Maozhi Li

Effect of local structures and atomic packing on glass forming ability in CuxZr100−x metallic glasses

Molecular dynamics simulations are performed for CuZr metallic alloys to study the structural and dynamical features for glass forming ability (GFA). Our analysis shows that in CuZr metallic system, although ⟨0,0,12,0⟩ icosahedral clusters are important, some Zr-centered clusters such as ⟨0,1,10,4⟩ and ⟨0,1,10,5⟩ play a key role in slowing down the dynamics. It is found that these Zr-centered clusters are intrinsically slow and fundamentally determine the stability and slow dynamics. Due to the strong spatial correlation between ⟨0,0,12,0⟩ and Zr-centered clusters, their relative population influences the dense packing and dynamics in metallic glasses, and further the GFA.

Effect of local structures on structural evolution during crystallization in undercooled metallic glass-forming liquids.

The effect of local structures on structural evolution during the crystallization of undercooled ZrCu metallic glass-forming liquid was studied via molecular dynamics simulations. It is found that body-centered-cubic (bcc)-like clusters play a key role in structural evolution during crystallization. In contrast to previous speculations, the number of bcc-like crystal nuclei does not change much before the onset of crystallization. Instead, the development of a bcc-like critical nucleus during annealing leads to a strong spatial correlation with other nuclei in its surroundings, forming a crystalline structure template. It is also found that the size distribution of bcc-like nuclei follows a power-law form with an exponential cutoff in the early stage of annealing, but changes to a pure power-law behavior just before the onset of crystallization. This implies that the crystalline structure template has fractal feature and the undercooled liquids evolve to a self-organized critical state before the onset of crystallization, which might trigger the subsequent rapid crystallization. According to the graph theory analysis, it is also found that the observed large scatter of the onset time of crystallization in different liquid samples results from the connectivity of the bcc-like clusters.

Characterization of mechanical heterogeneity in amorphous solids

The structural geometry and size distribution of the local atomic rearrangements induced by external stress in amorphous solids are investigated by molecular dynamics studies. We find that the size distribution exhibits a generic power-law behavior and their structural geometry shows fractal feature. This indicates that the local atomic rearrangements in amorphous solids are self-organized during deformation. A simple theoretical model based on the interaction of the heterogeneous elastic field sources is proposed which predicts the power-law scaling and characterizes the properties of the local atomic rearrangements in amorphous solids.

Structural signatures evidenced in dynamic crossover phenomena in metallic glass-forming liquids

Molecular dynamics simulations were performed to investigate dynamic evolution in metallic glass-forming liquids during quenching from high temperature above melting point down to supercooled region. Two crossover temperatures TA and TS (TA > TS) are identified, and their physical meanings are clarified. TA and TS are found to be not only the sign of dynamic crossover phenomena but also the manifestation of two key structure correlation lengths ξs. As temperature decreases below TA, ξs goes beyond the nearest-neighbor distance, resulting in the Arrhenius-to-non-Arrhenius transition of structural relaxation time and the failure of Stokes-Einstein (SE) relation. As TS is traversed, the increase rate of ξs reaches the maximum, leading to the simultaneous appearance of dynamical heterogeneity and fractional SE relation. It is further found that structure correlation increases much faster than dynamic correlation, playing a role of structural precursor for dynamic evolution in liquids. Thus, a structural link ...

Stress-versus temperature-induced structural evolution in metallic glasses

Structure evolution induced by shear deformation was investigated via molecular dynamic simulation on CuZr metallic glass system and compared with that induced by temperature. Voronoi tessellation analysis found that the local structures evolve to a liquid-like state as shear stress increases, similar to the temperature-induced structure evolution. However, shear stress induces little change to the radial distribution functions (RDFs) compared to temperature, indicating that the global glassy state still sustains. This is in contrast to the opinion that shear deformation may be similar to temperature increase and induce a metallic glass system to experience glass-liquid transition. The analysis of anisotropic part of RDFs reveals that shear deformation can induce significant anisotropic structural evolution, while pure increase of temperature cannot. Our findings demonstrate that shear deformation may induce different structural evolution in metallic glasses compared to temperature.

