Effect of crystal orientation on picosecond-laser bulk microstructuring and Raman lasing in diamond

In the paper we report on picosecond-laser bulk microstructuring and stimulated Raman scattering (SRS) in type IIa single-crystal diamond in the course of multipulse irradiation at λ=532 nm wavelength using an advanced ps-laser system equipped with additional setups for on-line video imaging and photoluminescence spectra measurements. The effect of crystal orientation (relative to the incident laser beam) on (i) optical breakdown thresholds, (ii) character of bulk modifications, and (iii) generation of stimulated Raman scattering in diamond during irradiation with picosecond pulses of different durations (τ ₁=10 ps and τ ₂=44 ps) is studied. It is shown that the processes of laser-induced breakdown in the bulk of diamond (at the backside of the crystals) and bulk microstructure growth are governed by the dielectric breakdown mechanism. It is found that generation of high-order stimulated Raman scattering in diamond crystals has a considerable effect on the threshold of laser-induced breakdown and bulk microstructuring. Conditions of the efficient SRS lasing are determined, depending on the pulse duration and the direction ([100] and [110]) of the laser beam incidence. A method of local temperature measurements in the bulk of diamond based on the Stokes-to-anti-Stokes intensity ratio in the recorded SRS spectra is proposed, its applicability to determine a “pre-breakdown” temperature of diamond during multipulse ps-laser irradiation is discussed.     

Temporal characteristics of picosecond stimulated Raman scattering in oxide crystals

The temporal characteristics of stimulated Raman scattering (SRS) under 22-ps laser excitation were studied in eight oxide crystals with a T ₂ optical-phonon dephasing time variable by up to two orders of magnitude. The measured SRS pulse width was shortened from 13.8 ps for Ba(NO₃)₂ (T ₂ = 26.5 ps) to 4 ps for the LiNbO₃ (T ₂ = 0.38 ps) crystal. The dependence of SRS pulse width on the dephasing time was analyzed in the framework of the known SRS theory.     

Raman scattering in monocrystal Bi3B5O12

Raman spectra of a Bi₃B₅O₁₂ monocrystal are investigated for the first time and compared with the Raman spectra of crystals α-Bi₂O₃ and Bi₁₂SiO₂₀. The most intensive lines observed in the Raman spectrum of Bi₃B₅O₁₂ are identified. Promising prospects of use of Bi₃B₅O₁₂ crystals as SRS converters of radiation are shown.     

自受激拉曼晶体Nd3+:SrMoO4的光谱性质研究

通过拉曼散射光谱，吸收光谱，荧光发射寿命和808 nm LD激发下的红外荧光光谱的实验测量，系统研究了Nd³⁺:SrMoO₄晶体的自受激拉曼光谱性质.分析指认了拉曼散射光谱中各拉曼峰所对应的晶格振动模式，得出了其SRS活性最强的声子频率约为898 cm^-1，对应于(MoO^2-₄)离子团的完全对称光学伸缩振动A_g模；通过J-O理论对晶体的吸收谱进行了全面的光谱参数计算，得出⁴F_3/2→⁴I_11/2跃迁的积分发射截面达0.57×10^-18 cm²，自发辐射概率为141.06 s^-1；同时，实验测得该跃迁的荧光发射寿命约为0.2 ms.最后，结合808 nm LD激发下的红外波段荧光光谱，论证了SrMoO₄晶体中Nd³⁺离子1068 nm发射通过拉曼频移获得1180 nm一级斯托克斯激光发射的可能性，为Nd³⁺:SrMoO₄晶体的自受激拉曼激光器研究提供了理论依据. 关键词： 3+离子')" href="#">d³⁺离子 4 晶体')" href="#">SrMoO₄ 晶体 自受激拉曼散射     

Multiphoton SRS-Lasing in a Monoclinic β-BaYb<Subscript>2</Subscript>F<Subscript>8</Subscript> Crystal

The discovery of stimulated Raman scattering (SRS) in monoclinic fluoride β-BaYb₂F₈ known as a host matrix for Ln³⁺ lasant ions was reported. All the recorded spectral components of Stokes and anti-Stokes χ⁽³⁾-nonlinear picosecond generation were assigned to the three SRS-active photon A_g- and B_g-modes of a crystal (ω_SRS1 ~ 362 cm^–1, ω_SRS2 ~ 295 cm^–1, and ω_SRS3 ~ 230 cm^–1).     

Polarized Raman and IR spectra of non‐centrosymmetric PbB4O7 single crystal

Polarized Raman and IR spectra of a PbB₄O₇ single crystal were measured. The obtained spectra are discussed within the factor group approach for the orthorhombic P2₁nm(C_2v⁷) space group with Z = 2 assuming that the crystal structure is built up of the (B₄O₇)_∞²⁻ framework and Pb²⁺ ions. It has been shown that vibrations of borate and Pb²⁺ units are observed above 240 and below 160 cm⁻¹, respectively. The results obtained for the spontaneous Raman scattering have also been used in the discussion of the stimulated Raman spectra of the material studied—a new Raman‐laser crystal. The obtained results revealed that mainly translational motions of Pb²⁺ ions participate efficiently in the SRS effect. Copyright © 2008 John Wiley & Sons, Ltd.     

