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Register a new userHarmonic Vibrational Excitations in Disordered Solids and the Boson Peak
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We consider a system of coupled classical harmonic oscillators with spatially fluctuating nearest-neighbor force constants on a simple cubic lattice. The model is solved both by numerically diagonalizing the Hamiltonian and by applying the single-bond coherent potential approximation. The results for the density of states $g(omega)$ are in excellent agreement with each other. As the degree of disorder is increased the system becomes unstable due to the presence of negative force constants. If the system is near the borderline of stability a low-frequency peak appears in the reduced density of states $g(omega)/omega^2$ as a precursor of the instability. We argue that this peak is the analogon of the boson peak, observed in structural glasses. By means of the level distance statistics we show that the peak is not associated with localized states.
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We study a disordered vibrational model system, where the spring constants k are chosen from a distribution P(k) ~ 1/k above a cut-off value k_min > 0. We can motivate this distribution by the presence of free volume in glassy materials. We show that the model system reproduces several important features of the boson peak in real glasses: (i) a low-frequency excess contribution to the Debye density of states, (ii) the hump of the specific heat c_V(T) including the power-law relation between height and position of the hump, and (iii) the transition to localized modes well above the boson peak frequency.
We show that a {em vibrational instability} of the spectrum of weakly interacting quasi-local harmonic modes creates the maximum in the inelastic scattering intensity in glasses, the Boson peak. The instability, limited by anharmonicity, causes a complete reconstruction of the vibrational density of states (DOS) below some frequency $omega_c$, proportional to the strength of interaction. The DOS of the new {em harmonic modes} is independent of the actual value of the anharmonicity. It is a universal function of frequency depending on a single parameter -- the Boson peak frequency, $omega_b$ which is a function of interaction strength. The excess of the DOS over the Debye value is $proptoomega^4$ at low frequencies and linear in $omega$ in the interval $omega_b ll omega ll omega_c$. Our results are in an excellent agreement with recent experimental studies.
We present a random matrix approach to study general vibrational properties of stable amorphous solids with translational invariance using the correlated Wishart ensemble. Within this approach, both analytical and numerical methods can be applied. Using the random matrix theory, we found the analytical form of the vibrational density of states and the dynamical structure factor. We demonstrate the presence of the Ioffe-Regel crossover between low-frequency propagating phonons and diffusons at higher frequencies. The reduced vibrational density of states shows the boson peak, which frequency is close to the Ioffe-Regel crossover. We also present a simple numerical random matrix model with finite interaction radius, which properties rapidly converges to the analytical results with increasing the interaction radius. For fine interaction radius, the numerical model demonstrates the presence of the quasilocalized vibrations with a power-law low-frequency density of states.
Disordered systems exhibit universal excitation, referred to as the boson peak, in the terahertz region. Meanwhile, the so-called fracton is expected to appear in the nanoscale region owing to the self-similar structure of monomers in polymeric glasses. We demonstrate that such excitations can be detected using terahertz spectroscopy. For the interaction between terahertz light and the vibrational density of states of the fractal structure, we formulate an infrared light-vibration coupling coefficient for the fracton region. Accordingly, we show that information concerning fractal and fracton dimensions appears in the exponent of the absorption coefficient. Finally, using terahertz time-domain spectroscopy and low-frequency Raman scattering, we experimentally observe these universal excitations in a protein lysozyme system that has an intrinsically disordered and self-similar nature in a single supramolecule. These findings are applicable to disordered and polymeric glasses in general and will be key to understanding universal dynamics of disordered systems by terahertz light.
Glasses have a large excess of low-frequency vibrational modes in comparison with continuous elastic body, the so-called Boson Peak, which appears to correlate with several crucial properties of glasses, such as transport or fragility. I review recent results showing that the Boson Peak is a necessary consequence of the weak connectivity of the solid. I explain why in assemblies repulsive spheres the boson peak shifts up to zero frequency as the pressure is lowered toward the jamming threshold, and derive the corresponding exponent. I show how these ideas capture the main low-frequency features of the vibrational spectrum of amorphous silica. These results extend arguments of Phillips on the presence of floppy modes in under-constrained covalent networks to glasses where the covalent network is rigid, or when interactions are purely radial.
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