Subscribe to the gold package and get unlimited access to Shamra Academy
Register a new userSpatial correlations in the dynamics of glassforming liquids: Experimental determination of their temperature dependence
94
0
0.0
(
0
)
Ask ChatGPT about the research
No Arabic abstract
We use recently introduced three-point dynamic susceptibilities to obtain an experimental determination of the temperature evolution of the number of molecules, N_corr, that are dynamically correlated during the structural relaxation of supercooled liquids. We first discuss in detail the physical content of three-point functions that relate the sensitivity of the averaged two-time dynamics to external control parameters (such as temperature or density), as well as their connection to the more standard four-point dynamic susceptibility associated with dynamical heterogeneities. We then demonstrate that these functions can be experimentally determined with a good precision. We gather available data to obtain the temperature dependence of N_corr for a large number of supercooled liquids over a wide range of relaxation timescales from the glass transition up to the onset of slow dynamics. We find that N_corr systematically grows when approaching the glass transition. It does so in a modest manner close to the glass transition, which is consistent with an activation-based picture of the dynamics in glassforming materials. For higher temperatures, there appears to be a regime where N_corr behaves as a power-law of the relaxation time. Finally, we find that the dynamic response to density, while being smaller than the dynamic response to temperature, behaves similarly, in agreement with theoretical expectations.
rate research
Read More
A relation between vibrational entropy and particles mean square displacement is derived in super-cooled liquids, assuming that the main effect of temperature changes is to rescale the vibrational spectrum. Deviations from this relation, in particular due to the presence of a Boson Peak whose shape and frequency changes with temperature, are estimated. Using observations of the short-time dynamics in liquids of various fragility, it is argued that (i) if the crystal entropy is significantly smaller than the liquid entropy at $T_g$, the extrapolation of the vibrational entropy leads to the correlation $T_Kapprox T_0$, where $T_K$ is the Kauzmann temperature and $T_0$ is the temperature extracted from the Vogel-Fulcher fit of the viscosity. (ii) The jump in specific heat associated with vibrational entropy is very small for strong liquids, and increases with fragility. The analysis suggests that these correlations stem from the stiffening of the Boson Peak under cooling, underlying the importance of this phenomenon on the dynamical arrest.
Correlations between different partitions of quantum systems play a central role in a variety of many-body quantum systems, and they have been studied exhaustively in experimental and theoretical research. Here, we investigate dynamical correlations in the time evolution of multiple parts of a composite quantum system. A rigorous measure to quantify correlations in quantum dynamics based on a full tomographic reconstruction of the quantum process has been introduced recently [A. Rivas et al., New Journal of Physics, 17(6) 062001 (2015).]. In this work, we derive a lower bound for this correlation measure, which does not require full knowledge of the quantum dynamics. Furthermore we also extend the correlation measure to multipartite systems. We directly apply the developed methods to a trapped ion quantum information processor to experimentally characterize the correlations in quantum dynamics for two- and four-qubit systems. The method proposed and demonstrated in this work is scalable, platform-independent and applicable to other composite quantum systems and quantum information processing architectures. We apply the method to estimate spatial correlations in environmental noise processes, which are crucial for the performance of quantum error correction procedures.
We obtain analytic expressions for the time correlation functions of a liquid of spherical particles, exact in the limit of high dimensions $d$. The derivation is long but straightforward: a dynamic virial expansion for which only the first two terms survive, followed by a change to generalized spherical coordinates in the dynamic variables leading to saddle-point evaluation of integrals for large $d$. The problem is thus mapped onto a one-dimensional diffusion in a perturbed harmonic potential with colored noise. At high density, an ergodicity-breaking glass transition is found. In this regime, our results agree with thermodynamics, consistently with the general Random First Order Transition scenario. The glass transition density is higher than the best known lower bound for hard sphere packings in large $d$. Because our calculation is, if not rigorous, elementary, an improvement in the bound for sphere packings in large dimensions is at hand.
In this work, we analytically derive the exact closed dynamical equations for a liquid with short-ranged interactions in large spatial dimensions using the same statistical mechanics tools employed to analyze Brownian motion. Our derivation greatly simplifies the original path-integral-based route to these equations and provides new insight into the physical features associated with high-dimensional liquids and glass formation. Most importantly, our construction provides a facile route to the exact dynamical analysis of important related dynamical problems, as well as a means to devise cluster generalizations of the exact solution in infinite dimensions. This latter fact opens the door to the construction of increasingly accurate theories of vitrification in three-dimensional liquids.
We numerically study the relaxation dynamics of several glass-forming models to their inherent structures, following quenches from equilibrium configurations sampled across a wide range of temperatures. In a mean-field Mari-Kurchan model, we find that relaxation changes from a power-law to an exponential decay below a well-defined temperature, consistent with recent findings in mean-field $p$-spin models. By contrast, for finite-dimensional systems, the relaxation is always algebraic, with a non-trivial universal exponent at high temperatures crossing over to a harmonic value at low temperatures. We demonstrate that this apparent evolution is controlled by a temperature-dependent population of localised excitations. Our work unifies several recent lines of studies aiming at a detailed characterization of the complex potential energy landscape of glass-formers.
Log in to be able to interact and post comments
comments
Fetching comments
Sign in to be able to follow your search criteria
