采用圆偏振啁啾飞秒激光脉冲操控CS2分子的相干拉曼散射过程

采用两束圆偏振啁啾飞秒激光脉冲,非共线相干激发三原子分子CS₂液体. 在相位匹配的方向上,探测到由CS₂频率为397 cm^-1的振动模式产生的强度对称分布的相干反斯托克斯拉曼散射(CARS)信号和相干斯托克斯拉曼散射(CSRS)信号. 当调整两束激发光的圆偏振状态时,CARS,CSRS信号的强度、偏振、波长均发生规律性的改变:CARS,CSRS信号的强度分布反映了CS₂ 在不同极化状态下的受激拉曼散射截面大小;信号光的 关键词： 啁啾脉冲 相干反斯托克斯拉曼散射(CARS) 相干斯托克斯拉曼散射(CSRS) 2')" href="#">CS₂     

基于光强传输方程相位成像的宽场相干反斯托克斯拉曼散射显微背景抑制

相干反斯托克斯拉曼散射(CARS)显微能够对样品的特殊化学组分进行选择性成像,无需荧光标记,在生物医学领域被广泛应用.然而,传统的CARS图像往往存在非共振背景信号.本文将基于光强传输方程的单光束相位成像技术用于CARS显微成像,来抑制CARS的非共振背景信号.该方法通过记录样品在三个相邻平面上的CARS图像,然后利用光强传输方程获取CARS光场的相位分布,最后利用共振CARS信号和非共振背景信号在相位上的差异,实现了对背景噪声的抑制.该方法无需参考光,通过三次测量可完成CARS的背景噪声抑制,具有良好的应用前景.     

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：     

单模光纤中超快受激拉曼散射的反斯托克斯波

由光纤中光的基本传输方程出发 ,利用慢变振幅近似 ,给出了包含反斯托克斯波的光纤超快受激拉曼散射的耦合波方程。以此为基础讨论连续、超快受激拉曼散射中泵浦波、斯托克斯和反斯托克斯波的耦合 ,分析了单模光纤相位匹配和群速匹配对光纤超快受激拉曼散射反斯托克斯波产生的影响     

燃烧流场线CARS测温技术研究

常规CARS采用凸透镜聚焦多束激光于空间一点,在满足相位匹配条件下产生携带该点温度信息的CARS信号。常规CARS一次只能测量一个空间点的温度,难以满足燃烧流场深入研究需要。为了提高CARS测量能力,使得CARS在一次测量中获得更多信息,提出了线CARS测量方法。线CARS测量方法在常规CARS基础上采用柱面凸透镜替换普通凸透镜,使得聚焦位置由焦点变为焦线。由于焦线上的点大部分满足相位匹配关系,因此可以同时获得多点CARS信号。后续光路同样采用柱面凸透镜替换普通凸透镜,通过光谱仪和ICCD相机将CARS信号传输至计算机,解析出聚焦线上CARS信号对应的温度信息,实现CARS测量能力由“点”到“线”的提升。基于平面火焰炉的燃烧实验结果表明：线CARS可以一次有效测量200个空间点的温度信息,空间测量长度约3.6 mm,空间分辨率约18 μm,测量结果相对不确定度优于7%,在保持测量精度的同时有效丰富了单次测量信息。     

光子晶体光纤中高效的反斯托克斯信号产生

基于四波混频的反斯托克斯变换, 被广泛应用于短波辐射高分辨率成像以及直接激发分子的电子跃迁等方面. 为了实现更加高效的反斯托克斯变换, 利用中心波长为810 nm脉冲宽度为120 fs的钛蓝宝石(Ti: sapphire)飞秒激光器作为抽运光源, 在长度为0.5 m和3 m的光子晶体光纤中分别实现了高阶模和基膜的简并四波混频. 实验中, 采用的光子晶体光纤的零色散波长在820 nm附近. 在基模相位匹配条件下, 在560 nm附近实现了高效地反斯托克斯信号的产生, 反斯托克斯信号与残余抽运信号的最大功率比为33:1; 反斯托克斯信号和斯托克斯信号的最大功率比25:1; 反斯托克斯信号最大功率转换效率P_a/P_p0为34%. 抽运波长从790 nm逐渐增加到810 nm过程中, 在长为3 m的光子晶体光纤中相位从不匹配状态转化为高阶模匹配状态后, 再转化为基模匹配状态. 通过实验研究得出了相位匹配程度随抽运功率、波长和光纤长度的变化规律, 同时分析了造成理论计算与实验结果存在差异的主要因素. 本文为研究在光子晶体光纤基模中实现相位匹配和产生高效反斯托克斯信号提供了理论和实验依据.     

