Dynamically correlated regions and configurational entropy in supercooled liquids.
نویسندگان
چکیده
When a liquid is cooled below its melting temperature, if crystallization is avoided, it forms a glass. This phenomenon, called glass transition, is characterized by a marked increase of viscosity, about 14 orders of magnitude, in a narrow temperature interval. The microscopic mechanism behind the glass transition is still poorly understood. However, recently, great advances have been made in the identification of cooperative rearranging regions, or dynamical heterogeneities, i.e., domains of the liquid whose relaxation is highly correlated. The growth of the size of these domains is now believed to be the driving mechanism for the increase of the viscosity. Recently a tool to quantify the size of these domains has been proposed. We apply this tool to a wide class of materials to investigate the correlation between the size of the heterogeneities and their configurational entropy, i.e., the number of states accessible to a correlated domain. We find that the relaxation time of a given system, apart from a material dependent prefactor, is a universal function of the configurational entropy of a correlated domain. As a consequence, we find that, at the glass transition temperature, the size of the domains and the configurational entropy per unit volume are anticorrelated, as originally predicted by the Adam-Gibbs theory. Finally, we use our data to extract some exponents defined in the framework of the random first-order theory, a recent quantitative theory of the glass transition.
منابع مشابه
String-like Correlated Motion in Supercooled Liquids and Polymers
Title of dissertation: SPATIALLY HETEROGENEOUS DYNAMICS AND STRING-LIKE CORRELATED MOTION IN SUPERCOOLED LIQUIDS AND POLYMERS Yeshitila Gebremichael, Doctor of Philosophy, 2004 Dissertation directed by: Professor Sharon C. Glotzer Chemical Engineering Department University of Michigan, Ann Arbor, MI Professor John D. Weeks Chemical Physics Program University of Maryland, College Park, MD Dense ...
متن کاملBarrier Softening near the onset of Non-Activated Transport in Supercooled Liquids: Implications for Establishing Detailed Connection between Thermodynamic and Kinetic Anomalies in Supercooled Liquids
According to the Random First Order Transition (RFOT) theory of glasses, the barriers for activated dynamics in supercooled liquids vanish as the temperature of a viscous liquid approaches the dynamical transition temperature from below. This occurs due to a decrease of the surface tension between local meta-stable molecular arrangements much like at a spinodal. The dynamical transition thus re...
متن کاملNovel approach to numerical measurements of the configurational entropy in supercooled liquids.
The configurational entropy is among the key observables to characterize experimentally the formation of a glass. Physically, it quantifies the multiplicity of metastable states in which an amorphous material can be found at a given temperature, and its temperature dependence provides a major thermodynamic signature of the glass transition, which is experimentally accessible. Measurements of th...
متن کاملConnection between Adam-Gibbs theory and spatially heterogeneous dynamics.
We investigate the spatially heterogeneous dynamics in the extended simple point charge model of water using molecular dynamics simulations. We relate the average mass n* of mobile particle clusters to the diffusion constant and the configurational entropy. Hence, n* can be interpreted as the mass of the "cooperatively rearranging regions" that form the basis of the Adam-Gibbs theory of the dyn...
متن کاملThe Viscous Slowing down of Supercooled Liquids and the Glass Transition: Phenomenology, Concepts, and Models
The viscous slowing down of supercooled liquids that leads to glass formation can be considered as a classical, and is assuredly a thoroughly studied, example of a ”jamming process”. In this review, we stress the distinctive features characterizing the phenomenon. We also discuss the main theoretical approaches, with an emphasis on the concepts (free volume, dynamic freezing and mode-coupling a...
متن کاملذخیره در منابع من
با ذخیره ی این منبع در منابع من، دسترسی به آن را برای استفاده های بعدی آسان تر کنید
عنوان ژورنال:
- The journal of physical chemistry. B
دوره 112 34 شماره
صفحات -
تاریخ انتشار 2008