Dispersive phonon linewidths: the E2 phonons of ZnO

Phonon linewidths can exhibit a large variation when either pressure or isotopic masses are changed. These effects yield detailed information about the mechanisms responsible for linewidths and lifetimes, e.g., anharmonicity or isotopic disorder. We report Raman measurements of the linewidth of the upper E2 phonons of ZnO crystals with several isotopic compositions and their dependence on pressure. Changes by a factor of 12 are observed at a given temperature. Comparison with calculated densities of one-phonon states, responsible for isotope scattering, and of two-phonon states, responsible for anharmonic decay, yields a consistent picture of these phenomena. Isotopic disorder broadening by 7 cm(-1) is found in samples with mixed 16O-18O content, whereas the anharmonic processes involve decay into sums and differences of two phonons.     

Phonon confinement and substitutional disorder in Cd1−xZnxS nanocrystals

1‐longitudinal optical (LO) phonons in free‐standing mixed Cd_1−xZn_xS nanocrystals, synthesized using chemical precipitation, are investigated using Raman spectroscopy. As expected for the nanocrystals, the 1‐LO modes are found to appear at slightly lower wavenumbers than those in the bulk mixed crystals and exhibit one‐mode behavior. On the other hand, the line broadening is found to be much more than that can be accounted on the basis of phonon confinement. From the detailed line‐shape analysis it turns out that the substitutional disorder in the mixed crystals contributes much more to the line broadening than the phonon confinement. The linewidth arising from these mechanisms are also extracted from the analysis. Copyright © 2009 John Wiley & Sons, Ltd.     

Normal phonon-phonon scattering processes and the thermal conductivity of germanium crystals with isotope disorder

The influence of the normal phonon-phonon scattering processes on the thermal conductivity was theoretically studied for germanium crystals with various degrees of the isotope disorder. The theory takes into account redistribution of the phonon momentum in the normal scattering processes both inside each oscillation branch (Simons mechanism) and between various phonon oscillation branches (Herring mechanism). Contributions to the thermal conductivity due to the drift mobility of the longitudinal and transverse phonons are analyzed. It is shown that the momentum redistribution between longitudinal and transverse phonons according to the Herring relaxation mechanism leads to a significant suppression of the drift motions (and to the corresponding drop in contribution to the thermal conductivity) of the longitudinal phonons in isotopically pure germanium crystals. The results of the thermal conductivity calculations involving the Herring relaxation mechanism agree well with the experimental data available for germanium crystals with various degrees of the isotope disorder.     

Decoherence of excitons in multichromophore systems: thermal line broadening and destruction of superradiant emission

We study the temperature-dependent dephasing rate of excitons in chains of chromophores, accounting for scattering on static disorder as well as acoustic phonons in the host matrix. From this we find a power-law temperature dependence of the absorption linewidth, in excellent quantitative agreement with experiments on dye aggregates. We also propose a relation between the linewidth and the exciton coherence length imposed by the phonons. The results indicate that the much debated steep rise of the fluorescence lifetime of pseudoisocyanine aggregates above 40 K results from the fact that this coherence length drops below the localization length imposed by static disorder.     

High-temperature slow relaxation of the magnetization in Ni10 magnetic molecules

We investigate a family of molecular crystals containing noninteracting Ni10 magnetic molecules. We find slow relaxation of the magnetization below a temperature as high as 17 K and we show that this behavior is not associated with an anisotropy energy barrier. Ni10 has a characteristic magnetic energy spectrum structured in dense bands, the lowest of which makes the crystal opaque to phonons of energy below about 1 meV. We ascribe the nonequilibrium behavior to the resulting resonant trapping of these low-energy phonons. Trapping breaks up spin relaxation paths leading to a novel kind of slow magnetic dynamics which occurs in the lack of anisotropy, magnetic interactions and quenched disorder.     

The effect of normal phonon-phonon scattering processes on the maximum thermal conductivity of isotopically pure silicon crystals

The effect of normal phonon-phonon scattering processes on the thermal conductivity of silicon crystals with various degrees of isotope disorder is considered. The redistribution of phonon momentum in normal scattering processes is taken into account within each oscillation branch (the Callaway generalized model), as well as between different oscillation branches of the phonon spectrum (the Herring mechanism). The values of the parameters are obtained that determine the phonon momentum relaxation in anharmonic scattering processes. The contributions of the drift motion of longitudinal and transverse phonons to the thermal conductivity are analyzed. It is shown that the momentum redistribution between longitudinal and transverse phonons in the Herring relaxation model represents an efficient mechanism that limits the maximum thermal conductivity in isotopically pure silicon crystals. The dependence of the maximum thermal conductivity on the degree of isotope disorder is calculated. The maximum thermal conductivity of isotopically pure silicon crystals is estimated for two variants of phonon momentum relaxation in normal phonon-phonon scattering processes.     

