Generation of multi-color stimulated raman emission from two-color linearly or circularly polarized pump beams

A laser beam at two different frequencies separated by 587 cm^–1 is focused into pressurized hydrogen (rotational transition energy, 587 cm^–1) to generate multi-color stimulated Raman emission. The polarization state and the pulse energy are measured for each generated emission line using linearly and circularly polarized pump beams. The effect of the polarization is discussed by using a parameter characterizing the polarizability of hydrogen and a conservation rule for the angular momentum in four-wave mixing. Many rotational lines are generated with linearly polarized pump beams through a four-wave mixing process. This is in striking contrast to the results obtained by using a single-color circularly polarized pump beam which generates only one rotational line through a conventional stimulated Raman process.     

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.     

Rotational Raman scattering dependence on pump polarization

The influence of the ellipticity degree of the pump radiation polarization on threshold energies and energy conversion efficiencies of stimulated rotational Raman scattering (SRRS) are investigated in H₂ with a XeCl excimer laser, by using different focusing geometries. For the first time, it is shown that the dependence of SRRS on pump radiation polarization is also affected by the focusing geometry, i.e. whether low- or high-angle focusing is applied. The experimentally determined threshold energies as a function of the pump radiation polarization are in accordance with theory mainly at high-angle focusing geometries. It is also shown for the first time that gain suppression effects on vibrational Raman scattering have to be considered in understanding the experimental results. Received: 5 January 1999 / Final version: 10 September 1999 / Published online: 8 March 2000     

Ultrahigh efficiency laser wavelength conversion in a gas-filled hollow core photonic crystal fiber by pure stimulated rotational Raman scattering in molecular hydrogen

We report on the generation of pure rotational stimulated Raman scattering in a hydrogen gas hollow-core photonic crystal fiber. Using the special properties of this low-loss fiber, the normally dominant vibrational stimulated Raman scattering is suppressed, permitting pure conversion to the rotational Stokes frequency in a single-pass configuration pumped by a microchip laser. We report 92% quantum conversion efficiency (40 nJ pulses in 2.9 m fiber) and threshold energies (3 nJ in 35 m) more than 1 x 10(6) times lower than previously reported. The control of the output spectral components by varying only the pump polarization is also shown. The results point to a new generation of highly engineerable and compact laser sources.     

Thermal loss mechanism in the generation of multifrequency laser emission via stimulated Raman scattering and four-wave Raman mixing studied by photothermal refraction spectroscopy

The heat produced in conjunction with the processes of stimulated Raman scattering and four-wave Raman mixing in hydrogen was measured by photothermal refraction spectroscopy. Many vibrational, rotational, and vibrationally shifted rotational Raman lines are exclusively/simultaneously generated by changing the polarization of the laser beam and the hydrogen pressure. Thermal loss occurs predominantly from vibrational Raman scattering, which can be ascribed to a large Raman shift frequency of 4155 cm^-1 for the vibrational transition. In contrast to stimulated Raman scattering, little or no thermal loss is observable during the process of four-wave Raman mixing. Received: 12 April 1999 / Revised version: 12 July 1999 / Published online: 20 October 1999     

测量时间分辨拉曼谱实验装置的研制

测量时间分辨拉曼谱实验装置的研制王晶晶金榕周赫田邹英华（北京大学物理系人工微结构及介观物理国家重点实验室北京１００８７１）孙志勇（北京理工大学四系４３１教研室北京１０００８１）ＴｈｅＥｘｐｅｒｉｍｅｎｔａｌＳｅｔｕｐｆｏｒＴｉｍｅ－ＲｅｓｏｌｖｅｄＲ...     

Tuning of group delay with stimulated Raman scattering-induced dispersion in gas-filled optical fiber

We report the first demonstration of group delay tuning with stimulated Raman scattering-induced dispersion in a hydrogen-filled hollow-core optical fiber. A pump laser induces a sharp refractive index change near the S_0(0)Raman transition of hydrogen molecules, enabling the control of the group velocity of signal pulses around the Stokes wavelength. Experiments with an 80-m-long hollow-core fiber filled with 2.5 bar hydrogen achieved continuous tuning of the pulse delay up to 1.42 ns by varying the Raman amplification from 0 to 10 dB. The tunable pulse delay is realized by changing the pump power as well as the hydrogen pressure. This work provides a new technique for controlling the pulse propagation in optical fibers with high flexibility.     

