全频域下窄线宽激光器光谱线宽的分析

窄线宽激光器的线宽表征方式通常采用延时自外差法测量技术。该技术是通过延时光纤差拍产生一个与待测激光线宽相关的洛伦兹频谱,因此该频谱只具有单一的线宽表现形式。为了能够观察到激光器的线宽和频率噪声在其傅里叶频率分布下的完整特性,报道了一种基于β算法计算窄线宽激光器线宽的方法。该方法是结合频率噪声中的白噪声和1/f噪声分别诱导不同激光线型的理论,从而确定激光线宽。首先,对β算法的基本原理进行了详细的分析说明。通过基于维纳-辛钦定理,分析了窄线宽激光器不同频率范围内的频率噪声和激光线宽的依赖关系。阐明了在截止频率趋于0和无穷大的两个范围条件时,激光频谱特性从高斯线型向洛伦兹线型演变。同时推导出使两种线型转换的截止频率表达式,并将其转换为频率噪声函数,该函数定义为β分子线。此时频率噪声分量中高斯线型的总和即为激光线宽计算公式;其次,对窄线宽激光器的频率噪声和激光线型进行数值仿真。将通过OEwaves公司的OE4000互相关零差相位/频率噪声自动测试系统测得的频率噪声谱密度,带入β算法理论公式中。结果显示：1/f噪声导致激光呈现高斯线型,线宽随截止频率的增加而增大。而白噪声将导致洛伦兹线型,线宽不再随截止频率而改变。此外,在低频区域,频率噪声电平远大于其傅里叶频率,噪声调制系数较高,该部分噪声可以决定线宽大小。因此,高斯线型区域对应的频率噪声的积分,即为待测激光器的线宽;在高频区域,频率噪声电平与其傅里叶频率相差较小,频率波动较快,噪声对线宽影响可以忽略。并且频率带宽在截止频率范围内,计算的线宽误差较小。最后,实验上运用β算法对RIO公司的1 550 nm低噪声窄线宽激光器的频率噪声功率谱密度进行积分计算,成功获得了其不同傅里叶频率分布下对应的激光线宽值。其中β分子线将频率噪声中的白噪声和1/f噪声分隔两部分：当频率噪声谱密度大于β分子线时,激光即为高斯线型,线宽随频率积分带宽的增加而减少;而频率噪声谱密度小于β分子线时,激光呈现洛伦兹线型,线宽为定值不再改变。同时为了对β算法进行实验验证,搭建了延迟光纤为50 km、移频频率为60 MHz的延时自外差法测量系统。对注入电流为110 mA的RIO 1 550 nm低噪声窄线宽激光器的线宽进行实验测量,测量结果表明激光线宽为1.8 kHz,与上述β算法中2.8 kHz的频率带宽积分结果一致。充分证明了此算法的准确性。β算法可以对任意类型的窄线宽激光器进行线宽表征,对窄线宽激光器的研究具有重要意义。     

获取生物分子完整拉曼谱的时间分辨相干反斯托克斯拉曼散射方法的理论研究

利用半经典理论分析了三束中心频率不同的窄线宽激光光场在样品中的相互耦合过程,得到一组描述相干反斯托克斯拉曼散射(CARS)过程的耦合波方程。结合时间分辨方法的原理,得到了描述使用窄线宽激光脉冲的时间分辨CARS(T-CARS)方法的耦合波方程。采用数值模拟方法研究了T-CARS方法中CARS信号和非共振背景噪声与入射光场之间的关系以及分子振动的弛豫过程。说明分子振动的退相时间可以作为区分成份和结构相近的分子以及监测样品所处微环境变化的依据。基于使用窄线宽激光光源的T-CARS方法的理论分析说明了使用宽谱激光具有同时获取生物分子完整拉曼光谱的能力。     

近距离激光外差探测光学极限位移分辨率

通过统计理论和维纳-辛钦定理推导出激光外差探测系统光电流的功率谱函数,分析了光电流谱线分布与激光光源线宽、中频信号频率以及信号光相对本振光传输延迟时间的关系,修正了相关文献中光电流功率谱的理论公式.根据信号与噪声理论建立了激光线宽引起的相位噪声的一维概率分布模型,并据此得到了基于激光波长、探测距离以及激光线宽的极限位移分辨率的数学模型.对光电流的功率谱和外差光学极限位移分辨率进行了相关的数值仿真,结果表明延迟时间与相干时间的关系决定光电流谱线分布的情况.当激光波长为532 nm,激光线宽在1 kHz,探测距离为100 m时,光学极限位移分辨率为0.266 nm,相关文献中的实验数据与理论推导结果相符合.     