Magnetostriktive Erzeugung transversaler Phononen im 10 GHz-Bereich unter Vermeidung eines äußeren Magnetfeldes

To generate transverse microwave phonons in nonpiezoelectric crystals one has to use ferromagnetic filmtransducers. This method needs a static magnetic field of some kOe. It is shown in this paper that it is possible to shift the resonance field to lower values by applying mechanical stress to the ferromagnetic film. Due to the broad linewidth even at zero field transverse phonons are generated. The measured conversion factor for generation and detection is ?50 dB each which is comparable with values by other methods. The conversion factor depends strongly on the conditions during evaporation of the film.     

Anisotropic attenuation of transverse ultrasound in cubic crystals of Ge,Si, and diamond with various isotopic compositions

The attenuation of transverse ultrasound in germanium, silicon, and diamond crystals is considered with allowance for competing isotopic and anharmonic scattering processes. The dependence of the attenuation of transverse ultrasound on the direction of the wave vector of quasi-transverse phonons is analyzed within an anisotropic continuum model. The Landau—Rumer mechanism is considered for anharmonic scattering processes. Given the second-and third-order elastic moduli, the parameters are found determining ultrasonic absorption in the above crystals with various degrees of isotopic disorder. The attenuation coefficients of transverse ultrasound associated with isotopic and anharmonic scattering processes are shown to have qualitatively different angular dependences. Therefore, from studying the anisotropic attenuation of ultrasound in cubic crystals, one can determine the dominant mechanism of ultrasonic absorption in isotopically modified crystals.     

Theorie des stimulierten Raman-Effekts

We consider stimulated Raman emission in solids, placed in a plane laser beam external to the cavity. The Hamiltonian of the system of phonons, electrons and electromagnetic fields is derived within the framework of a generalized adiabatic approximation for electrons and nuclei. It contains terms due to nonlinear interactions between electrons and phonons. Because the usual time-dependent perturbation theory cannot describe coherence effects properly we turn toHeisenberg's equations of motion for the operators of photons, phonons and electron excitations. In order to solve these equations in the steady state we apply an iteration procedure. We start with the light waves which give rise to electron transitions. The electrons such excited create phonons which then react on the electrons. Finally the electrons are coupled again to the lightfield. This procedure yields besides the usual wellknown Raman process two main processes occurring in stimulated Raman emission: a coupled two step Raman process and a parametric process. In the first one two phonons are involved. If the linewidth of phonons is comparable to the phonon frequencies the non-resonant parts of the above processes also become important. In solving the set of coupled equations for the light amplitudes, obtained from the iteration procedure, we only consider terms due to the first Stokes, the first anti-Stokes and the laser line. We then find frequency shifts of these lines due to the stimulated emission which are of the order of the linewidth of photons if this linewidth is very much smaller than that of phonons as it is the case in solids. This means that the coupled two step Raman process is dominant, in good agreement with measurements ofChiao andStoicheff in calcite.     

Raman scattering from crystalline and amorphous (GaSb)1-xGex semiconducting films

The first reported Raman scattering experiments have been performed on single crystal and amorphous films of the metastable alloy (GaSb)_1-xGe_x with compositions across the pseudobinary phase diagram. In crystalline films, the optical phonons exhibit a “one-two” type mode behavior. Broadening and softening of the Raman peaks with increasing alloy concentrations are attributed to a relaxation of q-vector selection rules due to substitutional disorder on both the cation and anion sublattices. Additionally, disorder induced scattering from the zone-edge acoustic phonons was observed. In amorphous alloy films, the reduced Raman spectra were compared to the one-phonon densities of states of the end-member crystals. The resulting apparent lack of polarization dependence indicated that the amorphous films were of the random network type.     

Infrared absorption by zone edge lattice vibrations in mixed gallium indium phosphide

The combinations of zone edge phonons of mixed Ga_1?xIn_xP have been studied by means of infrared absorption, these crystals exhibit a one mode behavior for both the zone center and the zone edge phonons.     

The mechanism of Landau-Rumer relaxation of thermal and high-frequency phonons in cubic crystals of germanium,silicon, and diamond

Transverse phonon relaxation according to the Landau-Rumer mechanism is considered for an isotropic medium and crystals of germanium, silicon, and diamond possessing a cubic symmetry. The energy of elastic deformation caused by the anharmonicity of vibrations of the cubic crystal lattice is expressed via the second-and third-order moduli of elasticity. Using the known values of these elastic moduli, parameters determining the frequencies of the transverse phonon relaxation in the Landau-Rumer mechanism are evaluated for the germanium, silicon, and diamond crystals. It is shown that the dependence of the relaxation frequency on the wavevector of thermal and high-frequency phonons sharply differs from the classical Landau-Rumer relationship both in the isotropic medium and in the cubic crystals. It is established that the observed peculiarities in the relaxation frequency are related to the angular dependence of the probability of anharmonic scattering and the anisotropy of elastic properties of the germanium, silicon, and diamond crystals. A new method is proposed for the experimental determination of the relaxation frequency of high-frequency phonons as a function of the wavevector using the temperature dependence of the coefficient of absorption of high-frequency ultrasound.     

