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.     

光解产生的铅原子中受激喇曼散射和共振激光辐射

用2660(?)的紫外激光解离PbCl_2分子时,发现在3740(?)和3734(?)波长上有较强的受激辐射输出.根据它们的光谱特性和铅原子的能级结构判断,这些辐射是基于双光子解离PbCl_2分子得到的铅原子在6p~(23)P_2亚稳能级上的布居而产生的光泵共振激光辐射和受激喇曼散射.提出了描述整个过程的理论模型,通过拟合实验结果,确定了2660(?)激光双光子解离PbCl_2产生6p~(23)P_2亚稳态铅原子的光解系数.当PbCl_2分子密度为N_(00)=6.21×10~(16)cm~(-3)时,光解产生的铅原子在6p~(23)P_2和6p~(21)D_2这两个亚稳态的最大布居数近似相等,称为2.0×10~(16)cm~(-3).     

351nm激光入射大腔靶的受激Raman散射光谱

 报道了“神光 Ⅱ”装置上Au大柱腔靶产生的受激Raman散射光谱。通过分析实验条件和测量结果，排除了散射光谱来自增强非相干Thomson散射的可能性，发现用丝化不稳定性与受激Raman散射的耦合能合理解释观测到的Raman光谱。考虑到丝化不稳定性与SRS的耦合，测量到的散射光谱依然能用于密度诊断，其结果与对流SRS理论的计算值相差不到10%。     

双包层光纤激光器的受激拉曼散射与热应力

 建立了高功率掺镱双包层光纤激光器的速率方程模型与热应力模型,对影响受激拉曼散射效应和热应力效应的关键参数（如纤芯半径、光纤长度、泵浦波长、泵浦方式）进行了数值模拟。结果表明:对于较小的纤芯半径,光纤内的斯托克斯光功率较大且增长迅速,因此增加纤芯半径能有效减弱受激拉曼散射效应;减小光纤长度能提高受激拉曼散射的阈值,而纤芯的热应力也增大,因此在不出现热应力引起光纤断裂的情况下,可以减小光纤长度以提高输出功率;采用976 nm波段泵浦源能提高输出功率,降低热应力的影响;两端均匀泵浦方式可以有效降低纤芯热应力,同时维持高功率输出。     

皮秒激光抽运高压H_2的受激拉曼散射研究

利用Nd :YAG锁模序列脉冲激光 (10 6 4nm)抽运充有高压H2 的拉曼池 ,输出光束经棱镜分光后投射在屏上 ,在可见光及近紫外光区用彩色胶卷摄得 15个受激拉曼散射光斑 ;经 1m光栅摄谱仪摄谱 ,在 36 5— 6 0 5nm波长范围内得到 6 5条受激拉曼谱线 .通过实验结果与理论计算值的比较 ,证明除了H2 的振动拉曼频移量 4 15 4 6cm- 1 外 ,还有多个振动及转动拉曼频移量共同参与作用 ,从而产生了从紫外到红外众多波长的受激拉曼散射光 .     

氢和甲烷混合气体的受激喇曼散射

使用调Q Nd~(3+):YAG激光的二次谐波(532nm)作为泵浦源,探讨了氢和甲烷混合气体的受激喇曼散射效应。利用光学光谱分析仪(OSA)监测,在不同比例的混合气体中,观测到氢和甲烷各自的SRS谱线以及两种气体的联合谱线,[m,n,=0,|±1,±2,…];观察到斯托克斯和反斯托克斯的谱线频移。实验表明两种气体的混合使得氢和甲烷的受激喇曼散射过程发生了竞争和耦合。     

Generation of high-order rotational lines by four-wave Raman mixing using a high-power picosecond Ti:Sapphire laser

More than thirty rotational lines equally spaced by 587 cm^–1 are generated simultaneously in the vicinity of the fundamental line by four-wave Raman mixing using a high-power picosecond Ti:Sapphire laser as a pump source and hydrogen as a Raman medium. Since the wavelength of this multifrequency laser emission extends from the near-infrared to the near-ultraviolet, it can be utilized as a tunable light source for picosecond spectroscopy. Because of the wide spectral bandwidth available, this procedure has great potential for the generation of ultrashort laser pulses by mode-locking these emission lines.     

