Tailoring local structures of atomically dispersed copper sites for highly selective CO_(2) electroreduction

Atomically‐dispersed copper sites coordinated with nitrogen‐doped carbon(Cu–N–C)can provide novel possibilities to enable highly selective and active electrochemical CO_(2) reduction reactions.However,the construction of optimal local electronic structures for nitrogen‐coordinated Cu sites(Cu–N_(4))on carbon remains challenging.Here,we synthesized the Cu–N–C catalysts with atomically‐dispersed edge‐hosted Cu–N_(4) sites(Cu–N_(4)C_(8))located in a micropore between two graphitic sheets via a facile method to control the concentration of metal precursor.Edge‐hosted Cu–N_(4)C_(8) catalysts outperformed the previously reported M–N–C catalysts for CO_(2)‐to‐CO conversion,achieving a maximum CO Faradaic efficiency(FECO)of 96%,a CO current density of–8.97 mA cm^(–2) at–0.8 V versus reversible hydrogen electrode(RHE),and over FECO of 90%from–0.6 to–1.0 V versus RHE.Computational studies revealed that the micropore of the graphitic layer in edge‐hosted Cu–N_(4)C_(8) sites causes the d‐orbital energy level of the Cu atom to shift upward,which in return decreases the occupancy of antibonding states in the*COOH binding.This research suggests new insights into tailoring the locally coordinated structure of the electrocatalyst at the atomic scale to achieve highly selective electrocatalytic reactions.

基于多尺度Scale-Unet的单样本图像翻译

随着生成对抗网络(GAN)的发展,基于单样本的无监督图像到图像翻译(UI2I)取得了重大进展。然而,以前方法无法捕获图像中的复杂纹理并保留原始内容信息。为解决这个问题,提出了一种基于尺度可变U-Net结构(Scale—Unet)的新型单样本图像翻译结构SUGAN。所提出的SUGAN使用Scale—Unet作为生成器,利用多尺度结构和渐进方法不断改进网络结构,以从粗到细地学习图像特征。同时,提出了尺度像素损失scale-pixel来更好地约束保留原始内容信息,防止信息丢失。实验表明,与SinGAN、TuiGAN、TSIT、StyTR2等公共数据集Summer■Winter、Horse■Zebra上的方法相比,该方法生成图像的SIFID值平均降低了30%。所提方法可更好地保留图像内容信息,同时生成详细逼真的高质量图像。

Laser machining fundamentals:micro,nano,atomic and close-to-atomic scales

With the rapid development in advanced industries,such as microelectronics and optics sectors,the functional feature size of devises/components has been decreasing from micro to nanometric,and even ACS for higher performance,smaller volume and lower energy consumption.By this time,a great many quantum structures are proposed,with not only an extreme scale of several or even single atom,but also a nearly ideal lattice structure with no material defect.It is almost no doubt that such structures play critical role in the next generation products,which shows an urgent demand for the ACSM.Laser machining is one of the most important approaches widely used in engineering and scientific research.It is high-efficient and applicable for most kinds of materials.Moreover,the processing scale covers a huge range from millimeters to nanometers,and has already touched the atomic level.Laser–material interaction mechanism,as the foundation of laser machining,determines the machining accuracy and surface quality.It becomes much more sophisticated and dominant with a decrease in processing scale,which is systematically reviewed in this article.In general,the mechanisms of laser-induced material removal are classified into ablation,CE and atomic desorption,with a decrease in the scale from above microns to angstroms.The effects of processing parameters on both fundamental material response and machined surface quality are discussed,as well as theoretical methods to simulate and understand the underlying mechanisms.Examples at nanometric to atomic scale are provided,which demonstrate the capability of laser machining in achieving the ultimate precision and becoming a promising approach to ACSM.