Capture zone area distributions for nucleation and growth of islands during submonolayer deposition

A fundamental evolution equation is developed to describe the distribution of areas of capture zones (CZs) associated with islands formed by homogeneous nucleation and growth during submonolayer deposition on perfect flat surfaces. This equation involves various quantities which characterize subtle spatial aspects of the nucleation process. These quantities in turn depend on the complex stochastic geometry of the CZ tessellation of the surface, and their detailed form determines the CZ area distribution (CZD) including its asymptotic features. For small CZ areas, behavior of the CZD reflects the critical island size, i. For large CZ areas, it may reflect the probability for nucleation near such large CZs. Predictions are compared with kinetic Monte Carlo simulation data for models with two-dimensional compact islands with i = 1 (irreversible island formation by diffusing adatom pairs) and i = 0 (adatoms spontaneously convert to stable nuclei, e.g., by exchange with the substrate).

From Initial to Late Stages of Epitaxial Thin Film Growth: STM Analysis and Atomistic or Coarse-Grained Modeling

Epitaxial thin film growth by vapor deposition or molecular beam epitaxy under ultra‐high vacuum conditions generally occurs in two stages: (i) nucleation and growth of well‐separated islands on the substrate; (ii) subsequent formation of a thicker continuous film with possible kinetic roughening. For homoepitaxial growth, two‐dimensional (2D) monolayer islands are formed during submonolayer deposition. Typically, the presence of a step‐edge barrier inhibits downward transport and leads to the formation of mounds (multilayer stacks of 2D islands) during multilayer growth. For heteroepitaxial growth, islands formed in the initial stages of deposition sometimes have a 2D monolayer structure. However, they may instead exhibit bilayer or 3D multilayer structure due to, e.g., a high film surface energy, strain, or quantum size effects. Various growth modes are possible for thicker films. Atomistic modeling provides the most detailed picture of film growth. For coherent (defect‐free) epitaxial films, lattice‐ga...

Kinetic Monte Carlo Simulation of Epitaxial Thin Film Growth: Formation of Submonolayer Islands and Multilayer Mounds

We consider homoepitaxy (or low‐misfit heteroepitaxy) via vapor deposition or MBE under UHV conditions. Thin film growth is initiated by nucleation and growth of 2D islands in the submonolayer regime. For atoms subsequently deposited on top of islands, a step edge barrier often inhibits downward transport and produces kinetic roughening during multilayer growth. Such unstable growth is characterized by the formation of 3D mounds (multilayer stacks of 2D islands). Kinetic Monte Carlo (KMC) simulation of suitable atomistic lattice‐gas models can address fundamental or general issues related to both submonolayer and multilayer film evolution, and can also provide a predictive tool for morphological evolution in specific systems. Examples of the successes of KMC modeling are provided for metal homoepitaxial film growth, specifically for contrasting behavior in the classic Ag/Ag(100) and Ag/Ag(111) systems.

Size effect on dynamics and glass transition in metallic liquids and glasses

The relaxation dynamics and glass transition in finite-sized metallic liquid droplets were investigated via molecular dynamic simulations in model monoatomic Ta and binary Cu50Zr50 metallic liquids. We find that the droplet size has a significant impact on liquid dynamics and glass transition. Glass transition temperature and structural relaxation time exhibit strong size dependence and decrease drastically as the droplet is smaller than a certain size. It is revealed that this results from a liquid-like surface layer (∼1 nm thick) of droplets, in which the dynamics is much faster than the interior of droplets. A proposed scaling relationship can well describe the size dependent behavior of the glass transition temperature in metallic liquid droplets. These findings provide insight into the dynamics of metallic liquid droplets and plausible understanding of recent novel experimental observations. Apart from temperature and pressure, size may be another important parameter for potentially tuning the properties of metallic liquids and glasses in nanometer scale.

Local environments of atomic clusters and the effect on dynamics in CuZr metallic glass-forming liquids

The effect of local environments of various atomic clusters on the dynamics in CuZr metallic glass-forming liquids was investigated via classical molecular dynamics simulations. It is found that atomic clusters exhibit different local connectivity, leading to different local environments, even for the same type of clusters. Moreover, local environments of atomic clusters are found to have a different impact on dynamics in supercooled liquids. For pentagon-rich clusters such as ⟨0,0,12,0⟩ and ⟨0,1,10,2⟩, the dynamics becomes slower with increasing connectivity in both α and β relaxation time scales. In contrast, as local connectivity increases, atomic mobility of connected ⟨0,3,6,4⟩ clusters is enhanced. The evolution of atomic symmetries in clusters with local connectivity is found to be the underlying structural basis for the correlation between local environments and dynamics of atomic clusters. These findings indicate that local environments of atomic clusters are more critical in the relaxation dynami...