Raman scattering using vortex light

We re-examine the theory of Raman scattering in cubic crystals. The unconventional vector potential of vortex light leads to new selection rules. We show that in this novel optical process, (a) silent phonon modes become active and (b) scattering tensors change for ordinary Raman active phonon modes. Calculation based on a simplified model shows that the vortex Raman scattering intensity can be comparable with that of ordinary Raman process.     

Additional Raman Scattering Mechanism due to Transverse Polar Modes

Longitudinal polar modes generate a macroscopic electric field in piezoelectric crystals and cause an additional mechanism of Raman scattering.The classical theory holds that transverse polar modes cannot produce such an additional mechanism.Our quantum theory shows that there is an additional Raman scattering mechanism arising from the electro-optic effect of transverse polar 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.     

The pH effects on the growth rate of KDP (KH2PO4) crystal by investigating Raman active lattice modes

We report on the dependence of the pH value on the growth rates of KDP single crystals. Extensive experimental work has been carried out in order to find the optimum pH ranges for growing KDP single crystals with suitable sizes and high optical quality. Different techniques including micro‐Raman back‐scattering spectroscopy, UV/vis/IR transmission spectroscopy and X‐ray diffraction have been employed for this investigation. Deuterated substituted single crystals of KDP and DKDP also have been grown for the investigation of growth rates and Raman active mode identification purposes. The molecular vibration modes of the grown crystals, including internal modes of PO₄ tetrahedrons molecular vibrations, external modes of optical phonons and hydrogen bonding modes have been determined exactly by micro‐Raman back‐scattering spectroscopy. The best pH values of the solution for the KDP crystal growth with reasonably higher growth rates from aqueous solutions that have been supersaturated ata temperature range of 30–50 °C have been found to be in the pH range of 3.2–5.4. Copyright © 2007 John Wiley & Sons, Ltd.     

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.     

ZnO晶体的偏振拉曼散射的深入研究

利用拉曼选择定则,设计了ZnO单晶的直角偏振几何配置。在室温下测量了ZnO单晶的各种振动模式的偏振拉曼散射光谱。与原先的文献相比较,初步讨论了各种振动模式的线宽和强度的变化原因。除ZnO晶体中包括非极性和极性拉曼基频振动,准横光学和准纵光学模式和振动属性被指认外,它们的高阶拉曼散射模式首先被确定。本研究结果为深入了解ZnO晶体和薄膜的宏观性质和微观结构提供了依据。     

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.     

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.     

拉曼光谱研究n型4H-和6H-SiC晶体的载流子浓度

半导体材料的纵光学声子与等离子体激元耦合模(LOPC模)能够提供材料电学方面的相关信息。本文在室温下测得了n型4H-和6H-SiC的拉曼光谱,分析了掺入的杂质对于SiC晶体拉曼光谱的影响,通过拟合n型4H-和6H-SiC晶体的LOPC模的线型得到等离子体频率,并由此从理论上计算了载流子浓度。载流子浓度的理论计算值与霍尔测量的结果符合得很好。研究结果进一步证实了对于n型4H-和6H-SiC晶体,可以通过分析LOPC模的线形来较准确地给出相关材料的载流子浓度。     

旋光性单轴晶体的喇曼光谱中TO和LO模的识别

本文提出一种简便识别旋光性单轴晶体喇曼光谱中横模和纵模的方法。应用90°散射几何配置x(z+Δy,xz)y,散射光的偏振方向与x轴成δ夹角。应用Loudon给出的单轴晶体极性声子的喇曼散射效率公式,计算TO和LO模的散射效率,它们依赖于喇曼张量元和δ角,其极大值分别位于δ_max^TO和δ_max^LO处,这两个角度的符号正好相反。因此,由判定δ_max的符号,可以将TO和LO模区分开来,并且从|δ_max|值可以了解喇曼张量的各向异性。 关键词：     

Vibrational modes symmetry and raman scattering in SnI4 crystals

A group-theoretical vibrational modes symmetry analysis of SnI₄ crystals has been made for the Brillouin zone center and polarized Raman scattering study in these crystals has been carried out. Correlation diagram showing the correspondence between the crystal vibrational modes and the free SnI₄ molecule modes has been built. The nature and peculiarities of the low frequencies spectrum have been considered.     

Raman scattering from GaSxSe1-x

The non resonant Raman scattering spectra of GaSe, GaS and of eight different mixed crystals GaS_xSe_1-x are presented. The frequencies of some vibrational modes shift continuosly from GaSe to GaS indicating that the mixed crystals are homogeneous. The discontinuous shift of some other modes is explained either by the change of the stacking of the layers, or by a ‘two mode’ behaviour as previously observed in other types of mixed crystals. Moreover, local vibrational modes are observed.     

Raman and Hyper-Rayleigh Scattering in Lithium Tetraborate Crystals

Experimental studies of Raman scattering and the infrared reflection spectra of lithium tetraborate crystals were carried out within a broad temperature range with various polarization geometries. The crystals studied are characterized by record values of radiation resistance, transparence within a broad spectral range including the ultraviolet region, and nonlinear optical properties. A group-theoretical analysis of the vibrational spectra of this crystal was performed and fundamental vibrational terms were assigned to the symmetry types of the point group as well as the polarizations of the corresponding modes. The effective Raman cross section was measured and was found to be one order of magnitude higher than those of the known crystals, in which the stimulated Raman scattering (SRS) was observed. The nonlinear optical and electrooptical coefficients were evaluated and were found to be consistent with the results of independent measurements. The effect of a drastic increase in the intensity of quasi-elastic light scattering at 253 K was registered. It was associated with the phase transition that consists of the disordering of lithium ions with respect to the rigid skeleton. The formation energy for Frenkel defects in the lithium sublattice and the activation energy of the ionic conduction when heating the sample were calculated from the obtained temperature dependences of the intensity of quasielastic and hyper-Rayleigh light scattering.     

