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 perf...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.展开更多
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 scal...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.展开更多
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 t...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.展开更多
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- t...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.展开更多
Reaction dynamics in gases at operating temperatures at the atomic level are the basis of heterogeneous gas-solid catalyst reactions and are crucial to the catalyst function.Supported noble metal nanocatalysts such as...Reaction dynamics in gases at operating temperatures at the atomic level are the basis of heterogeneous gas-solid catalyst reactions and are crucial to the catalyst function.Supported noble metal nanocatalysts such as platinum are of interest in fuel cells and as diesel oxidation catalysts for pollution control,and practical ruthenium nanocatalysts are explored for ammonia synthesis.Graphite and graphitic carbons are of interest as supports for the nanocatalysts.Despite considerable literature on the catalytic processes on graphite and graphitic supports,reaction dynamics of the nanocatalysts on the supports in different reactive gas environments and operating temperatures at the single atom level are not well understood.Here we present real time in-situ observations and analyses of reaction dynamics of Pt in oxidation,and practical Ru nanocatalysts in ammonia synthesis,on graphite and related supports under controlled reaction environments using a novel in-situ environmental(scanning) transmission electron microscope with single atom resolution.By recording snapshots of the reaction dynamics,the behaviour of the catalysts is imaged.The images reveal single metal atoms,clusters of a few atoms on the graphitic supports and the support function.These all play key roles in the mobility,sintering and growth of the catalysts.The experimental findings provide new structural insights into atomic scale reaction dynamics,morphology and stability of the nanocatalysts.展开更多
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 microstru...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.展开更多
Thermodynamic/dynamic modeling of liquid immiscibility in silicates is seriously hindered due to lack of in situ investigation on the structural evolution of the melt.In this work,atomic-scale structural evolution of ...Thermodynamic/dynamic modeling of liquid immiscibility in silicates is seriously hindered due to lack of in situ investigation on the structural evolution of the melt.In this work,atomic-scale structural evolution of a classic binary silicate immiscible system,SiO2–TiO2,is tracked by in situ high energy X-ray diffraction(HE-XRD).It is found that both the configuration of[SiO]and the polymerization between them are closely coupled with embedment and extraction of the metallic cations(Ti^4+).[SiO]monomer goes through deficit-oxygen and excess-polymerization before liquid–liquid separation and enables self-healing after liquid–liquid separation,which challenges the traditional cognition that[SiO4]monomer is immutable.Ti4+cations with tetrahedral oxygen-coordination first participate in the network construction before liquid separation.The four-fold Ti–O bond is broken during liquid separation,which may facilitate the movement of Ti4+across the Si–O network to form TiO2-rich nodules.The structural features of nodules were also investigated and they were found highly analogous to that of molten TiO2,which implies a parallel crystallization behavior in the two circumstances.Our results shed light on the structural evolution scenario in liquid immiscibility at atomic scale,which will contribute to constructing a complete thermodynamic/dynamic framework describing the silicate liquid immiscibility systems beyond current models.展开更多
The growth of (100} oriented CVD (Chemical Vapor Deposition) diamond film under Joe-Badgwell-Hauge (J-B-H) model is simulated at atomic scale by using revised KMC (Kinetic Monte Carlo) method. The results show that: (...The growth of (100} oriented CVD (Chemical Vapor Deposition) diamond film under Joe-Badgwell-Hauge (J-B-H) model is simulated at atomic scale by using revised KMC (Kinetic Monte Carlo) method. The results show that: (1) under Joe's model, the growth mechanism from single carbon species is suitable for the growth of (100) oriented CVD diamond film in low temperature; (2) the deposition rate and surface roughness (Rq) under Joe's model are influenced intensively by temperature (Ta) and not evident bymass fraction W of atom chlorine; (3)the surface roughness increases with the deposition rate, i.e. the film quality becomes worse with elevated temperature, in agreement with Grujicic's prediction; (4) the simulation results cannot make sure the role of single carbon insertion.展开更多
