Raman scattering and the low-frequency vibrational spectrum of glasses

We present a theory of low-frequency Raman scattering in glasses, based on the concept that light couples to the elastic strains via spatially fluctuating elasto-optic (Pockels) constants. We show that the Raman intensity is not proportional to the vibrational density of states (as was widely believed), but to a convolution of Pockels constant correlation functions with the dynamic strain susceptibilities of the glass. Using the dynamic susceptibilities of a system with fluctuating elastic constants we are able for the first time to describe the Raman intensity and the anomalous vibration spectrum of a glass on the same footing. Good agreement between the theory and experiment for the Raman spectrum, the density of states, and the specific heat is demonstrated at the example of glassy As(2)S(3).     

Elementary excitations in vibrational nuclei

We propose to describe the entire collective spectrum of vibrational nuclei in terms of few enteracting elementary excitation modes. We discuss in detail the case in which only two elementary modes are important (the quadrupole d and the octupole f-bosons). We give explicit expressions for the energy levels and transition matrix elements.     

Investigation of laser-induced depth damage and scattering of light in crystals and glasses

Laser-induced depth damage to sapphire crystals and to various glasses is investigated. The influence of self-focusing on the laser damage process is studied. The conditions under which self-focusing influences the damage are clarified. The influence of various impurities on the optical endurance of ruby laser crystals is determined. The damage mechanism is initiated by various types of absorbing inclusions and defects; a correlation is found between the light scattering and the damage threshold. A new criterion based on light scattering is introduced for the purity of transparent dielectrics.Translated from Trudy Ordena Lenina Fizicheskogo Instituta im. P. N. Lebedeva, Vol. 101, pp. 31–74, 1978.     

Hyper-Raman scattering in the LiNbO3 crystal

The hyper-Raman spectra in non-centrosvmmetric LiNbO₃ crystal were obtained using the multichannel recording technique. The hyper-Raman cross-section and non-linear susceptibility for the 151 cm^-1 band were measured.     

Magnetic excitations in ferromagnetic semiconductors,and their study by light scattering

The magnetic excitation spectrum of degenerate ferromagnetic semiconductors, described by the s-f interaction model, is investigated by calculating various Green functions which provide the dynamic response of the system. In addition to the usual acoustic spin-wave mode, there are also an optical spin-wave branch and the Stoner-like continuum of excitations. Some estimates are made for the first order light scattering from ferrmagnetic semiconductors at low temperatures T?T_c.     

Propagating vibrational excitations in molecular chains

We investigate quantum dynamics of vibrational excitations in one-dimensional (1D) molecular chain. Our model includes nearest neighbor interaction between identical molecular sites and one impurity atom placed in the middle (n = 0). We show that upon exciting the impurity site, its excess energy for relatively long for molecular scales time up to 100 ps is not redistributed uniformly among all other degrees of freedom. On the contrary an excitation propagates along the chain, reflected from the chain ends, and quantum interference of these waves yields to recurrence cycles and echo phenomena. For a critical cycle number k _c , echo components of the neighboring cycles start to overlap, and eventually for k ≫ k _c dynamics looks like chaotic one. The critical cycle number k _c depends on the coupling strength 0 ≤ C ≤ 1 of the impurity site with its neighbors n = ±1. k _c achieves the maximum for C ² = 1/2. Our results are in qualitative agreement with experimental data on vibrational excitations in various (CH₂) _n molecular chains, and besides offer a way for loss-free energy transfer between separated in space reaction centers.     

Raman scattering by electron and phonon excitations in FeSi

The temperature evolution of Raman scattering by electron and phonon excitations in FeSi is studied within the range of 10–500 K. At low temperatures, the frequency dependence for the spectra of light scattered by electrons exhibits vanishing intensity in the range up to 500–600 cm^–1, which suggests the existence of an energy gap of about 70 meV. The calculations of the electronic excitation spectra based on the band structure determined using the LDA+DMFT technique (local electron density + dynamic mean field approximation) are in good agreement with the low-temperature experimental data and confirm that FeSi is a material with intermediate electron correlations. The changes in the shape of the electronic excitation spectrum and in the self-energy of optical phonons indicate a transition to the metallic state above 100 K. The analysis of experimental data demonstrates an appreciable decrease in the electron lifetime with the growth of temperature determining the (insulator–poor metal) transition.     

