Friction is a phenomenon observed ubiquitously in daily life,yet its nature is complicated.Friction between rough surfaces is considered to arise primarily because of macroscopic roughness.In contrast,interatomic forc...Friction is a phenomenon observed ubiquitously in daily life,yet its nature is complicated.Friction between rough surfaces is considered to arise primarily because of macroscopic roughness.In contrast,interatomic forces dominate between clean and smooth surfaces.“Superlubricity”,where friction effectively becomes zero,occurs when the ratio of lattice parameters in the pair of surfaces becomes an irrational number.Superlubricity has been found to exist in a limited number of systems,but is a very important phenomenon both in industry and in mechanical engineering.New atomistic research on friction is under way,with the aim of refining theoretical models that consider interactions between atoms beyond mean field theory and experiments using ultrahigh vacuum non-contact atomic force microscopy.Such research is expected to help clarify the nature of microscopic friction,reveal the onset conditions of friction and superlubricity as well as the stability of superlubricity,discover new superlubric systems,and lead to new applications.展开更多
All-solid-state batteries(ASSBs)represent a next-generation energy storage technology,offering enhanced safety,higher energy density,and improved cycling stability compared to conventional liquid-electrolyte-based lit...All-solid-state batteries(ASSBs)represent a next-generation energy storage technology,offering enhanced safety,higher energy density,and improved cycling stability compared to conventional liquid-electrolyte-based lithium-ion batteries.Understanding and optimizing the complex chemistries and interfaces that underpin ASSB performance present significant challenges from both experimental and modeling perspectives.In particular,atomistic simulations face difficulties in capturing the complex structure,disorder,and dynamic evolution of materials and interfaces under practically relevant conditions.While established methods such as density functional theory and classical force fields have provided valuable insights,some questions remain difficult to address,particularly those involving large system sizes or long timescales.Recently,machine learning interatomic potentials(MLIPs)have emerged as a transformative tool,enabling atomistic simulations at length and time scales that were previously challenging to access with conventional approaches.By delivering near first-principles accuracy with much greater efficiency,MLIPs open new avenues for large-scale,long-timescale,and high-throughput simulations of solid-state battery materials.In this review,we present a comparative overview of density functional theory,classical force fields,and MLIPs,highlighting their respective strengths and limitations in ASSB research.We then discuss how MLIPs enable simulations that reach longer timescales,larger system sizes,and support high-throughput calculations,providing unique insights into ion transport and interfacial evolution in ASSBs.Finally,we conclude with a summary and outlook on current challenges and future opportunities for expanding MLIP capabilities and accelerating their impact in solid-state battery research.展开更多
Thermodynamically stable and ultra-thin “phase” at the interface, known as complexions, can significantly improve the mechanical properties of nanolayered composites. However, the effect of complexions features (e.g...Thermodynamically stable and ultra-thin “phase” at the interface, known as complexions, can significantly improve the mechanical properties of nanolayered composites. However, the effect of complexions features (e.g., crystalline orientation, crystalline structure and amorphous composition) on the plastic deformation remains inadequately investigated, and the correlation with the plastic transmission and mechanical response has not been fully established. Here, using atomistic simulations, we elucidate the different complexions-dominated plastic transmission and mechanical response. Complexions can alter the preferred slip system of dislocation nucleation, depending on the Schmid factor and interface structure. After nucleation, the dislocation density exhibits an inverse correlation with the stress magnitude, because the number of dislocations influences the initiation of plastic deformation and determines the stress release. For crystalline complexions with different structures and orientations, the ability of dislocation transmission is mainly dependent on the continuity of the slip system. The plastic transmission can easily proceed and exhibits relatively low flow stress when the slip system is well-aligned. In the case of amorphous complexions with different compositions, compositional variations impact the atomic percentage of shear transformation zones after loading, resulting in different magnitudes of plastic deformation. When smaller plastic deformation is produced, less stress can be released contributing to higher flow stress. These findings reveal the role of the complexions on plasticity behavior and provide valuable insights for the design of nanolayered composites.展开更多
Interstitial alloying has emerged as a powerful strategy to tune microstructure and microproperties of high-entropy alloys(HEAs) due to the strong interaction of interstitials with constituent elements and crystal def...Interstitial alloying has emerged as a powerful strategy to tune microstructure and microproperties of high-entropy alloys(HEAs) due to the strong interaction of interstitials with constituent elements and crystal defects,which enables the development of advanced alloys with superior mechanical and functional properties. The paper reviews the latest progress in the atomic-scale understanding of the effects of various interstitials, including carbon, boron, nitrogen, oxygen, and hydrogen, on the microstructure, stability, mechanical properties, and deformation behavior of HEAs. Emphases are placed on the in-depth insights on the interaction of interstitials with constituent elements and crystal defects, such as vacancies,stacking faults, and grain boundaries. Key parameters for rapid prediction of intrinsic properties of HEAs are also discussed. Finally, we highlight some unsolved issues and provide perspectives for future research directions.展开更多
Pronounced compositional fluctuations in CrMnFeCoNi high-entropy alloys(HEAs)lead to variations of the stacking-fault energy(SFE),which dominates the dislocation behavior and mechanical properties.However,studies on t...Pronounced compositional fluctuations in CrMnFeCoNi high-entropy alloys(HEAs)lead to variations of the stacking-fault energy(SFE),which dominates the dislocation behavior and mechanical properties.However,studies on the underlying dislocation behaviors and deformation mechanisms as a function of composition(Cr/Ni ratio)within CrMnFeCoNi HEAs are largely lacking,which hinders further understanding of the composition-structure-property relationships for the rational design of HEAs.Atomistic simulations were employed in this study to investigate the core structures and dynamic behaviors of a/2<110>edge dislocations in non-equiatomic CrMnFeCoNi HEA,as well as its plasticity mechanisms.The results show that the core structure of a/2<110>edge dislocations is planar after energy minimization,but with significant variations in the separation distance between two partial dislocations along the dislocation line owing to the complex local composition.The effects of the Cr/Ni ratio on the dislocation-solute interactions during dislocation gliding were calculated and discussed.Additionally,snapshots of dislocation motion under shear stress were analyzed.The observations indicate that the strengthening of the non-equiatomic CrMnFeCoNi HEA with increasing Cr concentration is not contributed by the expected solute/dislocation interactions,but the observed events of edge extended dislocation climbing through jog nucleation.The unusual but reasonable dislocation climbing phenomenon and the resultant strengthening observed in this study open extraordinary opportunities for obtaining outstanding mechanical properties in non-equiatomic CrMnFeCoNi HEAs by tailoring the compositional variations.展开更多