The growth of {100}-oriented CVD diamond film under two modifications ofJ-B-H model at low substrate temperatures was simulated by using a revised KMC method at atomicscale. The results were compared both in Cl-contai...The growth of {100}-oriented CVD diamond film under two modifications ofJ-B-H model at low substrate temperatures was simulated by using a revised KMC method at atomicscale. The results were compared both in Cl-containing systems and in C-H system as follows: (1)Substrate temperature can produce an important effect both on film deposition rate and on surfaceroughness; (2) Aomic Cl takes an active role for the growth of diamond film at low temperatures; (3){100}-oriented diamond film cannot deposit under single carbon insertion mechanism, which disagreeswith the predictions before; (4) The explanation of the exact role of atomic Cl is not provided inthe simulation results.展开更多
The mechanism of chemical-vapor-deposited (CVD) diamond film growth has attracted increasing attention recent years, mainly due to the fact that further technological advancement (such as obtaining high-quality films,...The mechanism of chemical-vapor-deposited (CVD) diamond film growth has attracted increasing attention recent years, mainly due to the fact that further technological advancement (such as obtaining high-quality films, controlling film growth, and heteroepitaxial growth, etc.) requires a more detailed understanding of the fundamental phenomena responsible for diamond growth.展开更多
Electrocatalysis has been extensively explored for the storage and conversion of renewable electric power.Understanding the physisorption and chemisorption processes at electrified solid–liquid interfaces(ESLIs)is cr...Electrocatalysis has been extensively explored for the storage and conversion of renewable electric power.Understanding the physisorption and chemisorption processes at electrified solid–liquid interfaces(ESLIs)is crucial for revealing the typical surface restructuring and catalyst dissolution during electrocatalysis.Although advanced in situ tools and theoretical models have been proposed[1,2],identifying the nature of the active sites with atomic-scale spatial resolution remains a challenge,especially at ESLIs.In a recent work published in Nature,Zhang et al.[3]reported a groundbreaking atomic-resolution imaging of the structural dynamics of Cu nanowire catalysts in ESLIs for electrochemical CO_(2)reduction(ECR).展开更多
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,e...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.展开更多
Precise synthesis at the atomic scale is a highly desirable and controllable route for the preparation of heterogeneous catalysts with the desired structure and properties,which promotes the rational design of highly ...Precise synthesis at the atomic scale is a highly desirable and controllable route for the preparation of heterogeneous catalysts with the desired structure and properties,which promotes the rational design of highly efficient catalysts and facilitates the understanding of structure-properties relationship.The precise construction of the active sites of the catalysts provides important opportunities for atomic insight into the correlation between structure and catalytic performance.In this review,the atomic-level tuning strategies for the precise synthesis of heterogeneous catalysts are summarized with the emphasis on the precise control of the structure of active sites,including single atom sites,dual atom sites and complex active sites.Furthermore,we illustrate the crucial role of atomic-level regulation of structure in determining the catalytic performance by providing typical catalysis examples in different reactions.In the end,some perspectives on the further development of precise synthesis of catalysts at the atomic level are presented.展开更多
Atomic and close-to-atomic scale manufacturing is the key technology for the production of next-generation devices with atomic precision.As an important approach of mechanical processing,cutting has evolved as a poten...Atomic and close-to-atomic scale manufacturing is the key technology for the production of next-generation devices with atomic precision.As an important approach of mechanical processing,cutting has evolved as a potential candidate to generate an atomically smooth surface;thus,exploring its ultimate capability is significant.In this paper,single-crystal graphite,whose lattice structure and chemical bond property are of representation for demonstration,is selected to study the mechanism of atomic layer removal using molecular dynamics.A localized workpiece,which is dynamically updated on the basis of the tool position,is used to improve the computation efficiency.The principle and bullet points of this modeling method are first introduced,followed by a series of simulations under various undeformed chip thicknesses and tool edge radi.In addition,different potentials for the tool-workpiece interaction are tested,and the effect on the material response is presented.Based on the analysis of deformation,the number of carbon layers removed,and cutting forces,the chip formation mechanism and further understanding of the controllability of cutting at atomic and close-to-atomic scale can be achieved.展开更多