Controlling vibrational excitations in C60 by laser pulse durations

Two similar off-resonant ultrafast laser experiments in C60 have reported two different vibrational modes that dominate the relaxation process: one predicts the A(g) modes while the other the H(g) modes. A systematical simulation presented here reveals that this experimental discrepancy results from the laser pulse duration. The numerical results show that since each mode nu has a distinctive optimal duration tau(nu)(o), the A(g) modes are strongly suppressed for durations longer than 40 fs, while the H(g) modes start to grow. For the off-resonant and low-intensity excitations, the period Omega(o)(nu) of the dominant mode and tau(nu)(o) satisfy the relation Omega(o)(nu)/tau(nu)(o) approximately 3.4. By carefully scanning the laser frequencies and pulse durations, a comprehensive excitation diagram is constructed, which can be used to guide experiments to selectively excite the A(g) and H(g) modes in C60 by an ultrafast laser. Its potential impact is also discussed.     

Low energy excitations in spin glasses

We discuss the nature of excitations that govern the low temperature thermodynamic behaviour of spin glasses and propose that the spin glass state is a space-time dependent ground state of a system of interacting spins wherein rotational invariance is broken spontaneously.     

Light scattering by spin excitations in copper-oxide-based materials

In this paper we present a study of spin dynamics in CuO, Bi₂CuO₄and CuGeO₃single crystals using Raman spectroscopy. The measurements of polarized Raman scattering spectra are performed in the temperature region from 10 to 300 K in various frequency ranges. We found and assigned the lines in the spectra that belong to magnetically ordered phases. The origin of these excitations, based on the temperature dependence of their energies, linewidths and symmetry arguments, is given. Also, we present calculations of two-magnon intensities, based on the densities of states, and compare them with experimental data.     

Transient stimulated raman scattering in crystals during motion of populations of vibrational states

Transient stimulated Raman scattering (SRS) in crystals is analyzed taking into account the motion of populations of vibrational states under the action of subpicosecond (shorter than the dephasing time) pump pulses. Analytic expressions describing the dynamics of excitation of vibrations in SRS are derived. It is found that for a small wavelength of SRS interaction and high intensities of pump radiation observed for femtosecond SRS in crystals, avalanche excitation of vibrations can be responsible for SRS suppression. It is shown that when phase matching of Stokes-anti-Stokes parametric coupling in transient SRS is ensured, it is possible to elevate the efficiency of frequency conversion under conditions of motion of populations of vibrational states; this explains recent successful results in the experimental implementation of femtosecond SRS in crystals pumped by a Bessel beam.     

Variety of vibrational excitations in 228Th

The level structure of ²²⁸Th was studied using mass-separated ²²⁸Pa sources and a γ - γ coincidence setup of 5 Compton suppressed Ge detectors. The complete octupole quadruplet, three excited K ^π = 0⁺ bands and two excited K ^π = 2⁺ bands were identified at excitation energies elow 1.4 MeV.     

Evolution of vibrational excitations in glassy systems

The equations of the mode-coupling theory (MCT) for ideal liquid-glass transitions are used for a discussion of the evolution of the density-fluctuation spectra of glass-forming systems for frequencies within the dynamical window between the band of high-frequency motion and the band of low-frequency-structural-relaxation processes. It is shown that the strong interaction between density fluctuations with microscopic wavelength and the arrested glass structure causes an anomalous-oscillation peak, which exhibits the properties of the so-called boson peak. It produces an elastic modulus which governs the hybridization of density fluctuations of mesoscopic wavelength with the boson-peak oscillations. This leads to the existence of high-frequency sound with properties as found by x-ray-scattering spectroscopy of glasses and glassy liquids. The results of the theory are demonstrated for a model of the hard-sphere system. It is also derived that certain schematic MCT models, whose spectra for the stiff-glass states can be expressed by elementary formulas, provide reasonable approximations for the solutions of the general MCT equations.