Theoretically,a twinning dislocation must stay on the twinning plane which is the first invariant plane of a twinning mode,because the glide of twinning dislocation linearly transforms the parent lattice to the twin l...Theoretically,a twinning dislocation must stay on the twinning plane which is the first invariant plane of a twinning mode,because the glide of twinning dislocation linearly transforms the parent lattice to the twin lattice.However,recent experimental observations showed that a{1011}{1012}twin variant could cross another variant during twin-twin interaction.It is well known that{1011}twinning is mediated by zonal twinning dislocations.Thus,how the zonal twinning dislocations transmute during twin-twin interaction is of great interest but not well understood.In this work,atomistic simulation is performed to investigate interaction between{1011}twin variants.Our results show that when an incoming twin variant impinges on the other which acts as a barrier,surprisingly,the barrier twin can grow at the expense of the incoming twin.Eventually one variant consumes the other.Structural analysis shows that the twinning dislocations of the barrier variant are able to penetrate the zone of twin-twin intersection,by plowing through the lattice of one variant and transform its lattice into the lattice of the other.Careful lattice correspondence analysis reveals that,the lattice transformation from one variant to the other is close to{1012}{1011}twinning,but the orientation relationship deviates by a minor lattice rotation.This deviation presents a significant energy barrier to the lattice transformation,and thus it is expected such a twin-twin interaction will increase the stress for twin growth.展开更多
To explore atomic-level phenomena in the Cu-Ni-Sn alloy,a second nearest-neighbor modified embedded-atom method(2NN MEAM)potential has been developed for the Cu-Ni-Sn system,building upon the work of other researchers...To explore atomic-level phenomena in the Cu-Ni-Sn alloy,a second nearest-neighbor modified embedded-atom method(2NN MEAM)potential has been developed for the Cu-Ni-Sn system,building upon the work of other researchers.This potential demonstrates remarkable accuracy in predicting the lattice constant,with a relative error of less than 0.5%when compared to density functional theory(DFT)results,and it achieves a 10%relative error in the enthalpy of formation compared to experimental data,marking substantial advancements over prior models.The bulk modulus is predicted with a relative error of 8%compared to DFT.Notably,the potential effectively simulates the processes of melting and solidification of Cu-15Ni-8Sn,with a simulated melting point that closely aligns with the experimental value,within a 7.5%margin.This serves as a foundation for establishing a 2NN MEAM potential for a flawless Cu-Ni-Sn system and its microalloying systems.展开更多
Grain boundary(GB)segregation substantially influences the mechanical properties and performance of magnesium(Mg).Atomic-scale modeling,typically using ab-initio or semi-empirical approaches,has mainly focused on GB s...Grain boundary(GB)segregation substantially influences the mechanical properties and performance of magnesium(Mg).Atomic-scale modeling,typically using ab-initio or semi-empirical approaches,has mainly focused on GB segregation at highly symmetric GBs in Mg alloys,often failing to capture the diversity of local atomic environments and segregation energies,resulting in inaccurate structure-property predictions.This study employs atomistic simulations and machine learning models to systematically investigate the segregation behavior of common solute elements in polycrystalline Mg at both 0 K and finite temperatures.The machine learning models accurately predict segregation thermodynamics by incorporating energetic and structural descriptors.We found that segregation energy and vibrational free energy follow skew-normal distributions,with hydrostatic stress,an indicator of excess free volume,emerging as an important factor influencing segregation tendency.The local atomic environment's flexibility,quantified by flexibility volume,is also crucial in predicting GB segregation.Comparing the grain boundary solute concentrations calculated via the Langmuir-Mc Lean isotherm with experimental data,we identified a pronounced segregation tendency for Nd,highlighting its potential for GB engineering in Mg alloys.This work demonstrates the powerful synergy of atomistic simulations and machine learning,paving the way for designing advanced lightweight Mg alloys with tailored properties.展开更多
The mechanical properties of Mg–Al–Ca alloys are significantly affected by their Laves phases,including the Al_(2)Ca phase.Laves phases are generally considered to be brittle and have a detrimental effect on the duc...The mechanical properties of Mg–Al–Ca alloys are significantly affected by their Laves phases,including the Al_(2)Ca phase.Laves phases are generally considered to be brittle and have a detrimental effect on the ductility of Mg.Recently,the Al_(2)Ca phase was shown to undergo plastic deformation in a dilute Mg-Al-Ca alloy to increase the ductility and work hardening of the alloy.In the present study,we investigated the extent to which the deformation of Al_(2)Ca is driven by dislocations in the Mg matrix by simulating the interactions between the basal edge dislocations and Al_(2)Ca particles.In particular,the effects of the interparticle spacing,particle orientation,and particle size were considered.Shearing of small particles and dislocation cross-slips near large particles were observed.Both events contribute to strengthening,and accommodate to plasticity.The shear resistance of the dislocation to bypass the particles increased as the particle size increased.The critical resolved shear stress(CRSS)for activating dislocations and stacking faults was easier to reach for small Al_(2)Ca particles owing to the higher local shear stress,which is consistent with the experimental observations.Overall,this work elucidates the driving force for Al_(2)Ca particles in Mg–Al–Ca alloys to undergo plastic deformation.展开更多
This paper investigates the temperature and loading rate dependencies of the critical stress intensity fac-tor(KIC)for dislocation nucleation at crack tips.We develop a new KIC formula with a generalized form by incor...This paper investigates the temperature and loading rate dependencies of the critical stress intensity fac-tor(KIC)for dislocation nucleation at crack tips.We develop a new KIC formula with a generalized form by incorporating the atomistic reaction pathway analysis into Transition State Theory(TST),which cap-tures the KIC of the first dislocation nucleation event at crack tips and its sensitivity to temperature and loading rates.We use this formula and atomistic modeling information to specifically calculate the KIC for quasi-two-dimensional crack tips located at various slant twin boundaries in nano-twinned TiAl al-loys across a wide range of temperatures and strain rates.Our findings reveal that twinning dislocation nucleation at the crack tip dominates crack propagation when twin boundaries(TBs)are tilted at 15.79°and 29.5°.Conversely,when TBs tilt at 45.29°,54.74°,and 70.53°,dislocation slip becomes the preferred mode.Additionally,at TB tilts of 29.5°and 70.53°,at higher temperatures above 800 K and typical exper-imental loading rates,both dislocation nucleation modes can be activated with nearly equal probability.This observation is particularly significant as it highlights scenarios that molecular dynamics simulations,due to their time scale limitations,cannot adequately explore.This insight underscores the importance of analyzing temperature and loading rate dependencies of the KIC to fully understand the competing mechanisms of dislocation nucleation and their impact on material behavior.展开更多