This paper presents a new approach for material removal on silicon at atomic and close-to-atomic scale assisted by photons.The corresponding mechanisms are also investigated.The proposed approach consists of two seque...This paper presents a new approach for material removal on silicon at atomic and close-to-atomic scale assisted by photons.The corresponding mechanisms are also investigated.The proposed approach consists of two sequential steps:surface modification and photon irradiation.The back bonds of silicon atoms are first weakened by the chemisorption of chlorine and then broken by photon energy,leading to the desorption of chlorinated silicon.The mechanisms of photon-induced desorption of chlorinated silicon,i.e.,SiCl_(2) and SiCl,are explained by two models:the Menzel-Gomer-Redhead(MGR)and Antoniewicz models.The desorption probability associated with the two models is numerically calculated by solving the Liouville-von Neumann equations for open quantum systems.The calculation accuracy is verified by comparison with the results in literatures in the case of the NO/Pt(111)system.The calculation method is then applied to the cases of SiCl_(2)/Si and SiCl/Si systems.The results show that the value of desorption probability first increases dramatically and then saturates to a stable value within hundreds of femtoseconds after excitation.The desorption probability shows a super-linear dependence on the lifetime of excited states.展开更多
The atomic time scale release system for multiple laboratories is completed by modular design according to the atomic clock data provided by eight domestic punctual laboratories.The system includes the three modules,t...The atomic time scale release system for multiple laboratories is completed by modular design according to the atomic clock data provided by eight domestic punctual laboratories.The system includes the three modules,the processing of atomic clock data,the calculation of atomic time scale and the release of atomic time scale data,using MATLAB for data processing and time scale calculation,and using GUI for data visualization design.The system has clear process of the algorithm,simple function modules and friendly human-machine interface.The operation results of actual data show that the time difference between the integrated atomic time scale of the system and UTC is better than±10ns,and the content of data release can meet the needs of the scientific research in related fields in China.展开更多
Zeolites,as a class of porous inorganic materials,are extensively employed across a range of industrial applications,including catalysis[1],and adsorption separation[2],owing to their exceptional thermal stability,hig...Zeolites,as a class of porous inorganic materials,are extensively employed across a range of industrial applications,including catalysis[1],and adsorption separation[2],owing to their exceptional thermal stability,highly ordered pore structures,and tunable acidic properties.These characteristics enable zeolites to perform with remarkable efficiency and versatility in various processes.However,in the commonly employed aluminosilicate zeolites,Al atoms,acting as the active centers of acidity.展开更多
The detailed understanding of various underlying processes at liquid/solid interfaces requires the development of interface-sensitive and high-resolution experimental techniques with atomic precision.In this perspecti...The detailed understanding of various underlying processes at liquid/solid interfaces requires the development of interface-sensitive and high-resolution experimental techniques with atomic precision.In this perspective,we review the recent advances in studying the liquid/solid interfaces at atomic level by electrochemical scanning tunneling microscope(EC-STM),non-contact atomic force microscopy(NC-AFM),and surface-sensitive vibrational spectroscopies.Different from the ultrahigh vacuum and cryogenic experiments,these techniques are all operated in situ under ambient condition,making the measurements close to the native state of the liquid/solid interface.In the end,we present some perspectives on emerging techniques,which can defeat the limitation of existing imaging and spectroscopic methods in the characterization of liquid/solid interfaces.展开更多