Anharmonic processes of scattering and relaxation of slow quasi-transverse phonons in cubic crystals

Relaxation of slow quasi-transverse phonons in anharmonic processes of scattering in cubic crystals with positive (Ge, Si, diamond) and negative (KCl, NaCl) anisotropies of the second-order elastic moduli has been considered. The dependences of the relaxation rates on the direction of the wave vector of phonons in scattering processes with the participation of three quasi-transverse phonons (the TTT relaxation mechanisms) are analyzed within the anisotropic continuum model. It is shown that the TTT relaxation mechanisms in crystals are associated with their cubic anisotropy, which is responsible for the interaction between noncollinear phonons. The dominant contribution to the phonon relaxation comes from large-angle scattering. For crystals with significant anisotropy of the elastic energy (Ge, Si, KCl, NaCl), the total contribution of the TTT relaxation mechanisms to the total relaxation rate exceeds the contribution of the Landau-Rumer mechanism either by several factors or by one to two orders of magnitude depending on the direction. The dominant role of the TTT relaxation mechanisms as compared to the Landau-Rumer mechanism is governed, to a considerable extent, by the second-order elastic moduli. The total relaxation rates of slow quasi-transverse phonons are determined. It is demonstrated that, when the anharmonic processes of scattering play the dominant role, the inclusion of one of the relaxation mechanisms (the Landau-Rumer mechanism or the mechanisms of relaxation of the slow quasi-transverse mode by two slow or two fast modes) is insufficient for describing the anisotropy of the total relaxation rates in cubic crystals.     

Ge_xSi_(1-x)/Si超晶格中周期不均匀对折叠声学声子拉曼线宽的影响

本文报导了在 Ge_Si_(1-x)/Si 超晶格中观察到了超晶格周期不均匀导致的折叠声学声子拉曼谱线展宽,这种谱线展宽与折叠指数(m)有关,折叠声学声子的谱线越宽,m 相同的折叠声学声子具有相同的线宽。     

Elastic waves and the Landau-Rumer mechanism of relaxation of quasi-transverse phonons in GaAs crystals

The dependences of the relaxation rate and the absorption coefficient of ultrasound in GaAs crystals on the direction of the wave vector of quasi-transverse phonons for the Landau-Rumer mechanism are analyzed in the framework of the anisotropic-continuum model. The calculations are performed with two sets of second-order and third-order elastic moduli experimentally measured by different authors. It is demonstrated that the angular dependences of the relaxation rates of quasi-transverse phonons and the ultrasonic absorption coefficients calculated from these data differ qualitatively. The correctness of the determination of the third-order elastic moduli available in the literature can be checked by measuring the ultrasonic absorption coefficients for GaAs crystals.     

Long-range order in quasi-one-dimensional conductors

We study the formation of the charge-density wave long-range order in a system of repulsive 1D electrons coupled to 3D phonons. We show that the charge-density wave can be stabilized by interaction with phonons in quasi-1D crystals and semiconducting nanowires. In the case of metallic atomic chains, interaction with phonons of a 3D substrate is not enough, and violation of the translational invariance by commensurable perturbation or disorder is needed. The possibility of stabilization of superconductivity in 1D electrons with attraction by means of tunnel coupling to a 3D metal is considered.     

Effect of the local coulomb interaction of strongly correlated electrons on phonon, elastic, and electronic properties of ZnSe crystals

The dispersions and densities of states of phonons in cubic ZnSe crystals have been calculated and the modification of these quantities with inclusion of the local Coulomb interaction U of strongly correlated 3d(Zn) electrons has been investigated. It has been found that the inclusion of U leads to a decrease in the frequencies of optical and longitudinal acoustic phonons and to an increase in the frequencies of transverse acoustic phonons in the entire Brillouin zone. To explain these specific features in the behavior of phonons, the modifications of elastic moduli and electron density of states with inclusion of U have been analyzed.     

Momentum-resolved electron-phonon interaction in lead determined by neutron resonance spin-echo spectroscopy

Neutron resonance spin-echo spectroscopy was used to monitor the temperature evolution of the linewidths of transverse acoustic phonons in lead across the superconducting transition temperature over an extended range of the Brillouin zone. For phonons with energies below the superconducting energy gap, a linewidth reduction of maximum amplitude was observed below . The electron-phonon contribution to the phonon lifetime extracted from these data is in satisfactory overall agreement with ab initio lattice-dynamical calculations, but significant deviations are found.     

Phase transition, order parameter, and their manifestation in optical spectra of Hg2Cl2

This paper reports on a high-precision study of the effects induced by the phase transition in Raman spectra of Hg₂Cl₂ crystals. The odd (acoustic and IR-active) phonons, including the soft modes, from the Brillouin zone (BZ) X points of the paraphase of these crystals, which are induced by the phase transition, unit cell doubling, and the X ?? ?? BZ folding, have been investigated both theoretically and experimentally. The temperature dependences of the intensities of these phonons, complemented by a theoretical analysis, have yielded the first information on the behavior of the transition order parameter. The corresponding critical exponents have been derived, which correlate in magnitude with the data obtained from X-ray diffraction measurements and, thus, imply the closeness of the phase transition in these crystals to the tricritical point.