Spurious forces are a significant challenge for multi-scale methods,e.g.,the coupled atomistic/discrete dislocation(CADD)method.The assumption of isotropic matter in the continuum domain is a critical factor leading t...Spurious forces are a significant challenge for multi-scale methods,e.g.,the coupled atomistic/discrete dislocation(CADD)method.The assumption of isotropic matter in the continuum domain is a critical factor leading to such forces.This study aims to minimize spurious forces,ensuring that atomic dislocations experience more precise forces from the continuum domain.The authors have already implemented this idea using a simplified and unrealistic slipping system.To create a comprehensive and realistic model,this paper considers all possible slip systems in the face center cubic(FCC)lattice structure,and derives the required relationships for the displacement fields.An anisotropic version of the three-dimensional CADD(CADD3D)method is presented,which generates the anisotropic displacement fields for the partial dislocations in all the twelve slip systems of the FCC lattice structure.These displacement fields are tested for the most probable slip systems of aluminum,nickel,and copper with different anisotropic levels.Implementing these anisotropic displacement fields significantly reduces the spurious forces on the slip systems of FCC materials.This improvement is particularly pronounced at greater distances from the interface and in more anisotropic materials.Furthermore,the anisotropic CADD3D method enhances the spurious stress difference between the slip systems,particularly for materials with higher anisotropy.展开更多
Lithium-ion batteries are at the forefront of modern energy storage technology.However,the accumulation of by-products such as ethylene and carbon dioxide during charging and discharging cycles reduces battery effecti...Lithium-ion batteries are at the forefront of modern energy storage technology.However,the accumulation of by-products such as ethylene and carbon dioxide during charging and discharging cycles reduces battery effective capacity and threatens large-scale safe performance.With significant advantages over ethylene carbonate(EC)electrolytes,fluorinated electrolytes can more effectively suppress internal gas evolution,thereby improving battery safety and cycling stability.To reveal the mechanism behind gas formation in lithium-ion batteries,our study investigated the transport behavior and interfacial products of fluorinated electrolytes under various operation conditions,including electrode material and electrolyte composition.Innovatively,we applied the reaction network integrator ReacNetGenerator to the analysis of the solid electrolyte interface(SEI)in lithium batteries,providing more molecular fingerprint information from the perspective of specific products.Using reactive molecular dynamics(MD)simulations with the ReaxFF force field and EChemDID,complemented by density functional theory(DFT)calculations,our results demonstrate that fluorinated electrolytes can effectively suppress the decomposition of LiPF_(6) to produce toxic gases PFs and PF_3.DFT analysis further reveals that highly fluorinated solvents(e.g.,FEMC)enhance the anti-reduction stability of PF_(6)~-through synergistic regulation of molecular orbital energy levels,thermodynamic electron affinity,charge transfer,and electrostatic potential distribution,thereby mitigating LiPF_(6) decomposition.Additionally,fluorinated electrolytes generate significantly more LiF components than non-fluorinated ones to promote the formation of a stable and durable solid electrolyte interface(SEI).Experimental validations via XPS and GC-MS confirm reduced CO_(2) generation and LiF-enriched SEI formation,aligning with simulation and DFT data.The findings provide valuable insights for the design of advanced electrolytes aimed at ensuring large-scale,safe energy storage solutions.展开更多
Molecular dynamics （MD） simulations of monocrystalline copper （100） surface during nanomachining process were performed based on a new 3D simulation model. The material removal mechanism and system temperature dis...Molecular dynamics （MD） simulations of monocrystalline copper （100） surface during nanomachining process were performed based on a new 3D simulation model. The material removal mechanism and system temperature distribution were discussed. The simulation results indicate that the system temperature distribution presents a roughly concentric shape, a steep temperature gradient is observed in diamond cutting tool, and the highest temperature is located in chip. Centrosymmetry parameter method was used to monitor defect structures. Dislocations and vacancies are the two principal types of defect structures. Residual defect structures impose a major change on the workpiece physical properties and machined surface quality. The defect structures in workpiece are temperature dependent. As the temperature increases, the dislocations are mainly mediated from the workpiece surface, while the others are dissociated into point defects. The relatively high cutting speed used in nanomachining results in less defect structures, beneficial to obtain highly machined surface quality.展开更多
A semi-empirical interatomic potential formalism,the second-nearest-neighbor modified embedded-atom method(2NN MEAM),has been applied to obtaining interatomic potentials for the Co-W and Al-W binary system using previ...A semi-empirical interatomic potential formalism,the second-nearest-neighbor modified embedded-atom method(2NN MEAM),has been applied to obtaining interatomic potentials for the Co-W and Al-W binary system using previously developed MEAM potentials of Co,Al and W.The potential parameters were determined by fitting the experimental data on the enthalpy of formation,lattice parameter,melting point and elastic constants.The present potentials generally reproduce the fundamental physical properties of the Co-W and Al-W systems accurately.The lattice parameters,the enthalpy of formation,the thermal stability and the elastic constants match well with experiment and the first-principles results.The enthalpy of mixing and the enthalpy of formation and mixing of liquid are in good agreement with CALPHAD calculations.The potentials can be easily combined with already-developed MEAM potentials for binary cobalt systems and can be used to describe Co-Al-W-based multicomponent alloys,especially for interfacial properties.展开更多
This article focuses on a new insight into the energy classification of sublayers. In this article, the study brings out very interesting and enriching information, knowledge and knowledge in atomistics. An affine fun...This article focuses on a new insight into the energy classification of sublayers. In this article, the study brings out very interesting and enriching information, knowledge and knowledge in atomistics. An affine function is represented in an orthonormal frame while assimilating a point to a sublayer. This made it possible to draw up a graph integrating each of the diagrams of the known energy levels. Our results are conclusive. We can then confirm that the research hypothesis is verified.展开更多
