽。而且，对有一个无限的限制潜力的光吸收的电子声子相互作用影响与一个有限限制潜力与那不同。

Electrically-driven ultrafast out-of-equilibrium light emission from hot electrons in suspended graphene/hBN heterostructures

Nanoscale light sources with high speed of electrical modulation and low energy consumption are key components for nanophotonics and optoelectronics.The record-high carrier mobility and ultrafast carrier dynamics of graphene make it promising as an atomically thin light emitter which can be further integrated into arbitrary platforms by van der Waals forces.However,due to the zero bandgap,graphene is difficult to emit light through the interband recombination of carriers like conventional semiconductors.Here,we demonstrate ultrafast thermal light emitters based on suspended graphene/hexagonal boron nitride(Gr/hBN)heterostructures.Electrons in biased graphene are significantly heated up to 2800 K at modest electric fields,emitting bright photons from the near-infrared to the visible spectral range.By eliminating the heat dissipation channel of the substrate,the radiation efficiency of the suspended Gr/hBN device is about two orders of magnitude greater than that of graphene devices supported on SiO2or hBN.Wefurther demonstrate that hot electrons and low-energy acoustic phonons in graphene are weakly coupled to each other and are not in full thermal equilibrium.Direct cooling ofhigh-temperature hot electrons to low-temperature acoustic phonons is enabled by the significant near-field heat transfer at the highly localized Gr/hBN interface,resulting in ultrafast thermal emission with up to 1 GHz bandwidth under electrical excitation.It is found thatsuspending the Gr/hBN heterostructures on the SiO2trenches significantly modifies the light emission due to the formation of the optical cavity and showed a~440%enhancement inintensity at the peak wavelength of 940 nm compared to the black-body thermal radiation.The demonstration of electrically driven ultrafast light emission from suspended Gr/hBNheterostructures sheds the light on applications of graphene heterostructures in photonicintegrated circuits,such as broadband light sources and ultrafast thermo-optic phase modulators.

Divergence angle consideration in energy spread measurement for high-quality relativistic electron beam in laser wakefield acceleration

The thorough exploration of the transverse quality represented by divergence angle has been lacking yet in the energy spread measurement of the relativistic electron beam for laser wakefield acceleration(LWFA). In this work, we fill this gap by numerical simulations based on the experimental data, which indicate that in a C-shape magnet, magnetic field possesses the beam focusing effect, considering that the divergence angle will result in an increase in the full width at half maxima(FWHM) of the electron density distribution in a uniformly isotropic manner, while the length-to-width ratio decreases. This indicates that the energy spread obtained from the electron deflection distance is smaller than the actual value, regardless of the divergence angle. A promising and efficient way to accurately correct the value is presented by considering the divergence angle(for instance, for an electron beam with a length-to-width ratio of 1.12, the energy spread correct from 1.2% to 1.5%), providing a reference for developing the high-quality electron beam source.

Electron Interaction Among the Noncovalently Engineered Graphene-methylene Blue Nanocomposites

The electron interaction among the noncovalently engineered graphene-methylene blue（MB） nanocompo- site with a dipolar pull-push hybrid model was studied. The π-π interaction between reduced graphene oxide（rGO） and MB molecule was studied by 1HNMR spectroscopy. The electrochemical investigation indicates MB has a stronger electron transfer interaction with rGO than with GO. The ability of graphene-MB nanocomposites to undergo photoinduced electron transfer was confirmed from the capability of the nanocomposites coated electrode to generate photocurrent in a photoelectrochemical cell. The role of graphene as electron acceptor in the opto-electronic assembly was discussed.

Electron–acoustic phonon interaction and mobility in stressed rectangular silicon nanowires

We investigate the effects of pre-stress and surface tension on the electron–acoustic phonon scattering rate and the mobility of rectangular silicon nanowires. With the elastic theory and the interaction Hamiltonian for the deformation potential, which considers both the surface energy and the acoustoelastic effects, the phonon dispersion relation for a stressed nanowire under spatial confinement is derived. The subsequent analysis indicates that both surface tension and pre-stress can dramatically change the electron–acoustic phonon interaction. Under a negative（positive） surface tension and a tensile（compressive） pre-stress, the electron mobility is reduced（enhanced） due to the decrease（increase） of the phonon energy as well as the deformation-potential scattering rate. This study suggests an alternative approach based on the strain engineering to tune the speed and the drive current of low-dimensional electronic devices.

Ab Initio Molecular Orbital Calculation on Dinuclear Gold(Ⅰ) Complexes──Metal-Metal Interaction and Electronic Structure of Binuclear Gold(Ⅰ) Complexes with Bridging Bidentate Ligands

The electronic structure and electronic absorption spectra of binuclear Au(Ⅰ) complexes with bidentate phophines and a bidentate ylid ligand have been studied using quasirelativistic pseudopotential ab initio calculations at the HF and MP2 levels by the LANL2DZ basis sets. The electronic properties of the spectral transition and Au(Ⅰ)—Au(Ⅰ) interaction were also discussed.

Towards a Methodology for Formal Design and Analysis of Agent Interaction Protocols ——An Investigation in Electronic Commerce

Various extensions of UML have been developed to meet the challenges of designing modern software systems, such as agent based electronic commerce applications. Recent advances in model checking technology have led it to be introduced into the development of approaches and tools to check the correctness of electronic commerce protocols. This paper focuses on the research of a method that connects an extension of AUML to model checker SPIN/Promela for the specification and verification of agent interaction protocols (AIP) in electronic commerce. The method presented here allows us to combine the benefits of visual specification with the power of some static analysis and model checking. Some algorithms and rules are developed to permit all visual modeling constructs translated mechanically into some Promela models of AIP, as supported by the model checker SPIN. Moreover, a process is illustrated to guide the specification and verification of AIP. The method is demonstrated thoroughly using the e commerce protocol NetBill as an example.

On the electron sheath theory and its applications in plasma–surface interactions

In this work,an improved understanding of electron sheath theory is provided using both fluid and kinetic approaches while elaborating on their implications for plasma–surface interactions.A fluid model is proposed considering the electron presheath structure,avoiding the singularity in electron sheath Child–Langmuir law which overestimates the sheath potential.Subsequently,a kinetic model of electron sheath is established,showing considerably different sheath proflles in respect to the fluid model due to non-Maxwellian electron velocity distribution function and flnite ion temperature.The kinetic model is then further generalized and involves a more realistic truncated ion velocity distribution function.It is demonstrated that such a distribution function yields a super-thermal electron sheath whose entering velocity at the sheath edge is greater than the Bohm criterion prediction.Furthermore,an attempt is made to describe the electron presheath–sheath coupling within the kinetic framework,showing a necessary compromise between a realistic sheath entrance and the inclusion of kinetic effects.Finally,the secondary electron emissions induced by sheath-accelerated plasma electrons in an electron sheath are analysed and the influence of backscattering is discussed.