This review covers a wide range of experimental and theoretical studies of two-level or tunnelling states in glasses. Emphasis is on fundamental physics rather than a detailed comparison of experiment and theory. Sections cover the static and dynamic properties of tunnelling states, their contribution to thermal properties and their response to weak and strong electric and acoustic fields, both steady state and pulsed. A section on metallic glasses focuses on the importance of electron tunnelling-state interactions, and a final section illustrates approaches to a microscopic description by means of selected examples.

https://iopscience.iop.org/article/10.1088/0034-4885/50/12/003/pdf

Two-level states in glasses

Amorphous metallic alloys, also called metallic glasses, are of considerable technological importance. The metastability of these systems, which gives rise to various rearrangement processes at elevated temperatures, calls for an understanding of their diffusional behavior. From the fundamental point of view, these metallic glasses are the paradigm of dense random packing. Since the recent discovery of bulk metallic glasses it has become possible to measure atomic diffusion in the supercooled liquid state and to study the dynamics of the liquid-to-glass transition in metallic systems. In the present article the authors review experimental results and computer simulations on diffusion in metallic glasses and supercooled melts. They consider in detail the experimental techniques, the temperature dependence of diffusion, effects of structural relaxation, the atom-size dependence, the pressure dependence, the isotope effect, diffusion under irradiation, and molecular-dynamics simulations. It is shown that diffusion in metallic glasses is significantly different from diffusion in crystalline metals and involves thermally activated, highly collective atomic processes. These processes appear to be closely related to low-frequency excitations. Similar thermally activated collective processes were also found to mediate diffusion in the supercooled liquid state well above the caloric glass transition temperature. This strongly supports the mode-coupling scenario of the glass transition, which predicts an arrest of liquidlike flow already at a critical temperature well above the caloric glass transition temperature.

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Diffusion in Metallic Glasses and Supercooled Melts

We take familiar inorganic oxide glasses and non-oxide glasses and the liquids from which they derive to review the current understanding of their atomic structure, ranging from the local environments of individual atoms to the long-range order which can cover many interatomic distances. The structural characteristics of important glasses and melts, like silicates, borates, alumino-silicates, halides and chalcogenides, are drawn from the results of recent spectroscopy and scattering experiments. The techniques include Nuclear Magnetic Resonance (NMR) and X-ray Absorption Fine Structure (XAFS), Neutron Scattering (NS) and Small- and Wide-angle X-ray Scattering measurements (SAXS/WAXS), and are often combined with computer simulation experiments in order to obtain detailed images of structure and diffusion in the glassy as well as in the molten state. We then review the current understanding of relaxation in glasses, liquids and polyamorphic states. This includes phenomenological models and theories of rela...

Inorganic glasses, glass-forming liquids and amorphizing solids

This article describes the advances that have been made over the past ten years on the problem of fracton excitations in fractal structures. The relevant systems to this subject are so numerous that focus is limited to a specific structure, the percolating network. Recent progress has followed three directions: scaling, numerical simulations, and experiment. In a happy coincidence, large-scale computations, especially those involving array processors, have become possible in recent years. Experimental techniques such as light- and neutron-scattering experiments have also been developed. Together, they form the basis for a review article useful as a guide to understanding these developments and for charting future research directions. In addition, new numerical simulation results for the dynamical properties of diluted antiferromagnets are presented and interpreted in terms of scaling arguments. The authors hope this article will bring the major advances and future issues facing this field into clearer focus, and will stimulate further research on the dynamical properties of random systems.

/pdf/dynamical-properties-of-fractal-networks-scaling-numerical-34gns79y2x.pdf

Dynamical properties of fractal networks: Scaling, numerical simulations, and physical realizations

Type-I clathrate compounds have attracted a great deal of interest in connection with the search for efficient thermoelectric materials. These compounds constitute networked cages consisting of nano-scale tetrakaidecahedrons (14 hedrons) and dodecahedrons (12 hedrons), in which the group 1 or 2 elements in the periodic table are encaged as the so-called rattling guest atom. It is remarkable that, though these compounds have crystalline cubic-structure, they exhibit glass-like phonon thermal conductivity over the whole temperature range depending on the states of rattling guest atoms in the tetrakaidecahedron. In addition, these compounds show unusual glass-like specific heats and THz-frequency phonon dynamics, providing a remarkable broad peak almost identical to those observed in topologically disordered amorphous materials or structural glasses, the so-called Boson peak. An efficient thermoelectric effect is realized in compounds showing these glass-like characteristics. This decade, a number of experimental works dealing with type-I clathrate compounds have been published. These are diffraction experiments, thermal and spectroscopic experiments in addition to those based on heat and electronic transport. These form the raw materials for this article based on advances this decade. The subject of this article involves interesting phenomena from the viewpoint of not only physics but also from the view point of the practical problem of elaborating efficient thermoelectric materials. This review presents a survey of a wide range of experimental investigations of type-I clathrate compounds, together with a review of theoretical interpretations of the peculiar thermal and dynamic properties observed in these materials.

/pdf/phonon-glass-electron-crystal-thermoelectric-clathrates-2jojtwpik8.pdf

Phonon-glass electron-crystal thermoelectric clathrates : Experiments and theory

Measurements of the elastic and inelastic neutron scattering from vitreous silica in the frequency range 0.3 to 4 THz and with scattering vectors in the range 0.2 to 5.3 A${\r{}}^{\mathrm{\ensuremath{-}}1}$ are analyzed in conjunction with heat-capacity measurements on the same samples to provide a microscopic description of low-frequency vibrational modes. The results show that additional harmonic excitations coexist with sound waves below 1 THz, and that these excitations correspond to relative rotation of ${\mathrm{SiO}}_{4}$ tetrahedra.

Low-frequency modes in vitreous silica

The vibrations in amorphous germanium between 160 GHz and 4 THz have been studied by inelastic neutron scattering. From the observed dynamic structure factor, one finds essentially sound waves at low frequencies and essentially bond bending modes akin to the crystalline TA zone boundary modes at 2 THz. In contrast to the crystalline case, these bond bending modes extend down to lower frequencies and coexist with the sound waves below 1 THz. The total vibrational density of states determined at 293 K is in good agreement with measured specific-heat data between 5 and 30 K.

Neutron scattering from low-frequency excitations in amorphous germanium

Inelastic neutron scattering from vitreous silica reveals that, in addition to the sound waves, there is a strong contribution from other vibrational modes in the frequency region above 150 GHz. From an analysis of their inelastic structure factor, we have put forward a simple model which can describe satisfactorily the measured data. The additional modes are identified as coupled rotations of SiO 4 tetrahedra and their density of states is determined on an absolute scale. The specific heat calculated from this density of states, in addition to the Debye term, is in good agreement with data in the literature. Some comments are made on the fracton interpretation of the vibrational density of states of amorphous solids.

M. Prager

Papers

Low-frequency modes in vitreous silica

Neutron scattering from low-frequency excitations in amorphous germanium

Low frequency excitations in vitreous silica