Deformation twinning, i.e., twin nucleation and twin growth （or twin boundary migration, TBM） activated by impinged basal slip at a symmetrical tilt grain boundary in HCP Mg, was examined with molecular dynamics （M...Deformation twinning, i.e., twin nucleation and twin growth （or twin boundary migration, TBM） activated by impinged basal slip at a symmetrical tilt grain boundary in HCP Mg, was examined with molecular dynamics （MD） simulations. The results show that the {1^-1^-21}-type twinning acts as the most preferential mode of twinning. Once such twins are formed, they are almost ready to grow. The TBM of such twins is led by pure atomic shuffling events. A secondary mode of twinning can also occur in our simulations. The {112^-2} twinning is observed at 10 K as the secondary twin. This secondary mode of twinning shows different energy barriers for nucleation as well as for growth compared with the {1^-1^-21}-type twining. In particular, TBMs in this case is triggered intrinsically by pyramidal slip at its twin boundary.展开更多
Coupled atomistic/dislocation/continuum simulation of interfacial fracture is performed in this paper.The model consists of a nanoscopic core made by atomistic assembly and a surrounding elastic continuum with discret...Coupled atomistic/dislocation/continuum simulation of interfacial fracture is performed in this paper.The model consists of a nanoscopic core made by atomistic assembly and a surrounding elastic continuum with discrete dislocations. Atomistic dislocations nucleate from the crack tip and move to the continuum layer where they glide according to the dislocation dynamics curve.An atoms/continuum overlapping belt is devised to facilitate the transition between the two scales.The continuum constraint on the atomic assembly is imposed through the mechanics at- mosphere along the overlapping belt.Transmissions of mechanics parameters such as displacements,stresses,masses and momenta across the belt are realized.The present model allows us to explore interfacial fracture processes under different mode mixity.The effect of atomistic zigzag interface on the fracture process is revealed:it hinders dislocation emission from the crack tip,especially under high mode mixity.展开更多
The phenomenon of interfacial fracture, as manifested by atom- istic cleavage, debonding and dislocation emission, provides a challenge for combined atomistic-continuum analysis. As a precursor for fully coupled atomi...The phenomenon of interfacial fracture, as manifested by atom- istic cleavage, debonding and dislocation emission, provides a challenge for combined atomistic-continuum analysis. As a precursor for fully coupled atomistic-continuum simulation of interfacial fracture, we focus here on the atomistic behavior within a nanoscopic core surrounding the crack tip. The inter-atomic potential under Em- bedded Atom Method is recapitulated to form an essential framework of atomistic simulation. The calculations are performed for a side-cracked disc configuration un- der a remote K field loading. It is revealed that a critical loading rate defines the brittle-to-ductile transition of homogeneous materials. We further observe that the near tip mode mixity dictates the nanoscopic profile near an interfacial crack tip. A zigzag interface structure is simulated which plays a significant role in the dislocation emission from an interfacial crack tip, as will be explored in the second part of this investigation.展开更多
Al,Ca,and Zn are representative commercial alloying elements for Mg alloys.To investigate the effects of these elements on the deformation and recrystallization behaviors of Mg alloys,we develop interatomic potentials...Al,Ca,and Zn are representative commercial alloying elements for Mg alloys.To investigate the effects of these elements on the deformation and recrystallization behaviors of Mg alloys,we develop interatomic potentials for the Al-Ca,Al-Zn,Mg-Al-Ca and Mg-Al-Zn systems based on the second nearest-neighbor modified embedded-atom method formalism.The developed potentials describe structural,elastic,and thermodynamic properties of compounds and solutions of associated alloy systems in reasonable agreement with experimental data and higher-level calculations.The applicability of these potentials to the present investigation is confirmed by calculating the generalized stacking fault energy for various slip systems and the segregation energy on twin boundaries of the Mg-Al-Ca and Mg-Al-Zn alloys,accompanied with the thermal expansion coefficient and crystal structure maintenance of stable compounds in those alloys.展开更多
When wood-based activated carbon was tailored with quaternary ammonium/epoxide(QAE) forming compounds(QAE-AC), this tailoring dramatically improved the carbon's effectiveness for removing perfluorooctanoic acid(PF...When wood-based activated carbon was tailored with quaternary ammonium/epoxide(QAE) forming compounds(QAE-AC), this tailoring dramatically improved the carbon's effectiveness for removing perfluorooctanoic acid(PFOA) from groundwater. With favorable tailoring, QAE-AC removed PFOA from groundwater for 118,000 bed volumes before halfbreakthrough in rapid small scale column tests, while the influent PFOA concentration was 200 ng/L. The tailoring involved pre-dosing QAE at an array of proportions onto this carbon, and then monitoring bed life for PFOA removal. When pre-dosing with 1 mL QAE, this PFOA bed life reached an interim peak, whereas bed life was less following 3 mL QAE pre-dosing, then PFOA bed life exhibited a steady rise for yet subsequently higher QAE pre-dosing levels. Large-scale atomistic modelling was used herein to provide new insight into the mechanism of PFOA removal by QAE-AC. Based on experimental results and modelling, the authors perceived that the QAE's epoxide functionalities cross-linked with phenolics that were present along the activated carbon's graphene edge sites, in a manner that created mesopores within macroporous regions or created micropores within mesopores regions. Also, the QAE could react with hydroxyls outside of these pore, including the hydroxyls of both graphene edge sites and other QAE molecules. This latter reaction formed new pore-like structures that were external to the activated carbon grains. Adsorption of PFOA could occur via either charge balance between negatively charged PFOA with positively charged QAE, or by van der Waals forces between PFOA's fluoro-carbon tail and the graphene or QAE carbon surfaces.展开更多
文摘Friction is a phenomenon observed ubiquitously in daily life,yet its nature is complicated.Friction between rough surfaces is considered to arise primarily because of macroscopic roughness.In contrast,interatomic forces dominate between clean and smooth surfaces.“Superlubricity”,where friction effectively becomes zero,occurs when the ratio of lattice parameters in the pair of surfaces becomes an irrational number.Superlubricity has been found to exist in a limited number of systems,but is a very important phenomenon both in industry and in mechanical engineering.New atomistic research on friction is under way,with the aim of refining theoretical models that consider interactions between atoms beyond mean field theory and experiments using ultrahigh vacuum non-contact atomic force microscopy.Such research is expected to help clarify the nature of microscopic friction,reveal the onset conditions of friction and superlubricity as well as the stability of superlubricity,discover new superlubric systems,and lead to new applications.