Atomically Dispersed Ruthenium Catalysts with Open Hollow Structure for Lithium-Oxygen Batteries

Lithium–oxygen battery with ultrahigh theoretical energy density is considered a highly competitive next-generation energy storage device,but its practical application is severely hindered by issues such as difficult decomposition of discharge products at present.Here,we have developed N-doped carbon anchored atomically dispersed Ru sites cathode catalyst with open hollow structure(h-RuNC)for Lithium–oxygen battery.On one hand,the abundance of atomically dispersed Ru sites can effectively catalyze the formation and decomposition of discharge products,thereby greatly enhancing the redox kinetics.On the other hand,the open hollow structure not only enhances the mass activity of atomically dispersed Ru sites but also improves the diffusion efficiency of catalytic molecules.Therefore,the excellent activity from atomically dispersed Ru sites and the enhanced diffusion from open hollow structure respectively improve the redox kinetics and cycling stability,ultimately achieving a high-performance lithium–oxygen battery.

Atomically Substitutional Engineering of Transition Metal Dichalcogenide Layers for Enhancing Tailored Properties and Superior Applications

Transition metal dichalcogenides(TMDs)are a promising class of layered materials in the post-graphene era,with extensive research attention due to their diverse alternative elements and fascinating semiconductor behavior.Binary MX2 layers with different metal and/or chalcogen elements have similar structural parameters but varied optoelectronic properties,providing opportunities for atomically substitutional engineering via partial alteration of metal or/and chalcogenide atoms to produce ternary or quaternary TMDs.The resulting multinary TMD layers still maintain structural integrity and homogeneity while achieving tunable(opto)electronic properties across a full range of composition with arbitrary ratios of introduced metal or chalcogen to original counterparts(0–100%).Atomic substitution in TMD layers offers new adjustable degrees of freedom for tailoring crystal phase,band alignment/structure,carrier density,and surface reactive activity,enabling novel and promising applications.This review comprehensively elaborates on atomically substitutional engineering in TMD layers,including theoretical foundations,synthetic strategies,tailored properties,and superior applications.The emerging type of ternary TMDs,Janus TMDs,is presented specifically to highlight their typical compounds,fabrication methods,and potential applications.Finally,opportunities and challenges for further development of multinary TMDs are envisioned to expedite the evolution of this pivotal field.

Atomic Dispersed Hetero‑Pairs for Enhanced Electrocatalytic CO_(2)Reduction

Electrochemical carbon dioxide reduction reaction(CO_(2)RR)involves a variety of intermediates with highly correlated reaction and ad-desorption energies,hindering optimization of the catalytic activity.For example,increasing the binding of the*COOH to the active site will generally increase the*CO desorption energy.Breaking this relationship may be expected to dramatically improve the intrinsic activity of CO_(2)RR,but remains an unsolved challenge.Herein,we addressed this conundrum by constructing a unique atomic dispersed hetero-pair consisting of Mo-Fe di-atoms anchored on N-doped carbon carrier.This system shows an unprecedented CO_(2)RR intrinsic activity with TOF of 3336 h−1,high selectivity toward CO production,Faradaic efficiency of 95.96%at−0.60 V and excellent stability.Theoretical calculations show that the Mo-Fe diatomic sites increased the*COOH intermediate adsorption energy by bridging adsorption of*COOH intermediates.At the same time,d-d orbital coupling in the Mo-Fe di-atom results in electron delocalization and facilitates desorption of*CO intermediates.Thus,the undesirable correlation between these steps is broken.This work provides a promising approach,specifically the use of di-atoms,for breaking unfavorable relationships based on understanding of the catalytic mechanisms at the atomic scale.

Atomically dispersed Fe sites on hierarchically porous carbon nanoplates for oxygen reduction reaction