LiNi_(0.8)Co_(0.1)Mn_(0.1)O_(2)(NCM811)layered oxides have been regarded as promising alternative cathodes for the next generation of high-energy lithium ion batteries(LIBs)due to high discharge capacities and energy ...LiNi_(0.8)Co_(0.1)Mn_(0.1)O_(2)(NCM811)layered oxides have been regarded as promising alternative cathodes for the next generation of high-energy lithium ion batteries(LIBs)due to high discharge capacities and energy densities at high operation voltage.However,the capacity fading under high operation voltage still restricts the practical application.Herein,the capacity degradation mechanism of NCM811 at atomic-scale is studied in detail under various cut-off voltages using aberration-corrected scanning transmission electron microscopy(STEM).It is observed that the crystal structure of NCM811 evolution from a layered structure to a rock-salt phase is directly accompanied by serious intergranular cracks under 4.9 V,which is distinguished from the generally accepted structure evolution of layered,disordered layered,defect rock salt and rock salt phases,also observed under 4.3 and 4.7 V.The electron energy loss spectroscopy analysis also confirms the reduction of Ni and Co from the surface to the bulk,not the previously reported only Li/Ni interlayer mixing.The degradation mechanism of NCM811 at a high cut-off voltage of4.9 V is attributed to the formation of intergranular cracks induced by defects,the direct formation of the rock salt phase,and the accompanied reduction of Ni^(2+)and Co^(2+)phases from the surface to the bulk.展开更多
The physicochemical properties of surfaces have a great effect on the micro-morphologies of the crystal structures which are in contact with them.Understanding the interaction mechanism between the internal driving fo...The physicochemical properties of surfaces have a great effect on the micro-morphologies of the crystal structures which are in contact with them.Understanding the interaction mechanism between the internal driving forces of the crystal and external inducing forces of the surfaces is the prerequisite of controlling and obtaining the desirable morphologies.In this work,the dynamic density functional theory was applied to construct the free energy functional expression of polyethylene(PE)lattice,and the micro-dynamic evolution processes of PE lattice morphology near the surfaces with different properties were observed to reveal the interaction mechanism at atomic scale.The results showed that the physical and chemical properties of the external surfaces synergistically affect the morphologies in both the defect shapes and the distribution of the defect regions.In the absence of the contact surfaces,driven by the oriented interactions among different CH2 groups,PE lattices gradually grow and form a defect-free structure.Conversely,the presence of contact surfaces leads to lattice defects in the interfacial regions,and PE lattice shows different self-healing abilities around different surfaces.展开更多
基金supported by the National Natural Science Foundation of China(Nos.52035009,52105475).
文摘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.
文摘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.
基金The authors gratefully acknowledge the support from the National Science Foundation of China(Grant Nos.51320105009,61635008,and 61675149)and the Science Foundation Ireland(SFI)(Grant Nos.15/RP/B3208 and 18/FIP/3555).
文摘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.
基金Supported by the National Natural Science Foundation of China(No.90922034)
文摘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.
基金the Engineering and Physical Science Research Council(EPSRC),U.K.for the award of a research grant EP/J0118058/1 and postdoctoral research assistantships(PDRAs) to M.R.W.and R.W.M.from the grant。
文摘Reaction dynamics in gases at operating temperatures at the atomic level are the basis of heterogeneous gas-solid catalyst reactions and are crucial to the catalyst function.Supported noble metal nanocatalysts such as platinum are of interest in fuel cells and as diesel oxidation catalysts for pollution control,and practical ruthenium nanocatalysts are explored for ammonia synthesis.Graphite and graphitic carbons are of interest as supports for the nanocatalysts.Despite considerable literature on the catalytic processes on graphite and graphitic supports,reaction dynamics of the nanocatalysts on the supports in different reactive gas environments and operating temperatures at the single atom level are not well understood.Here we present real time in-situ observations and analyses of reaction dynamics of Pt in oxidation,and practical Ru nanocatalysts in ammonia synthesis,on graphite and related supports under controlled reaction environments using a novel in-situ environmental(scanning) transmission electron microscope with single atom resolution.By recording snapshots of the reaction dynamics,the behaviour of the catalysts is imaged.The images reveal single metal atoms,clusters of a few atoms on the graphitic supports and the support function.These all play key roles in the mobility,sintering and growth of the catalysts.The experimental findings provide new structural insights into atomic scale reaction dynamics,morphology and stability of the nanocatalysts.
文摘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.