文摘All-solid-state batteries(ASSBs)represent a next-generation energy storage technology,offering enhanced safety,higher energy density,and improved cycling stability compared to conventional liquid-electrolyte-based lithium-ion batteries.Understanding and optimizing the complex chemistries and interfaces that underpin ASSB performance present significant challenges from both experimental and modeling perspectives.In particular,atomistic simulations face difficulties in capturing the complex structure,disorder,and dynamic evolution of materials and interfaces under practically relevant conditions.While established methods such as density functional theory and classical force fields have provided valuable insights,some questions remain difficult to address,particularly those involving large system sizes or long timescales.Recently,machine learning interatomic potentials(MLIPs)have emerged as a transformative tool,enabling atomistic simulations at length and time scales that were previously challenging to access with conventional approaches.By delivering near first-principles accuracy with much greater efficiency,MLIPs open new avenues for large-scale,long-timescale,and high-throughput simulations of solid-state battery materials.In this review,we present a comparative overview of density functional theory,classical force fields,and MLIPs,highlighting their respective strengths and limitations in ASSB research.We then discuss how MLIPs enable simulations that reach longer timescales,larger system sizes,and support high-throughput calculations,providing unique insights into ion transport and interfacial evolution in ASSBs.Finally,we conclude with a summary and outlook on current challenges and future opportunities for expanding MLIP capabilities and accelerating their impact in solid-state battery research.
基金supported by the National Natural Science Foundation of China(Nos.U23A20543,52071124)the Natural Science Foundation of the Hebei Province(No.E2021202135).
文摘Thermodynamically stable and ultra-thin “phase” at the interface, known as complexions, can significantly improve the mechanical properties of nanolayered composites. However, the effect of complexions features (e.g., crystalline orientation, crystalline structure and amorphous composition) on the plastic deformation remains inadequately investigated, and the correlation with the plastic transmission and mechanical response has not been fully established. Here, using atomistic simulations, we elucidate the different complexions-dominated plastic transmission and mechanical response. Complexions can alter the preferred slip system of dislocation nucleation, depending on the Schmid factor and interface structure. After nucleation, the dislocation density exhibits an inverse correlation with the stress magnitude, because the number of dislocations influences the initiation of plastic deformation and determines the stress release. For crystalline complexions with different structures and orientations, the ability of dislocation transmission is mainly dependent on the continuity of the slip system. The plastic transmission can easily proceed and exhibits relatively low flow stress when the slip system is well-aligned. In the case of amorphous complexions with different compositions, compositional variations impact the atomic percentage of shear transformation zones after loading, resulting in different magnitudes of plastic deformation. When smaller plastic deformation is produced, less stress can be released contributing to higher flow stress. These findings reveal the role of the complexions on plasticity behavior and provide valuable insights for the design of nanolayered composites.
基金the financial support from National Natural Science Foundation of China(No.52171162)Research Grants Council of Hong Kong(Nos.15202824,15227121,C5002-24Y,C1017D21GF,and C1020D21GF)+4 种基金Shenzhen Science and Technology Program(No.JCYJ20210324142203009)the Research Institute for Advanced Manufacturing Fund(No.P0046108)PolyU Fund(Nos.P0044243 and P0043467)Guangdong Science and Technology Innovation Foundation(No.2023A1515240061)Open access funding provided by The Hong Kong Polytechnic University
文摘Interstitial alloying has emerged as a powerful strategy to tune microstructure and microproperties of high-entropy alloys(HEAs) due to the strong interaction of interstitials with constituent elements and crystal defects,which enables the development of advanced alloys with superior mechanical and functional properties. The paper reviews the latest progress in the atomic-scale understanding of the effects of various interstitials, including carbon, boron, nitrogen, oxygen, and hydrogen, on the microstructure, stability, mechanical properties, and deformation behavior of HEAs. Emphases are placed on the in-depth insights on the interaction of interstitials with constituent elements and crystal defects, such as vacancies,stacking faults, and grain boundaries. Key parameters for rapid prediction of intrinsic properties of HEAs are also discussed. Finally, we highlight some unsolved issues and provide perspectives for future research directions.
基金supported by the National Natural Science Foundation of China(No.52275352)the National Key Research and Development Program of China(No.2022YFB3706902)Inner Mongolia-SJTU Science and Technology Cooperation Special Project(No.2023XYJG0001-01-01).
文摘Pronounced compositional fluctuations in CrMnFeCoNi high-entropy alloys(HEAs)lead to variations of the stacking-fault energy(SFE),which dominates the dislocation behavior and mechanical properties.However,studies on the underlying dislocation behaviors and deformation mechanisms as a function of composition(Cr/Ni ratio)within CrMnFeCoNi HEAs are largely lacking,which hinders further understanding of the composition-structure-property relationships for the rational design of HEAs.Atomistic simulations were employed in this study to investigate the core structures and dynamic behaviors of a/2<110>edge dislocations in non-equiatomic CrMnFeCoNi HEA,as well as its plasticity mechanisms.The results show that the core structure of a/2<110>edge dislocations is planar after energy minimization,but with significant variations in the separation distance between two partial dislocations along the dislocation line owing to the complex local composition.The effects of the Cr/Ni ratio on the dislocation-solute interactions during dislocation gliding were calculated and discussed.Additionally,snapshots of dislocation motion under shear stress were analyzed.The observations indicate that the strengthening of the non-equiatomic CrMnFeCoNi HEA with increasing Cr concentration is not contributed by the expected solute/dislocation interactions,but the observed events of edge extended dislocation climbing through jog nucleation.The unusual but reasonable dislocation climbing phenomenon and the resultant strengthening observed in this study open extraordinary opportunities for obtaining outstanding mechanical properties in non-equiatomic CrMnFeCoNi HEAs by tailoring the compositional variations.
