Space-time Thermodynamics of the Glass Transition

We consider the probability distribution for fluctuations in dynamical action and similar quantities related to dynamic heterogeneity. We argue that the so-called "glass transition" is a manifestation of low action tails in these distributions where the entropy of trajectory space is sub-extensive in time. These low action tails are a consequence of dynamic heterogeneity and an indication of phase coexistence in trajectory space. The glass transition, where the system falls out of equilibrium, is then an order-disorder phenomenon in space-time occurring at a temperature T_g which is a weak function of measurement time. We illustrate our perspective ideas with facilitated lattice models, and note how these ideas apply more generally.Comment: 5 pages, 4 figure

Dynamics and Thermodynamics of the Glass Transition

The principal theme of this paper is that anomalously slow, super-Arrhenius relaxations in glassy materials may be activated processes involving chains of molecular displacements. As pointed out in a preceding paper with A. Lemaitre, the entropy of critically long excitation chains can enable them to grow without bound, thus activating stable thermal fluctuations in the local density or molecular coordination of the material. I argue here that the intrinsic molecular-scale disorder in a glass plays an essential role in determining the activation rate for such chains, and show that a simple disorder-related correction to the earlier theory recovers the Vogel-Fulcher law in three dimensions. A key feature of this theory is that the spatial extent of critically long excitation chains diverges at the Vogel-Fulcher temperature. I speculate that this diverging length scale implies that, as the temperature decreases, increasingly large regions of the system become frozen and do not contribute to the configurational entropy, and thus ergodicity is partially broken in the super-Arrhenius region above the Kauzmann temperature $T_K$. This partially broken ergodicity seems to explain the vanishing entropy at $T_K$ and other observed relations between dynamics and thermodynamics at the glass transition.Comment: 20 pages, no figures, some further revision

Unexpected drop of dynamical heterogeneities in colloidal suspensions approaching the jamming transition

As the glass (in molecular fluids\cite{Donth}) or the jamming (in colloids and grains\cite{LiuNature1998}) transitions are approached, the dynamics slow down dramatically with no marked structural changes. Dynamical heterogeneity (DH) plays a crucial role: structural relaxation occurs through correlated rearrangements of particle ``blobs'' of size $\xi$\cite{WeeksScience2000,DauchotPRL2005,Glotzer,Ediger}. On approaching these transitions, $\xi$ grows in glass-formers\cite{Glotzer,Ediger}, colloids\cite{WeeksScience2000,BerthierScience2005}, and driven granular materials\cite{KeysNaturePhys2007} alike, strengthening the analogies between the glass and the jamming transitions. However, little is known yet on the behavior of DH very close to dynamical arrest. Here, we measure in colloids the maximum of a ``dynamical susceptibility'', $\chi^*$, whose growth is usually associated to that of $\xi$\cite{LacevicPRE}. $\chi^*$ initially increases with volume fraction $\phi$, as in\cite{KeysNaturePhys2007}, but strikingly drops dramatically very close to jamming. We show that this unexpected behavior results from the competition between the growth of $\xi$ and the reduced particle displacements associated with rearrangements in very dense suspensions, unveiling a richer-than-expected scenario.Comment: 1st version originally submitted to Nature Physics. See the Nature Physics website fro the final, published versio

Activity phase transition for constrained dynamics

We consider two cases of kinetically constrained models, namely East and FA-1f models. The object of interest of our work is the activity A(t) defined as the total number of configuration changes in the interval [0,t] for the dynamics on a finite domain. It has been shown in [GJLPDW1,GJLPDW2] that the large deviations of the activity exhibit a non-equilibirum phase transition in the thermodynamic limit and that reducing the activity is more likely than increasing it due to a blocking mechanism induced by the constraints. In this paper, we study the finite size effects around this first order phase transition and analyze the phase coexistence between the active and inactive dynamical phases in dimension 1. In higher dimensions, we show that the finite size effects are also determined by the dimension and the choice of boundary conditions.Comment: 38 pages, 3 figure

Fragility, Stokes-Einstein violation, and correlated local excitations in a coarse-grained model of an ionic liquid

Dynamics of a coarse-grained model for the room-temperature ionic liquid, 1-ethyl-3-methylimidazolium hexafluorophosphate, couched in the united-atom site representation are studied via molecular dynamics simulations. The dynamically heterogeneous behavior of the model resembles that of fragile supercooled liquids. At or close to room temperature, the model ionic liquid exhibits slow dynamics, characterized by nonexponential structural relaxation and subdiffusive behavior. The structural relaxation time, closely related to the viscosity, shows a super-Arrhenius behavior. Local excitations, defined as displacement of an ion exceeding a threshold distance, are found to be mainly responsible for structural relaxation in the alternating structure of cations and anions. As the temperature is lowered, excitations become progressively more correlated. This results in the decoupling of exchange and persistence times, reflecting a violation of the Stokes-Einstein relation.Comment: Published on the Phys. Chem. Chem. Phys. websit