基金supported by the National Natural Science Foundation of China-Excellent Young Scholars(No.51922068)the National Key Research and Development Program(No.2017YFA0403800)+1 种基金the National Natural Science Foundation of China(Nos.51727802,51821001 and 51971138)Shanghai Pujiang Program(No.19PJ1404400)。
文摘Thermodynamic/dynamic modeling of liquid immiscibility in silicates is seriously hindered due to lack of in situ investigation on the structural evolution of the melt.In this work,atomic-scale structural evolution of a classic binary silicate immiscible system,SiO2–TiO2,is tracked by in situ high energy X-ray diffraction(HE-XRD).It is found that both the configuration of[SiO]and the polymerization between them are closely coupled with embedment and extraction of the metallic cations(Ti^4+).[SiO]monomer goes through deficit-oxygen and excess-polymerization before liquid–liquid separation and enables self-healing after liquid–liquid separation,which challenges the traditional cognition that[SiO4]monomer is immutable.Ti4+cations with tetrahedral oxygen-coordination first participate in the network construction before liquid separation.The four-fold Ti–O bond is broken during liquid separation,which may facilitate the movement of Ti4+across the Si–O network to form TiO2-rich nodules.The structural features of nodules were also investigated and they were found highly analogous to that of molten TiO2,which implies a parallel crystallization behavior in the two circumstances.Our results shed light on the structural evolution scenario in liquid immiscibility at atomic scale,which will contribute to constructing a complete thermodynamic/dynamic framework describing the silicate liquid immiscibility systems beyond current models.
基金[This work was financially supported by National Natural Science Founds of China (No. 59872003).]
文摘The growth of (100} oriented CVD (Chemical Vapor Deposition) diamond film under Joe-Badgwell-Hauge (J-B-H) model is simulated at atomic scale by using revised KMC (Kinetic Monte Carlo) method. The results show that: (1) under Joe's model, the growth mechanism from single carbon species is suitable for the growth of (100) oriented CVD diamond film in low temperature; (2) the deposition rate and surface roughness (Rq) under Joe's model are influenced intensively by temperature (Ta) and not evident bymass fraction W of atom chlorine; (3)the surface roughness increases with the deposition rate, i.e. the film quality becomes worse with elevated temperature, in agreement with Grujicic's prediction; (4) the simulation results cannot make sure the role of single carbon insertion.
基金This project was supported by National Natural Science Foundation of China (No.59872003).]
文摘The growth of {100}-oriented CVD diamond film under two modifications ofJ-B-H model at low substrate temperatures was simulated by using a revised KMC method at atomicscale. The results were compared both in Cl-containing systems and in C-H system as follows: (1)Substrate temperature can produce an important effect both on film deposition rate and on surfaceroughness; (2) Aomic Cl takes an active role for the growth of diamond film at low temperatures; (3){100}-oriented diamond film cannot deposit under single carbon insertion mechanism, which disagreeswith the predictions before; (4) The explanation of the exact role of atomic Cl is not provided inthe simulation results.
文摘The mechanism of chemical-vapor-deposited (CVD) diamond film growth has attracted increasing attention recent years, mainly due to the fact that further technological advancement (such as obtaining high-quality films, controlling film growth, and heteroepitaxial growth, etc.) requires a more detailed understanding of the fundamental phenomena responsible for diamond growth.
基金financially supported by the Natural Science Foundation of Shandong(ZR2023ME014)。
文摘Electrocatalysis has been extensively explored for the storage and conversion of renewable electric power.Understanding the physisorption and chemisorption processes at electrified solid–liquid interfaces(ESLIs)is crucial for revealing the typical surface restructuring and catalyst dissolution during electrocatalysis.Although advanced in situ tools and theoretical models have been proposed[1,2],identifying the nature of the active sites with atomic-scale spatial resolution remains a challenge,especially at ESLIs.In a recent work published in Nature,Zhang et al.[3]reported a groundbreaking atomic-resolution imaging of the structural dynamics of Cu nanowire catalysts in ESLIs for electrochemical CO_(2)reduction(ECR).