Chirped-pulse four-wave Raman mixing in molecular hydrogen

Four-wave Raman mixing (FWRM) in molecular hydrogen was studied using chirped pump and Stokes pulses emitting at 802 and 1,203 nm, respectively. The group delay dispersion (GDD) of the anti-Stokes pulse was examined employing a frequency-resolved optical gating system at different GDDs of the pump and Stokes pulses (0 or ±1,000 fs²). As a result, the energy and the sign of GDD for the anti-Stokes pulse remained unchanged, when the pump and Stokes pulses had the GDD with the same sign. When the sign was not the same, the energy decreased and only the portion useful for resonant FWRM was converted into a Raman emission. This technique has a potential for use in compensation of dispersion by passing the negatively chirped high-order Raman sidebands through the optics with positive chirps in the spectral region from the deep-ultraviolet to the near-infrared, to generate multiple transform-limited Raman pulses and then to produce an ultrashort optical pulse by a Fourier synthesis of these Raman emissions.     

Efficient rotational Raman conversion of XeCl laser radiation in H2

2 is investigated with a XeCl laser. It is shown that energy conversion to rotational Stokes radiation can be efficiently obtained by properly choosing the focusing geometry of pump radiation and the pressure of the Raman medium even at moderate pulse energies. Energy conversion to the first rotational Stokes at 313.8 nm with efficiencies as high as 38% is obtained with a circularly polarised XeCl pump beam of 10-mJ energy focused in 30 bar of H₂. The spectral and optical characteristics of the pump and the rotational Stokes radiation are analysed. Received: 29 May 1996/Revised version: 7 March 1997     

Backward Raman amplification in a plasma waveguide

Backward Raman amplification of a short laser pulse in a plasma waveguide is demonstrated. With a guided seed pulse of 0.8-microJ energy and a pump pulse of 345-mJ energy in a 9-mm-long optically preformed plasma waveguide, 910-fold energy amplification is achieved. Heating of the plasma by the long pump pulse is identified to be a key issue for plasma-waveguide-based backward Raman amplifiers.     

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。     

拉曼效应和参量放大共同作用下增益谱特性

根据激光脉冲在双折射光纤中传输时, 拉曼效应和参量放大共同作用下所所遵循的耦合模方程, 基于平行拉曼增益的洛伦兹模型, 给出了输入抽运波偏振方向沿相互正交的双折射轴时, 拉曼效应和参量放大共同作用所导致的增益. 讨论并分析了在不同色散区相关参量对增益谱特性的影响. 结果表明, 拉曼效应改变了非线性和色散的相互平衡, 使得参量放大斯托克斯波与反斯托克斯波增益谱彼此不对称; 当输入功率一定时, 其增益谱结构确定, 非线性系数和色散系数两者之间相对变化时, 增益谱的强度和展宽有所改变.     

利用拉曼孤子实现宽带拉曼脉冲压缩

从拉曼散射方程的出发,研究了利用拉曼孤子实现宽带拉曼脉冲压缩的机制,发现孤子脉冲的宽度随拉曼增益的增加减小,并与 运光的脉冲形状及相位结构有关。实验中利用ＸｅＣｌ激光／Ｈ２系统初步实现了５０％的压缩率,并将实验结果与理论进行了比较。     

光纤拉曼放大器中增益的偏振相关特性研究

提出了一种改进的、可用于计算偏振相关拉曼增益的光纤拉曼放大器的非线性耦合波方程。建立了单模双折射光纤拉曼增益的数学模型,分析了线偏振抽运光以与光纤快轴成45°激励的单模双折射光纤拉曼放大器模型与实际具有随机双折射的光纤拉曼放大器的拉曼增益偏振相关特性的等价性。基于上述模型,提出了一个可定量表征单模光纤偏振模色散统计特性的拉曼增益偏振相关因子,用以替代常规的光纤拉曼放大器非线性耦合波方程中的偏振相关因子。计算结果与已报道文献的实验数据非常吻合。同时对抽运增益在同向和反向抽运方式下截然不同的增益偏振相关特性给出了合理的解释。     

Stimulated Raman amplification characteristics in long span single-mode silica fibers

Spectral Raman amplification characteristics have been measured directly for a tunable pumping source, taking the relative polarization states of pump and signal waves into consideration. Raman amplification has been observed, even with an orthogonal polarization pump, in a long span single mode fiber. Raman amplification causes significant crosstalk in wave-length-multiplexed systems.     

