arXiv subjects

Bu Wang

Publications and source records attributed to Bu Wang.

15 recordsLinked to original sources

arXiv2026

Asymmetric Energy Landscapes Control Diffusion in Glasses

While diffusion in crystalline solids is quantitatively understood through defect-mediated atomic hops, no comparable quantitative framework exists for glasses. In these systems, the origin of large diffusion activation energies remains puzzling, despite local rearrangements involving low barriers. Using molecular dynamics simulations of metallic glasses, we decompose diffusion into random-walk and correlation contributions and find that back-and-forth correlated motion, not local rearrangement barriers, dominates the activation energy, resolving how low-barrier rearrangements yield large macroscopic activation energies. These correlations arise from asymmetry between forward and reverse barriers, a generic feature of disordered energy landscapes. We find that the correlation-driven mechanism is active beyond metallic glass alloys, including SiO2 and a single-component Lennard-Jones glass. The latter demonstrates that the correlation originates from structural disorder rather than chemical complexity. The framework also explains accelerated surface diffusion, where reduced activation energies arise primarily from weaker correlations rather than changes in local rearrangement barriers. Our results establish a direct, quantitative link between atomic-scale dynamics and macroscopic transport, providing a predictive basis for kinetics in disordered materials.

cond-mat.mtrl-sci↗

arXiv2025

Physical regularized Hierarchical Generative Model for Metallic Glass Structural Generation and Energy Prediction

Disordered materials such as glasses, unlike crystals, lack long range atomic order and have no periodic unit cells, yielding a high dimensional configuration space with widely varying properties. The complexity not only increases computational costs for atomistic simulations but also makes it difficult for generative AI models to deliver accurate property predictions and realistic structure generation. In this work, we introduce GlassVAE, a hierarchical graph variational autoencoder that uses graph representations to learn compact, rotation, translation, and permutation invariant embeddings of atomic configurations. The resulting structured latent space not only enables efficient generation of novel, physically plausible structures but also supports exploration of the glass energy landscape. To enforce structural realism and physical fidelity, we augment GlassVAE with two physics informed regularizers, a radial distribution function (RDF) loss that captures characteristic short and medium range ordering and an energy regression loss that reflects the broad configurational energetics. Both theoretical analysis and experimental results highlight the critical impact of these regularizers. By encoding high dimensional atomistic data into a compact latent vector and decoding it into structures with accurate energy predictions, GlassVAE provides a fast, physics aware path for modeling and designing disordered materials.

cs.CE↗

arXiv2025

Silk-Nano-Fibroin Aerogels: A Bio-Derived, Amine-Rich Platform for Rapid and Reversible CO2 Capture

Despite growing interest in bio-based materials, rapid, low-temperature CO2 capture using amine-rich natural sorbents has received limited attention. In recent years, various porous solid sorbents have drawn significant research interest as promising carbon capture materials. However, high synthesis cost, limited CO2 adsorption capacity, sluggish adsorption-desorption kinetics, high sorbent regeneration temperature, and poor operational stability remain major challenges for their practical implementation. Here, we present silk-nano-fibroin aerogels derived from natural mulberry silk as a sustainable, amine-rich, and support-free sorbent platform for energy-efficient CO2 capture. The aerogels exhibit a CO2 adsorption capacity competitive with state-of-the-art amino acid and amino acid ionic liquid-based solid sorbents. Thermogravimetric analysis confirms high thermal stability up to 250C, substantially higher than that of conventional amine sorbents, while complete sorbent regeneration occurs at only 60 C. Furthermore, the silk-nano-fibroin aerogels demonstrate rapid adsorption-desorption kinetics, excellent multicycle stability, and full retention of CO2 adsorption capacity under humid conditions. Spectroscopic analyses (XPS, FTIR, Raman, and solid-state 13C NMR) confirm reversible CO2 chemisorption through intrinsic amine sites within the silk-fibroin backbone. Overall, this work establishes silk-nano-fibroin aerogels as a sustainable and low-cost route toward energy-efficient CO2 capture.