基金support from U.S.National Science Foundation(NSF)(CMMI-2016263,2032483).
文摘Theoretically,a twinning dislocation must stay on the twinning plane which is the first invariant plane of a twinning mode,because the glide of twinning dislocation linearly transforms the parent lattice to the twin lattice.However,recent experimental observations showed that a{1011}{1012}twin variant could cross another variant during twin-twin interaction.It is well known that{1011}twinning is mediated by zonal twinning dislocations.Thus,how the zonal twinning dislocations transmute during twin-twin interaction is of great interest but not well understood.In this work,atomistic simulation is performed to investigate interaction between{1011}twin variants.Our results show that when an incoming twin variant impinges on the other which acts as a barrier,surprisingly,the barrier twin can grow at the expense of the incoming twin.Eventually one variant consumes the other.Structural analysis shows that the twinning dislocations of the barrier variant are able to penetrate the zone of twin-twin intersection,by plowing through the lattice of one variant and transform its lattice into the lattice of the other.Careful lattice correspondence analysis reveals that,the lattice transformation from one variant to the other is close to{1012}{1011}twinning,but the orientation relationship deviates by a minor lattice rotation.This deviation presents a significant energy barrier to the lattice transformation,and thus it is expected such a twin-twin interaction will increase the stress for twin growth.
基金sponsored by the Science and Technology Foundation of Guizhou Provincial Education Department(No.QJJ[2024]60)Guizhou Provincial Basic Research Program(Natural Science)(No.QKHJC[2024]Youth 214)+1 种基金Science and Technology Foundation of Guizhou Minzu University(No.GZMUZK[2024]QD21)Research Projects of Anshun University(No.asxybsjj202413).
文摘To explore atomic-level phenomena in the Cu-Ni-Sn alloy,a second nearest-neighbor modified embedded-atom method(2NN MEAM)potential has been developed for the Cu-Ni-Sn system,building upon the work of other researchers.This potential demonstrates remarkable accuracy in predicting the lattice constant,with a relative error of less than 0.5%when compared to density functional theory(DFT)results,and it achieves a 10%relative error in the enthalpy of formation compared to experimental data,marking substantial advancements over prior models.The bulk modulus is predicted with a relative error of 8%compared to DFT.Notably,the potential effectively simulates the processes of melting and solidification of Cu-15Ni-8Sn,with a simulated melting point that closely aligns with the experimental value,within a 7.5%margin.This serves as a foundation for establishing a 2NN MEAM potential for a flawless Cu-Ni-Sn system and its microalloying systems.
基金Z.X.and T.A.S.acknowledge the financial support by the German Research Foundation(DFG)(Grant Nr.505716422)T.A.S.are grateful for the financial support from the DFG(Grant Nr.AL1343/7-1,AL1343/8-1 and Yi 103/3-1)+4 种基金Z.X.,S.K.K.and U.K.acknowledge financial support by the DFG through the projects A05,A07 and C02 of the SFB1394 StructuralChemical Atomic Complexity-From Defect Phase Diagrams to Material Properties,project ID 409476157Additionally,Z.X.and S.K.K.are grateful for funding from the European Research Council(ERC)under the European Union’s Horizon 2020 research and innovation program(grant agreement No.852096 FunBlocks)J.G.acknowledges funding from the French National Research Agency(ANR),Grant ANR-21-CE08-0001(ATOUUM)and ANR-22-CE92-0058-01(SILA)The authors gratefully acknowledge the computing time provided to them at the NHR Center NHR4CES at RWTH Aachen University(project number p0020431 and p0020267)。
文摘Grain boundary(GB)segregation substantially influences the mechanical properties and performance of magnesium(Mg).Atomic-scale modeling,typically using ab-initio or semi-empirical approaches,has mainly focused on GB segregation at highly symmetric GBs in Mg alloys,often failing to capture the diversity of local atomic environments and segregation energies,resulting in inaccurate structure-property predictions.This study employs atomistic simulations and machine learning models to systematically investigate the segregation behavior of common solute elements in polycrystalline Mg at both 0 K and finite temperatures.The machine learning models accurately predict segregation thermodynamics by incorporating energetic and structural descriptors.We found that segregation energy and vibrational free energy follow skew-normal distributions,with hydrostatic stress,an indicator of excess free volume,emerging as an important factor influencing segregation tendency.The local atomic environment's flexibility,quantified by flexibility volume,is also crucial in predicting GB segregation.Comparing the grain boundary solute concentrations calculated via the Langmuir-Mc Lean isotherm with experimental data,we identified a pronounced segregation tendency for Nd,highlighting its potential for GB engineering in Mg alloys.This work demonstrates the powerful synergy of atomistic simulations and machine learning,paving the way for designing advanced lightweight Mg alloys with tailored properties.
基金funded by the National Natural Science Foundation of China(nos.51631006 and 51825101)。
文摘The mechanical properties of Mg–Al–Ca alloys are significantly affected by their Laves phases,including the Al_(2)Ca phase.Laves phases are generally considered to be brittle and have a detrimental effect on the ductility of Mg.Recently,the Al_(2)Ca phase was shown to undergo plastic deformation in a dilute Mg-Al-Ca alloy to increase the ductility and work hardening of the alloy.In the present study,we investigated the extent to which the deformation of Al_(2)Ca is driven by dislocations in the Mg matrix by simulating the interactions between the basal edge dislocations and Al_(2)Ca particles.In particular,the effects of the interparticle spacing,particle orientation,and particle size were considered.Shearing of small particles and dislocation cross-slips near large particles were observed.Both events contribute to strengthening,and accommodate to plasticity.The shear resistance of the dislocation to bypass the particles increased as the particle size increased.The critical resolved shear stress(CRSS)for activating dislocations and stacking faults was easier to reach for small Al_(2)Ca particles owing to the higher local shear stress,which is consistent with the experimental observations.Overall,this work elucidates the driving force for Al_(2)Ca particles in Mg–Al–Ca alloys to undergo plastic deformation.
