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Register a new userInherent-Structure Dynamics and Diffusion in Liquids
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The self-diffusion constant D is expressed in terms of transitions among the local minima of the potential (inherent structure, IS) and their correlations. The formulae are evaluated and tested against simulation in the supercooled, unit-density Lennard-Jones liquid. The approximation of uncorrelated IS-transition (IST) vectors, D_{0}, greatly exceeds D in the upper temperature range, but merges with simulation at reduced T ~ 0.50. Since uncorrelated IST are associated with a hopping mechanism, the condition D ~ D_{0} provides a new way to identify the crossover to hopping. The results suggest that theories of diffusion in deeply supercooled liquids may be based on weakly correlated IST.
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Thermal energy can be conducted by different mechanisms including by single particles or collective excitations. Thermal conductivity is system-specific and shows a richness of behaviors currently explored in different systems including insulators, strange metals and cuprate superconductors. Here, we show that despite the seeming complexity of thermal transport, the thermal diffusivity $alpha$ of liquids and supercritical fluids has a lower bound which is fixed by fundamental physical constants for each system as $alpha_m=frac{1}{4pi}frac{hbar}{sqrt{m_em}}$, where $m_e$ and $m$ are electron and molecule masses. The newly introduced elementary thermal diffusivity has an absolute lower bound dependent on $hbar$ and the proton-to-electron mass ratio only. We back up this result by a wide range of experimental data. We also show that theoretical minima of $alpha$ coincide with the fundamental lower limit of kinematic viscosity $ u_m$. Consistent with experiments, this points to a universal lower bound for two distinct properties, energy and momentum diffusion, and a surprising correlation between the two transport mechanisms at their minima. We observe that $alpha_m$ gives the minimum on the phase diagram except in the vicinity of the critical point, whereas $ u_m$ gives the minimum on the entire phase diagram.
The mechanism of diffusion in supercooled liquids is investigated from the potential energy landscape point of view, with emphasis on the crossover from high- to low-T dynamics. Molecular dynamics simulations with a time dependent mapping to the associated local mininum or inherent structure (IS) are performed on unit-density Lennard-Jones (LJ). New dynamical quantities introduced include r2_{is}(t), the mean-square displacement (MSD) within a basin of attraction of an IS, R2(t), the MSD of the IS itself, and g_{loc}(t) the mean waiting time in a cooperative region. At intermediate T, r2_{is}(t) posesses an interval of linear t-dependence allowing calculation of an intrabasin diffusion constant D_{is}. Near T_{c} diffusion is intrabasin dominated with D = D_{is}. Below T_{c} the local waiting time tau_{loc} exceeds the time, tau_{pl}, needed for the system to explore the basin, indicating the action of barriers. The distinction between motion among the IS below T_{c} and saddle, or border dynamics above T_{c} is discussed.
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.
We study the diffusive motion of a test particle in a two-dimensional comb structure consisting of a main backbone channel with continuously distributed side branches, in the presence of stochastic Markovian resetting to the initial position of the particle. We assume that the motion along the infinitely long branches is biased by a confining potential. The crossover to the steady state is quantified in terms of a large deviation function, which is derived for the first time for comb structures in present paper. We show that the relaxation region is demarcated by a nonlinear light-cone beyond which the system is evolving in time. We also investigate the first-passage times along the backbone and calculate the mean first-passage time and optimal resetting rate.
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.
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