Developing cost-effective,robust and stable non-precious metal catalysts for oxygen reduction reaction(ORR) is of paramount importance for electrochemical energy conversion devices such as fuel cells and metal-air batteries.Although Fe-N-C single atom catalysts(SACs) have been hailed as the most promising candidate due to the optimal binding strength of ORR intermediates on the Fe-N_(4) sites,they suffer from serious mass transport limitations as microporous templates/substrates,i.e.,zeolitic imidazolate frameworks(ZIFs),are usually employed to host the active sites.Motivated by this challenge,we herein develop a hydrogen-bonded organic framework(HOF)-assisted pyrolysis strategy to construct hierarchical micro/mesoporous carbon nanoplates for the deposition of atomically dispersed Fe-N_(4) sites.Such a design is accomplished by employing HOF nanoplates assembled from 2-aminoterephthalic acid(NH_(2)-BDC) and p-phenylenediamine(PDA) as both soft templates and C,N precursors.Benefitting from the structural merits inherited from HOF templates,the optimized catalyst(denoted as Fe-N-C SAC-950) displays outstanding ORR activity with a high half-wave potential of 0.895 V(vs.reversible hydrogen electrode(RHE)) and a small overpotential of 356 mV at 10 mA cm^(-2) for the oxygen evolution reaction(OER).More excitingly,its application potential is further verified by delivering superb rechargeability and cycling stability with a nearly unfading charge-discharge gap of 0.72 V after 160 h.Molecular dynamics(MD) simulations reveal that micro/mesoporous structure is conducive to the rapid mass transfer of O_(2),thus enhancing the ORR performance.In situ Raman results further indicate that the conversion of O_(2) to~*O_(2)-the rate-determining step(RDS) for Fe-N-C SAC-950.This work will provide a versatile strategy to construct single atom catalysts with desirable catalytic properties.

Fractal Behaviour of Atomic Scale Microstructures:an Introduction

The properties of all materials depend largely on their chemical compositions.Compositional analysis by using the atom probe suggests that it is necessary to invent new parameters to describe some aspects of microstructures.Experimental and calculation work indicates that fractal dimension can be used to describe structural aspects not readily expressible with normal parameters.The application of fractal concept in mate- rials studies will enable us to understand from a brand-new angle the ultra-fine microstructures of materials.

The Tension Cosmology, Largest Cosmic Structures and Explosions of Supernovae from SST

Here, using the Scale-Symmetric Theory (SST) we explain the cosmological tension and the origin of the largest cosmic structures. We show that a change in value of strong coupling constant for cold baryonic matter leads to the disagreement in the galaxy clustering amplitude, quantified by the parameter S8. Within the same model we described the Hubble tension. We described also the mechanism that transforms the gravitational collapse into an explosion—it concerns the dynamics of virtual fields that lead to dark energy. Our calculations concern the Type Ia supernovae and the core-collapse supernovae. We calculated the quantized masses of the progenitors of supernovae, emitted total energy during explosion, and we calculated how much of the released energy was transferred to neutrinos. Value of the speed of sound in the strongly interacting matter measured at the LHC confirms that presented here model is correct. Our calculations show that the Universe is cyclic.

Atomic-Scale AES-EELS Analysis of Structure-Phase State and Growth Mechanism of Layered Nanostructures

A review of our experience in range of electron spectroscopy of the physical vapor-phase deposition and growth of single- and multilayer nanostructures with atomic scale interfaces is presented. The foundation of an innovative methodology for the combined AES-EELS analysis of layered nanostructures is developed. The methodology includes: 1) determination of the composition, thickness, and the mechanism of phase transitions in nanocoatings under the probing depth most appropriated for the range of film thickness 1 - 10 ML;2) quantitative iteration Auger-analysis of the composition, thickness and growth mechanism of nanocoating;3) structural and phase analysis of nanocoatings with use of the analysis of position, shape and energy of the plasmon EELS peak and with subtracting the contribution from the substrate;4) analysis of phase transitions with use of the shift of the plasmon Auger-satellite and 5) non-destructive profiling of the composition of nanocoatings over depth with use of a dependence of the intensity and energy of EELS peaks on the value of the primary electron energy.

A combined multiscale modeling and experimental study on surface modification of high-volume micro-nanoparticles with atomic accuracy

