Determination of the composition of mixtures of organic liquids by CARS spectroscopy

Two methods of realization of coherent anti-Stokes Raman scattering (CARS) spectroscopy of organic liquids are described: with a tunable dye laser and by means of biharmonic laser pumping based on stimulated Raman scattering. The second method is applied to liquids for the first time. The possibilities of the two methods are compared. CARS spectroscopy is applied for the first time to the analysis of a mixture of two organic liquids.     

超短超强激光与气体靶相互作用中的背向受激Raman散射

 实验诊断测量了超短超强激光与气体靶相互作用产生的背向受激Raman散射,在实验条件下呈现强耦合模式,背向受激Raman散射出现非线性Stokes多峰伴线结构,峰值的频率间隔小于等离子体波的频率,可以大致地推断出激光打靶过程中产生的等离子体密度偏低,其结果与等离子体强耦合理论计算结果一致。     

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.     

一种用弱信号光调制的宽带光纤拉曼相干光源

本文考察了光纤中外加可调谐信号光条件下的受激拉曼散射现象,提出一种新的宽带光纤拉曼相干光源的设想。这种光源是利用波长可调的弱信号光来调制固定波长的强泵浦光在光纤中产生的高阶受激拉曼散射,使得高阶受激拉曼散射Stokes峰值波长随弱信号光的波长改变而改变。从而获得一个输出均匀而频带又比信号光宽得多的高强度相干光。     

碘激光的H2振动受激拉曼阈值研究

首次实现了脉冲光解碘激光作为基频光的氢气振动受激拉曼变频,对碘激光的波长转换有着重要意义。在碘激光单脉冲能量100~130 mJ(脉宽100 ns)的条件下, 采用双次聚焦技术降低了高压氢气的振动受激拉曼变频的阈值,获得了波长为2900 nm中红外激光,光子转化效率最高达到8.7%。实验发现当拉曼介质氢气气压大于1 MPa后,一级斯托克斯光的拉曼转化效率不再随气压变化,并对这一现象进行了理论分析和归属。     

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.     

Stimulated Raman scattering and spontaneous Raman solitons in ammonia

In this study we report the first observation of spontaneous Raman solitons in stimulated Raman scattering (SRS) by the gas NH₃. The scattered radiation is called Stokes radiation. Raman solitons are of considerable interest, because their existence can be explained by quantum-mechanical fluctuations of the electromagnetic field in vacuum. We have observed spontaneous Raman solitons in a forward SRS configuration for two different molecular transitions of NH₃, the laser emissions at 58 μm and 72.6 μm wavelength. These are optically pumped by 10 μm CO₂-laser pulses with a duration of 100 ns and an energy of 150 mJ. Spontaneous Raman solitons are short spikes in the pump pulse which occur during its depletion. Their origin is the rapid π phase change of the Stokes seed. In contrast to other laboratories we have used single-pass cells. Thus, we have succeeded in observing multiple spontaneous Raman solitons during one pump pulse. Previous experiments with multi-pass cells never showed multiple solitons. Since multiple spontaneous Raman solitons have already been reported in an earlier experiment with a single-pass cell filled with hydrogen at high pressure, we conclude that such multiple Raman solitons can be observed mainly in this type of gas cell. Subsequently, we have performed statistical measurements on the delay time and the height of the spontaneous Raman solitons in the depleted pump pulse for the 58 μm-NH₃ emission. We have compared these statistics with theory and equivalent experimental results of other laboratories. They are in good agreement with the assumption that quantum-mechanical fluctuations are the origin of spontaneous Raman solitons. The most recent theories postulate that the origin of the formation of spontaneous Raman solitons can be explained by the rapid π phase change of the Stokes seed as well as that of the laser or polarization wave. Therefore, we have determined the phase of the spontaneous Raman solitons relative to the depleted pump pulse. Although, such changes of sign of the relative phase have already been observed in an earlier SRS experiment with hydrogen at high pressure, we did not detect any in our experiment. Therefore, we conclude that in this experiment the π phase change occurs in the Stokes or polarization wave.     