基金supported by the China Scholarship Council(Grant No.202007865002)the National Natural Science Foundation of China(Grant Nos.51865027,52065036,and 52065037)+2 种基金the Educational Unveiling Leadership Project of Gansu Province of China(Grant No.2021jyjbgs01)the support by JSPS KAKENHI(Grant No.JP23K20037)MEXT Programs(Grant Nos.JPMXP1122684766,JPMXP1020230325,and JPMXP1020230327).
文摘This paper investigates the temperature and loading rate dependencies of the critical stress intensity fac-tor(KIC)for dislocation nucleation at crack tips.We develop a new KIC formula with a generalized form by incorporating the atomistic reaction pathway analysis into Transition State Theory(TST),which cap-tures the KIC of the first dislocation nucleation event at crack tips and its sensitivity to temperature and loading rates.We use this formula and atomistic modeling information to specifically calculate the KIC for quasi-two-dimensional crack tips located at various slant twin boundaries in nano-twinned TiAl al-loys across a wide range of temperatures and strain rates.Our findings reveal that twinning dislocation nucleation at the crack tip dominates crack propagation when twin boundaries(TBs)are tilted at 15.79°and 29.5°.Conversely,when TBs tilt at 45.29°,54.74°,and 70.53°,dislocation slip becomes the preferred mode.Additionally,at TB tilts of 29.5°and 70.53°,at higher temperatures above 800 K and typical exper-imental loading rates,both dislocation nucleation modes can be activated with nearly equal probability.This observation is particularly significant as it highlights scenarios that molecular dynamics simulations,due to their time scale limitations,cannot adequately explore.This insight underscores the importance of analyzing temperature and loading rate dependencies of the KIC to fully understand the competing mechanisms of dislocation nucleation and their impact on material behavior.
文摘Spurious forces are a significant challenge for multi-scale methods,e.g.,the coupled atomistic/discrete dislocation(CADD)method.The assumption of isotropic matter in the continuum domain is a critical factor leading to such forces.This study aims to minimize spurious forces,ensuring that atomic dislocations experience more precise forces from the continuum domain.The authors have already implemented this idea using a simplified and unrealistic slipping system.To create a comprehensive and realistic model,this paper considers all possible slip systems in the face center cubic(FCC)lattice structure,and derives the required relationships for the displacement fields.An anisotropic version of the three-dimensional CADD(CADD3D)method is presented,which generates the anisotropic displacement fields for the partial dislocations in all the twelve slip systems of the FCC lattice structure.These displacement fields are tested for the most probable slip systems of aluminum,nickel,and copper with different anisotropic levels.Implementing these anisotropic displacement fields significantly reduces the spurious forces on the slip systems of FCC materials.This improvement is particularly pronounced at greater distances from the interface and in more anisotropic materials.Furthermore,the anisotropic CADD3D method enhances the spurious stress difference between the slip systems,particularly for materials with higher anisotropy.
基金funding support from the National Natural Science Foundation of China(Grant No.52302302)the National Key R&D Program of China(Grant No.2022YFE0208000)+1 种基金the Fundamental Research Funds for the Central Universitiesthe Special Funds of Tongji University for“Sino-German Cooperation 2.0 Strategy”。
文摘Lithium-ion batteries are at the forefront of modern energy storage technology.However,the accumulation of by-products such as ethylene and carbon dioxide during charging and discharging cycles reduces battery effective capacity and threatens large-scale safe performance.With significant advantages over ethylene carbonate(EC)electrolytes,fluorinated electrolytes can more effectively suppress internal gas evolution,thereby improving battery safety and cycling stability.To reveal the mechanism behind gas formation in lithium-ion batteries,our study investigated the transport behavior and interfacial products of fluorinated electrolytes under various operation conditions,including electrode material and electrolyte composition.Innovatively,we applied the reaction network integrator ReacNetGenerator to the analysis of the solid electrolyte interface(SEI)in lithium batteries,providing more molecular fingerprint information from the perspective of specific products.Using reactive molecular dynamics(MD)simulations with the ReaxFF force field and EChemDID,complemented by density functional theory(DFT)calculations,our results demonstrate that fluorinated electrolytes can effectively suppress the decomposition of LiPF_(6) to produce toxic gases PFs and PF_3.DFT analysis further reveals that highly fluorinated solvents(e.g.,FEMC)enhance the anti-reduction stability of PF_(6)~-through synergistic regulation of molecular orbital energy levels,thermodynamic electron affinity,charge transfer,and electrostatic potential distribution,thereby mitigating LiPF_(6) decomposition.Additionally,fluorinated electrolytes generate significantly more LiF components than non-fluorinated ones to promote the formation of a stable and durable solid electrolyte interface(SEI).Experimental validations via XPS and GC-MS confirm reduced CO_(2) generation and LiF-enriched SEI formation,aligning with simulation and DFT data.The findings provide valuable insights for the design of advanced electrolytes aimed at ensuring large-scale,safe energy storage solutions.
基金Project (50925521) supported by the National Natural Science Fund for Distinguished Young Scholars of China
文摘Molecular dynamics （MD） simulations of monocrystalline copper （100） surface during nanomachining process were performed based on a new 3D simulation model. The material removal mechanism and system temperature distribution were discussed. The simulation results indicate that the system temperature distribution presents a roughly concentric shape, a steep temperature gradient is observed in diamond cutting tool, and the highest temperature is located in chip. Centrosymmetry parameter method was used to monitor defect structures. Dislocations and vacancies are the two principal types of defect structures. Residual defect structures impose a major change on the workpiece physical properties and machined surface quality. The defect structures in workpiece are temperature dependent. As the temperature increases, the dislocations are mainly mediated from the workpiece surface, while the others are dissociated into point defects. The relatively high cutting speed used in nanomachining results in less defect structures, beneficial to obtain highly machined surface quality.
