Multiple length and time scales of dynamic heterogeneities in model glass-forming liquids: a systematic analysis of multi-point and multi-time correlations.

نویسندگان

  • Kang Kim
  • Shinji Saito
چکیده

We report an extensive and systematic investigation of the multi-point and multi-time correlation functions to reveal the spatio-temporal structures of dynamic heterogeneities in glass-forming liquids. Molecular dynamics simulations are carried out for the supercooled states of various prototype models of glass-forming liquids such as binary Kob-Andersen, Wahnström, soft-sphere, and network-forming liquids. While the first three models act as fragile liquids exhibiting super-Arrhenius temperature dependence in their relaxation times, the last is a strong glass-former exhibiting Arrhenius behavior. First, we quantify the length scale of the dynamic heterogeneities utilizing the four-point correlation function. The growth of the dynamic length scale with decreasing temperature is characterized by various scaling relations that are analogous to the critical phenomena. We also examine how the growth of the length scale depends upon the model employed. Second, the four-point correlation function is extended to a three-time correlation function to characterize the temporal structures of the dynamic heterogeneities based on our previous studies [K. Kim and S. Saito, Phys. Rev. E 79, 060501(R) (2009); and J. Chem. Phys. 133, 044511 (2010)]. We provide comprehensive numerical results obtained from the three-time correlation function for the above models. From these calculations, we examine the time scale of the dynamic heterogeneities and determine the associated lifetime in a consistent and systematic way. Our results indicate that the lifetime of the dynamical heterogeneities becomes much longer than the α-relaxation time determined from a two-point correlation function in fragile liquids. The decoupling between the two time scales is remarkable, particularly in supercooled states, and the time scales differ by more than an order of magnitude in a more fragile liquid. In contrast, the lifetime is shorter than the α-relaxation time in tetrahedral network-forming strong liquid, even at lower temperatures.

برای دانلود متن کامل این مقاله و بیش از 32 میلیون مقاله دیگر ابتدا ثبت نام کنید

ثبت نام

اگر عضو سایت هستید لطفا وارد حساب کاربری خود شوید

منابع مشابه

Anomalous diffusion in heterogeneous glass-forming liquids: temperature-dependent behavior.

In a preceding paper, Langer and Mukhopadhyay [Phys. Rev. E 77, 061505 (2008)] studied the diffusive motion of a tagged molecule in an heterogeneous glass-forming liquid at temperatures just above a glass transition. Among other features of this system, we postulated a relation between heterogeneity and stretched-exponential decay of correlations, and we also confirmed that systems of this kind...

متن کامل

Spontaneous and induced dynamic fluctuations in glass formers. I. General results and dependence on ensemble and dynamics.

We study theoretically and numerically a family of multipoint dynamic susceptibilities that quantify the strength and characteristic length scales of dynamic heterogeneities in glass-forming materials. We use general theoretical arguments (fluctuation-dissipation relations and symmetries of relevant dynamical field theories) to relate the sensitivity of averaged two-time correlators to temperat...

متن کامل

Dynamics and correlation length scales of a glass-forming liquid in quiescent and sheared conditions.

We numerically study dynamics and correlation length scales of a colloidal liquid in both quiescent and sheared conditions to further understand the origin of slow dynamics and dynamic heterogeneity in glass-forming systems. The simulation is performed in a weakly frustrated two-dimensional liquid, where locally preferred order is allowed to develop with increasing density. The four-point densi...

متن کامل

Spatial correlations in glass-forming liquids across the mode-coupling crossover

We discuss a novel approach, the point-to-set correlation functions, that allows to determine relevant static and dynamic length scales in glass-forming liquids. We find that static length scales increase monotonically when the temperature is lowered, whereas the measured dynamic length scale shows a maximum around the critical temperature of mode-coupling theory. We show that a similar non-mon...

متن کامل

Threshold F-policy and N-policy for multi-component machining system with warm standbys

The integration of marketing and demand with logistics and inventories (supply side of companies) may cause multiple improvements; it can revolutionize the management of the revenue of rental companies, hotels, and airlines. In this paper, we develop a multi-objective pricing-inventory model for a retailer. Maximizing the retailer's profit and the service level are the objectives, and shorta...

متن کامل

ذخیره در منابع من


  با ذخیره ی این منبع در منابع من، دسترسی به آن را برای استفاده های بعدی آسان تر کنید

برای دانلود متن کامل این مقاله و بیش از 32 میلیون مقاله دیگر ابتدا ثبت نام کنید

ثبت نام

اگر عضو سایت هستید لطفا وارد حساب کاربری خود شوید

عنوان ژورنال:
  • The Journal of chemical physics

دوره 138 12  شماره 

صفحات  -

تاریخ انتشار 2013