physics.chem-ph↗

arXiv2023

How close are the classical two-body potentials to ab initio calculations? Insights from linear machine learning based force matching

In this work, we propose a linear machine learning force matching approach that can directly extract pair atomic interactions from ab initio calculations in amorphous structures. The local feature representation is specifically chosen to make the linear weights a force field as a force/potential function of the atom pair distance. Consequently, this set of functions is the closest representation of the ab initio forces given the two-body approximation and finite scanning in the configurational space. We validate this approach in amorphous silica. Potentials in the new force field (consisting of tabulated Si-Si, Si-O, and O-O potentials) are significantly softer than existing potentials that are commonly used for silica, even though all of them produce the tetrahedral network structure and roughly similar glass properties. This suggests that those commonly used classical force fields do not offer fundamentally accurate representations of the atomic interaction in silica. The new force field furthermore produces a lower glass transition temperature ($T_g\sim$1800 K) and a positive liquid thermal expansion coefficient, suggesting the extraordinarily high $T_g$ and negative liquid thermal expansion of simulated silica could be artifacts of previously developed classical potentials. Overall, the proposed approach provides a fundamental yet intuitive way to evaluate two-body potentials against ab initio calculations, thereby offering an efficient way to guide the development of classical force fields.

cond-mat.mtrl-sci↗

arXiv2022

Distribution of atomic rearrangement vectors in a metallic glass

Short-timescale atomic rearrangements are fundamental to the kinetics of glasses and frequently dominated by one atom moving significantly (a rearrangement), while others relax only modestly. The rates and directions of such rearrangements (or hops) are dominated by the distributions of activation barriers (Eact) for rearrangement for a single atom and how those distributions vary across the atoms in the system. We have used molecular dynamics simulations of Cu50Zr50 metallic glass below Tg in an isoconfigurational ensemble to catalog the ensemble of rearrangements from thousands of sites. The majority of atoms are strongly caged by their neighbors, but a tiny fraction has a very high propensity for rearrangement, which leads to a power-law variation in the cage-breaking probability for the atoms in the model. In addition, atoms generally have multiple accessible rearrangement vectors, each with its own Eact. However, atoms with lower Eact (or higher rearrangement rates) generally explored fewer possible rearrangement vectors, as the low Eact path is explored far more than others. We discuss how our results influence future modeling efforts to predict the rearrangement vector of a hopping atom.

cond-mat.mtrl-sci↗

arXiv2022

Understanding the fragile-to-strong transition in silica from microscopic dynamics

In this work, we revisit the fragile-to-strong transition (FTS) in the simulated BKS silica from the perspective of microscopic dynamics in an effort to elucidate the dynamical behaviors of fragile and strong glass-forming liquids. Softness, which is a machine-learned feature from local atomic structures, is used to predict the microscopic activation energetics and long-term dynamics. The FTS is found to originate from a change in the temperature dependence of the microscopic activation energetics. Furthermore, results suggest there are two diffusion channels with different energy barriers in BKS silica. The fast dynamics at high temperatures is dominated by the channel with small energy barriers ($<\sim$1 eV), which is controlled by the short-range order. The rapid closing of this diffusion channel when lowering temperature leads to the fragile behavior. On the other hand, the slow dynamics at low temperatures is dominated by the channel with large energy barriers controlled by the medium-range order. This slow diffusion channel changes only subtly with temperature, leading to the strong behavior. The distributions of barriers in the two channels show different temperature dependences, causing a crossover at $\sim$3100 K. This transition temperature in microscopic dynamics is consistent with the inflection point in the configurational entropy, suggesting there is a fundamental correlation between microscopic dynamics and thermodynamics.

cond-mat.dis-nn↗

arXiv2020

Structural Signatures for Thermodynamic Stability in Vitreous Silica: Insight from Machine Learning and Molecular Dynamics Simulations

