High frequency sound waves in vitreous silica

We report a molecular dynamics simulation study of the sound waves in vitreous silica in the mesoscopic exchanged momentum range. The calculated dynamical structure factors are in quantitative agreement with recent experimental inelastic neutron and x-ray scattering data. The analysis of the longitudinal and transverse current spectra allows to discriminate between opposite interpretations of the existing experimental data in favour of the propagating nature of the high frequency sound waves.Comment: 4 pages, Revtex, 4 ps figures; to be published in Phys. Rev. Lett., February 198

The D+H2(v=1,j)→HD(v′,j′)+H reaction. A detailed quasiclassical trajectory study

Thorough quasiclassical trajectory (QCT) calculations have been carried out for the D+H2(v =1,j) exchange reaction. These calculations include integral and differential cross sections, rate constants, reaction probabilities as a function of total energy, opacity functions, and distributions of internal states of the HD product in the range of collision energies from the reaction threshold to 1.5 eV and initial j values from 0 to 12. An overall good agreement with some discrepancies is found between the present QCT results and those from experiments and accurate quantum-mechanical calculations. © 1994 American Institute of Physics.German-Spanish scientific exchange program >Acciones Integradas HispanoAlemanas,> under Project No. HA-063. Financial support by the DGICYT under Project No. PB92-0219-C03.Peer Reviewe

Fragility and compressibility at the glass transition

Isothermal compressibilities and Brillouin sound velocities from the literature allow to separate the compressibility at the glass transition into a high-frequency vibrational and a low-frequency relaxational part. Their ratio shows the linear fragility relation discovered by x-ray Brillouin scattering [1], though the data bend away from the line at higher fragilities. Using the concept of constrained degrees of freedom, one can show that the vibrational part follows the fragility-independent Lindemann criterion; the fragility dependence seems to stem from the relaxational part. The physical meaning of this finding is discussed. [1] T. Scopigno, G. Ruocco, F. Sette and G. Monaco, Science 302, 849 (2003)Comment: 4 pages, 2 figures, 2 tables, 33 references. Slightly changed after refereein

Phonons from neutron powder diffraction

The spherically averaged structure function \soq obtained from pulsed neutron powder diffraction contains both elastic and inelastic scattering via an integral over energy. The Fourier transformation of \soq to real space, as is done in the pair density function (PDF) analysis, regularizes the data, i.e. it accentuates the diffuse scattering. We present a technique which enables the extraction of off-center phonon information from powder diffraction experiments by comparing the experimental PDF with theoretical calculations based on standard interatomic potentials and the crystal symmetry. This procedure (dynamics from powder diffraction(DPD)) has been successfully implemented for two systems, a simple metal, fcc Ni, and an ionic crystal, CaF$_{2}$. Although computationally intensive, this data analysis allows for a phonon based modeling of the PDF, and additionally provides off-center phonon information from powder neutron diffraction

Dielectric and thermal relaxation in the energy landscape

We derive an energy landscape interpretation of dielectric relaxation times in undercooled liquids, comparing it to the traditional Debye and Gemant-DiMarzio-Bishop pictures. The interaction between different local structural rearrangements in the energy landscape explains qualitatively the recently observed splitting of the flow process into an initial and a final stage. The initial mechanical relaxation stage is attributed to hopping processes, the final thermal or structural relaxation stage to the decay of the local double-well potentials. The energy landscape concept provides an explanation for the equality of thermal and dielectric relaxation times. The equality itself is once more demonstrated on the basis of literature data for salol.Comment: 7 pages, 3 figures, 41 references, Workshop Disordered Systems, Molveno 2006, submitted to Philosophical Magazin

Observation of Umklapp processes in non-crystalline materials

Umklapp processes are known to exist in cristalline materials, where they control important properties such as thermal conductivity, heat capacity and electrical conductivity. In this work we report the provocative observation of Umklapp processes in a non-periodical system, namely liquid Lithium. The lack of a well defined periodicity seems then not to prevent the existence of these scattering processes mechanisms provided that the local order of the systems i.e. the maxima of the static structure factor supply the equivalent of a reciprocal lattice vector in the case of cristalline materials.Comment: 13 pages P

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

The Raman coupling function in amorphous silica and the nature of the long wavelength excitations in disordered systems

New Raman and incoherent neutron scattering data at various temperatures and molecular dynamic simulations in amorphous silica, are compared to obtain the Raman coupling coefficient $C(\omega)$ and, in particular, its low frequency limit. This study indicates that in the $\omega \to 0$ limit $C(\omega)$ extrapolates to a non vanishing value, giving important indications on the characteristics of the vibrational modes in disordered materials; in particular our results indicate that even in the limit of very long wavelength the local disorder implies non-regular local atomic displacements.Comment: Revtex, 4 ps figure

Some Finite Size Effects in Simulations of Glass Dynamics

We present the results of a molecular dynamics computer simulation in which we investigate the dynamics of silica. By considering different system sizes, we show that in simulations of the dynamics of this strong glass former surprisingly large finite size effects are present. In particular we demonstrate that the relaxation times of the incoherent intermediate scattering function and the time dependence of the mean squared displacement are affected by such finite size effects. By compressing the system to high densities, we transform it to a fragile glass former and find that for that system these types of finite size effects are much weaker.Comment: 12 pages of RevTex, 4 postscript figures available from W. Ko

Crystal-like high frequency phonons in the amorphous phases of solid water

The high frequency dynamics of low- (LDA) and high-density amorphous-ice (HDA) and of cubic ice (I_c) has been measured by inelastic X-ray Scattering (IXS) in the 1-15 nm^{-1} momentum transfer (Q) range. Sharp phonon-like excitations are observed, and the longitudinal acoustic branch is identified up to Q = 8nm^{-1} in LDA and I_c and up to 5nm^{-1} in HDA. The narrow width of these excitations is in sharp contrast with the broad features observed in all amorphous systems studied so far. The "crystal-like" behavior of amorphous ices, therefore, implies a considerable reduction in the number of decay channels available to sound-like excitations which is assimilated to low local disorder.Comment: 4 pages, 3 figure