Vibrational origin of the fast relaxation processes in molecular glass-formers

We study the interaction of the relaxation processes with the density fluctuations by molecular dynamics simulation of a flexible molecule model for o-terphenyl (oTP) in the liquid and supercooled phases. We find evidence, besides the structural relaxation, of a secondary vibrational relaxation whose characteristic time, few ps, is slightly temperature dependent. This i) confirms the result by Monaco et al. [Phys. Rev, E 62, 7595 (2000)] of the vibrational nature of the fast relaxation observed in Brillouin Light Scattering (BLS) experiments in oTP; and ii) poses a caveat on the interpretation of the BLS spectra of molecular systems in terms of a purely center of mass dynamics.Comment: RevTeX, 5 pages, 4 eps figure

Correlations between the mechanical loss and atomic structure of amorphous TiO2-doped Ta2O5 coatings

<p>Highly reflective dielectric mirror coatings are critical components in a range of precision optics applications including frequency combs, optical atomic clocks, precision interferometry and ring laser gyroscopes. A key limitation to the performance in these applications is thermal noise, arising from the mechanical loss of the coatings. The origins of the mechanical loss from these coatings is not well understood.</p> <p>Recent work suggests that the mechanical loss of amorphous Ta2O5 coatings can drop by as much as 40% when it is doped with TiO2. We use a combination of electron diffraction data and atomic modelling using molecular dynamics to probe the atomic structure of these coatings, and examine the correlations between changes in the atomic structure and changes in the mechanical loss of these coatings. Our results show the first correlation between changes in the mechanical loss and experimentally measured changes in the atomic structure resulting from variations in the level of TiO2 doping in TiO2-doped Ta2O5 coatings, in that increased homogeneity at the nearest-neighbour level appears to correlate with reduced mechanical loss. It is demonstrated that subtle but measurable changes in the nearest-neighbour homogeneity in an amorphous material can correlate with significant changes in macroscopic properties.</p&gt

Energy landscape - a key concept for the dynamics of glasses and liquids

There is a growing belief that the mode coupling theory is the proper microscopic theory for the dynamics of the undercooled liquid above a critical temperature T_c. In addition, there is some evidence that the system leaves the saddlepoints of the energy landscape to settle in the valleys at this critical temperature. Finally, there is a microscopic theory for the entropy at the calorimetric glass transition T_g by Mezard and Parisi, which allows to calculate the Kauzmann temperature from the atomic pair potentials. The dynamics of the frozen glass phase is at present limited to phenomenological models. In the spirit of the energy landscape concept, one considers an ensemble of independent asymmetric double-well potentials with a wide distribution of barrier heights and asymmetries (ADWP or Gilroy-Phillips model). The model gives an excellent description of the relaxation of glasses up to about T_g/4. Above this temperature, the interaction between different relaxation centers begins to play a role. One can show that the interaction reduces the number of relaxation centers needed to bring the shear modulus down to zero by a factor of three.Comment: Contribution to the III Workshop on Nonequilibrium Phenomena in Supercooled Fluids, Glasses and Amorphous Materials, 22-27 September 2002, Pisa; 14 pages, 3 figures; Version 3 takes criticque at Pisa into account; final version 4 will be published in J.Phys.: Condens.Matte

Spectral Shape of Relaxations in Silica Glass

Precise low-frequency light scattering experiments on silica glass are presented, covering a broad temperature and frequency range (9 GHz < \nu < 2 THz). For the first time the spectral shape of relaxations is observed over more than one decade in frequency. The spectra show a power-law low-frequency wing of the relaxational part of the spectrum with an exponent $\alpha$ proportional to temperature in the range 30 K < T < 200 K. A comparison of our results with those from acoustic attenuation experiments performed at different frequencies shows that this power-law behaviour rather well describes relaxations in silica over 9 orders of magnitude in frequency. These findings can be explained by a model of thermally activated transitions in double well potentials.Comment: 4 pages, 3 figures, submitted to Phys. Rev. Let

Minimal model for beta relaxation in viscous liquids

Contrasts between beta relaxation in equilibrium viscous liquids and glasses are rationalized in terms of a double-well potential model with structure-dependent asymmetry, assuming structure is described by a single order parameter. The model is tested for tripropylene glycol where it accounts for the hysteresis of the dielectric beta loss peak frequency and magnitude during cooling and reheating through the glass transition.Comment: Phys. Rev. Lett. (in press

Molecular dynamics simulation of the fragile glass former ortho-terphenyl: a flexible molecule model

We present a realistic model of the fragile glass former orthoterphenyl and the results of extensive molecular dynamics simulations in which we investigated its basic static and dynamic properties. In this model the internal molecular interactions between the three rigid phenyl rings are described by a set of force constants, including harmonic and anharmonic terms; the interactions among different molecules are described by Lennard-Jones site-site potentials. Self-diffusion properties are discussed in detail together with the temperature and momentum dependencies of the self-intermediate scattering function. The simulation data are compared with existing experimental results and with the main predictions of the Mode Coupling Theory.Comment: 20 pages and 28 postscript figure

Mechanical Relaxation in Glasses and at the Glass Transition

The Gilroy-Phillips model of relaxational jumps in asymmetric double-well potentials, developed for the Arrhenius-type secondary relaxations of the glass phase, is extended to a formal description of the breakdown of the shear modulus at the glass transition, the flow process.Comment: 13 pages, 11 figures, 49 ref

Corresponding States of Structural Glass Formers

The variation with respect to temperature T of transport properties of 58 fragile structural glass forming liquids (68 data sets in total) are analyzed and shown to exhibit a remarkable degree of universality. In particular, super-Arrhenius behaviors of all super-cooled liquids appear to collapse to one parabola for which there is no singular behavior at any finite temperature. This behavior is bounded by an onset temperature To above which liquid transport has a much weaker temperature dependence. A similar collapse is also demonstrated, over the smaller available range, for existing numerical simulation data.Comment: 6 pages, 2 figures. Updated References, Table Values, Submitted for Publicatio

Time-temperature superposition in viscous liquids

Dielectric relaxation measurements on supercooled triphenyl phosphite show that at low temperatures time-temperature superposition (TTS) is accurately obeyed for the primary (alpha) relaxation process. Measurements on 6 other molecular liquids close to the calorimetric glass transition indicate that TTS is linked to an $\omega^{-1/2}$ high-frequency decay of the alpha loss, while the loss peak width is nonuniversal.Comment: 4 page

The crossover from propagating to strongly scattered acoustic modes of glasses observed in densified silica

Spectroscopic results on low frequency excitations of densified silica are presented and related to characteristic thermal properties of glasses. The end of the longitudinal acoustic branch is marked by a rapid increase of the Brillouin linewidth with the scattering vector. This rapid growth saturates at a crossover frequency Omega_co which nearly coincides with the center of the boson peak. The latter is clearly due to additional optic-like excitations related to nearly rigid SiO_4 librations as indicated by hyper-Raman scattering. Whether the onset of strong scattering is best described by hybridization of acoustic modes with these librations, by their elastic scattering (Rayleigh scattering) on the local excitations, or by soft potentials remains to be settled.Comment: 14 pages, 6 figures, to be published in a special issue of J. Phys. Condens. Matte