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Relaxation processes play a crucial role in glassy materials. However, current dielectric or mechanical spectroscopy typically reaches a lower limit of around 10−1 or 10−2 Hz, which restricts the exploration of long-time dynamics and stability. Here, we propose a mechanical protocol that enables the probing of relaxation processes down to 10−5 Hz, extending the lower limit by ∼3–4 orders of magnitude. The effectiveness of this method is demonstrated in investigating metallic glasses, where the primary and secondary relaxations are detected over an extended timescale. An additional relaxation process has been captured below 10−4 Hz, indicating the emergence of more complex relaxation phenomena over longer timescales. This progress in probing long-term dynamics opens up new possibilities for advancing glassy physics and material properties. [ABSTRACT FROM AUTHOR]

Establishing the structure–property relationship is an important goal of glassy materials, but it is usually impeded by their disordered structure and non-equilibrium nature. Recent studies have illustrated that secondary (β) relaxation is closely correlated with several properties in a range of glassy materials. However, it has been challenging to identify the pertinent structural features that govern it. In this work, we show that the so-called polyamorphous transition in metallic glasses offers an opportunity to distinguish the structural length scale of β relaxation. We find that, while the glass transition temperature and medium-range orders (MROs) change rapidly across the polyamorphous transition, the intensity of β relaxation and the short-range orders (SROs) evolve in a way similar to those in an ordinary reference glass without polyamorphous transition. Our findings suggest that the MRO accounts mainly for the global stiffening of the materials and the glass transition, while the SRO contributes more to β relaxation per se. [ABSTRACT FROM AUTHOR]

A new glass forming method is essential for broadening the scope of liquid and glassy metal–organic frameworks due to the limitations of the conventional melt-quenching method. Herein, we show that in situ mechanical vibration can facilitate the framework melting at a lower temperature and produce glassy metal–organic frameworks (MOFs) with unique properties. Using zeolitic imidazolate framework (ZIF)-62 as a concept-proofing material, in situ mechanical vibration enables low-temperature melting at 653 K, far below its melting point (713 K). The resultant vibrated ZIF-62 glass exhibited a lower glass transition temperature of 545 K, improved gas accessible porosity, and pronounced short-to-medium range structures compared to the corresponding melt-quenched glass. We propose that vibration-facilitated surface reconstruction facilitates pre-melting, which could be the cause of the lowered melting temperature. The vibration assisted method represents a new general method to produce MOF glasses without thermal decomposition. [ABSTRACT FROM AUTHOR]

Self-healing coatings, which possess the ability to repair damage and restore corrosion resistance without significant human intervention, have become a hot topic in corrosion protection research. In this paper, (±)-10-camphorsulfonic acid-doped polyaniline is synthesized and then combined with copolyurethane (copPU) to form the photothermal shape memory composite polymer (CSPA-copPU). An aggregation-induced emission agent, named N',2-bis[(E)-5-chloro-2-hydroxybenzylidene] hydrazine-1-carbohydrazide, is synthesized and applied to create a synergistic fluorescence system with a prepared chelation-enhanced fluorescence (CHEF) agent, named Rhodamine Benzimidazole. Under the CHEF behavior in response to Fe3+ and the fluorescence resonance energy transfer effect, the system exhibits a strong and sensitive fluorescence response to corrosion-generated Fe3+. Using electrospinning technology, CSPA-copPU@Fl fibers are prepared with CSPA-copPU as the shell and a mixture of fluorescent agents as the core solution and applied to create the composite coatings. The coatings effectively indicate damage in the form of fluorescence, providing guidance for infrared laser repair. CSPA facilitates the passivation of exposed steel. Under irradiation by an infrared laser, the surface temperature reaches the glass transition temperature of copPU and the epoxy binder. Through softening expansion and diffusion entanglement of molecular chains, scratches in the coatings are closed and repaired, and the corrosion resistance is restored to a level of intact coatings. [ABSTRACT FROM AUTHOR]

We investigate the fast β- and Johari–Goldstein (JG) β-relaxation processes, along with the elastic scattering response of glass-forming (GF) liquids and the boson peak, in a simulated Al–Sm GF material exhibiting a fragile–strong (FS) transition. These dynamical processes are universal in "ordinary" GF fluids and collectively describe their "fast dynamics," and we find these relaxation processes also arise in a GF liquid exhibiting a FS transition. String-like particle motion, having both an irreversible and a reversible nature (stringlets) component, occurs in the fast-dynamics regime, corresponding to a ps timescale. String-like collective motion associated with localized unstable modes facilitates irreversible and intermittent particle "jumping" events at long times associated with the JG β-relaxation process, while stringlets associated with localized stable modes and corresponding perfectly reversible atomic motion give rise to the boson peak. To further clarify the origin of the boson peak, we calculate the density of states for both the stringlet particles and the "normal" particles and find that the stringlet particles give rise to a boson peak, while the normal atoms do not. The growth of stringlets upon heating ultimately also leads to the "softening" of these excitations, and the boson peak frequency and shear modulus drop in concert with this softening. The growth of string-like collective motion upon heating in the fast-dynamics regime is further shown to be responsible for the growth in the intensity of the fast relaxation process. Relaxation in cooled liquids clearly involves a hierarchy of relaxation processes acting on rather different timescales and spatial scales. [ABSTRACT FROM AUTHOR]

Glassy materials are nonequilibrium and their energy states have crucial influences on properties. Recent studies have shown that oscillating deformations (vibrations) can cause either accelerated aging (lowering energy) or rejuvenation (elevating energy); however, the underlying atomic mechanisms remain elusive. Using metallic glasses (MGs) as model systems, we show that the vibration-induced accelerated aging is correlated with the strain field of the stringlike atomic motions stemming from the Johari-Goldstein (β) relaxation, whereas the rejuvenation is associated with nonlinear response and the formation of nanoscale shear bands attributing to the activation of α relaxation. Both processes are affected by thermal fluctuations, which result in an optimal temperature for accelerated aging. These results suggest intrinsic correlations among relaxation dynamics, mechanical properties, and the vibration induced structural rearrangements in MGs. [ABSTRACT FROM AUTHOR]

Solid materials, whether crystalline or glasses, are characterized by their elasticity. Generally, elasticity is independent of the probing strain if it is not exceeding the yielding point. Here, by contrast, we experimentally capture a pronounced strain-dependent elasticity in metallic glasses, as manifested by nonlinear mechanical damping in the apparent elastic deformation regime (∼1/100 of the yielding strain). Normal damping behaviors recover at higher temperatures but still below the glass transition. Atomistic simulations reproduce these features and reveal that they could be related to avalanche-like local structural instabilities. Our findings demonstrate that the standard elasticity is not held for metallic glasses at low temperatures and plastic events can be triggered at small perturbations. These results are consistent with previous simulations of model glasses and a scenario of hierarchical free-energy landscape of mean-field theory. [ABSTRACT FROM AUTHOR]