Stimulated Raman scattering and four-wave Raman mixing seeded by a supercontinuum generated in dibromomethane using picosecond and femtosecond laser sources

Stimulated Raman emission from liquid dibromomethane (vibrational Raman shift frequency, 588 cm⁻¹) is introduced into hydrogen gas (rotational Raman shift frequency, 587 cm⁻¹) as a seed beam, in order to generate numerous rotational lines by four-wave Raman mixing. Unexpectedly, a supercontinuum, which is generated by self-phase modulation in dibromomethane, acted as a seed beam to exclusively generate vibrational lines; the rotational lines are generated only when the supercontinuum is minimal. The former is explained by a competition between the high-gain vibrational and low-gain rotational Raman effects when strongly seeded by a supercontinuum. The latter is explained by stimulated Raman gain under the seed effect exclusively to the first-Stokes rotational line.     

双折射光纤中拉曼效应对参量放大增益谱的影响

根据激光脉冲在光纤中传输时, 所满足的波动方程, 导出了拉曼效应和参量放大共同作用下, 在双折射光纤中所遵循的耦合模方程, 并引入平行拉曼增益的洛伦兹模型, 给出了输入抽运波偏振方向同双折射轴成45^o 时, 拉曼效应和参量放大共同作用所导致的增益. 讨论并分析了拉曼效应在不同色散区对参量放大增益谱的影响. 结果表明, 在考虑拉曼效应后, 使得参量放大斯托克斯波与反斯托克斯波增益谱彼此不对称; 在反常色散区, 产生的增益以反斯托克斯波为主, 正常色散区则以斯托克斯波为主.     

Raman gap solitons

We show that an intense pump pulse, detuned far from the Bragg resonance of a nonlinear periodic structure, can excite a gap soliton at a wavelength within the band gap that corresponds to the Raman shift of the medium. This Raman gap soliton is a stable, long-lived, quasistationary excitation that exists within the grating even after the pump pulse has passed. We find both stationary solitons as well as slow Raman gap solitons with velocities as low as 1% of the speed of light. The predicted phenomena should be observable in fiber Bragg gratings and other nonlinear photonic band gap structures.     

受激旋转拉曼散射效应对基频光光束质量的影响

 采用瞬态受激旋转拉曼散射(SRRS)和空间相位扰动模型，定量分析了泵浦光强度和脉冲宽度对基频光在空气长程传输过程中产生的SRRS效应的阈值距离和转换效率的影响，讨论了泵浦光空间相位畸变对长程传输后的基频光光束质量的影响。研究结果表明：SRRS效应的阈值距离随着泵浦光强度和脉宽的增大而变短；空间相位畸变对斯托克斯光和泵浦光的光强分布存在一定影响，对斯托克斯光相位分布的影响比对泵浦光相位的影响大；SRRS效应的存在将导致基频光光束质量明显变差，对谐波转换效率产生明显影响。     

Origin of spectral interferences in femtosecond stimulated Raman microscopy

In femtosecond stimulated Raman microscopy (FSRM), a spectrally narrow (Raman pump) pulse and a broad (Raman probe) laser pulse are employed to generate the Raman spectra of microscopic objects. The resulting spectra exhibit, in addition to the Raman bands, spectral modulations of comparable amplitude. Here a model is devised that attributes these modulations to a four‐wave mixing (FWM) process. Two light fields of the probe pulse and one field of the pump pulse serve as input fields. The resulting FWM field experiences a heterodyne amplification by the probe field. Simulations based on this model reproduce the appearance of the spectral modulations. Furthermore, the amplitude of the modulations exhibits dependences on the energies of pump and probe pulses as well as on the nonlinear refractive index n₂, which are in line with the model. Copyright © 2011 John Wiley & Sons, Ltd.