强紫外激光在空气中长程传输受激旋转拉曼散射效应

 采用瞬态受激旋转拉曼散射（SRRS）模型，详细考虑了激光脉冲波形、介质的非线性极化、泵浦光的衰减、斯托克斯光的非线性放大以及拉曼线宽等诸多因素，对强紫外激光束在空气中长程传输过程产生的SRRS效应进行了研究。讨论了产生SRRS效应的阈值条件，详细分析了SRRS效应对激光光束质量的影响。     

水的低频受激拉曼散射

利用532 nm的脉冲激光进行了水的受激拉曼散射研究. 水的低激发光能量下主要表现为受激Stocks和反Stocks 3426 cm^-1谱线; 在能量大于140 mJ时出现低频率313 cm^-1受激Stocks谱线, 同时出现后向3389和3268 cm^-1 的受激Stocks谱线. 实验结果表明, 在较强的激光作用下, 水的结构表现为冰的Ⅷ相.     

皮秒激光瞬态受激喇曼散射的实验研究

本文采用对撞脉冲锁模Nd:YAG激光器输出10ps脉冲串,经KTP非线性晶体腔外倍频,泵浦喇曼介质为二甲亚砜(DMSO)液体.实验研究了不同透镜焦长、焦点位置及不同喇曼介质氏度对瞬态受激喇曼散射的影响,获得了能量转换效率分别为45.6%和10.5%的前、后向一阶斯托克斯-喇曼散射光,并对实验结果进行了讨论.     

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.     

2 ns,351 nm激光黑腔靶受激Raman散射实验研究

 介绍了在神光Ⅱ装置上开展的长脉冲2 ns,351 nm激光与黑腔靶相互作用的实验,报道了受激Raman散射光时间分辨谱图及能量测量的实验结果。长脉冲2 ns激光注入小腔靶（Ø700 mm×1 250 mm）时,激光辐照缝靶产生的SRS光能量是激光与全腔靶作用产生的SRS光能量的1.3倍。在2 ns激光与不同尺寸黑腔靶作用的情况下,激光辐照小腔靶产生的SRS光能量比标准腔靶(Ø800 mm×1 350 mm)产生的SRS光能量高1.6倍。由于激光功率密度下降,2 ns激光打靶SRS散射光要弱于短脉冲1 ns激光打靶,但持续时间稍长。实验结果表明：长脉冲2 ns激光与标准腔靶相互作用时,等离子体“堵腔效应”比较严重,标准腔靶尺寸不再合适。     

Thermal dissipation effects of the entangled photon generated by four-wave mixing process in a nonlinear ring resonator

We firstly analyze the thermal dissipation effects of the entangled photons generated by a nonlinear optical ring resonator. To obtain the corresponding equation of motion of the entangled photons generated by a four-wave mixing process within the system, we propose the Markov approximation to repel the reservoir operators. The system master equation in the interaction picture for both degenerate and non-degenerate cases is analyzed and obtained. The established system can be used to characterize the optimum entangled photons in some cases where the thermal dissipation effects may be introduced noise into the system. In this work, the entangled photons can be generated into two forms, firstly, the two entangled photon states is generated, the other, the four entangled photon states can be easily obtained. Results obtained have shown that the optimum entangled photon in term of entangled photon visibility can be compensated (i.e. unchanged) under thermal dissipation effects.     

部分离化激光等离子体的受激喇曼散射不稳定性

由于部分离化激光等离子体中存在束缚电子，它可显著改变其参量不稳定性。本文分析了部分离化激光等离子体的受激喇曼散射的非线性色散关系，计算了钕玻璃倍频和三倍频激光受激喇曼散射的增长率，结果表明，前向受激喇曼散射显著增强，后向受激喇曼散射影响不大。     

Stimulated Raman scattering in light and heavy water under picosecond laser excitation

The spectra of stimulated Raman scattering in ordinary and heavy water under excitation by second harmonic of a picosecond Nd:YAG laser were compared. It was shown that when stimulated Raman scattering is excited in water in cavities of a photonic crystal (synthetic opal matrix constructed of silica nanoglobules) or a photonic glass in the form of close-packed monodimensional millimeter-size amorphous-quartz balls, the efficiency of stimulated Raman scattering increases significantly compared to a uniform liquid medium.     