Detection of stimulated Raman scattering in the LiYbF<Subscript>4</Subscript> crystal

Stimulated Raman scattering (SRS) has been observed for the first time in a tetragonal LiYbF₄ crystal. The recorded Stokes and anti-Stokes components of χ⁽³⁾ nonlinear lasing are attributed to the two SRS-active phonon modes with ω_SRS1 ~ 325 cm^–1 and ω_SRS2 ~ 432 cm^–1 of this crystal.     

Enhanced stimulated Raman scattering in H<Subscript>2</Subscript> by seeding an SRS line into an H-ɛ Balmer line: Amplification-coupled laser wavelength shifter

The stimulated Raman scattering (SRS) in H₂ gas above the dissociation energy limit was recorded using a 266-nm UV laser. All of the observed Stokes and anti-Stokes SRS lines showed a normal behavior except the third Stokes SRS lines at 397.8 nm, which showed a substantial intensity enhancement of about a 36%-conversion efficiency of the pump energy. This enhancement in the SRS line is attributed to the seeding of the SRS line into the Balmer H-? line at 397 nm in molecular hydrogen. To the best of our knowledge, there is no report of any work on enhanced stimulated Raman scattering in H₂ by the seeding of the H-? Balmer line into the SRS line and attaining a very high intensity at the third Stokes SRS lines at 397.8 nm. The cell pressure and the laser pulse energy dependence of these SRS lines substantiate our explanation.     

Control of radiation spatial coherence under synchronous amplification in crystalline LiF:F 2 − amplifier

A technique of spatial coherence control, based on the synchronous amplification of a radiation in LiF crystals with F ₂ ^? color centers, is demonstrated. Spatial radiation distributions of stimulated Raman scattering (SRS) in oxide crystals were investigated under picosecond laser excitation. Low spatial radiation coherence was revealed for both the transient and quasi-stationary SRS. Spatially incoherent SRS was transformed to spatially coherent radiation as a result of phase—locked picosecond synchronous laser pumping of nonlinear Raman and LiF: F ₂ ^? crystals and the Stokes radiation amplification in the color center crystal.     

Polarization resolved stimulated raman scattering: probing depolarization ratios of liquids

Polarization resolved stimulated Raman scattering (SRS) signal is described in the case of isotropic media and linearly polarized incident fields. The model gives simple expressions for the two perpendicularly polarized SRS signals I_X and I_Y, detected along the X and Y directions, respectively, as a function of the incident pump and Stokes polarization angles. We find that Raman depolarization ratio can be simply obtained from the ratio of the SRS intensities detected along the X and Y axis. These theoretical findings are supported by polarization resolved SRS measurements performed on polarized and depolarized bands of cyclohexane. Copyright © 2011 John Wiley & Sons, Ltd.     

Investigation of the spatial profile of stimulated Raman scattering beams in D<Subscript>2</Subscript> and H<Subscript>2</Subscript> gases using a pulsed Nd:YAG laser at 266 nm

The stimulated Raman scattering (SRS) beam spatial mode structure is studied in H₂ and D₂ gases, in a 60 cm-long high-pressure Raman cell, using a pulsed Nd:YAG laser at 266 nm. The conversion efficiencies of the first and second Stokes in H₂, D₂ and H₂/D₂ mixtures have been measured precisely in the 1–14 atm range. The SRS beam profiles were recorded for different gas pressures in the high-pressure Raman cell and interesting behaviour is revealed. Homogeneous SRS spatial profiles were obtained only for pressures higher than 7 atm. For lower pressures the profiles are either in the form of a ring or of a more complicated shape. The results are explained in terms of nonlinear self-focusing processes during the pump beam propagation in the Raman cell. Also, from our measurements, a more precise value of the nonlinear index of refraction for the H₂ and D₂ at 266 nm is proposed. PACS 42.65.Dr; 42.60.Jf; 42.60.Lh; 42.65.Jx     

Raman spectra of TiO2-II,TiO2-III,SnO2, and GeO2 at high pressure

Raman spectra of the orthorhombic (II) and high pressure (III) phases of titanium dioxide at pressures to 372 kbar and effects of temperature and hydrostatic pressure on Raman spectra of the tetagonal cassiterite-like phases of TiO₂, GeO₂ and SnO₂ are described. At room temperature, the TiO₂ II–III transition is sluggish, and metastable coexistence was observed from 200 to 300 kbar. The Raman spectra of TiO₂-III imply that its primitive cell contains at least four formula units; however, the structure could not be established from the Raman spectra and available powder X-ray diffraction patterns.The temperature and pressure dependences of the spectrum of the tetragonal MO₂ phases together with bulk moduli and thermal expansion data were used to evaluate the pure-volume and pure-temperature contributions to the isobaric temperature dependence of the Raman frequencies. Large anharmonicities in TiO₂ are attributed to hybridization of the oxygen p states with the d states of the Ti ion. GeO₂, where p-electron bonding is involved, is much less Enharmonic.     