基金supported by the National Natural Science Foundation of China(51835005 and 51911540476)National Key Research and Development Program of China(2020YFB2010401)+3 种基金Hubei Province Natural Science Foundation for innovative research groups(2020CFA030)Independent Innovation Research Fund of HUST(2019kfyXMBZ025)Tencent Foundationthe Engineering and Physical Sciences Research Council project(EP/T019085/1).
文摘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.
基金the National Natural Science Foundation of China(22171157)he Banting Postdoctoral Fellowships of Canada。
文摘Precise synthesis at the atomic scale is a highly desirable and controllable route for the preparation of heterogeneous catalysts with the desired structure and properties,which promotes the rational design of highly efficient catalysts and facilitates the understanding of structure-properties relationship.The precise construction of the active sites of the catalysts provides important opportunities for atomic insight into the correlation between structure and catalytic performance.In this review,the atomic-level tuning strategies for the precise synthesis of heterogeneous catalysts are summarized with the emphasis on the precise control of the structure of active sites,including single atom sites,dual atom sites and complex active sites.Furthermore,we illustrate the crucial role of atomic-level regulation of structure in determining the catalytic performance by providing typical catalysis examples in different reactions.In the end,some perspectives on the further development of precise synthesis of catalysts at the atomic level are presented.
基金the Science Challenge Project(No.TZ2018006-0201-01)National Natural Science Foundation of China(Nos.52035009,61635008).
文摘Atomic and close-to-atomic scale manufacturing is the key technology for the production of next-generation devices with atomic precision.As an important approach of mechanical processing,cutting has evolved as a potential candidate to generate an atomically smooth surface;thus,exploring its ultimate capability is significant.In this paper,single-crystal graphite,whose lattice structure and chemical bond property are of representation for demonstration,is selected to study the mechanism of atomic layer removal using molecular dynamics.A localized workpiece,which is dynamically updated on the basis of the tool position,is used to improve the computation efficiency.The principle and bullet points of this modeling method are first introduced,followed by a series of simulations under various undeformed chip thicknesses and tool edge radi.In addition,different potentials for the tool-workpiece interaction are tested,and the effect on the material response is presented.Based on the analysis of deformation,the number of carbon layers removed,and cutting forces,the chip formation mechanism and further understanding of the controllability of cutting at atomic and close-to-atomic scale can be achieved.
基金This work was supported by the Science Foundation Ireland(SFI)(No.15/RP/B3208)the National Natural Science Foundation of China(NSFC)(No.52035009)。
文摘This paper presents a new approach for material removal on silicon at atomic and close-to-atomic scale assisted by photons.The corresponding mechanisms are also investigated.The proposed approach consists of two sequential steps:surface modification and photon irradiation.The back bonds of silicon atoms are first weakened by the chemisorption of chlorine and then broken by photon energy,leading to the desorption of chlorinated silicon.The mechanisms of photon-induced desorption of chlorinated silicon,i.e.,SiCl_(2) and SiCl,are explained by two models:the Menzel-Gomer-Redhead(MGR)and Antoniewicz models.The desorption probability associated with the two models is numerically calculated by solving the Liouville-von Neumann equations for open quantum systems.The calculation accuracy is verified by comparison with the results in literatures in the case of the NO/Pt(111)system.The calculation method is then applied to the cases of SiCl_(2)/Si and SiCl/Si systems.The results show that the value of desorption probability first increases dramatically and then saturates to a stable value within hundreds of femtoseconds after excitation.The desorption probability shows a super-linear dependence on the lifetime of excited states.
文摘The atomic time scale release system for multiple laboratories is completed by modular design according to the atomic clock data provided by eight domestic punctual laboratories.The system includes the three modules,the processing of atomic clock data,the calculation of atomic time scale and the release of atomic time scale data,using MATLAB for data processing and time scale calculation,and using GUI for data visualization design.The system has clear process of the algorithm,simple function modules and friendly human-machine interface.The operation results of actual data show that the time difference between the integrated atomic time scale of the system and UTC is better than±10ns,and the content of data release can meet the needs of the scientific research in related fields in China.