Surface modification for micro-nanoparticles at the atomic and close-to-atomic scales is of great importance to enhance their performance in various applications,including high-volume battery,persistent luminescence,etc.Fluidized bed atomic layer deposition(FB-ALD)is a promising atomic-scale manufacturing technology that offers ultrathin films on large amounts of particulate materials.Nevertheless,nanoparticles tend to agglomerate due to the strong cohesive forces,which is much unfavorable to the film conformality and also hinders their real applications.In this paper,the particle fluidization process in an ultrasonic vibration-assisted FB-ALD reactor is numerically investigated from micro-scale to macro-scale through the multiscale computational fluid dynamics and discrete element method(CFD-DEM)modeling with experimental verification.Various vibration amplitudes and frequencies are investigated in terms of their effects on the fluid dynamics,distribution of particle velocity and solid volume fraction,as well as the size of agglomerates.Results show that the fluid turbulent kinetic energy,which is the key power source for the particles to obtain the kinetic energy for overcoming the interparticle agglomeration forces,can be strengthened obviously by the ultrasonic vibration.Besides,the application of ultrasonic vibration is found to reduce the mean agglomerate size in the FB.This is bound to facilitate the heat transfer and precursor diffusion in the entire FB-ALD reactor and the agglomerates,which can largely shorten the coating time and improve the film conformality as well as precursor utilization.The simulation results also agree well with our battery experimental results,verifying the validity of the multiscale CFD-DEM model.This work has provided momentous guidance to the mass manufacturing of atomic-scale particle coating from lab-scale to industrial applications.

Structural Stabilities and Electronic Structures of Ga Atomic Chains

The structural stabilities and electronic structures of Ga atomic chains are studied by the first-principles plane wave pseudopotential method based on the density functional theory. The present calculations show that gallium can form planar chains in linear-, zigzag- and ladder-form one-dimensional structures. The most stable one among the studied structures is the zigzag chain with a unit cell rather close to equilateral triangles with four nearest neighbors, and all the other structures are metastable. The relative structural stability, the energy bands and the charge densities are discussed based on the ab initio calculations and the Jahn-Teller effect.

Atomic and close-to-atomic scale manufacturing: perspectives and measures

This article presents the three paradigms of manufacturing advancement:Manufacturing I,craft-based manufacturing by hand,as in the Stone,Bronze,and Iron Ages,in which manufacturing precision was at the millimeter scale;ManufacturingⅡ,precision-controllable manufacturing using machinery whereby the scales of material removal,migration,and addition were reduced from millimeters to micrometers and even nanometers;and Manufacturing Ⅲ,manufacturing objectives and processes are directly focused on atoms,spanning the macro-through the micro-to the nanoscale,whereby manufacturing is based on removal,migration,and addition at the atomic scale,namely,atomic and close-to-atomic scale manufacturing(ACSM).A typical characteristic of ACSM is that energy directly impacts the atom to be removed,migrated,and added.ACSM,as the next generation of manufacturing technology,will be employed to build atomic-scale features for required functions and performance with the capacity of mass production.It will be the leading development trend in manufacturing technology and will play a significant role in the manufacturing of high-end components and future products.

Thin Film of Perovskite Oxide with Atomic Scale p-n Junctions

Thin films of perovskite manganese oxide Lao.66Ca0.29K0.05MnO3（LCKMO） on Au/ITO（ITO=indium tin oxide） substrates were prepared by off-axis radio frequency magnetron sputtering and characterized by X-ray diffrac- tion（XRD）, high-resolution transmission electron microscopy（HRTEM）, and conductive atomic force microscopy （C-AFM） at room temperature. The thin films with thickness ranged from 100 nm to 300 nm basically show cubic structures with a=0.3886 nm, the same as that of the raw material used, but the structures are highly modulated. C-AFM results revealed that the atomic scale p-n junction feature of the thin films was the same as that of the single crystals. The preparation of the thin films thus further confirms the possibility of their application extending from micrometer-sized single crystals to macroscopic thin film.

AN EXPERIMENTAL STUDY OF THE LARGE SCALE COHERENT STRUCTURES IN A FORCED FREE SHEAR LAYER

The dynamic characteristics of the large scale coherent structures in a forced free shear layer are experi- mentally studied by means of flow visualization. The quantitative measurements are acquired by the use of a LDV. It is shown that the development of the coherent structures can be greatly influenced by upstream artificial perturbations and as a result the mixing in the layer can be controlled. Like vortex merging, vortex splitting is also a common evolu- tion pattern in the development of the coherent structures.

