Raman spectra of single-crystal C60

We have analysed the Raman spectra of C₆₀ single crystals between room temperature and 10K and studied the temperature-induced phase transition in this material. The spectra show crystal field splitting of the internal Raman modes but no evidence for a line shift near the phase transition. The photo-induced transformation of the crystals and its implication on the interpretation of the Raman spectra is discussed. In the low temperature phase we observed two lines at 30 cm^–1 and 41 cm^–1 which we assign to the librational modes of the crystal.     

Study of vibrational spectra of lanthanum sulphate nonahydrate at different temperatures in the region from 4000–50 cm−1

Infrared spectra of lanthanum sulphate nonahydrate are studied over the 4000–50 cm⁻¹ range. The bands pertaining to different internal and external modes of sulphate ion and water molecules are observed and assigned. It is shown that coordinated water molecules exist at two site symmetries C₁ and C_i, which provides confirmation of crystallographic data. Lattice water is not found in these crystals. The effect of low temperature on librational modes of coordinated water and their lattice vibrations are studied in the 550–50 cm⁻¹ region. The potential force field constants are calculated for rocking, wagging and twisting librational modes of water at 290 K, 80 K and 60 K. The higher value of the potential constant for the rocking mode from the wagging librational mode shows the in-plane bend of the hydrogen bond in lanthanum sulphate crystals.     

Normal vibrational modes in benzil crystals

A group-theoretical analysis of the vibrational spectrum of benzil crystals was carried out. The selection rules and normal coordinates were found. Raman scattering spectra of benzil single crystals were studied in polarized light within a broad temperature range from 100 K to the melting point (T _m=96°C). The experimental data were found to correlate with theory. The temperature dependences of the spectral-line half-widths were used to separate the observed vibrations into translational and librational modes, and the correspondence between the experimentally observed vibrations and their normal coordinates was established in some cases.     

Anharmonic self energy shift of a librational mode

A sizable anharmonic self energy shift of the Raman active librational modes in KN₃ has been found and shown to be a linear function of temperature above the Debye characteristic temperature of the solid (ca. 351°K). The Grüneisen parameter for the librational mode is estimated from the data to be 1.40. The Raman active mode involving the translation of the K⁺ ion shows a negligibly small anharmonic shift.     

Lattice modes of the chirally pure and racemic phases of tyrosine crystals

High-Q librational modes have been found to be present in the infrared absorption and Raman spectra of chirally pure L-tyrosine. Such modes can serve as terahertz radiation detectors and generators in chirally pure biostructures.     

负膨胀材料Zn(CN)_2和Cd(CN)_2的晶格振动分析

运用群论理论对负膨胀系数材料Zn(CN)2和Cd(CN)2的晶格振动进行了对称性分类,利用第一性原理密度泛函理论计算了它们布里渊区中心点的声子频率和Grüneisen参数,根据计算得到的各个模式所对应的本征矢对各个振动模式进行了指认,根据各模式Grüneisen参数讨论了负膨胀机理。在11个光学振动模式中,一个属于Zn/Cd原子的晶格振动模,位于223 cm-1/154 cm-1;5个属于C≡N刚性单元平移振动模;3个属于C≡N刚性单元天平动;2个属于C≡N刚性单元内振动。有7个振动模为拉曼活性,4个振动模为红外活性,两个振动模红外和拉曼均为非活性。C≡N刚性单元的3个低频平移振动模和全部天平动模的Grüneisen参数为负,对负热膨胀的产生有贡献,振动频率为47 cm-1的平移振动模具有最大的负Grüneisen参数,对负膨胀贡献最大。     

Raman study of squaric acid

Raman spectra of squaric acid have been measured at various temperatures below and above the transition temperature. Six low frequency bands below 300 cm^?1 are assigned to translational and librational modes of the squaric molecule on the basis of the recent crystal determination by X-ray diffraction. A discussion is given of the striking temperature dependence of these external modes in the ordered phase in connection with the phase transition.     