Corresponding States of Structural Glass Formers

The variation with respect to temperature T of transport properties of 58 fragile structural glass forming liquids (68 data sets in total) are analyzed and shown to exhibit a remarkable degree of universality. In particular, super-Arrhenius behaviors of all super-cooled liquids appear to collapse to one parabola for which there is no singular behavior at any finite temperature. This behavior is bounded by an onset temperature To above which liquid transport has a much weaker temperature dependence. A similar collapse is also demonstrated, over the smaller available range, for existing numerical simulation data.Comment: 6 pages, 2 figures. Updated References, Table Values, Submitted for Publicatio

Thermodynamic formalism for systems with Markov dynamics

The thermodynamic formalism allows one to access the chaotic properties of equilibrium and out-of-equilibrium systems, by deriving those from a dynamical partition function. The definition that has been given for this partition function within the framework of discrete time Markov chains was not suitable for continuous time Markov dynamics. Here we propose another interpretation of the definition that allows us to apply the thermodynamic formalism to continuous time. We also generalize the formalism --a dynamical Gibbs ensemble construction-- to a whole family of observables and their associated large deviation functions. This allows us to make the connection between the thermodynamic formalism and the observable involved in the much-studied fluctuation theorem. We illustrate our approach on various physical systems: random walks, exclusion processes, an Ising model and the contact process. In the latter cases, we identify a signature of the occurrence of dynamical phase transitions. We show that this signature can already be unravelled using the simplest dynamical ensemble one could define, based on the number of configuration changes a system has undergone over an asymptotically large time window.Comment: 64 pages, LaTeX; version accepted for publication in Journal of Statistical Physic

X-ray fluorescence microscopy of light elements in cells: self-absorption correction by integration of compositional and morphological measurements

We present here a new methodology for quantitative mapping of light elements in cells, based on combination of compositional and morphological information, derived respectively by X-ray Fluorescence Microscopy (XRFM), Atomic Force Microscopy and Scanning Transmission X-ray Microscopy (STXM). Since XRFM of light elements (carbon, nitrogen, oxygen, sodium and magnesium), are strongly influenced by self-absorption, we developed an algorithm to correct for this effect, using the morphological and structural information provided by AFM and STXM. Finally, the corrected distributions have been obtained, thus allowing quantitative mapping

First results from the full-scale prototype for the Fluorescence detector Array of Single-pixel Telescopes

The Fluorescence detector Array of Single-pixel Telescopes (FAST) is a design concept for the next generation of ultrahigh-energy cosmic ray (UHECR) observatories, addressing the require- ments for a large-area, low-cost detector suitable for measuring the properties of the highest en- ergy cosmic rays. In the FAST design, a large field of view is covered by a few pixels at the focal plane of a mirror or Fresnel lens. Motivated by the successful detection of UHECRs using a prototype comprised of a single 200 mm photomultiplier-tube and a 1 m2 Fresnel lens system [Astropart.Phys. 74 (2016) 64-72], we have developed a new full-scale prototype consisting of four 200 mm photomultiplier-tubes at the focus of a segmented mirror of 1.6 m in diameter. In October 2016 we installed the full-scale prototype at the Telescope Array site in central Utah, USA, and began steady data taking. We report on first results of the full-scale FAST prototype, including measurements of artificial light sources, distant ultraviolet lasers, and UHECRs.Toshihiro Fujii, Max Malacari, Justin Albury, Jose A. Bellido, John Farmer, Aygul Galimova, Pavel Horvath, Miroslav Hrabovsky, Dusan Mandat, Ariel Matalon, John N. Matthews, Maria Merolle, Xiaochen Ni, Libor Nozka, Miroslav Palatka, Miroslav Pech, Paolo Privitera, Petr Schovanek, Stan B. Thomas, Petr Travnicek (FAST Collaboration

Simulating rare events in dynamical processes

Atypical, rare trajectories of dynamical systems are important: they are often the paths for chemical reactions, the haven of (relative) stability of planetary systems, the rogue waves that are detected in oil platforms, the structures that are responsible for intermittency in a turbulent liquid, the active regions that allow a supercooled liquid to flow... Simulating them in an efficient, accelerated way, is in fact quite simple. In this paper we review a computational technique to study such rare events in both stochastic and Hamiltonian systems. The method is based on the evolution of a family of copies of the system which are replicated or killed in such a way as to favor the realization of the atypical trajectories. We illustrate this with various examples