The structure-thermodynamic stability relationship in vitreous silica is investigated using machine learning and a library of 24,157 inherent structures generated from melt-quenching and replica exchange molecular dynamics simulations. We find the thermodynamic stability, i.e., enthalpy of the inherent structure ($e_{\mathrm{IS}}$), can be accurately predicted by both linear and nonlinear machine learning models from numeric structural descriptors commonly used to characterize disordered structures. We find short-range features become less indicative of thermodynamic stability below the fragile-to-strong transition. On the other hand, medium-range features, especially those between 2.8-~6 $\unicode{x212B}$;, show consistent correlations with $e_{\mathrm{IS}}$ across the liquid and glass regions, and are found to be the most critical to stability prediction among features from different length scales. Based on the machine learning models, a set of five structural features that are the most predictive of the silica glass stability is identified.

cond-mat.dis-nn↗

arXiv2018

A New Transferable Interatomic Potential for Molecular Dynamics Simulations of Borosilicate Glasses

Borosilicate glasses are traditionally challenging to model using atomic scale simulations due to the composition and thermal history dependence of the coordination state of B atoms. Here, we report a new empirical interatomic potential that shows a good transferability over a wide range of borosilicate glasses--ranging from pure silicate to pure borate end members--while relying on a simple formulation and a constant set of energy parameters. In particular, we show that our new potential accurately predicts the compositional dependence of the average coordination number of boron atoms, glass density, overall short-range and medium-range order structure, and shear viscosity values for several borosilicate glasses and liquids. This suggests that our new potential could be used to gain new insights into the structure of a variety of advanced borosilicate glasses to help elucidate composition-structure-property relationships--including in complex nuclear waste immobilization glasses.

cond-mat.dis-nn↗

arXiv2017

Cooling-Rate Effects in Sodium Silicate Glasses: Bridging the Gap between Molecular Dynamics Simulations and Experiments

Although molecular dynamics (MD) simulations are commonly used to predict the structure and properties of glasses, they are intrinsically limited to short time scales, necessitating the use of fast cooling rates. It is therefore challenging to compare results from MD simulations to experimental results for glasses cooled on typical laboratory time scales. Based on MD simulations of a sodium silicate glass with varying cooling rate (from 0.01 to 100 K/ps), here we show that thermal history primarily affects the medium-range order structure, while the short-range order is largely unaffected over the range of cooling rates simulated. This results in a decoupling between the enthalpy and volume relaxation functions, where the enthalpy quickly plateaus as the cooling rate decreases, whereas density exhibits a slower relaxation. Finally, we demonstrate that the outcomes of MD simulations can be meaningfully compared to experimental values if properly extrapolated to slower cooling rates.

cond-mat.mtrl-sci↗

arXiv2016

Topological Control on Atomic Networks' Relaxation Under Stress

Upon loading, atomic networks can feature delayed viscoplastic relaxation. However, the effect of composition and structure on such a relaxation remains poorly understood. Herein, relying on accelerated molecular dynamics simulations and topological constraint theory, we investigate the relationship between atomic topology and stress-induced relaxation, by taking the example of creep deformations in calcium--silicate--hydrates, the binding phase of concrete. Under constant shear stress, C--S--H is found to feature delayed logarithmic shear deformations. We demonstrate that the propensity for relaxation is minimum for isostatic atomic networks, which are characterized by the simultaneous absence of floppy internal modes of relaxation and eigen stress. This suggests that topological nano-engineering could lead to the discovery of non-aging materials.

cond-mat.mtrl-sci↗

arXiv2015

Nano-Ductility in Silicate Glasses is Driven by Topological Heterogeneity

The existence of nanoscale ductility during the fracture of silicate glasses remains controversial. Here, based on molecular dynamics simulations coupled with topological constraint theory, we show that nano-ductility arises from the spatial heterogeneity of the atomic network's rigidity. Specifically, we report that localized floppy modes of deformation in under-constrained regions of the glass enable plastic deformations of the network, resulting in permanent change in bond configurations. Ultimately, these heterogeneous plastic events percolate, thereby resulting in a non-brittle mode of fracture. This suggests that nano-ductility is intrinsic to multi-component silicate glasses having nanoscale heterogeneities.