基于拟合衰减差自补偿的分布式光纤温度传感器

针对斯托克斯光和反斯托克斯光的本质损耗、附加损耗使分布式光纤温度传感器产生测温误差的问题,通过对分布式光纤温度传感器的温度解调原理的研究,提出了拟合斯托克斯光与反斯托克斯光之间衰减差的方法实现温度自补偿,以此减小测温误差.以传感光纤上不同位置的两部分作为参考段和测温段,参考段的光信号作为测温段拟合多阶衰减差和解调温度的参量,通过引入多阶拟合结果解调温度,减小因斯托克斯光和反斯托克斯光的本质损耗、附加损耗导致的温度误差,实现温度的初步修正.改变光纤上同一位置的温度,取3组不同温度值及对应信号值计算引入拟合衰减差前后的瑞利噪声,分析了瑞利噪声与光纤长度和温度的关系,通过引入拟合衰减差消除瑞利噪声,减小了斯托克斯光和反斯托克斯光的本质损耗、附加损耗导致的瑞利噪声误差,实现温度的再次修正.分析比较多阶衰减差拟合结果对测温误差以及消除瑞利噪声的影响,获得最优拟合阶次.在拟合因参考段的附加损耗而导致的测温段的附加误差后,通过拟合结果进行温度补偿,完成了最终温度修正.实验结果表明,在30-90℃,引入一阶线性拟合结果的温度修正效果最好,经过三次修正后,测温误差从10.50℃降低至0.90℃.     

PLIF法定量测量甲烷-空气火焰二维温度场分布

利用平面激光诱导荧光(PLIF)技术，通过选择适合的OH自由基激励线，定量测量了甲烷-空气燃烧火焰的二维温度场分布。给出炉面中心上方火焰温度随离炉面高度的变化和距炉面12 mm高处沿炉面水平方向变化的实验测量结果并进行了讨论与分析。与利用相干反斯托克斯喇曼散射（CARS）技术进行测温的实验结果相比，该测量的相对不确定度优于5％。     

甲烷-空气预混V形火焰的CARS实验研究

本文将相干反斯托克斯(CARS)理论光谱计算和实验光谱分析的方法应用于预混V形火焰燃烧的温度测量实验,利用N2的Q支CARS谱线,使用单脉冲宽带方法获得了预混V形火焰的CARS信号光谱强度特性,测量了V形火焰水平方向和竖直方向上的温度分布特征,从中得出了火焰锋面的厚度,分析了火焰锋面的皱褶与摆动对CARS信号的影响。同时测量了不同燃料系数下V形火焰燃烧产物的温度,得出了温度随燃料系数的变化趋势,为进一步研究预混 V形火焰的结构提供了依据。     

可调空间分辨USEDCARS技术研究

相干反斯托克斯拉曼散射（CARS）技术是一种非常重要的燃烧诊断技术,该技术具有非常强的抗干扰能力和非常高的测量精度。但空间分辨力不足会使CARS技术产生很强的空间平均效应,引起成CARS光谱畸变,进而造成CARS光谱分析困难,无法通过CARS光谱反演燃烧场参数。针对非稳腔空间增强探测CARS（USEDCARS）技术存在的空间分辨不足以及空间分辨力不易改变的特点,分析了影响USEDCARS技术测量空间分辨力的各种因素,采用一组轴棱锥对USEDCARS系统中的泵浦激光进行环状光束整形,并通过调节轴棱锥之间的距离获得了不同直径的环状光束,在此基础上,建立了空间分辨可调USEDCARS诊断系统。开展了空间分辨力分析实验,获得了CARS信号强度随空间位置的分布数据,以CARS信号总强度95%包含的空间区域代表CARS的纵向空间分辨力,以此计算得到了CARS系统空间分辨力为1.7～6.5 mm连续可调。其中,高分辨力情况,达到了现有BOXCARS技术的空间分辨力。利用所建立的空间分辨可调USEDCARS诊断系统测量了酒精/空气预混火焰温度参数,获得了不同空间分辨条件下的CARS光谱。空间分辨力为1.7 mm时,获得了高质量CARS光谱,通过光谱拟合给出了所测火焰的温度信息。分辨力分别为4.9和6.5 mm时获得了较强的CARS信号,但存在光谱畸变。结果显示,空间分辨力对CARS信号的强度和空间平均效应有很大地影响,提高测量的空间分辨力可以有效消除空间平均效应,获得准确的CARS光谱,增强光谱拟合精度,同时空间分辨可调的特性使该系统能够更好地适应不同实验条件下的诊断工作。     

