关于超Raman效应中散射强度的计算

本文根据辐射的量子理论,对超Raman散射强度进行了计算。从理论上直接断言:所有具有振动红外活性的Raman介质都同时具有振动超Raman活性。由于偶极跃迁几率只对反Stokes超Raman散射线有贡献,所以反Stokes线与Stokes线的强度公式不对称,前者含有更丰富的频谱。并且对于低波数频移,即使在室温条件下,两者也几乎有同数量级的强度。最后讨论了超Raman散射中的共振效应。 关键词：     

High-spectral-resolution coherent anti-Stokes Raman scattering with interferometrically detected broadband chirped pulses

To achieve high-spectral-resolution multiplex coherent anti-Stokes Raman scattering (CARS), one typically uses a narrowband pump pulse and a broadband Stokes pulse. This is to ensure a correspondence between anti-Stokes and vibrational frequencies. We obtain high-resolution CARS spectra of isopropanol, using a broadband chirped pump pulse and a broadband Stokes pulse, by detecting the anti-Stokes pulse with spectral interferometry. With the temporally resolved anti-Stokes signal, we can remove the chirp of the anti-Stokes pulse and restore high spectral resolution while also rejecting nonresonant scattering.     

Diode-pumped nonresonant continuous-wave Raman laser in H2 with resonant optical feedback stabilization

We demonstrate a nonresonant cw Raman laser pumped by an optically locked diode laser at 790 nm that produces cw Stokes (1178-nm) and coherent anti-Stokes (595-nm) emission. Considering the modest pump powers, relative low cost, and predicted spectral purity, we expect that frequency downconversion of tunable diode lasers through stimulated Raman scattering will provide an attractive source for remote sensing, spectroscopic, and atomic physics applications. The Stokes laser threshold is 240+/-19muW pump power, and emission is observed over a roughly 10-nm range by adjustment of the optical locking feedback phase. Photon-conversion efficiency rises throughout the pump-power region, with a peak value of 15+/-2% .     

Multimode stimulated Raman scattering with squeezed light

Stimulated Raman scattering of a multimode pump light on an one-mode phonon system is examined. The pump light is expected to be strong, so that it can be treated classically. The phonon mode and scattered Stokes and anti-Stokes modes are described quantally. The phonon is prepared in a coherent state and the scattered modes are prepared in displaced and squeezed states at the input.The author would like to thank Dr. J. Peina for fruitful discussions, and Dr. A. Luk for comments on the results.     

Coherent anti-Stokes Raman scattering velocimetry with nearly degenerate pumps

The time evolution of the anti-Stokes signal produced from the non-linear interaction of a short Stokes pulse and two long pump pulses that are nearly degenerate in frequency has been investigated. It is shown that this approach allows us to specify the accuracy of CARS (coherent anti-Stokes Raman scattering) velocimetry and to extend the range of operation of the method. In addition, an original optical scheme capable of delivering short visible pulses with good spatial and spectral properties is reported. The optical bench has been used for the characterisation of a low-pressure laminar Mach-10 flow. Received: 24 October 2001 / Revised version: 8 January 2002 / Published online: 14 March 2002     

Generation of anti-Stokes radiation upon amplification of stokes pulses in transient stimulated Raman scattering

An analytical solution is obtained for equations of transient stimulated Raman scattering for short samples and a weak seed Stokes wave in the approximation of a given pump field, and a numerical solution for more extended media or more intense input Stokes pulses with allowance for pump depletion. The dependence of the anti-Stokes wave energy on its spatial mismatch with the Stokes and laser waves is studied. The optimum angle of the anti-Stokes generation is found as a function of the length of the system, transverse relaxation rate, laser pulse energy, and intensity ratio of the Stokes and pump pulses at the entrance of the sample.     

Calculation of the Stokes-component amplification with bias illumination in the anti-Stokes region

The effect of Raman absorption in the anti-Stokes region on Stakes-component Raman scattering is discussed for the case of stimulated Raman scattering. It is shown that the Raman interaction leads to a significant amplification of the Stokes-component radiation and that the anti-Stokes radiation converts into Stokes radiation in proportion to the ratio _s/ _as.Translated from Izvestiya Vysshikh Uchebnykh Zavedenii, Fizika, Vol. 12, No. 7, pp. 112–115, July, 1969.     