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.     

混合溶液中CARS过程的非共振信号实验研究

相干反斯托克斯拉曼散射是一种非线性四波混频效应,但是通过探测共振信号不易进行物质成分的定量光谱分析。本文利用单频相干反斯托克斯拉曼散射光谱分析法,对不同体积比混合的乙醇溶液在远离双光子共振跃迁及其远离溶质与溶剂的特征拉曼共振态位置进行了光谱探测。通过对实验结果进行分析发现,在共振位置2 876 cm-1的信号强度随混合溶液中的乙醇的体积比增加而增加,呈二次方关系。而在远离共振态位置的非共振信号强度随混合溶液中乙醇的体积比增加而增加,且呈线性关系,进而说明了非共振信号强度随着分子数浓度N呈线性变化关系。因此,通过探测非共振信号强度与分子数浓度关系可以为混合物中特定成分的定量光谱分析提供一种研究途径。     

光纤维中的喇曼混频

我们在656厘米^-1到1343厘米^-1的频率范围研究了光纤维的调谐喇曼混频(RM)效应。在实验中观察到下列现象:相干反斯托克斯喇曼散射(CARS)的大小与逆喇曼吸收(VRA)的大小成反比;RM对受激喇曼散射(SRS)的强度分布有强烈影响。除了观测到相干斯托克斯(CSRS)和CARS辐射,还观测到二级相干斯托克斯(SOCSRS)和相干反斯托克斯(SOCARS)辐射。对实验结果进行了讨论。 关键词：     

用染料激光增益降低二元混合物中少量化合物的受激拉曼散射可探测浓度

在二元混合物构成的圆形谐振腔中,用染料的激光增益增强了少量化合物(乙醇溶液中的甲醇、水溶液中的乙醇)的受激拉曼散射（SRS）光谱,将少量化合物在悬垂液滴中的瞬态SRS探测极限提高了近一个数量级. 用受激拉曼散射理论,解释了增强少量化合物SRS的机理. 关键词： 受激拉曼散射 染料激光增益 二元混合物 最小可探测浓度     

非线性拉曼激光雷达测量CO2气体的研究

提出了利用气体的受激拉曼散射(SRS)效应激光雷达光源来探测大气中的CO2气体的新方法,设计出探测大气中CO2气体含量的非线性拉曼增益激光雷达,用Nd:YAG激光器(1064 nm)的三倍频光(354.7 nm)通过分别装有CO2气体和N2气体的拉曼管,分别得到CO2气体和N2气体的受激拉曼散射的一阶斯托克斯线(S1),并用S1线作为雷达的种子发射光源.通过实验得到拉曼管中的气压与S1能量的变化关系,对其优化条件和物理机制进行了分析.该实验方法已经成功测出了大气中CO2气体的回波电压信号.     

罗丹明B荧光增强苯受激拉曼散射研究

将液芯光纤技术与荧光增强受激拉曼散射技术相结合,能够大大增强受激拉曼散射光谱强度,降低受激拉曼散射阈值。通过对罗丹明B苯溶液在液芯光纤中的受激拉曼散射进行研究,结果表明:荧光染料Rhodamine B可以降低苯溶液的各阶受激拉曼散射阈值近一个数量级;在一定浓度范围内(10-6mol/L~10-8mol/L)各阶Stokes阈值随浓度降低而降低,并在理论上给出了解释。并且理论推导了在荧光种子作用下的四阶耦合波方程。液芯光纤中的受激拉曼光谱技术在对实现宽带受激辐射激光器、种子激光,以及生物大分子结构研究、生物分子的非生物过程研究等领域等有光明应用前景。     

驱动激光束间相干性以及对背向散射影响的研究

早期的研究表明, 束匀滑技术能够有效地抑制高功率激光与等离子体相互作用中产生的各种参量不稳定性, 大大减少受激布里渊散射和受激拉曼散射. 但在NIF最近的实验研究中发现, 受激布里渊散射和受激拉曼散射份额远远高于预期, 原因可能与驱动激光束间的相干性有关. 本文利用"神光II"装置两路倍频纳秒激光辐照金平面靶, 研究了小口径取样情况下两者背向散射的能量和光谱在不同驱动激光相干条件下的变化情况. 初步结果表明, 激光束间存在着较强的相干性, 并且随着束间相干程度的增加, 背向散射也逐渐增强.     