基金Project(51274167)supported by the National Natural Science Foundation of ChinaProject(LQ14E010002)supported by the Zhejiang Provincial Natural Science Foundation of ChinaProject(2E24692)supported by the KIST Institutional Programs,Korea
文摘A semi-empirical interatomic potential formalism,the second-nearest-neighbor modified embedded-atom method(2NN MEAM),has been applied to obtaining interatomic potentials for the Co-W and Al-W binary system using previously developed MEAM potentials of Co,Al and W.The potential parameters were determined by fitting the experimental data on the enthalpy of formation,lattice parameter,melting point and elastic constants.The present potentials generally reproduce the fundamental physical properties of the Co-W and Al-W systems accurately.The lattice parameters,the enthalpy of formation,the thermal stability and the elastic constants match well with experiment and the first-principles results.The enthalpy of mixing and the enthalpy of formation and mixing of liquid are in good agreement with CALPHAD calculations.The potentials can be easily combined with already-developed MEAM potentials for binary cobalt systems and can be used to describe Co-Al-W-based multicomponent alloys,especially for interfacial properties.
文摘This article focuses on a new insight into the energy classification of sublayers. In this article, the study brings out very interesting and enriching information, knowledge and knowledge in atomistics. An affine function is represented in an orthonormal frame while assimilating a point to a sublayer. This made it possible to draw up a graph integrating each of the diagrams of the known energy levels. Our results are conclusive. We can then confirm that the research hypothesis is verified.
基金Project(2012CB932202)supported by the National Basic Research Program of ChinaProjects(50890174,50971088)supported by the National Natural Science Foundation of China
文摘Deformation twinning, i.e., twin nucleation and twin growth （or twin boundary migration, TBM） activated by impinged basal slip at a symmetrical tilt grain boundary in HCP Mg, was examined with molecular dynamics （MD） simulations. The results show that the {1^-1^-21}-type twinning acts as the most preferential mode of twinning. Once such twins are formed, they are almost ready to grow. The TBM of such twins is led by pure atomic shuffling events. A secondary mode of twinning can also occur in our simulations. The {112^-2} twinning is observed at 10 K as the secondary twin. This secondary mode of twinning shows different energy barriers for nucleation as well as for growth compared with the {1^-1^-21}-type twining. In particular, TBMs in this case is triggered intrinsically by pyramidal slip at its twin boundary.
基金The project supported by the National Natural Science Foundation of China
文摘Coupled atomistic/dislocation/continuum simulation of interfacial fracture is performed in this paper.The model consists of a nanoscopic core made by atomistic assembly and a surrounding elastic continuum with discrete dislocations. Atomistic dislocations nucleate from the crack tip and move to the continuum layer where they glide according to the dislocation dynamics curve.An atoms/continuum overlapping belt is devised to facilitate the transition between the two scales.The continuum constraint on the atomic assembly is imposed through the mechanics at- mosphere along the overlapping belt.Transmissions of mechanics parameters such as displacements,stresses,masses and momenta across the belt are realized.The present model allows us to explore interfacial fracture processes under different mode mixity.The effect of atomistic zigzag interface on the fracture process is revealed:it hinders dislocation emission from the crack tip,especially under high mode mixity.
基金The project supported by the National Natural Science Foundation of China
文摘The phenomenon of interfacial fracture, as manifested by atom- istic cleavage, debonding and dislocation emission, provides a challenge for combined atomistic-continuum analysis. As a precursor for fully coupled atomistic-continuum simulation of interfacial fracture, we focus here on the atomistic behavior within a nanoscopic core surrounding the crack tip. The inter-atomic potential under Em- bedded Atom Method is recapitulated to form an essential framework of atomistic simulation. The calculations are performed for a side-cracked disc configuration un- der a remote K field loading. It is revealed that a critical loading rate defines the brittle-to-ductile transition of homogeneous materials. We further observe that the near tip mode mixity dictates the nanoscopic profile near an interfacial crack tip. A zigzag interface structure is simulated which plays a significant role in the dislocation emission from an interfacial crack tip, as will be explored in the second part of this investigation.
文摘Al,Ca,and Zn are representative commercial alloying elements for Mg alloys.To investigate the effects of these elements on the deformation and recrystallization behaviors of Mg alloys,we develop interatomic potentials for the Al-Ca,Al-Zn,Mg-Al-Ca and Mg-Al-Zn systems based on the second nearest-neighbor modified embedded-atom method formalism.The developed potentials describe structural,elastic,and thermodynamic properties of compounds and solutions of associated alloy systems in reasonable agreement with experimental data and higher-level calculations.The applicability of these potentials to the present investigation is confirmed by calculating the generalized stacking fault energy for various slip systems and the segregation energy on twin boundaries of the Mg-Al-Ca and Mg-Al-Zn alloys,accompanied with the thermal expansion coefficient and crystal structure maintenance of stable compounds in those alloys.
基金funding from Evoqua Companythe National Natural Science Foundation of China (Nos. 51878090 and 51808066)the Chinese Scholarship Council for financial support。
文摘When wood-based activated carbon was tailored with quaternary ammonium/epoxide(QAE) forming compounds(QAE-AC), this tailoring dramatically improved the carbon's effectiveness for removing perfluorooctanoic acid(PFOA) from groundwater. With favorable tailoring, QAE-AC removed PFOA from groundwater for 118,000 bed volumes before halfbreakthrough in rapid small scale column tests, while the influent PFOA concentration was 200 ng/L. The tailoring involved pre-dosing QAE at an array of proportions onto this carbon, and then monitoring bed life for PFOA removal. When pre-dosing with 1 mL QAE, this PFOA bed life reached an interim peak, whereas bed life was less following 3 mL QAE pre-dosing, then PFOA bed life exhibited a steady rise for yet subsequently higher QAE pre-dosing levels. Large-scale atomistic modelling was used herein to provide new insight into the mechanism of PFOA removal by QAE-AC. Based on experimental results and modelling, the authors perceived that the QAE's epoxide functionalities cross-linked with phenolics that were present along the activated carbon's graphene edge sites, in a manner that created mesopores within macroporous regions or created micropores within mesopores regions. Also, the QAE could react with hydroxyls outside of these pore, including the hydroxyls of both graphene edge sites and other QAE molecules. This latter reaction formed new pore-like structures that were external to the activated carbon grains. Adsorption of PFOA could occur via either charge balance between negatively charged PFOA with positively charged QAE, or by van der Waals forces between PFOA's fluoro-carbon tail and the graphene or QAE carbon surfaces.