双折射光纤受激拉曼散射偏光特性的实验研究

对椭圆芯光纤受激拉曼散射偏光特性进行了系统的实验研究。实验巾观察到8级斯托克斯线和2级反斯托克斯线,对不同偏振态的抽运光激励下各级斯托克斯线的偏振特性、拉曼频移等参量进行了分析,并给出了经验公式。其结果与实验数据符合良好。实验表明,双折射光纤受激拉曼谱的各级斯托克斯线的偏振状态不但与拉曼介质有关还与抽运光的偏振态有关,入射抽运光偏振态对低阶次的斯托克斯线拉曼频移的影响较小,而对高级斯托克斯线拉曼频移影响较大。     

Selective excitation and suppression of coherent anti-Stokes Raman scattering by shaping femtosecond pulses

Femtosecond coherent anti-Stokes Raman scattering (CARS) suffers from poor selectivity between neighbouring Raman levels due to the large bandwidth of the femtosecond pulses. This paper provides a new method to realize the selective excitation and suppression of femtosecond CARS by manipulating both the probe and pump (or Stokes) spectra. These theoretical results indicate that the CARS signals between neighbouring Raman levels are differentiated from their indistinguishable femtosecond CARS spectra by tailoring the probe spectrum, and then their selective excitation and suppression can be realized by supplementally manipulating the pump (or Stokes) spectrum with the $\pi $ spectral phase step.     

斯托克斯和反斯托克斯拉曼位移差与时间反演对称性

首先列出若干Stokes和anti-Stokes位移不对称的事例,并在此基础上指出,如果将anti-Stokes散射严格定义为Stokes散射的时间反演行为,则对于初态或末态具有Kramers简并的体系,Stokes和anti-Stokes散射的拉曼位移可以不同.这是因为时间的正过程和反演过程各对应于不同的跃迁途径,其位移大小的差别与简并能级的分裂值相关.     

Relation of pump-beam quality and conversion efficiency in the Raman downward conversion

To investigate the full conversion of pump power to the Stokes waves in stimulated Raman scattering with a single-pass cell, unconverted pump energies have been analyzed in detail in relation to the first Stokes, second Stokes and first anti-Stokes energies. Adoption of a long focusing configuration with a high-pressure cell was found to be effective but insufficient to suppress the four-wave mixing effect, because a small amount of pump energy always remained undepleted. Comparison of the results using pump beams of various spectral and spatial mode characteristics from alexandrite and Nd:YAG lasers revealed that the spatial mode quality was the most critical parameter for full depletion of a pump pulse.     

On the spectra of resonant coherent Raman scattering

The spectra of resonant coherent anti-Stokes and Stokes Raman scattering of excited molecules are calculated and discussed. The interaction of light and molecules is treated semi-classically. The energy level diagram of four energy levels describing the process is used in four modifications possible for excited molecules. It is shown that non-vibrational resonances give extra maxima in some of the spectra. Comparison of the spectral structure in the Stokes and anti-Stokes components gives information on which of the four schemes the interaction is realized by. The influence of the pumping detuning on the Stokes component shape is pointed out.     

Observation of intense stokes and anti-stokes lines in CH4 pumped by 355 nm of a Nd:YAG laser

The stimulated Raman scattering (SRS) and four-wave mixing (FWM) processes have been studied in detail in CH₄ gas pumped by the third-harmonic of Nd:YAG laser at =355 nm. The conversion efficiency and average output energy have been measured for the various Stokes and anti-Stokes lines at different experimental conditions. The threshold input energy at various CH₄ pressures has been calculated for the unguided and capillary waveguide Raman cells. The calculated values for the capillary case have been compared with the measured values at different CH₄ pressures and the two results are in good agreement.     

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：     

Influence of the scattering matrix elements on the gain of Stokes and anti-Stokes components in the nonstationary regime

The influence of the scattering matrix elements that are responsible for the amplification of the Stokes and anti-Stokes components on the process of stimulated Raman scattering in the essentially nonstationary regime is analyzed. It is demonstrated that the optimum proportion between the scattering matrix elements, which maximizes the anti-Stokes component, is determined by the ratio between the optical frequencies of the components and the initial proportion between the intensities of the pump and initiating pulses. In the case of the optimum proportion between the scattering matrix elements, the variation in the excitation of a medium compensates the self-induced modulation of gain, and the efficiency of converting the radiation energy into the Stokes and anti-Stokes components increases substantially.     