Raman scattering from the molecular charge transfer crystal anthracene-PMDA

The Raman spectrum of the mixed stack charge transfer (CT) crystal anthracene-PMDA, has been measured in the wavelength region near the lowest CT transition at 5458 Å. Six low frequency modes are observed below 140 cm^?1, the mode at 130 cm^?1 showing strong resonance enhancement. These modes are assigned as librational motion of the anthracene and PMDA molecules by rigid body analysis of X-ray structural data.     

Rotational barrier height for diatomic molecular impurities in alkali halides

A general expression for the coupling constants according to Devonshire's model for the hindered rotation of diatomic molecules in cubic crystals is derived. The treatment is confined to alkali halides with polarizable point ions. The results are applied to the librational modes of OH^? and OD^? impurities in KCl-, KBr- and KI-lattices.     

Vibrational and calorimetric study of polymorphism in 2-fluoro and 2-chloronaphtalene—nature of disorder

The heat capacity of 2-chloro and 2-fluoronaphtalene has been measured from 4.2 K to 300 K. Two solid-solid transitions are found for 2-chloronaphtalene, one only for 2-fluoronaphtalene. Far IR and Raman spectra of single crystals have been recorded. The phase stable below the melting point, phase I, is disordered in each case. Short range order, similar to the order of phase II of 2-chloronaphtalene is found in phase I of both compounds; it yields a local symmetry different from the average one obtained from X-ray measurements. In these phases I a librational mode is overdamped.     

Elemental sulfur under high hydrostatic pressure. An up-to-date Raman study

We report a high pressure Raman study of orthorhombic elemental sulfur from ambient pressure to ～ 25 GPa. Using a near infrared laser and low laser intensity on the scattering volume, we achieve off-resonant conditions up to larger pressures in comparison with previous studies. Raman spectra were recorded over the full spectral range including external (librational, translational) and internal (bond bending and bond stretching) modes. Drastic changes are observed as regards the peak frequencies, relative intensities and band splitting of degenerate modes. The main outcome of the present study is the observation of a “structural” transition at ～ 16 GPa manifested as slope changes of certain frequencies and sudden relative intensities changes. The present findings are discussed in the context of previous pressure Raman studies and comparison with existing X-ray diffraction as well as ab initio molecular dynamics results is attempted.     

Raman Spectrum Study on the Doping Effect in LiNbO3: MgO Crystals

Raman spectra of LiNbO₃: MgO crystals have been obtained and compared with Raman spectra of pure LiNbO₃ crystals. For both of the two kinds of Raman active modes (4A₁+9E), no changes of the numbers, frequency-shifts, and relative intensities of the Raman spectral lines are found. However, it is observed that some modes coupled to each other at room temperature. The observed modes coupling phenomena, disappeared at low temperature. It is shown from these results that the Raman spectral lines of A₁ (TO) and E (TO) vibrational modes are mainly determined by the (NbO₆) oxygen octahedra characteristic groups of LiNbO₃ crystals.     

Raman evidence of librational fluctuations in KNCS phase transition

A marked divergence of the line width of the Raman spectra of the librational modes of the NCS^- ion is observed in KNCS as the temperature is raised through the transition temperature. The effect is attributed to the onset of fluctuations of the orientation of the NCS^- ion between two energetically equivalent positions.     

Features of the structure and dynamics of Me1−x (NH4) x SCN (Me = K, Rb) mixed crystals