文摘Zeolites,as a class of porous inorganic materials,are extensively employed across a range of industrial applications,including catalysis[1],and adsorption separation[2],owing to their exceptional thermal stability,highly ordered pore structures,and tunable acidic properties.These characteristics enable zeolites to perform with remarkable efficiency and versatility in various processes.However,in the commonly employed aluminosilicate zeolites,Al atoms,acting as the active centers of acidity.
文摘The detailed understanding of various underlying processes at liquid/solid interfaces requires the development of interface-sensitive and high-resolution experimental techniques with atomic precision.In this perspective,we review the recent advances in studying the liquid/solid interfaces at atomic level by electrochemical scanning tunneling microscope(EC-STM),non-contact atomic force microscopy(NC-AFM),and surface-sensitive vibrational spectroscopies.Different from the ultrahigh vacuum and cryogenic experiments,these techniques are all operated in situ under ambient condition,making the measurements close to the native state of the liquid/solid interface.In the end,we present some perspectives on emerging techniques,which can defeat the limitation of existing imaging and spectroscopic methods in the characterization of liquid/solid interfaces.
基金supported by the National Natural Science Foundation of China(U2032131)the Key R&D Program of Shaanxi Province(2021GY-118)the Shanxi-Zheda Institute of Advanced Materials and Chemical Engineering(2022SX-TD012 and 2021SXTD012)。
文摘LiNi_(0.8)Co_(0.1)Mn_(0.1)O_(2)(NCM811)layered oxides have been regarded as promising alternative cathodes for the next generation of high-energy lithium ion batteries(LIBs)due to high discharge capacities and energy densities at high operation voltage.However,the capacity fading under high operation voltage still restricts the practical application.Herein,the capacity degradation mechanism of NCM811 at atomic-scale is studied in detail under various cut-off voltages using aberration-corrected scanning transmission electron microscopy(STEM).It is observed that the crystal structure of NCM811 evolution from a layered structure to a rock-salt phase is directly accompanied by serious intergranular cracks under 4.9 V,which is distinguished from the generally accepted structure evolution of layered,disordered layered,defect rock salt and rock salt phases,also observed under 4.3 and 4.7 V.The electron energy loss spectroscopy analysis also confirms the reduction of Ni and Co from the surface to the bulk,not the previously reported only Li/Ni interlayer mixing.The degradation mechanism of NCM811 at a high cut-off voltage of4.9 V is attributed to the formation of intergranular cracks induced by defects,the direct formation of the rock salt phase,and the accompanied reduction of Ni^(2+)and Co^(2+)phases from the surface to the bulk.
基金supported by the National Natural Science Foundation of China(Nos.21476007,21673197,21621091)the National Key R&D Program of China(No.2018YFA0209500)+4 种基金the 111 Project(No.B16029)the Fundamental Research Funds for the Central Universities of China(No.20720190037)the Natural Science Foundation of Fujian Province of China(No.2018J06003)the Special Project of Strategic Emerging Industries from Fujian Development and Reform CommissionChemcloudcomputing of Beijing University of Chemical Technology。
文摘The physicochemical properties of surfaces have a great effect on the micro-morphologies of the crystal structures which are in contact with them.Understanding the interaction mechanism between the internal driving forces of the crystal and external inducing forces of the surfaces is the prerequisite of controlling and obtaining the desirable morphologies.In this work,the dynamic density functional theory was applied to construct the free energy functional expression of polyethylene(PE)lattice,and the micro-dynamic evolution processes of PE lattice morphology near the surfaces with different properties were observed to reveal the interaction mechanism at atomic scale.The results showed that the physical and chemical properties of the external surfaces synergistically affect the morphologies in both the defect shapes and the distribution of the defect regions.In the absence of the contact surfaces,driven by the oriented interactions among different CH2 groups,PE lattices gradually grow and form a defect-free structure.Conversely,the presence of contact surfaces leads to lattice defects in the interfacial regions,and PE lattice shows different self-healing abilities around different surfaces.