色散位移光纤中拉曼散射与参量放大增益谱

由斯托克斯波和反斯托克斯波所满足的耦合微分方程,考虑泵浦波是线偏振光,其偏振方向沿x轴,推导出了同偏振方向受激拉曼散射和参量放大同时作用下,斯托克斯波和反斯托克斯波的增益谱.引入平行拉曼散射增益系数的洛伦兹模型,研究了色散位移光纤中斯托克斯波和反斯托克斯波的增益谱随相关参数的变化关系.结果表明,斯托克斯波与反斯托克斯波...     

强激光照射下,α-LiIO3晶体中晶格振动的多模激发和模之间的相互作用

本文叙述了用调Q倍频YAG脉冲激光照射α-LiIO₃晶体,在不同的散射配置下,获得了各种散射谱图。实验表明,当用e光入射时,可以比用o光入射激发起更多不同模的晶格振动;获得了E₂模的很强的一阶、二阶斯托克斯散射线和反斯托克斯散射线,E₁模Polariton的一阶、二阶、三阶斯托克斯线和反斯托克斯线,还获得了反斯托克斯频率区一条频移为469cm^-1的新线,认为是不同模的Polariton之间的相互作用引起的。最后,提到实验中初步观察到的晶体拉曼活性的“疲劳现象”。 关键词：     

SRS generation of anti-Stokes radiation under phase quasi-matching conditions

New methods of generation of anti-Stokes radiation of stimulated Raman scattering in media with changeable parameters of the third-order nonlinearity χ⁽³⁾ along the longitudinal coordinate are proposed. The conditions of obtaining phase quasi-matching in different media and reaching the maximum efficiency of conversion into the anti-Stokes component of stimulated scattering are determined by numerical methods. The dependence of the efficiency of energy transfer from the pump wave to the anti-Stokes wave on the ratio of intensities of the pump and Stokes waves at the input of the medium is studied. The models of the media in which the efficiency of generation of anti-Stokes radiation exceeds 30% are obtained. The results of the investigation can be used for the development of new efficient nonlinear optical devices upconverting the laser radiation frequency.     

Coherent anti-Stokes Raman scattering and normal anti-Stokes Raman scattering due to LO phonons in GaP using cw diode lasers

Coherent anti-Stokes Raman scattering (CARS) and normal anti-Stokes Raman scattering (NARS) have been measured in (001) GaP at room temperature due to the 403 cm⁻¹ LO phonons using a continuous wave (CW) 785.0 nm fixed-wavelength pump laser and a CW Stokes laser tunable in the 800-830 nm wavelength range. CARS measurements are normally made using pulsed lasers. The use of CW diode lasers allows a more accurate comparison between the measured and calculated values of the CARS signal. The pump and Stokes laser beams were linearly polarized perpendicular to each other, same as the pump and normal Stokes/anti-Stokes scattered light for the GaP sample used in this work. The pump and Stokes laser powers incident upon the GaP sample, located in the focal plane of a 20 mm effective focal length lens, were <20 and 50 mW, respectively. The diameter of the laser beams in the focal plane of the focusing lens was determined to 40±5 μm. The pump and Stokes laser beam intensities incident upon the 0.3 mm thick GaP sample were <2 and 5 kW cm², respectively. The powers of the CARS and NARS signals were measured using a Raman spectrometer. The signal output of the Raman spectrometer was calibrated using the pump laser and several neutral density filters. The Raman linewidth (full-width at half-maximum) of the LO phonons was determined to be 0.95±0.05 cm⁻¹, using the variation of the CARS signal with the wavelength of the Stokes laser. The measured powers of the CARS and NARS signals are about a factor of 5 and 1.5, respectively, smaller than those calculated from the corresponding theoretical expressions.     

High-sensitivity vibrational imaging with frequency modulation coherent anti-Stokes Raman scattering (FM CARS) microscopy

We demonstrate a new approach to coherent anti-Stokes Raman scattering (CARS) microscopy that significantly increases the detection sensitivity. CARS signals are generated by collinearly overlapped, tightly focused, and raster scanned pump and Stokes laser beams, whose difference frequency is rapidly modulated. The resulting amplitude modulation of the CARS signal is detected through a lock-in amplifier. This scheme efficiently suppresses the nonresonant background and allows for the detection of far fewer vibrational oscillators than possible through existing CARS microscopy methods.