Broadband dielectric spectroscopy on benzophenone: alpha relaxation, beta relaxation, and mode coupling theory

We have performed a detailed dielectric investigation of the relaxational dynamics of glass-forming benzophenone. Our measurements cover a broad frequency range of 0.1 Hz to 120 GHz and temperatures from far below the glass temperature well up into the region of the small-viscosity liquid. With respect to the alpha relaxation this material can be characterized as a typical molecular glass former with rather high fragility. A good agreement of the alpha relaxation behavior with the predictions of the mode coupling theory of the glass transition is stated. In addition, at temperatures below and in the vicinity of Tg we detect a well-pronounced beta relaxation of Johari-Goldstein type, which with increasing temperature develops into an excess wing. We compare our results to literature data from optical Kerr effect and depolarized light scattering experiments, where an excess-wing like feature was observed in the 1 - 100 GHz region. We address the question if the Cole-Cole peak, which was invoked to describe the optical Kerr effect data within the framework of the mode coupling theory, has any relation to the canonical beta relaxation detected by dielectric spectroscopy.Comment: 11 pages, 7 figures; revised version with new Fig. 5 and some smaller changes according to referees' demand

Viscoelastic behaviour of polymethyl methacrylate networks with different crosslinking degrees

The influence of the cross-linking degree on the dynamics of the segmental motions close to the glass transition of poly(methyl methacrylate), PMMA, networks was investigated by three different mechanical spectroscopy techniques: thermally stimulated recovery (TSR), dynamic mechanical analysis (DMA), and creep. The application of the time-temperature superposition principle to isothermal DMA and creep results permitted to successfully construct master curves for PMMA networks with distinct cross-linking degrees. The former results were fitted to the KWW equation. The obtained variation of âKWW for the distinct networks indicated that the relaxation curves tend to broaden as the cross-linking degree increases. TSR results clearly revealed a significant shift of the R-relaxation to longer times and a broader relaxation as the cross-linking degree increases, what was also observed by DMA and creep. A change from a Vogel to an Arrhenius behavior was detected by the three techniques with the decrease of temperature below Tg. The temperature dependence of the apparent activation energies (Ea) was calculated from DMA, creep, and TSR experiments; above Tg a good agreement was seen between the Ea values for all the techniques. Furthermore, the effect of the cross-linking degree on the fragility of PMMA networks was evaluated. For these materials an increase of fragility with increasing cross-linking degree was observed

Non exponential relaxation in fully frustrated models

We study the dynamical properties of the fully frustrated Ising model. Due to the absence of disorder the model, contrary to spin glass, does not exhibit any Griffiths phase, which has been associated to non-exponential relaxation dynamics. Nevertheless we find numerically that the model exhibits a stretched exponential behavior below a temperature T_p corresponding to the percolation transition of the Kasteleyn-Fortuin clusters. We have also found that the critical behavior of this clusters for a fully frustrated q-state spin model at the percolation threshold is strongly affected by frustration. In fact while in absence of frustration the q=1 limit gives random percolation, in presence of frustration the critical behavior is in the same universality class of the ferromagnetic q=1/2-state Potts model.Comment: 7 pages, RevTeX, 11 figs, to appear on Physical Review

Broadband Dielectric Spectroscopy on Glass-Forming Propylene Carbonate

Dielectric spectroscopy covering more than 18 decades of frequency has been performed on propylene carbonate in its liquid and supercooled-liquid state. Using quasi-optic submillimeter and far-infrared spectroscopy the dielectric response was investigated up to frequencies well into the microscopic regime. We discuss the alpha-process whose characteristic timescale is observed over 14 decades of frequency and the excess wing showing up at frequencies some three decades above the peak frequency. Special attention is given to the high-frequency response of the dielectric loss in the crossover regime between alpha-peak and boson-peak. Similar to our previous results in other glass forming materials we find evidence for additional processes in the crossover regime. However, significant differences concerning the spectral form at high frequencies are found. We compare our results to the susceptibilities obtained from light scattering and to the predictions of various models of the glass transition.Comment: 13 pages, 9 figures, submitted to Phys. Rev.

Measurement of Cosmic-ray Muons and Muon-induced Neutrons in the Aberdeen Tunnel Underground Laboratory

We have measured the muon flux and production rate of muon-induced neutrons at a depth of 611 m water equivalent. Our apparatus comprises three layers of crossed plastic scintillator hodoscopes for tracking the incident cosmic-ray muons and 760 L of gadolinium-doped liquid scintillator for producing and detecting neutrons. The vertical muon intensity was measured to be $I_{\mu} = (5.7 \pm 0.6) \times 10^{-6}$ cm$^{-2}$s$^{-1}$sr$^{-1}$. The yield of muon-induced neutrons in the liquid scintillator was determined to be $Y_{n} = (1.19 \pm 0.08 (stat) \pm 0.21 (syst)) \times 10^{-4}$ neutrons/($\mu\cdot$g$\cdot$cm$^{-2}$). A fit to the recently measured neutron yields at different depths gave a mean muon energy dependence of $\left\langle E_{\mu} \right\rangle^{0.76 \pm 0.03}$ for liquid-scintillator targets.Comment: 14 pages, 17 figures, 3 table

Evidence of coexistence of change of caged dynamics at Tg and the dynamic transition at Td in solvated proteins

Mossbauer spectroscopy and neutron scattering measurements on proteins embedded in solvents including water and aqueous mixtures have emphasized the observation of the distinctive temperature dependence of the atomic mean square displacements, , commonly referred to as the dynamic transition at some temperature Td. At low temperatures, increases slowly, but it assume stronger temperature dependence after crossing Td, which depends on the time/frequency resolution of the spectrometer. Various authors have made connection of the dynamics of solvated proteins including the dynamic transition to that of glass-forming substances. Notwithstanding, no connection is made to the similar change of temperature dependence of obtained by quasielastic neutron scattering when crossing the glass transition temperature Tg, generally observed in inorganic, organic and polymeric glass-formers. Evidences are presented to show that such change of the temperature dependence of from neutron scattering at Tg is present in hydrated or solvated proteins, as well as in the solvents used unsurprisingly since the latter is just another organic glass-formers. The obtained by neutron scattering at not so low temperatures has contributions from the dissipation of molecules while caged by the anharmonic intermolecular potential at times before dissolution of cages by the onset of the Johari-Goldstein beta-relaxation. The universal change of at Tg of glass-formers had been rationalized by sensitivity to change in volume and entropy of the beta-relaxation, which is passed onto the dissipation of the caged molecules and its contribution to . The same rationalization applies to hydrated and solvated proteins for the observed change of at Tg.Comment: 28 pages, 10 figures, 1 Tabl