纳米流体激光自混频功率谱及其计算

激光自混频技术可用于纳米颗粒和纳米流体的探测。在纳米流体自混频信号自相关函数的基础上,理论推导了功率谱函数的表达式。结果表明,纳米流体的激光自混频信号功率谱是洛伦兹线型和高斯线型的卷积,即佛赫特(Voigt)线型。通过数值计算研究了各种典型情况下激光自混频信号功率谱的频谱特征,颗粒定向运动速度决定了多普勒频移和高斯线宽,颗粒粒度决定了洛伦兹线型的宽度,颗粒粒度和速度与功率谱之间的对应关系为纳米流体的测量提供了理论基础。     

多色宽带相干反斯托克斯拉曼散射过程的理论与实验研究

宽带相干反斯托克斯拉曼散射(coherent anti-Stokes Raman scattering,CARS)光谱技术能够同时获取完整的分子CARS光谱信息,以准确识别和定量分析混合物中的不同成分或未知成分.在宽带CARS光谱技术中,由于超连续谱激光有效光谱范围内各光谱成分的作用不同,分别会产生双色和三色CARS过程.这里我们在理论上分析了宽带激发条件下两种CARS过程的产生条件,以及不同CARS光谱信号强度与各激发光功率之间的关系.在此基础上,搭建了基于SC激光的宽带CARS光谱系统,分别实现了双色和三色CARS过程.通过对获得的苯甲腈样品的CARS光谱信号进行函数拟合分析,实验验证了上述两个过程中CARS信号的强度与各激发光强度之间的函数关系.理论和实验研究结果为进一步优化宽带时间分辨CARS光谱探测和显微系统,实现同时获取物质分子完整的CARS光谱信号提供了指导.     

利用CARS技术研究激发态Rb2和H2的碰撞转移

利用相干反斯托克斯拉曼光谱(coherent anti-stokes Raman spectroscopy,CARS)探测技术,研究了激发态Rb2与H<,2>间的电子-振转能级的碰撞转移.扫描CARS谱确认了H<,2>分子仅在v=1,J=1,2及v=2,J=0,1,2能级上有布居,用n1,n2,n3,n4,n5分别表示...     

用于互组跃迁谱测量的窄线宽激光系统

采用Pound-Drerer-Hall稳频技术将689 nm激光锁定在高精细度超稳极低膨胀系数材料腔上,实现用于探测锶原子互组跃迁谱的窄线宽激光.利用光腔衰荡光谱技术,测量了不同阶次多横模情况下腔的精细度,并在理论上分析了平凹型Fabry-Perot腔的损耗与多横模阶次的关系.考虑了光开关延时及探测器响应时间在测量中的影响,对腔衰荡时间的实验测量值进行了修正.利用光纤飞秒光频梳测量了激光器的频率漂移,测出窄线宽激光频率稳定度的秒稳优于2.8×10-13.利用窄线宽激光在锶原子束上观测到具有高信噪比的窄线宽原子跃迁谱线,实验测得谱线的线宽为55 kHz,该窄线宽原子谱线可应用于锶原子二级冷却激光绝对频率的精确测量及锶原子互组跃迁谱的四种同位素位移测量.     

宽带相干反斯托克斯喇曼散射法诊断固体燃剂燃烧场

 报道了采用单次脉冲非稳腔空间增强探测 相干反斯托克斯喇曼散射（USED CARS）技术诊断常压下固体燃剂瞬态燃烧场温度和氮气浓度。采用宽带USED CARS技术，在固体燃剂瞬态燃烧场获得了较高信噪比的单次激光脉冲氮气Q支CARS实验谱，用CARS理论计算软件拟合CARS实验谱，给出了固体燃剂瞬态燃烧场温度和氮气浓度在不同高度的分布，固体燃剂燃烧场温度约2 250K、氮气相对浓度16%～20%。     