Scattering of light in a ferroelectric with incommensurate phase: K2ZnCl4

We presented and analyzed spectra of Raman scattering in various phase states of K₂ZnCl₄ crystals, including the incommensurate phase. On the basis of this analysis we determined the parameters of modes associated with internal and external motions of ions. We found that the phase mode reveals itself in the Raman scattering spectra; this mode is responsible for the instability of the crystal lattice in the vicinity of the incommensurate phase transition.     

The Raman effect in crystals

A review is given of progress in the theoretical and experimental study of the Raman effect in crystals during the past ten years. Attention is given to the theory of those properties of long-wavelength lattice vibrations in both cubic and uniaxial crystals which can be studied by Raman scattering. In particular the phenomena observed in the Raman scattering from crystals which lack a centre of inversion are related to the theory. The angular variations of the scattering by any type of lattice vibration in a crystal having any symmetry can be easily calculated using a complete tabulation of the Raman tensor. Recent measurements of first-order lattice vibration spectra are listed. A discussion of Brillouin scattering is included. The relation of second-order Raman spectra to critical points in the lattice vibration density of states is discussed, and measurements of the second-order spectra of diamond and the alkali halides are reviewed. The theory and experimental results for Raman scattering by electronic levels of ions in crystals are examined, and proposals for Raman scattering by spin waves, electronic excitations across the superconductive gap and by plasmons are collected together. Finally, the prospects for applying lasers as sources for Raman spectroscopy are discussed, and progress in the new technique of stimulated Raman scattering is reviewed.     

Raman scattering from 2H and 3R–NbS2

Raman scattering experiments have been carried out on 2H-NbS₂ crystals and 3R-NbS₂ crystals. The spectra obtained from both compounds have been found to contain all the Raman active modes predicted by group theory. A nearest-neighbour lattice dynamics model has also been used to analyze the spectra and qualitative agreement with the experimental results is obtained. The results are also discussed in terms of the modifications expected in the Raman spectra obtained from different polytypes of the same layered compound. Some discrepancies with previously reported results are found.     

The Raman effect in crystals

A review is given of progress in the theoretical and experimental study of the Raman effect in crystals during the past ten years. Attention is given to the theory of those properties of long-wavelength lattice vibrations in both cubic and uniaxial crystals which can be studied by Raman scattering. In particular the phenomena observed in the Raman scattering from crystals which lack a centre of inversion are related to the theory. The angular variations of the scattering by any type of lattice vibration in a crystal having any symmetry can be easily calculated using a complete tabulation of the Raman tensor. Recent measurements of first-order lattice vibration spectra are listed. A discussion of Brillouin scattering is included. The relation of second-order Raman spectra to critical points in the lattice vibration density of states is discussed, and measurements of the second-order spectra of diamond and the alkali halides are reviewed.

The theory and experimental results for Raman scattering by electronic levels of ions in crystals are examined, and proposals for Raman scattering by spin waves, electronic excitations across the superconductive gap and by plasmons are collected together.

Finally, the prospects for applying lasers as sources for Raman spectroscopy are discussed, and progress in the new technique of stimulated Raman scattering is reviewed.     

Raman spectroscopy and Fermi resonance in Mn-doped ZnO bulk single crystal

For the first time the bulk oriented single crystals ZnO:Mn are obtained and the polarized Raman spectra are studied at excitation in the visible and near infrared regions. The resonance enhancing of the Raman scattering by Mn-related modes is found at the visible excitation due to the extra optical absorption in ZnO at the addition of Mn. It is shown that the resonance-enhanced overtone of Mn-related silent modes may be responsible for an appearance of anomalous modes of the A₁ symmetry at 500-600 cm⁻¹. A Fermi resonance between the overtone and one-phonon mode is analyzed.     

From high resolution spectroscopy to the modeling of potential energy surfaces

Methods and recipes used to establish potential energy surfaces in condensed molecular phases are discussed. The reliability of calculations is tested by confrontation with spectroscopic measurements in crystals. Optical spectroscopy, in particular, hole burning as a line-narrowing technique, as well as high resolution inelastic neutron scattering (INS), are used to resolve tunneling level structures corresponding to large-amplitude atomic and molecular motions. Rotational tunneling of methyl groups is discussed, and new measurements by INS are presented for crystals that are proposed as suitable candidates for optical studies. Translational tunneling in benzoic acid crystals and the role of promoting modes are reviewed, and new measurements of vibrational spectra by inelastic x-ray scattering are compared with INS and Raman spectra.     

KDP晶体拉曼散射角度特性

利用群理论详细分析了磷酸二氢钾(KDP)晶体的拉曼振动模式,得出了其拉曼振动模的归类。并采用拉曼光谱仪测量了Z切退火KDP晶体X(ZZ)珡X,Z(XY)珚Z和Y(XY)X三种散射配置和未退火KDP晶体Z(XY)珚Z配置下的拉曼光谱。根据拉曼选择定则得出X(ZZ)珡X,Z(XY)珚Z和Y(XY)X散射配置下的拉曼峰分别对应A1,B2(LO),B2(TO)对称类振动模,但在Z(XY)珚Z配置下的拉曼光谱中除了B2模,还观察到了A1模,而在Y(XY)X配置下的拉曼光谱中只有B2模,且退火和未退火晶体Z(XY)珚Z配置下的拉曼光谱无明显差别,此结果表明KDP晶体的对称性降低,在背向散射时A1模也具有角度特性,但与晶体的内应力无关,这是由KDP晶体内部结构决定的。