空气中O2和N2摩尔分数的拉曼散射多通道测量

开发了一套基于激光拉曼散射的多通道气体光学检测系统,应用于空气中主要组分的摩尔分数定量测量.针对性的设计了532 nm激光脉冲展宽器,能有效地避免脉冲激光在高能量状态下造成气体裂解、石英玻璃损伤等现象的发生,提高了气体拉曼散射的信噪比.在实验室环境压力和温度下,对气体样池内空气进行了长66 mm×直径1 mm激发区域同步10通道(每通道长约6.6 mm)的拉曼散射实验.得到了各通道下氧气(O2)和氮气(N2)的拉曼光谱和摩尔分数,及O2相对于N2的相对响应因子RO2.完成了26次重复性实验,每次为200个激光脉冲激发自发拉曼光谱的累加.结果表明,各通道间计算的平均的氧摩尔分数x-O2和相对于氮气的相对响应因子-RO2的标准偏差分别为0.015和0.024,但它们的平均值与10通道合并方式下的实验结果完全相同,准确率达98%,完全满足实时地并具有时空分辨力的定量测量混合气体摩尔分数的要求.该系统可满足于各种动态燃烧过程的光谱检测与分析.     

Laser diagnostics of ultrasonic outgassing of an insulating liquid

The efficiency of hydrogen evolution from transformer oil into a vacuum and into air under normal pressure is studied for the case when the oil is exposed to focused ultrasonic radiation. The study is performed by the method of spectroscopy of biharmonic-pumping coherent anti-Stokes Raman scattering (CARS) based on stimulated Raman scattering (SRS). Ultrasonic radiation at a frequency of 1.76 MHz is excited by a spherical piezoceramic transducer mounted on the bottom of the vessel and is focused on the surface of the oil. This causes the intense stirring of the oil with the formation of a fountain. The room-temperature diffusion coefficient of hydrogen in the transformer oil, 10⁻⁷ m²/s, is found by approximating experimental data by a theoretical relationship for hydrogen evolution into air. It is shown that ultrasonic radiation with a power density of 2.2 kW/m² accelerates diffusion processes ten-to fifteen-fold.     

H2的振动及转动受激喇曼散射研究

本文研究了不同泵浦光偏振态及氢气气压时,氢的振动及转动受激喇曼散射的竞争效应.在5atm的氢喇曼池中,以波长为532nm的椭偏激光为泵浦源,当椭圆的压缩系数为tg26°～tg32°时,获得了60多条Q(1)和S(1)混合谱线.并在低压氢及线偏或准线偏光泵浦条件下,观察到迄今尚未见报道的受激R(1)喇曼谱线.     

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.     

Stimulated Raman scattering of lattice translational modes in liquid heavy water

A study was conducted on stimulated Raman scattering (SRS) when laser-induced plasma is formed in heavy water by focusing an intense picosecond pulsed Nd:YAG laser beam with wavelength 532 nm at room temperature. An unexpected 280 cm(-1) low frequency SRS line attributed to the lattice translational modes is observed. This SRS line and the internal-mode SRS lines indicate that the ice VII structure is formed in heavy water under the condition of laser-induced shockwave production.     

Lidar Probing of a Mixture of Hydrogen Sulfide and Methane Molecules in the Atmosphere from a Flying Platform

Optics and Spectroscopy - The results of numerical solution of the lidar equation for the Raman scattering on the molecules of a gas mixture of hydrogen sulfide and methane in the 180°...