Towards atomic and close-to-atomic scale manufacturing

Human beings have witnessed unprecedented developments since the 1760s using precision tools and manufacturing methods that have led to ever-increasing precision,from millimeter to micrometer,to single nanometer,and to atomic levels.The modes of manufacturing have also advanced from craft-based manufacturing in the Stone,Bronze,and Iron Ages to precisioncontrollable manufacturing using automatic machinery.In the past 30 years,since the invention of the scanning tunneling microscope,humans have become capable of manipulating single atoms,laying the groundwork for the coming era of atomic and close-to-atomic scale manufacturing(ACSM).Close-to-atomic scale manufacturing includes all necessary steps to convert raw materials,components,or parts into products designed to meet the user’s specifications.The processes involved in ACSM are not only atomically precise but also remove,add,or transform work material at the atomic and close-to-atomic scales.This review discusses the history of the development of ACSM and the current state-of-the-art processes to achieve atomically precise and/or atomic-scale manufacturing.Existing and future applications of ACSM in quantum computing,molecular circuitry,and the life and material sciences are also described.To further develop ACSM,it is critical to understand the underlying mechanisms of atomic-scale and atomically precise manufacturing;develop functional devices,materials,and processes for ACSM;and promote high throughput manufacturing.

Review of chip-scale atomic clocks based on coherent population trapping

Research on chip-scale atomic clocks （CSACs） based on coherent population trapping （CPT） is reviewed. The back- ground and the inspiration for the research are described, including the important schemes proposed to improve the CPT signal quality, the selection of atoms and buffer gases, and the development of micro-cell fabrication. With regard to the re- liability, stability, and service life of the CSACs, the research regarding the sensitivity of the CPT resonance to temperature and laser power changes is also reviewed, as well as the CPT resonance＇s collision and light of frequency shifts. The first generation CSACs have already been developed but its characters are still far from our expectations. Our conclusion is that miniaturization and power reduction are the most important aspects calling for further research.

A Scheme for Calculating Atomic Structures beyond the Spherical Approximation

We present a scheme for calculating atomic single-particle wave functions and spectra with taking into ac-count the nonspherical effect explicitly. The actual calculation is also performed for the neutral carbon atom within the Hartree-Fock-Slater approximation. As compared with the conventional atomic structure of the spherical approximation, the degenerate energy levels are split partially. The ground state values of the total orbital and spin angular momenta are estimated to be both about unity, which corresponds to the term P3PP in the LS-multiplet theory. This means that the nonspherical effect may play an essential role on the description of the magnetization caused by the orbital polarization.

MULTI-SCALE FE COMPUTATION FOR THE STRUCTURES OF COMPOSITE MATERIALS WITH SMALL PERIODIC CONFIGURATION UNDER CONDITION OF COUPLED THERMOELASTICITY

In this paper,the multi-scale computational method for a structure of composite materials with a small periodic configuration under the coupled thermoelasticity condition is presented. The two-scale asymptotic(TSA)expression of the displacement and the increment of temperature for composite materials with a small periodic configuration under the condition of thermoelasticity are briefly shown at first,then the multi-scale finite element algorithms based on TSA are discussed.Finally the numerical results evaluated by the multi-scale computational method are shown.It demonstrates that the basic configuration and the increment of temperature strongly influence the local strains and local stresses inside a basic cell.

Integrated physics package of a chip-scale atomic clock

The physics package of a chip-scale atomic clock （CSAC） has been successfully realized by integrating vertical cavity surface emitting laser （VCSEL）, neutral density （ND） filter, λ/4 wave plate, 87Rb vapor cell, photodiode （PD）, and magnetic coil into a cuboid metal package with a volume of about 2.8 cm3. In this physics package, the critical component, 87Rb vapor cell, is batch-fabricated based on MEMS technology and in-situ chemical reaction method. Pt heater and thermistors are integrated in the physics package. A PTFE pillar is used to support the optical elements in the physics package, in order to reduce the power dissipation. The optical absorption spectrum of 87Rb D1 line and the microwave frequency correction signal are successfully observed while connecting the package with the servo circuit system. Using the above mentioned packaging solution, a CSAC with short-term frequency stability of about 7 × 10^-10τ-1/2 has been successfully achieved, which demonstrates that this physics package would become one promising solution for the CSAC.