Stimulated Raman scattering in three-dimensional photonic crystals

The results of experimental studies of stimulated Raman scattering of light (SRS) excited in three-dimensional photonic crystals — synthetic opal matrices infiltrated with Raman active media are presented. It is shown that the SRS threshold in such structures decreases with respect to the SRS threshold in Raman active bulk materials. The influence of the photonic-band structure of the active materials used on the SRS properties is estimated.     

Transient stimulated raman scattering in crystals during motion of populations of vibrational states

Transient stimulated Raman scattering (SRS) in crystals is analyzed taking into account the motion of populations of vibrational states under the action of subpicosecond (shorter than the dephasing time) pump pulses. Analytic expressions describing the dynamics of excitation of vibrations in SRS are derived. It is found that for a small wavelength of SRS interaction and high intensities of pump radiation observed for femtosecond SRS in crystals, avalanche excitation of vibrations can be responsible for SRS suppression. It is shown that when phase matching of Stokes-anti-Stokes parametric coupling in transient SRS is ensured, it is possible to elevate the efficiency of frequency conversion under conditions of motion of populations of vibrational states; this explains recent successful results in the experimental implementation of femtosecond SRS in crystals pumped by a Bessel beam.     

Detection of a new SRS‐promoting phonon mode and cross‐cascaded χ(3)‐nonlinear lasing in single crystals of calcite (trigonal CaCO3)

For calcite (CaCO₃), one of the pioneer crystals in nonlinear optics, new results of stimulated Raman scattering (SRS) spectroscopy are presented. Among them are the discovery of a new SRS‐promoting vibration mode with ω_SRS2 ≈︁ 282 cm^‐1 and its participation, together with the main SRS mode ω_SRS1 ≈︁ 1086.5 cm^‐1, in cross‐cascaded (χ⁽³⁾ ↔ χ⁽³⁾) nonlinear‐lasing generation, as well as the observation of efficient self‐upconversion via cascaded parametric four‐wave processes of one‐micron Stokes and anti‐Stokes χ⁽³⁾‐lasing into the UV‐region of third harmonic generation. The investigations show that calcite is able to generate a χ⁽³⁾‐lasing comb of more than two octaves bandwidth. The article also gives a brief review on the discovery and study of the SRS‐effect in natural crystals (minerals), which have expanded our ability to study the photon‐phonon nonlinear‐laser interactions in crystalline materials. A short summary of information about χ⁽³⁾‐lasing properties of the triangular planar structure units in SRS‐active crystals is included.     

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.     

A method for reducing the stimulated Raman scattering threshold in liquids embedded into photonic crystals

We study stimulated Raman scattering (SRS) in liquids (water and ethanol) embedded into photonic crystals (artificial opals) under excitation with 60 ps laser pulses at 532 nm. We observe a substantial decrease of the SRS threshold when the focused laser beam excites the crystals near their surface. The spatial distance between the beam center and the surface of the crystals is close to their nanoscale structure. The decrease in the SRS threshold is due to a substantial increase in the photonic-state density near the edges of the photonic crystal stop zones and the so-called Mie resonances in active media near the nanosized globules. This leads to a considerable increase in the local-electric-field intensity, causing the SRS threshold reduction. Such a method of reducing the SRS threshold opens up a way of creating new efficient laser sources based on photonic crystals and their use for different applications in nanotechnologies.     

SRS generation under phase matching conditions for four-wave interactions of SRS components in birefringent Raman-active crystals

The possibilities of efficient four-wave SRS generation in the schemes of cavity and cavity-amplifier SRS converters with the implementation of phase matching conditions for four-wave mixing of different SRS radiation components at an appropriate orientation of birefringent SRS crystals have been considered based on a numerical simulation. The threshold characteristics and achievable energetic parameters of the SRS generation of different frequency radiation components have been analyzed under the conditions of implementation of phase matching for four-wave mixing. Conditions have been found for a low-threshold SRS-four-wave mixing generation of an anti-Stokes wave with a conversion efficiency of up to 40%, as well as of the first, second, and third Stokes SRS components with conversion efficiencies of up to 90, 80, and 30%, respectively.     

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.     

Low-threshold parametric Raman generation of high-order Raman components in crystals

The theoretical and experimental study of the axial transient multiwave parametric Raman generation via four-wave mixing of arbitrary neighboring Stokes components in simple tungstate crystals is carried out. In agreement of the theoretical modeling with the experimental results, we have found that because of the four-wave mixing of arbitrary Stokes components in the short crystals, the stimulated Raman scattering (SRS) generation thresholds of the high-order Stokes components are significantly reduced relative to the values defined by the cascade-like mechanism of SRS.     

