Theoretical polarization dependence of the two-phonon double-resonant Raman spectra of graphene

The experimental Raman spectra of graphene exhibit a few intense two-phonon bands, whichare enhanced through double-resonant scattering processes. Though there are manytheoretical papers on this topic, none of them predicts the spectra within a single model.Here, we present results for the two-phonon Raman spectra of graphene calculated by meansof the quantum-mechanical perturbation theory. The electronic and phonon dispersions,electronic lifetime, electron-photon and electron-phonon matrix elements, are all obtainedwithin a density-functional-theory-based non-orthogonal tight-binding model. We studysystematically the overtone and combination two-phonon Raman bands, and, in particular,the energy and polarization dependence of their Raman shift and intensity. We find thatthe ratio of the integrated intensities for parallel and cross polarized light for alltwo-phonon bands is between 0.33 and 0.42. Our results are in good agreement with theavailable experimental data.     

Squeezed states in two-phonon devices

New variables called two-mode quadrature-phase amplitudes are used in order to analyze squeezing in two-phonon devices. The Fokker-Planck equation obtained for two-mode quasiprobability distributions presents a diffusion matrix independent of the non-linear coupling and with non-negative eigenvalues. Assuming that the initial state is a two-mode coherent state, the uncertainties in the two-mode quadrature-phase amplitudes have been obtained, and the dependence of squeezing in the non-linear coupling, the pumping phase and the modulation frequency has been studied.     

Possible two-phononβγ-vibration in 156Dy

The level structure of ¹⁵⁶Dy has been investigated with the (p, t) reaction at E_p = 29.9 MeV. A strong (7.7% of ground-state strength) transition is observed to a state at 1520 keV, assigned J^π = 2⁺. It is suggested that this state is the two-phonon βγ-vibration predicted by the theory of Davydov. Possible connections to the “super-band” in ¹⁵⁶Dy are discussed.     

On collective two-phonon states in deformed nuclei

The centroid energies of the two-phonon states in doubly even deformed nuclei are calculated within the quasiparticle-phonon nuclear model taking into account the Pauli principle in the two-phonon components of the wave functions. It is shown that the collective two-phonon energies are shifted by 1–2 MeV to higher energies due to the Pauli principle. A strong fragmentation of the two-phonon collective states over many nuclear levels occurs at the excitation energies of 3–4 MeV. It is concluded that the two-phonon states cannot exist in deformed nuclei. The analysis of the available experimental data on the two-phonon states shows that the experimental data do not contradict the results of these calculations.     

Temperature dependence of infrared spectra

A simple form of cell for the study of infrared absorption spectra at low and high temperatures is described. Preliminary results of a study of the temperature-phase dependence of fluorobenzene and m-toluic acid spectra are reported.     

Theory of two-phonon modes in layered charge-density-wave systems

A theoretical model with electron-phonon and anharmonic interactions is proposed to explain the two-phonon mode observed in the Raman spectra of layered transition metal dichalcogenides, which exhibit charge density wave (cdw) phase transition. The phonon self-energy, which involves the electron response function and the two-phonon Green’s function, is calculated using the double-time Green’s function formalism. It is shown that in these low-dimensional systems there exists an anharmonicity-mediated two-phonon mode in the phonon spectral function both in the normal and in thecdw phases. In the normal phase since the phonon Raman scattering proceeds through a single optic phonon the calculations are carried out for zero wave vector and hence the contribution of the electron response function to the self-energy vanishes. On the other hand explicit evaluation of the two-phonon Green’s function shows that the frequency of the two-phonon mode is twice that of the Kohn anomaly phonon and decreases with decreasing temperature. The strength of two-phonon peak is found to be comparable to that of the original optic phonon. In thecdw phase the phonon which enters into the Raman scattering is taken to be the one with thecdw wave vectorQ, which when zone-folded becomes equivalent to zero wave vector. The evaluation of the electron response function in this phase generates a phonon corresponding to thecdw-amplitude mode. The two-phonon Green’s function is assumed to be of similar form as in the normal phase. The spectral function evaluated at zero temperature shows a weak two-phonon peak besides the prominentcdw-amplitude mode. Numerical results are presented for the system 2H-NbSe₂ and are found to be in qualitative agreement with the experimental data.     