Ultrafast Raman loss spectroscopy

This paper deals with a new form of nonlinear Raman spectroscopy called ‘ultrafast Raman loss spectroscopy (URLS)’. URLS is analogous to stimulated Raman spectroscopy (SRS) but is much more sensitive than SRS. The signals are background (noise) free unlike in coherent anti‐Stokes Raman spectroscopy (CARS) and it provides natural fluorescence rejection, which is a major problem in Raman spectroscopy. In addition, being a self‐phase matching process, the URLS experiment is much easier than CARS, which requires specific phase matching of the laser pulses. URLS is expected to be alternative if not competitive to CARS microscopy, which has become a popular technique in applications to materials, biology and medicine. Copyright © 2009 John Wiley & Sons, Ltd.     

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.     

Phase‐locking of two independent degenerate coherent anti‐Stokes Raman scattering processes: concept,proposed all‐optical implementation,and potential applications

A novel approach toward phase‐locking of two independently produced yet energetically degenerate coherent anti‐Stokes Raman scattering (CARS) processes is put forward. The proposed all‐optical implementation involves a modified Mach–Zehnder interferometer, which is utilized to transfer phase coherence from three totally uncorrelated laser beams into two degenerate CARS beams that are produced in two distinct Raman active samples. Such a CARS interferometer based on coherent phase transport allows explicit measurement and control of phase differences between the two phase‐locked degenerate CARS processes, and hence may find applications in pertinent research fields such as CARS spectroscopy (tomography) as well as quantum information processing and transfer. Copyright © 2011 John Wiley & Sons, Ltd.     

Ultrabroadband (>2000 cm-1) multiplex coherent anti-Stokes Raman scattering spectroscopy using a subnanosecond supercontinuum light source

We have developed ultrabroadband (>2000 cm(-1)) multiplex coherent anti-Stokes Raman scattering (CARS) spectroscopy using a subnanosecond (sub-ns) microchip laser source. A photonic crystal fiber specifically designed for sub-ns supercontinuum (SC) generation has been used for obtaining ultrabroadband Stokes radiation, which enables us to achieve simultaneous vibrational excitation in the range from 800 to 3000 cm(-1). We have successfully obtained multiplex CARS spectra for several molecular liquids. Since the CARS system using the sub-ns SC is simple and compact, it can be easily applied to ultrabroadband multiplex CARS microspectroscopy.     

Single‐beam coherent anti‐Stokes Raman scattering (CARS) spectroscopy of gas‐phase CO2 via phase and polarization shaping of a broadband continuum

Coherent anti‐Stokes Raman scattering (CARS) spectroscopy of gas‐phase CO₂ is demonstrated using a single femtosecond (fs) laser beam. A shaped ultrashort laser pulse with a transform‐limited temporal width of ∼7 fs and spectral bandwidth of ∼225 nm (∼3500 cm⁻¹) is employed for simultaneous excitation of the CO₂ Fermi dyads at ∼1285 and ∼1388 cm⁻¹. CARS signal intensities for the two Raman transitions and their ratio as a function of pressure are presented. The signal‐to‐noise ratio of the single beam–generated CO₂ CARS signal is sufficient to perform concentration measurements at a rate of 1 kHz. The implications of these experiments for measuring CO₂ concentrations and rapid pressure fluctuations in hypersonic and detonation‐based chemically reacting flows are also discussed. Copyright © 2010 John Wiley & Sons, Ltd.     

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.     

Tunable light source for coherent anti-Stokes Raman scattering microspectroscopy based on the soliton self-frequency shift

We present a photonic crystal fiber (PCF)-based light source for generating tunable excitation pulses (pump and Stokes) that are applicable to coherent anti-Stokes Raman scattering (CARS) microspectroscopy. The laser employed is an unamplified Ti:sapphire femtosecond laser oscillator. The CARS pump pulse is generated by spectral compression of a laser pulse in a PCF. The Stokes pulse is generated by redshifting a laser pulse in a PCF through the soliton self-frequency shift. This setup allows for probing up to 4000 cm(-1) with a spectral resolution of approximately 25 cm(-1). We characterize the stability and robustness of CARS microspectroscopy employing this light source.