Chemical composition of matrix-embedded ternary II–VI nanocrystals derived from first- and second-order Raman spectra

A one- and multiphonon Raman scattering study is performed for an extensive set of CdS_1–xSe_x, Cd_1–yZn_yS, Cd_1–yZn_ySe, and CdSe_1–xTe_x nanocrystals to investigate the applicability of first- and second-order Raman spectra for the determination of the matrix-embedded ternary nanocrystal composition. For one-mode ternary systems both the LO and 2LO phonon frequencies in the Raman spectra are shown to be a good measure of the nanocrystal composition. For two-mode systems, the approaches based on the difference of the LO phonon frequencies (first-order Raman spectra) or double LO overtone and combination tone frequencies (second-order Raman spectra) as well as on the LO phonon band intensity ratios are analysed. The weak electron–phonon coupling in the II–VI nanocrystals and the polaron constant values for the nanocrystal sublattices are discussed.     

非均匀等离子体中受激Raman散射非线性行为

鉴于实际中等离子体不均匀性和非周期性边界条件，建立了受激Ｒａｍａｎ散射（ＳＲＳ）和受激Ｂｒｉｌｌｏｕｒｉｎ散射（ＳＢＳ）非线性耦合模型。ＳＢＳ对ＳＲＳ的影响主要表现在两方面：１）Ｌａｎｇｍｕｉｒ波与离子声波的非线性相互作用，２）ＳＢＳ与ＳＲＳ的竞争。本文研究了离子声衰变不稳定性、离子声波对Ｌａｎｇｍｕｉｒ波的非共振散射两种非线性过程在ＳＲＳ发展过程中的作用，给出一维不均匀等离子体中ＳＲＳ发展图象。Ｌａｎｇｍｕｉｒ波向短波转换，从而被强烈阻尼是抑制ＳＲＳ的重要机制。文中给出了ＳＢＳ／ＳＲＳ耦合过程中决定ＳＲ 关键词：     

Vibrational spectroscopy at very high pressures—XX Raman and far-IR study of the phase transition in paratellurite

Raman and far-IR spectra have been obtained up to ca. 45 kbar [4.5 GPa] for paratellurite (Te0₂) in a diamond anvil cell. At the D₄⁴ to D₂⁴ phase transition ca. 9 kbar an E symmetry mode initially at 122cm^?1 was found to split into two components in both IR and Raman spectra: their coincidence in both types of spectra shows that one component in the Raman spectrum cannot be an LO mode. No other E modes were seen to split. A further phase transition claimed ca. 30 kbar was not confirmed.Paratellurite is exceptionally sensitive to the presence of non-hydrostatic stresses, which greatly influence the phonon frequencies. This behaviour is illustrated by Raman spectra obtained under varying degrees of shear stress.     

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.     

Cerussite,PbCO3 – a new Stimulated Raman Scattering (SRS)‐active crystal with high‐order Stokes and anti‐Stokes lasing

Orthorhombic PbCO₃, known as natural crystal cerussite, is presented as a new Stimulated Raman Scattering (SRS)‐active crystal. With picosecond laser pumping high‐order Raman‐induced χ⁽³⁾ generation is observed. All registered Stokes and anti‐Stokes sidebands in the visible and near‐IR are identified and attributed to the SRS‐promoting phonon mode A_1g of the carbonate group, with ω_SRS ≈ 1054 cm⁻¹. The first Stokes steady‐state Raman gain coefficient in the visible spectral range is estimated as well to a value not less than 4.6 cm·GW⁻¹.     

Three-phonon stimulated Raman scattering in an orthorhombic LuAlO<Subscript>3</Subscript> crystal

High-order stimulated Raman scattering (SRS) has been revealed in a LuAlO₃ crystal upon stationary picosecond laser excitation. All recorded Stokes and anti-Stokes χ⁽³⁾-nonlinear laser components are attributed to three SRS-promoting А _g vibrational modes of its octahedral anionic units (AlO₃)^–3.     

“Negative” absorption and “negative” emission in nonlinear optics

The nonlinear susceptibilities X³ (ω₂ = ω₁ ? ω₁ + ω₂) calculated for stimulated Raman scattering (SRS) and two- photon absorption (TPA) under the condition of one-photon resonance in the case of a multilevel system with broad overlapping absorption bands (corresponding to polyatomic molecules) are discussed. Spectra of Im X³ with changed sign in some spectral regions are shown. The result is connected with a disbalance of the system, due to the large relaxation constants.     

Long wavelength lattice vibrations in GaS and GaSe

The first order Raman spectra and far infrared absorption spectra of GaS and GaSe have been investigated and interpreted. A correspondence is drawn between the observed vibrational modes of the two crystals and a Raman active polar longitudinal mode has been identified in GaSe. The results are consistent with the existence of GaS in a β-polytype (D_6h) and GaSe in an ?-polytype (D_3h).