光谱的精密仿真技术及NO的高分辨LMR谱的仿真研究

LMR(Laser Magnetic Resonance)光谱技术采用磁场扫描及磁场调制获得顺磁分子吸收谱线,其谱线具有Voigt线型及各不相同的磁场线宽.本文考虑线型理论模型和实验条件,提出了一种实现LMR谱精密仿真的方法,并设计了相应仿真计算程序.对¹⁵N¹⁶O的X²Π_3/2v=1←0,Q₂(2.5)在激光频率为1842.8160cm^-1处的塞曼跃迁谱进行了仿真,得到了理想的仿真效果.该方法可作为复杂光谱分析标识的有效辅助工具.     

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。     

高阶相干喇曼散射光谱研究

本文报道了利用YAG激光系统CARS装置研究方解石的高阶相干喇曼散射(CRS)的实验结果,观察到1—6阶相干反斯托克斯喇曼散射谱(CARS)和1—2阶的相干斯托克斯喇曼散射谱(CSRS),讨论了影响高阶CRS产生的因素及有关的问题。 关键词：     

Generalization of the lineshape useful in magnetic resonance spectroscopy

A new lineshape function is derived from the Tsallis distribution to describe electron paramagnetic resonance (EPR) spectra, and possibly nuclear magnetic resonance (NMR) spectra as well. This lineshape generalizes the Gaussian and Lorentzian lineshapes that are widely used in simulations. The main features of this lineshape function are presented: the normalization, moments, and first derivative. A number of experimental EPR spectra are compared with the results of simulations employing the new lineshape function. The results show that the new lineshape often provides a better approximation of the experimental spectrum. It is also shown that the new parameter of the lineshape function can be used to quantify the intermolecular spin-spin interactions.     

激发态Cs2和H2的电子-振转能级的碰撞转移

利用相干反斯托克斯拉曼光谱(CARS)探测技术, 研究了激发态Cs2与H2间的电子-振转能级的碰撞转移。用波长为532 nm和中心波长为716 nm的两束激光同时聚焦到样品池中, 扫描CARS谱确认了H2分子的S支(△v =1, △J=2)仅在v=1, J=4,5及v=2, J=3,4能级上有布居, 用n1、n2、n3、n4分别表示(2,4)、(2,3)、(1,4)及(1,5)上的粒子数密度。从CARS线的峰值得到n2/n1、n3/n1、n4/n1分别为6.34±1.27、3.66±0.73和1.45±0.29。转移能配置到振动、转动和平动的比例分别为0.44、0.06和0.50, 能量主要分配在振动和平动上。在T=523 K和PH2=2.5×103 Pa条件下, 通过求解速率方程组和对时间分辨CARS线轮廓的分析, 得到碰撞转移速率系数k1=(6.0±1.2)×10-14 cm-3s-1和k2=(4.0±0.8)×10-13cm-3 s-1。     

Theoretical modeling of single-laser-shot, chirped-probe-pulse femtosecond coherent anti-Stokes Raman scattering thermometry

Chirped-probe-pulse (CPP) femtosecond (fs) coherent anti-Stokes Raman scattering (CARS) spectroscopy for single-laser-shot temperature measurements in flames is discussed. In CPP fs CARS, a giant Raman coherence is created in the medium by impulsive pump-Stokes excitation, and the temperature-dependent temporal decay of this initial coherence is mapped into the frequency of the CARS signal using a CPP. The theory of the CPP fs CARS technique is presented. A computer code has been developed to calculate theoretical CPP fs CARS spectra. The input parameters for the calculation of the theoretical spectra include the temperature, probe time delay, ratio of the resonant and nonresonant susceptibilities, and parameters for characterizing the pump, Stokes and probe pulses. The parameters for characterizing the pump, Stokes and probe pulses are determined from the best fit of theoretical spectra to experimental spectra acquired from calibration flames at a known temperature. For spectra acquired in subsequent measurements, these laser parameters are fixed and temperature is determined as one of the fit parameters from the best fit of theoretical spectra to experimental spectra. For single-laser-shot CPP fs CARS temperature measurements performed in steady, near-adiabatic flames, the best-fit temperature distribution width is typically less than 1.5% of the mean temperature. The mean temperature is accurate to within approximately 3% with respect to the adiabatic flame temperature. The most significant limitation on temperature measurement accuracy is associated with the evaluation of the theoretical laser parameters. Significant improvements in the temperature measurement accuracy are expected once monitoring equipment capable of characterizing the spectrum and phase of each laser pulse is incorporated in the experiments.     