Bound-exciton cathodoluminescence in ZnSe crystals and two-phonon resonance

A study has been made of the cathodoluminescence of ZnSe crystals annealed in vacuum [ZnSe(Vac)], in vacuum and, subsequently, in antimony melt [(ZnSe(Vac)(Sb)], or in a zinc melt with subsequent annealing in antimony [ZnSe(Zn)(Sb)]. The emission of all samples contained the I ₁ ^s,d -nLO series. The LO-phonon replicas of the emission line I ₁ ^s observed in ZnSe(Vac) samples are accompanied by single-plasmon satellites. The plasmon energy determining the replica separation is ?ω_p?10 meV. The emission lines of ZnSe(Zn)(Sb) samples have the smallest half-width. We report the first observation of anomalous broadening of the zero-phonon line I ₁ ^s in ZnSe(Vac) samples caused by a high zinc vacancy content. A theory on the shape of the emission spectrum under two-phonon resonance is developed including bound-exciton interaction with mixed plasmon-phonon vibrational modes. It is shown that the splitting of the I ₁ ^d line at T?2 K may originate from resonance exciton-phonon interaction between exciton-impurity complexes.     

Theory of two-phonon absorption processes in liquid paraffins

Calculated absorption spectra are given for linear C₈H₁₈, C₁₀H₂₂, C₁₆H₃₄ and C₂₀H₄₂ chains, based on the assumption of a two-phonon absorption mechanism. In the present work the normal modes of vibration of different finite chains are computed directly, without recourse to the Pitzer sampling approximation and without the assumption of strict k-selection rules. The calculated spectra are found to be much more sensitive to chain length than the experimental spectra. A possible explanation of the relative insensitivity of the observed spectra is suggested in terms of a characteristic chain segment length common to all the chains. Ironically, the apparent importance of chain segmentation in the two-phonon absorption suggests that one-phonon transitions may also play a significant rôle in the absorption process.     

Fragmentation of the two-phonon γ-vibration in166Er

Two-phonon γ-vibrational states in¹⁶⁶Er have been populated using Coulomb excitation. The K^π=4⁺ component of the vibration appears to be fragmented over several states, whereas only one K^π=0⁺ state is observed.     

Lifetime of the two-phonon vibrational state in232Th

We report on a measurement of the lifetime of the 1414 keV state in²³²Th by the Doppler-shift recoil-distance method. This 4⁺ state shows all characteristics of a nearly-harmonic two-phonon-vibrational excitation. The result for the B(E2) value obtained from the lifetime,=3.2 ± 0.7 ps, is in agreement with an earlier estimate of the collectivity from Coulomb-excitation yields and supports the interpretation of the 1414 keV state as a two-phonon-vibrational excitation.We would like to thank the accelerator crew of the Max-Planck-Institut für Kernphysik for the excellent running conditions they maintain. We are also indebted to Dr. H.J. Maier, University Munich for supplying us with the²³²Th targets. This work was supported by the Bundesminister für Forschung und Technologie under contract numbers 06BN601 and 06HD5251.     

Temperature dependent peaks in secondary electron emission spectra

Peaks in the secondary emission spectra not associated with Auger effects have been observed in various metals (particularly copper and cobalt). These peaks are suppressed at elevated temperature and appear to have amplitudes which are unique functions of temperature. They are characteristic of well ordered, and, particularly, clean surfaces, and are interpreted in terms of the diffraction of the emitted secondary electrons.     

受激Raman谱中的宏观极化干涉

研究了Rb⁸⁵原子蒸气D1线系统中的受激Raman增益与损耗现象. 实验中观察到 随着抽运光失谐量的增大, 受激Raman谱明显地呈现出一个从增益到损耗的陡峭转变. 从缀饰态模型出发, 我们提出这是对探测光有相反贡献的不同速度原子群之间极化干涉的结果. 关键词： 受激Raman谱 电磁感应透明 极化干涉     

Relaxation effects in resonance Raman spectra

A density-matrix theory of resonance scattering spectroscopy is presented to characterize the relaxation processes which may be studied in these spectra. The distinction between Resonance Raman and Fluorescence emerges clearly from this treatment. It is shown that novel properties of the rotational and vibrational relaxation may be obtained from the lineshape of the scattered light. A new effect is discovered in the Resonance Raman excitation profile which, in principle, could be used to study the relaxation rate between specific vibronic levels of an excited electronic state.