Neutron scattering is used to study the structure and dynamics of Me_{1 − x} (NH₄) _x SCN (Me = K, Rb) mixed crystals along the concentration section of 0.0 < x < 1.0 at room temperature 10 and 290 K. Phase transitions in Me_{1 − x} (NH₄) _x SCN mixed crystals are analyzed by neutron powder diffraction. The measured spectra of inelastic incoherent neutron scattering from mixed crystals in a concentration range of 0.0 < x < 1.0 at 10 are transformed into the generalized phonon density of states G(E) in the one-phonon incoherent approximation. Using G(E), we determine the changes in ammonium ion dynamics during phase transitions. Low energy resonance and local translational (two bands) and librational (two bands) modes are observed in the disordered rhombic phase at 10 K. The low energy resonance mode is not found in the ordered monoclinic phase at 10 K, though the local translational mode in the form of two bands and the local librational mode in the form of four bands are present there. The low energy resonance mode appears due to hybridization of the phonon spectrum of the host crystal with rotational tunneling modes of the split librational ground state of the impurity’s molecular ammonium ion.     

Hydrogen local vibrational modes in zinc oxide

Using Raman backscattering spectroscopy we have observed six local vibrational modes in as-grown state-of-the-art nominally undoped zinc oxide single crystals. The local vibrational modes are located at nu=2854, 2890, 2918, 2948, 2988, and 3096 cm(-1). Some specimens were annealed up to 950 degrees C to remove hydrogen. A subsequent Raman backscattering measurement revealed that the local vibrational modes disappeared. This establishes that the observed local vibrational modes are caused by the presence of hydrogen in the ZnO crystals.     

Raman spectra of undoped and uranium doped CaF2 single crystals

Raman scattering experiments for nominally pure and uranium doped CaF2 single crystals were presented.In all crystals, the Raman active T2g vibration mode of CaF2 was observed, whose frequency shift and fullwidth at half-maximum (FWHM) broadening correspond well with defects and impurities in CaF2 lattice.Additional Raman peaks develop in nominally pure CaF2 with high etch pits density and U6+:CaF2crystals. Part of additional Raman peaks in the experimental results, which are assumed due to vibration modes from F- interstitials and vacancies, are in well agreement with the theoretical predications by employing the Green-function formulation.     

Optical phonons in Rb<Subscript>2</Subscript>TeBr<Subscript>6</Subscript> and Cs<Subscript>2</Subscript>TeBr<Subscript>6</Subscript> crystals

Raman scattering in Rb₂TeBr₆ and Cs₂TeBr₆ crystals is studied. The phonon spectra of the crystals are calculated using the factor group method. The number of Raman-active modes, their symmetries, and selection rules are found. Observed Raman spectrum lines are identified with atomic vibration modes of the crystal.     

Light scattering spectra of guided wave polaritons in thin crystals: Experiment

Guided wave polaritons (GWP) of thin crystals have been studied by near- forward Raman scattering experiments on GaP crystals of ≈ 5–35 μm thickness. The dispersion of these modes agrees well with theoretical predictions, but their Raman scattering intensities cannot be described completely by bulk Raman tensors. We discuss the temperature dependence of the observed frequencies of the modes.     

Neutron Scattering and Vibrational Spectra of Molecular Crystals

Infrared and Raman spectra of a number of molecular crystals have been measured for studying molecular vibrations and the intermolecular and intramolecular force fields. The infrared absorption bands arise from interaction of the electric wave with the oscillating dipole moment of the crystal. Raman scattering covers inelastic photon scattering processes and accordingly Raman lines arise from the oscillating polarizability of the crystal. Thus, the vibrational modes observed in infrared absorption or Raman scattering spectra are k = 0 modes, for which translationally equivalent molecules vibrate in phase.     

Nonlinear-laser effects in χ(<Superscript>3</Superscript>)-and χ(<Superscript>2</Superscript>)-active organic single crystals

The process of stimulated Raman scattering (SRS) allows one to convert laser emission wavelength of crystals, providing suitable molecular or lattice modes which contribute to third-order nonlinear optical susceptibility. Renewed interest in this field emerged because of the discovery of SRS in crystals that contain molecular units exhibiting Raman active modes. Particularly, organic nonlinear optical crystals used so far for frequency doubling and third harmonic generation seem to have a great potential for SRS application. This review paper reported same results on efficient SRS lasing effects that were discovered recently in organic crystals.