Hydrogen CARS thermometry in H2–N2 mixtures at high pressure and medium temperatures: influence of linewidths models

In order to improve the accuracy of H₂ CARS thermometry, H₂ Q-branch CARS spectra have been recorded for various H₂-N₂ mixtures in a high-pressure cell at different pressures and temperatures (up to 40 bar and 875 K). Due to the low spectral resolution of broadband CARS experiments, the relevant spectral lineshape factor is the linewidth ratio &(Q(3))/&(Q(1)), since Q(1) and Q(3) are the most intense lines of the Q-branch spectrum in this temperature range. For the first time, the speed-inhomogeneous effects are accounted for in the simulation of the CARS profiles. The evaluated temperatures are in good agreement with reference values obtained by thermocouples. The specific role on the accuracy of H₂ CARS thermometry of the speed inhomogeneity is carefully analyzed, in connection with the influence of the nitrogen concentration.     

Background-free cars studies of carbon monoxide in a flame

Background-free coherent anti-Stokes Raman spectra (CARS) of carbon monoxide have been obtained in a rich methane-air flat flame. Use of this background rejection method, requiring only two laser frequencies, results in an increase in signal-to-noise of over 200 in the |x⁽³⁾|² spectrum in comparison with normal CARS. In addition, this technique provides a means for determining the symmetry of observed Raman transitions. The principles of background-free CARS are derived, and the capabilities are demonstrated with experimental data.     

Effects of laser linewidth on coherent antiStokes Raman spectroscopy

Expressions for the generated antiStokes spectral density in coherent antiStokes Raman spectroscopy (CARS) are obtained, which take into account the finite linewidths of laser sources and which may be used to analyse observed spectra. Lorentzian and gaussian laser lineshapes are taken as special cases, which enable further analytic results for single and multiline CARS spectra to be derived. Emphasis is placed on scanning and broadband (multiplex) CARS techniques, and the choice of laser sources discussed from the spectral point of view. As examples of multiline spectra an analytical account of a periodic spectrum is presented and temperature measurement from Q-branch spectra is treated.     

1维非稳腔空间增强探测CARS技术对稳态燃烧场温度的测量

 建立了1维非稳腔空间增强探测CARS实验系统，该系统由光源（YAG激光器、染料激光器）、实验光路和信号采集系统组成。分别测量了空气和化学平衡比为1，甲烷流量为0.7 L/min的甲烷-空气预混火焰中的氮气Q支的CARS实验谱。给出了火焰不同高度处小范围内的温度分布结果，并对实验结果进行了分析，结果表明：预混火焰温度随高度的增加呈下降趋势，测量结果的不确定度优于7%。该技术可用于稳态燃烧场温度的测量。     

Spectral Intensity and Lineshape Measurements in the First Overtone Band of HF Using Tunable Diode Lasers

High-resolution absorption lineshapes for the P(3) and P(6) transitions of the first overtone (v = 2-0) band of HF at 296 K have been measured using a pair of distributed feedback diode lasers operating near 1.31 and 1.34 μm, respectively. Spectral line intensities and self-broadening parameters were determined by fitting the measured spectra with Voigt, Galatry, and Rautian lineshape models. Voigt profiles fit the low-pressure (<10 Torr) spectra of the P(3) transition reasonably well due to the relatively strong collisional broadening effect. Lineshape measurements of the P(6) transition (for pressures ranging from 5 to 60 Torr) show significant variation from the Voigt lineshape model due to velocity-changing collisions that effectively reduce the Doppler component of the spectral line. Lineshape models that include motional (Dicke) narrowing effects, Galatry (soft collision) and Rautian (hard collision) profiles yield significant improvements in the spectral lineshape fits compared with Voigt profiles. The collisional broadening coefficient (gamma) of the P(6) transition obtained from a Voigt fit is approximately 4% lower than those found with either Galatry or Rautian profile fits. The measured intensities and self-broadening coefficients are compared with values in the HITRAN database and previous measurements. Copyright 1999 Academic Press.