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Register a new userProbing the Local Response of Glass-forming Liquids by Laser Excitations
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The glass is a disordered solid that processes distinct dynamical and elastic properties compared with crystal. How heterogeneous glassy materials can be and to what extent dynamics is encoded with structure and elasticity are long-standing puzzles in glass science. In this experiment, we probed the responses of binary colloidal glasses towards the excitations induced by highly focused laser pulses. We observed very similar excitation patterns when the laser was repeated in the linear region; directly proving that the dynamical heterogeneity is strongly encoded with structure. In the non-linear region, we identified a non-monotonic dynamical length scale as a function of area fraction, resulting from the non-monotonic coupling of momentum transfer in radial and orthogonal directions. Surprisingly, the excitation size and radius of gyration conformed to a universal scaling relation that covered both linear and non-linear regions. Our experiments offered a new strategy of actively probing the response of glassy materials on the microscopic level.
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This work aims at reconsidering several interpretations coexisting in the recent literature concerning non-linear susceptibilities in supercooled liquids. We present experimental results on glycerol and propylene carbonate showing that the three independent cubic susceptibilities have very similar frequency and temperature dependences, both for their amplitudes and phases. This strongly suggests a unique physical mechanism responsible for the growth of these non-linear susceptibilities. We show that the framework proposed by two of us [BB, Phys. Rev. B 72, 064204 (2005)], where the growth of non-linear susceptibilities is intimately related to the growth of glassy domains, accounts for all the salient experimental features. We then review several complementary and/or alternative models, and show that the notion of cooperatively rearranging glassy domains is a key (implicit or explicit) ingredient to all of them. This paves the way for future experiments which should deepen our understanding of glasses.
It was recently shown that the real part of the frequency-dependent fluidity for several glass-forming liquids of different chemistry conforms to the prediction of the random barrier model (RBM) devised for ac electrical conduction in disordered solids [S. P. Bierwirth textit{et al.}, Phys. Rev. Lett. {bf 119}, 248001 (2017)]. Inspired by these results we introduce a crystallization-resistant modification of the Kob-Andersen binary Lennard-Jones mixture for which the results of extensive graphics-processing unit (GPU)-based molecular-dynamics simulations are presented. We find that the low-temperature mean-square displacement is fitted well by the RBM prediction, which involves no shape parameters. This finding highlights the challenge of explaining why a simple model based on hopping of non-interacting particles in a fixed random energy landscape can reproduce the complex and highly cooperative dynamics of glass-forming liquids.
One of the central problems of the liquid-glass transition is whether there is a structural signature that can qualitatively distinguish different dynamic behaviors at different degrees of supercooling. Here, we propose a novel structural characterization based on the spatial correlation of local density and we show the locally dense-packed structural environment has a direct link with the slow dynamics as well as dynamic heterogeneity in glass-formers. We find that particles with large local density relax slowly and the size of cluster formed by the dense-packed particles increases with decreasing the temperature. Moreover, the extracted static length scale shows clear correlation with the relaxation time at different degrees of supercooling. This suggests that the temporarily but continuously formed locally dense-packed structural environment may be the structural origin of slow dynamics and dynamic heterogeneity of the glass-forming liquids.
Via molecular dynamics simulations of a generic glass former in the supercooled and normal liquid states, it is shown that spatial correlations of strain fluctuations exhibit a crossover from the well-established power-law $sim 1/r^3$-decay at long wavelengths to an exponential behavior, $sim exp(-r/l_{text {c}})$ at intermediate distances. The characteristic length of the exponential decay grows both with temperature and time via, $l_{text {c}}^2 propto D(T), t$, with $D(T)$ being the temperature-dependent diffusion coefficient. This suggests that the crossover between the power-law and exponential decays is governed by a diffusion process.
The slow down of dynamics in glass forming liquids as the glass transition is approached has been characterised through the Adam-Gibbs relation, which relates relaxation time scales to the configurational entropy. The Adam-Gibbs relation cannot apply simultaneously to all relaxation times scales unless they are coupled, and exhibit closely related temperature dependences. The breakdown of the Stokes-Einstein relation presents an interesting situation to the contrary, and in analysing it, it has recently been shown that the Adam-Gibbs relation applies to diffusion coefficients rather than to viscosity or structural relaxation times related to the decay of density fluctuations. However, for multi-component liquids -- the typical cases considered in computer simulations, metallic glass formers, etc. -- such a statement raises the question of which diffusion coefficient is described by the Adam-Gibbs relation. All diffusion coefficients can be consistently described by the Adam-Gibbs relation if they bear a power law relationship with each other. Remarkably, we find that for a wide range of glass formers, and for a wide range of temperatures spanning the normal and the slow relaxation regimes, such a relationship holds. We briefly discuss possible rationalisations of the observed behaviour.
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