cond-mat.mtrl-sci↗

arXiv2015

Direct Experimental Evidence for Differing Reactivity Alterations of Minerals following Irradiation: The Case of Calcite and Quartz

Concrete, a mixture formed by mixing cement, water, and fine and coarse mineral aggregates is used in the construction of nuclear power plants (NPPs), e.g., to construct the reactor cavity concrete that encases the reactor pressure vessel, etc. In such environments, concrete may be exposed to radiation (e.g., neutrons) emanating from the reactor core. Until recently, concrete has been assumed relatively immune to radiation exposure. Direct evidence acquired on Ar$^+$-ion irradiated calcite and quartz indicates, on the contrary, that, such minerals, which constitute aggregates in concrete, may be significantly altered by irradiation. Specifically, while quartz undergoes disordering of its atomic structure resulting in a near complete lack of periodicity, i.e., similar to glassy silica, calcite only experiences random rotations, and distortions of its carbonate groups. As a result, irradiated quartz shows a reduction in density of around 15%, and an increase in chemical reactivity, described by its dissolution rate, similar to a glassy silica; i.e., an increase of around 3 orders of magnitude. Calcite however, shows little change in dissolution rates - although its density noted to reduce by around 9%. These differences are correlated with the nature of bonds in these minerals, i.e., being dominantly ionic or covalent, and the rigidity of the mineral's atomic network that is characterized by the number of topological constraints (n$_c$) that are imposed on the atoms in the network. The outcomes are discussed within the context of the durability of concrete structural elements formed with calcitic/quartzitic aggregates in nuclear power plants.

cond-mat.mtrl-sci↗

arXiv2015

Fracture Toughness of Silicate Glasses: Insights from Molecular Dynamics Simulations

Understanding, predicting and eventually improving the resistance to fracture of silicate materials is of primary importance to design new glasses that would be tougher, while retaining their transparency. However, the atomic mechanism of the fracture in amorphous silicate materials is still a topic of debate. In particular, there is some controversy about the existence of ductility at the nano-scale during the crack propagation. Here, we present simulations of the fracture of three archetypical silicate glasses using molecular dynamics. We show that the methodology that is used provide realistic values of fracture energy and toughness. In addition, the simulations clearly suggest that silicate glasses can show different degrees of ductility, depending on their composition.

cond-mat.mtrl-sci↗

arXiv2015

Nature of Radiation-Induced Defects in Quartz

Although quartz ($\rm α$-form) is a mineral used in numerous applications wherein radiation exposure is an issue, the nature of the atomistic defects formed during radiation-induced damage have not been fully clarified. Especially, the extent of oxygen vacancy formation is still debated, which is an issue of primary importance as optical techniques based on charged oxygen vacancies have been utilized to assess the level of radiation damage in quartz. In this paper, molecular dynamics (MD) simulations are applied to study the effects of ballistic impacts on the atomic network of quartz. We show that the defects that are formed mainly consist of over-coordinated Si and O, as well as Si--O connectivity defects, e.g., small Si--O rings and edge-sharing Si tetrahedra. Oxygen vacancies, on the contrary, are found in relatively low abundance, suggesting that characterizations based on $E^{\prime}$ centers do not adequately capture radiation-induced structural damage in quartz. Finally, we evaluate the dependence on the incident energy, of the amount of each type of the point defects formed, and quantify unambiguously the threshold displacement energies for both O and Si atoms. These results provide a comprehensive basis to assess the nature and extent of radiation damage in quartz.

cond-mat.mtrl-sci↗

arXiv2015

Stretched Exponential Relaxation of Glasses at Low Temperature

The question of whether glass continues to relax at low temperature is of fundamental and practical interest. Here, we report a novel atomistic simulation method allowing us to directly access the long-term dynamics of glass relaxation at room temperature. We find that the potential energy relaxation follows a stretched exponential decay, with a stretching exponent $β= 3/5$, as predicted by Phillips' diffusion-trap model. Interestingly, volume relaxation is also found. However, it is not correlated to the energy relaxation, but is rather a manifestation of the mixed alkali effect.

cond-mat.dis-nn↗