Connection between Mechanical Relaxation and Equilibration Kinetics in a High-Entropy Metallic Glass.

The slow transition from an out-of-equilibrium glass towards a supercooled liquid is a complex relaxation phenomenon. In this Letter, we study the correlation between mechanical relaxation and equilibration kinetics in a Pd_{20}Pt_{20}Cu_{20}Ni_{20}P_{20} high-entropy metallic glass. The evolution of stress relaxation with aging time was obtained with an unprecedented detail, allowing us to pinpoint new interesting features. The long structural relaxation towards equilibrium contains a wide distribution of activation energies, instead of being just associated to the ß relaxation as commonly accepted. The stress relaxation time can be correlated with the equilibration rate and we observe a decrease of microstructural heterogeneity which contrasts with an increase of dynamic heterogeneity. These results significantly enhance our insight of the interplay between relaxation dynamics and thermodynamics in metallic glasses.

Dynamics-Entropy Relationship in Metallic Glasses.

Establishing a robust quantitative correlation between thermodynamics and dynamics in amorphous matter remains a significant challenge in condensed matter physics. Although the classical Adam-Gibbs relationship represents a pivotal step in this direction and the correlation between relaxation time and configurational entropy has been partially verified in simple liquids, this quantitative link has yet to be tested in realistic glass-forming systems where complex many-body interactions are present. Here we conduct free energy samplings and lattice dynamics analysis to distinguish vibrational entropy from configurational entropy in a realistic Cu-Zr model of a metallic glass. Our calculations unveil a power-law relationship (with a substantial exponent of ∼3) between the logarithmic relaxation time and configurational entropy, surpassing the linear prediction of the original Adam-Gibbs relationship. This nonlinear entropy driven relaxation time variation likely originates from anisotropic nature of atomic many-body interactions, suggesting that factors beyond thermodynamics contribute to the glass transition phenomenon.

Intrinsic Correlation between the Fraction of Liquidlike Zones and the ß Relaxation in High-Entropy Metallic Glasses.

Lacking the structural information of crystalline solids, the origin of the relaxation dynamics of metallic glasses is unclear. Here, we report the evolution of stress relaxation of high-entropy metallic glasses with distinct ß relaxation behavior. The fraction of liquidlike zones, determined at each temperature by the intensity of stress decay, is shown to be directly related to both the aging process and the spectrum of relaxation modes obtained by mechanical spectroscopy. The results shed light on the intrinsic correlation between the static and dynamic mechanical response in high-entropy and conventional metallic glasses, pointing toward a sluggish diffusion high-entropy effect in the liquid dynamics.

Prediction of the RNA Secondary Structure Using a Multi-Population Assisted Quantum Genetic Algorithm.

Quantum-inspired genetic algorithms (QGAs) were recently introduced for the prediction of RNA secondary structures, and they showed some superiority over the existing popular strategies. In this paper, for RNA secondary structure prediction, we introduce a new QGA named multi-population assisted quantum genetic algorithm (MAQGA). In contrast to the existing QGAs, our strategy involves multi-populations which evolve together in a cooperative way in each iteration, and the genetic exchange between various populations is performed by an operator transfer operation. The numerical results show that the performances of existing genetic algorithms (evolutionary algorithms [EAs]), including traditional EAs and QGAs, can be significantly improved by using our approach. Moreover, for RNA sequences with middle-short length, the MAQGA improves even this state-of-the-art software in terms of both prediction accuracy and sensitivity.

Structural Parameter of Orientational Order to Predict the Boson Vibrational Anomaly in Glasses.

It has so far remained a major challenge to quantitatively predict the boson peak, a THz vibrational anomaly universal for glasses, from features in the amorphous structure. Using molecular dynamics simulations of a model Cu_{50}Zr_{50} glass, we decompose the boson peak to contributions from atoms residing in different types of Voronoi polyhedra. We then introduce a microscopic structural parameter to depict the "orientational order," using the vector pointing from the center atom to the farthest vertex of its Voronoi coordination polyhedron. This order parameter represents the most probable direction of transverse vibration at low frequencies. Its magnitude scales linearly with the boson peak intensity, and its spatial distribution accounts for the quasilocalized modes. This correlation is shown to be universal for different types of glasses.

Assessing the utility of structure in amorphous materials.

This paper presents a set of general strategies for the analysis of structure in amorphous materials and a general approach to assessing the utility of any selected structural description. Two measures of structure are defined, "diversity" and "utility," and applied to two model glass forming binary atomic alloys, Cu50Zr50 and a Lennard-Jones A80B20 mixture. We show that the change in diversity associated with selecting Voronoi structures with high localization or low energy, while real, is too weak to support claims that specific structures are the prime cause of these local physical properties. In addition, a new structure-free measure of incipient crystal-like organization in mixtures is introduced, suitable for cases where the stable crystal is a compound structure.

Oxyhydroxide of metallic nanowires in a molecular H2O and H2O2 environment and their effects on mechanical properties.

To avoid unexpected environmental mechanical failure, there is a strong need to fully understand the details of the oxidation process and intrinsic mechanical properties of reactive metallic iron (Fe) nanowires (NWs) under various aqueous reactive environmental conditions. Herein, we employed ReaxFF reactive molecular dynamics (MD) simulations to elucidate the oxidation of Fe NWs exposed to molecular water (H2O) and hydrogen peroxide (H2O2) environment, and the influence of the oxide shell layer on the tensile mechanical deformation properties of Fe NWs. Our structural analysis shows that oxidation of Fe NWs occurs with the formation of different iron oxide and hydroxide phases in the aqueous molecular H2O and H2O2 oxidizing environments. We observe that the resulting microstructure due to pre-oxide shell layer formation reduces the mechanical stress via increasing the initial defect sites in the vicinity of the oxide region to facilitate the onset of plastic deformation during tensile loading. Specifically, the oxide layer of Fe NWs formed in the H2O2 environment has a relatively significant effect on the deterioration of the mechanical properties of Fe NWs. The weakening of the yield stress and Young modulus of H2O2 oxidized Fe NWs indicates the important role of local oxide microstructures on mechanical deformation properties of individual Fe NWs. Notably, deformation twinning is found as the primary mechanical plastic deformation mechanism of all Fe NWs, but it is initially observed at low strain and stress level for the oxidized Fe NWs.