Picosecond stimulated Raman scattering in crystals

The comparative values of the peak and integral cross sections of spontaneous Raman scattering and the optical dephasing time of molecular vibrations were determined for several oxide crystals by spontaneous Raman spectroscopy. The spectral, time, and energy parameters of stimulated Raman scattering (SRS) were measured for ten crystals using picosecond YLF: Nd laser pumping with a radiation wavelength of 1047 nm. An analysis of the experimental dependence of the threshold energy of pumping SRS on the integral and peak cross sections of spontaneous Raman scattering showed that the SRS gain increment explicitly depended on the integral cross section and was independent of the peak cross section of spontaneous Raman scattering as the ratio between the pumping pulse width (11 ps) and the time of optical dephasing of molecular vibrations changed from 0.42 to 9.3. The gain coefficients of steady-state stimulated Raman scattering under threshold stimulated Raman scattering conditions were determined for all the crystals studied on the basis of the measured threshold SRS pumping energies, the duration and width of the spectrum of pulses, the nonlinear interaction length, the intensity of pumping, and the theoretical dependences that relate the steady-state and transient SRS gain increments. The steady-state SRS gain coefficients obtained in this work fitted well a linear dependence on the peak cross sections of spontaneous Raman scattering, which substantiated the correctness of our analysis and measurements.     

Two-photon absorption of high-power picosecond pulses in PbWO<Subscript>4</Subscript>, ZnWO<Subscript>4</Subscript>, PbMoO<Subscript>4</Subscript>, and CaMoO<Subscript>4</Subscript> crystals

The nonlinear process of two-photon interband absorption is studied in tungstate and molybdate oxide crystals excited by a sequence of high-power picosecond pulses with a wavelength of 523.5 nm. The transmission of the crystals is measured for the excitation pulse intensity up to 100 GW/cm². The pulse intensity in the crystals initially transparent at a wavelength of 523.5 nm is strongly limited due to two-photon absorption (TPA), and the reciprocal transmission in PbWO₄ and ZnWO₄ crystals reaches 50–60. In all crystals, TPA induces long-lived one-photon absorption, which affects the nonlinear process dynamics and leads to a hysteresis in the dependence of the transmission on the laser excitation intensity. Absorption dichroism manifests itself in a significant difference in the transmission intensities when the principal orthogonal optical axes of the crystals are excited. The TPA coefficients are determined during the excitation of two optical axes of the crystals. TPA coefficients β for the crystals vary over a wide range, namely, from β = 2.4 cm/GW for PbMoO₄ to β = 0.14 cm/GW for CaMoO₄, and the values of β can differ almost threefold when different optical axes of a crystal are excited. Good agreement is achieved between the measured intensities limited by TPA and the estimates calculated from the measured nonlinear coefficients. Stimulated Raman scattering (SRS) upon excitation at a wavelength of 523.5 nm is only detected in two of the four crystals under study. The experimental results make it possible to explain the suppression of SRS by its competition with TPA, and the measured nonlinear coefficients are used to estimate this suppression.     

Pump spectral linewidth influence on stimulated Brillouin scattering (SBS) and stimulated Raman scattering (SRS) and self‐termination behavior of SRS in liquids

The threshold, temporal behavior, and conversion efficiency of stimulated Brillouin scattering (SBS) and stimulated Raman scattering (SBS) in three liquids (benzene, hexane, and dimethyl sulfoxide) and two crystals (calcite and barium nitrate) have been investigated under three largely different spectral linewidth conditions. Pumped with 532‐nm and nanosecond duration laser pulses of ≤ 0.01 cm^?1 linewidth, only SBS can be generated in all tested liquids with a high nonlinear reflectivity. However when the pump spectral linewidth is ～0.07 cm^?1 or ～0.8 cm^?1, both SBS and SRS can be observed in benzene while only SRS can be generated in dimethyl sulfoxide; in all these cases SRS is the dominant contribution to the stimulated scattering but the efficiency values are drastically decreased due to the self‐termination behavior of SRS in liquids, which arises from the thermal self‐defocusing of both pump beam and SRS beam owing to Stokes‐shift related opto‐heating effect. In contrast, for SRS process in the two crystals, the thermal self‐defocusing influence is negligible benefitting from their much greater thermal conductivity, and a higher conversion efficiency of SRS generation can be retained under all three pump conditions.

     

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.     