高功率双包层光纤激光器受激拉曼散射和热效应的理论研究

 受激拉曼散射和热效应会限制光纤激光器功率的提高。利用高功率光纤激光器的速率方程和热传导方程,理论研究了双端泵浦和分布泵浦下双包层光纤激光器的受激拉曼散射和热效应,得到了光纤中的泵浦光、激光和斯托克斯光的功率分布,光纤激光器的输出特性以及光纤中的温度分布。分析表明,当泵浦功率增大到一定值时,光纤激光器中出现SRS,一部分激光功率会转移给斯托克斯光,影响激光功率进一步提高;与双端泵浦方式相比,分布泵浦下光纤激光器的斜率效率和最大输出功率相差不大,但是,光纤中的温度分布被有效地降低,因此,分布泵浦方式更为有效。     

Temperature measurements in condensed phases using non‐resonant femtosecond stimulated Raman scattering

We have previously demonstrated the capability of femtosecond stimulated Raman scattering (FSRS) data to measure the temperature (T) of condensed matter at the molecular vibrational level. [Phys. Rev. Lett. 2011, 107, 43001] In this paper, we expand the theory for the FSRS temperature dependence by considering the effects of an isolated change of T as well as a coupled change of T and chemical concentration. We point out that the origin of the temperature sensitivity of the Stokes to anti‐Stokes ratio of FSRS lies in the exponential nonlinearity of the gain and loss. We establish that FSRS of two Raman modes can be used to simultaneously determine the vibrational temperature and the change in concentration of the species contributing to those two modes. Single‐shot experimental results using FSRS are presented to demonstrate over four orders of magnitude higher efficiency than spontaneous Raman in small volume samples with picosecond resolution. Copyright © 2012 John Wiley & Sons, Ltd.     

基于超连续光谱激发的时间分辨相干反斯托克斯拉曼散射方法与实验研究

采用钛宝石飞秒激光器输出的一部分光抽运光子晶体光纤以产生超连续光谱,作为抽运光和斯托克斯光,另一部分飞秒激光作为探测光,并结合时间延迟方法,建立超连续光谱激发时间分辨相干反斯托克斯拉曼散射(CARS)实验系统,测试了具有较宽拉曼光谱的二甲基亚砜样品.实验结果表明,所建立的实验系统能有效抑制非共振背景噪声,并且通过一次测量,即可获得二甲基亚砜在690—3200cm-1范围内的CARS光谱信息,获得的二甲基亚砜CARS光谱范围达到2500cm-1.同时给出了所采用的光子晶体光纤光谱展宽的实验结果.     

钡蒸气的受激喇曼散射及碰撞诱导受激辐射

在宽带XeCl激光泵浦的钡蒸气中,观察到波长分别为472.6nm,582.6nm和648.3nm的碰撞诱导受激辐射以及波长为475nm的受激喇曼散射.碰撞锈导受激辐射脉宽为3ns左右的自终止型短脉冲,其强度随缓冲气体压力的升高而上升.喇曼光脉冲前沿与泵浦光脉冲前沿之间有长20ns的时间延迟,喇曼转换效率随缓冲气体压力的升高而下降     

Stimulated Brillouin scattering limited intensity-dependent four-wave mixing between pump and signal in a non-zero dispersion shifted fiber

The intensity-dependent four-wave mixing (FWM) efficiency is derived by the nonlinear Schrodinger equations including the self phase modulation and cross phase modulation between the two Fabry–Perot modes of a pump and a single-wavelength signal. The maximum FWM for mixing the pump with signal in non-zero dispersion shifted fiber is explained as the minimum phase mismatch for FWM due to equal group delay for the pump and signal. It was also found that the experimental measurements for the generated FWM power are limited by the stimulated Brillouin scattering (SBS) threshold. Under the SBS threshold, the experimental results are still coincided well with the theoretical calculations of the FWM generated power ratio to have the difference of 0.12 dB for the input signal power of 12 mW.