Neutron and light scattering study of supercooled glycerol

Wuttke, Joachim; Hernández, José Carlos Rodríguez; Li, G.; Coddens, G.; Cummins, H. Z.; Fujara, F.; Petry, W.; Sillescu, H.

doi:10.1103/physrevlett.72.3052

Cited by 213 publications

(187 citation statements)

References 25 publications

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“…4,5,8 As a matter of fact, as shown in Ref. 8, the spectra for frequencies above 1 THz can easily be superimposed after scaling by the Bose factor for temperatures within the range 170-313 K, thus indicating that at least for such frequencies, the vibrations in the glass and liquid share rather similar characteristics.…”

Section: Introductionmentioning

confidence: 92%

Microscopic dynamics of glycerol in its crystalline and glassy states

et al. 1996

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The dynamics of crystalline glycerol are studied by means of Raman spectroscopy and lattice dynamics calculations employing a semiflexible model to represent the low-lying molecular vibrations. The latter is validated against structural, thermodynamic, and spectroscopic data. The results serve to set an absolute frequency scale for glassy glycerol, which is also studied by Raman and incoherent inelastic-neutron scattering. Some implications of the present findings regarding ensuing discussions on glassy dynamics are finally commented on.

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Section: Introductionmentioning

confidence: 92%

Microscopic dynamics of glycerol in its crystalline and glassy states

et al. 1996

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“…[16][17][18][19][20] Moreover, molecular dynamics (MD) simulations have been performed in order to explore the dynamics of this glass-forming liquid. 21 An early and quite extensive analysis of QENS data on glycerol was performed by Wuttke et al [22][23][24] in the context of mode coupling theory (MCT). This study made extensive use of phenomenological Kohlrausch-Williams-Watts (KWW) line shapes to describe the slow dynamics.…”

Section: Introductionmentioning

confidence: 99%

A robust comparison of dynamical scenarios in a glass-forming liquid

Vispa

Büsch

Tamarit

et al. 2016

Phys. Chem. Chem. Phys.

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We use Bayesian inference methods to provide fresh insights into the sub-nanosecond dynamics of glycerol, a prototypical glass-forming liquid. To this end, quasielastic neutron scattering data as a function of temperature have been analyzed using a minimal set of underlying physical assumptions. On the basis of this analysis, we establish the unambiguous presence of three distinct dynamical processes in glycerol, namely, translational diffusion of the molecular centre of mass and two additional localized and temperature-independent modes.The neutron data also provide access to the characteristic length scales associated with these motions in a model-independent manner, from which we conclude that the faster (slower) localized motions probe longer (shorter) length scales. Careful Bayesian analysis of the entire scattering law favors a heterogeneous scenario for the microscopic dynamics of glycerol, where molecules undergo either the faster and longer or the slower and shorter localized motions.

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“…[15][16][17][18] More recently, experimental studies have been carried out of the short-time dynamics in nonfragile glass-formers, such as ZnCl 2 , 21 B 2 O 3 , 22 and glycerol. 6,8 In these "intermediate liquids", no prominent fast process is observed, notwithstanding the MCT prediction of its presence in both fragile and nonfragile liquids. To reconcile this deviation from MCT, it has been suggested that masking by a dominant boson peak causes the apparent absence of a fast -process in nonfragile liquids.…”

Section: Introductionmentioning

confidence: 99%

“…Short-time relaxational processes in glass-forming-liquids have been the subject of intense research, using various techniques including quasielastic neutron scattering, [1][2][3][4][5][6] dynamic light scattering, [7][8][9] and molecular dynamics simulations. [10][11][12] Much of this activity has been stimulated by mode coupling theory (MCT), 13 for example, in assessing the theory's prediction of a fast (ca.…”

Section: Introductionmentioning

confidence: 99%

“…3 These fast processes have not always been identified as the -process of MCT but rather as another possiblity as described below. 4,5,[15][16][17][18] The materials exhibiting a fast process are all considered "fragile" glass-formers [1][2][3][4][5][6][7][8][9][10][11][12][13][14] (i.e., exhibiting relaxation times that decrease markedly with a change in T gnormalized temperature 19 ). The expectation from MCT is that all glass-formers, "fragile" or "strong" (both terms referring to the temperature sensitivity of the relaxation times), will exhibit a fast -process.…”

Section: Introductionmentioning

confidence: 99%

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Short-Time Relaxational Dynamics of the “Strong” Glass-Former Methanol

Ngai

Roland

1997

J. Phys. Chem. B

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According to the coupling model of relaxation, structural relaxation in glass-forming liquids is comprised of an intermolecularly uncorrelated step ("fast R-relaxation process") in the picosecond time range followed by a slowed, intermolecularly cooperative, "slow R" process. Molecular dynamics simulation data [Sindzingre, P.; Klein, M. J. Chem. Phys. 1992, 96, 4681] have shown that for the "strong" liquid methanol, the fast relaxation step is absent. This finding is in contrast to the prominent fast relaxation appearing in fragile liquids about the glass transition temperature. The differing behavior of methanol can be accounted for from an analysis of the self part of the intermediate scattering function, F S (k,t) according to the coupling model. The latter relates the magnitude of the fast R-relaxation to the relaxation time, τ*, and to the exponent of the slow R-process described by the stretched exponential function exp[-(t/τ*) ]. This function fits the experimental F S (k,t) for t longer than 2 ps. The apparent absence of a fast relaxation step in methanol is shown to be a consequence of the weak intermolecular constraints governing the dynamics in "strong" liquids, a result consistent with the prominence of the fast process in polymers and other fragile glass-formers. This conclusion is supported by dielectric relaxation data (frequencies up to 90 GHz) and far-infrared data (>150 GHz) on methanol.

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Neutron and light scattering study of supercooled glycerol

Cited by 213 publications

References 25 publications

Microscopic dynamics of glycerol in its crystalline and glassy states

Microscopic dynamics of glycerol in its crystalline and glassy states

A robust comparison of dynamical scenarios in a glass-forming liquid

Short-Time Relaxational Dynamics of the “Strong” Glass-Former Methanol

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