Ba(NO3)2晶体受激拉曼散射的角度分布和脉冲压缩

报道了利用重复频率为30 Hz,波长为532 nm 的Nd∶YAG倍频激光单次通过抽运硝酸钡（Ba(NO3)2）晶体（晶体由水溶液降温法生长,长度为48 mm,横截面为10 mm×10 mm）,获得高效率的一阶（563 nm）,二阶（599 nm）和三阶（639 nm）斯托克斯光的实验结果.硝酸钡晶体沿着［110］晶轴方向切割.观测到一、二、三阶斯托克斯光呈锥形环分布,一、二、三阶斯托克斯光的散射外边缘与抽运光轴线间的夹角大小分别为1.7°,3.5°,5.0°.同时也观测到Ba(NO3)2的SRS角度分布与抽运光强度无关.定性分析认定,Ba(NO3)2的SRS角度分布主要是由相位匹配过程决定的.测得抽运光、一、二、三阶斯托克斯光的脉宽分别为11.6 ns,9.8 ns,8.4 ns和4.5 ns.当抽运光功率密度约为150 W/cm2时,获得一、二、三阶斯托克斯光的最大光光转换效率,分别为33.5%,8.8%和3.4%. 此外,由于晶体中的热沉积效应,观察到了Ba(NO3)2晶体的SRS转换效率饱和现象.     

Frequency comb expansion in a monolithic self‐mode‐locked laser concurrent with stimulated Raman scattering

The discovery of a novel phase‐locked frequency comb generated from a monolithic laser with the concurrent processes of self‐mode locking (SML) and stimulated Raman scattering (SRS) is reported. It is experimentally shown that the width of the Raman gain can be exploited to considerably expand the frequency comb of a monolithic SML crystal laser via the SRS process. At a pump power of 6.5 W, an output power of 140 mW in the Stokes wave with a pulse width as narrow as 2.9 ps at a pulse repetition rate of 6.615 GHz is obtained. The present finding not only provides useful insights into the monolithic intracavity SRS process but also paves the way for generating mode‐locked pulses based on monolithic self‐Raman crystals.     

Stimulated Raman scattering of picosecond pulses in a YVO<Subscript>4</Subscript> crystal

Stimulated Raman scattering (SRS) with a picosecond pulse in YVO₄ crystals in a transient state was investigated. The picosecond gain of YVO₄ crystals pumped by a 532-nm laser evaluated by means of the threshold was 16.13 cm/GW.     

钨酸锌晶体的受激拉曼散射和光致发光研究

采用皮秒532nm 激光激发，研究了ZnWO₄晶体的受激拉曼散射和本征荧光发射.在SRS光谱中观察到一级(558.7nm)和二级(588.6nm)斯托克斯光，线宽分别为130和77cm^－1, 一级斯托克斯光的抽运阈值为6.8mJ.在532nm激光抽运下ZnWO₄晶体的荧光光谱呈现出由能量为2.30，2.45和2.83eV的3个高斯分量组成的独特结构.光致发光表明晶体具有从400nm到650nm的宽带本征发光，其峰值波长为472.0nm，相应于钨氧之间的辐射跃迁. 关键词： 晶体 钨酸锌 受激拉曼散射 闪烁体     

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.     

KDP晶体受激拉曼散射特性

详细比较了磷酸二氢钾(KDP)晶体的自发拉曼散射和受激拉曼散射光谱,在受激拉曼散射(SRS)中观察到了自发拉曼散射中最强的振动模的三阶Stokes光(559.43,589.74,623.50nm),由于其他振动模的受激拉曼散射增益系数较小,其SRS光谱未观察到。另外,比较了传统生长的未退火和退火后的KDP晶体及快速生长的锥区和柱区KDP晶体的受激拉曼散射增益系数,结果表明生长方法和热退火对KDP晶体的受激拉曼散射增益系数无明显影响。     

Steady-state Raman gain in visible and near-infrared waveband of Sr WO_4 and Ba WO_4 crystals

The steady-state stimulated Raman scattering （SRS） gain with different excitation wavelengths ranging from 400 to 1100 nm of tungstate crystals, SrWO4 and BaWO4, is systematically researched. As excitation frequency is close to electronic transition frequency, molecular polarizability is not a constant, which has to be taken into account in our work. The experiment and theory agree well with each other and show that SRS gain is not only proportional to Stokes light frequency, but is also inversely proportional to biquadratic excitation frequency.     

A practical method for diameter,number density and material characterization of 40–90 µm size droplets by stimulated Raman scattering

We demonstrate that the technique of Stimulated Raman Scattering (SRS) is a practical method for the simultaneous characterization of diameter, number density and constituent material of microsize droplets. The method is applicable to all Raman active materials and to droplets with a diameter of at least 8 µm. Our experimental study was focused on water and ethanol monodisperse droplets in the diameter range of 40–90 µm. Results of a single laser pulse and multiple pulses are analyzed, indicating that the SRS method can diagnose droplets of mixed liquids and ensembles of polydisperse droplets.