Cage-jump motion reveals universal dynamics and non-universal structural features in glass forming liquids

Pastore, Raffaele; Coniglio, Antonio; Candia, A. de; Fierro, Annalisa; Ciamarra, Massimo Pica

doi:10.1088/1742-5468/2016/05/054050

Cited by 29 publications

(36 citation statements)

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“…Cage breakings have been modelled [11,12] using a Continuous Time Random Walk (CTRW) [13], a popular coarse-graining device recently criticized in [14,15]. Other approaches to coarse-graining are e.g.…”

Section: Introductionmentioning

confidence: 99%

“…To summarize, the phenomenology of glass formers and aging HSC is experimentally [1,2,4,5,7,29] and numerically [3,6,9,10] well described, but a unified theoretical description [11,12,28] is not yet available. RD has been proposed [15,24,28] as a viable candidate and its validity is investigated in the present work by extensive MD simulations of three dimensional HSC which extend over 6 order of magnitude in time.…”

Section: Introductionmentioning

confidence: 99%

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Dynamics of dense hard sphere colloidal systems: A numerical analysis

Sibani

Svaneborg

2019

Phys. Rev. E

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The applicability to dense hard sphere colloidal suspensions of a general coarse-graining approach called Record Dynamics (RD) is tested by extensive molecular dynamics simulations. We reproduce known results as logarithmic diffusion and the logarithmic decay of the average potential energy per particle. We provide quantitative measures for the cage size and identify the displacements of single particles corresponding to cage breakings. We then partition the system into spatial domains. Within each domain, a subset of intermittent events called quakes is shown to constitute a log-Poisson process, as predicted by Record Dynamics. Specifically, these events are shown to be statistically independent and Poisson distributed with an average depending on the logarithm of time. Finally, we discuss the nature of the dynamical barriers surmounted by quakes and link RD to the phenomenology of aging hard sphere colloids.

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Section: Introductionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

Dynamics of dense hard sphere colloidal systems: A numerical analysis

Sibani

Svaneborg

2019

Phys. Rev. E

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“…Pastore et al have recently developed a cage-jump model to predict the long-time diffusivity from the shorttime cage dynamics in supercooled liquids. [26][27][28][29][30][31] In the study, a trajectory of a single particle is segmented into a) Electronic mail: kk@cheng.es.osaka-u.ac.jp b) Electronic mail: nobuyuki@cheng.es.osaka-u.ac.jp caged and jumping states. The segmentation criterion was given by the MSD plateau value.…”

Section: Introductionmentioning

confidence: 99%

Diffusion dynamics of supercooled water modeled with the cage-jump motion and hydrogen-bond rearrangement

Kikutsuji

Kim

Matubayasi

2019

The Journal of Chemical Physics

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The slow dynamics of glass-forming liquids is generally ascribed to the cage-jump motion. In the cage-jump picture, a molecule remains in a cage formed by neighboring molecules, and after a sufficiently long time, it jumps to escape from the original position by cage-breaking. The clarification of the cage-jump motion is therefore linked to unraveling the fundamental element of the slow dynamics. Here, we develop a cagejump model for the dynamics of supercooled water. The caged and jumping states of a water molecule are introduced with respect to the hydrogen-bond (H-bond) rearrangement process, and describe the motion in supercooled states. It is then demonstrated from the molecular dynamics simulation of the TIP4P/2005 model that the characteristic length and time scales of cage-jump motions provide a good description of the selfdiffusion constant that is determined in turn from the long-time behavior of the mean square displacement. Our cage-jump model thus enables to connect between H-bond dynamics and molecular diffusivity. arXiv:1903.06060v2 [cond-mat.soft]

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“…In the literature, DH is considered to be one of the fingerprints of vitrification, and its cause is attributed to consecutive intermittent jump motions of particles escaping out of cages [45][46][47][48][49]. To begin with, the system-size dependence of the self-part of the intermediate scattering function…”

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confidence: 99%

Unveiling Dimensionality Dependence of Glassy Dynamics: 2D Infinite Fluctuation Eclipses Inherent Structural Relaxation

et al. 2016

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By using large-scale molecular dynamics simulations, the dynamics of two-dimensional (2D) supercooled liquids turns out to be dependent on the system size, while the size dependence is not pronounced in three dimensional (3D) systems. It is demonstrated that the strong system-size effect in 2D amorphous systems originates from the enhanced fluctuations at long wavelengths, which are similar to those of 2D crystal phonons. This observation is further supported by the frequency dependence of the vibrational density of states, consisting of the Debye approximation in the low-wavenumber-limit. However, the system-size effect in the intermediate scattering function becomes negligible when the length scale is larger than the vibrational amplitude. This suggests that the finite-size effect in a 2D system is transient and also that the structural relaxation itself is not fundamentally different from that in a 3D system. In fact, the dynamic correlation lengths estimated from the bond-breakage function, which do not suffer from those enhanced fluctuations, are not size dependent in either 2D or 3D systems. PACS numbers: 62.60.+v, 61.20.Lc, Dimensionality plays a key role in the physics of solids and liquids -from high to low dimensions -and fluctuation shows up differently, as typically observed in phase transitions [1,2]. Indeed, two-dimensional (2D) systems often exhibit enhanced fluctuations, leading to various anomalies that are not experienced in three-dimensional (3D) systems. The melting of a 2D solid is a marked example [3][4][5][6][7][8][9], where the long-wavelength structural correlation is induced by thermal fluctuations sthat span an infinite length. For the glass transition from supercooled liquids to amorphous solids, the dimensionality dependence of the fluctuation has become an issue only recently. Gigantic fluctuation in 2D supercooled liquids has been observed that is far stronger than that in their 3D counterparts [10][11][12]. The aim of this Letter is to elucidate the similarity of this fluctuation to that in crystals [13], and also to investigate the heterogeneous dynamics in both 2D and 3D systems.For a crystalline solid of monodisperse particle assemblies, the mean-squared thermal displacement (MSTD) is given by using the vibrational density of state (VDOS) g(ω) as a function of angular frequency ω aswhere m the particle mass, d the spatial dimension, and (k B T ) −1 the inverse temperature. Under the Debye approximation for the VDOS of acoustic plane waves, g(ω) becomes proportional to ω d−1 [14]. It leads to divergence of the integral in 2D systems owing to the low-frequency acoustic waves, while it converges in 3D systems. As a result, the long-range translation order is prohibited in 2D systems [15,16]. Integration of Eq. (1) over ω ≥ 2πc/L provides us with its dependence on the linear system size L aswhere µ and K are shear and bulk moduli, σ 0 is the particle radius, and c is the velocity of sound. Such fluctuation is the source of the size-dependent behavior of 2D solids undergoing melting...

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Cage-jump motion reveals universal dynamics and non-universal structural features in glass forming liquids

Cited by 29 publications

References 50 publications

Dynamics of dense hard sphere colloidal systems: A numerical analysis

Dynamics of dense hard sphere colloidal systems: A numerical analysis

Diffusion dynamics of supercooled water modeled with the cage-jump motion and hydrogen-bond rearrangement

Unveiling Dimensionality Dependence of Glassy Dynamics: 2D Infinite Fluctuation Eclipses Inherent Structural Relaxation

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