Polarization coherent anti‐stokes Raman scattering using noisy light

Several polarization studies on the noisy light version of coherent anti‐Stokes Raman scattering (CARS) exist in the literature. However, the full advantages of polarization CARS (P‐CARS), which are so useful in conventional and short‐pulse CARS methods, have not yet been exploited in the noisy light version. This work presents experimental realization of fully functional P‐CARS using noisy light. Several examples demonstrate the advantages brought by P‐CARS. This includes the ‘classic’ example of benzene in carbon tetrachloride. Also presented are the carbon–carbon double bond stretches in acrylonitrile and 1‐hexene. An interesting, and not fully understood, detection polarization angle dependence is discussed. Applications to an m‐xylene/benzene mixture and an alkaline solution of the amino acid phenylalanine are presented. Copyright © 2006 John Wiley & Sons, Ltd.     

氢分子振动态与铯分子基态碰撞中转动-振动能量转移

利用受激拉曼泵浦将H2激发到v=1,J=3态,研究了H2(1, 3)态与Cs2分子碰撞(1, 3)态的弛豫及Cs2(X1+g)振动态的激发过程。利用相干反斯托克斯拉曼散射(CARS)检测H2的振转态分布,由CARS峰值得到密度比[H2(1, 3)]/[H2(0, 3)]和[H2(1, 1)]/[H2(1, 3)],由H2(v=0)振转态的Boltzmann分布确定H2(0, 3)的密度,由此得到[H2(1, 3)]和[H2(1, 1)]态的密度。激光诱导荧光光谱(LIF)确定被碰撞激发的Cs2(X1+g, v=11-15)各态。利用单模半导体激光作瞬时光吸收,对于v= 11, 12, 13, 14和15,积分吸收系数(单位：106cm-1s-1)分别是6.5,7.9,7.0,6.1和4.7,结合H2(1, 3)的密度,得到H2(1, 3)Cs2(X1+g, v)的转移速率系数,对于v=11-15,分别是(单位：10-13cm-1s-1)1. 40. 6,1.70. 7,1.50. 6,1.30.5和1.00. 4。利用吸收线Doppler增宽测量分别得到了Cs2(X1+g, v=11-15)的平动能。     

Raman spectroscopy and CARS microscopy of stem cells and their derivatives

The characterisation of stem cells is of vital importance to regenerative medicine. Failure to separate out all stem cells from differentiated cells before therapies can result in teratomas—tumours of multiple cell types. Typically, characterisation is performed in a destructive manner with fluorescent assays. A truly non‐invasive method of characterisation would be a major breakthrough in stem cell‐based therapies. Raman spectroscopy has revealed that DNA and RNA levels drop when a stem cell differentiates into other cell types, which we link to a change in the relative sizes of the nucleus and cytoplasm. We also used Raman spectroscopy to investigate the biochemistry within an early embryo, or blastocyst, which differs greatly from colonies of embryonic stem cells. Certain cell types that differentiate from stem cells can be identified by directly imaging the biochemistry with CARS microscopy; examples presented are hydroxyapatite—a precursor to bone, and lipids in adipocytes. Copyright © 2011 John Wiley & Sons, Ltd.     

Applying the method of Coherent Anti‐stokes Raman microscopy for imaging of carotenoids in microalgae and cyanobacteria

Coherent anti‐stokes Raman scattering microscopy (CARS) was applied to visualize carotenoids in microalgae and cyanobacteria. Nonlinear light–matter interaction utilized in CARS microscopy inevitably induces a number of competing nonlinear processes, such as multiphoton excitation fluorescence. Microalgae and cyanobacteria being an intrinsically well‐fluorescent object generates a strong two‐photon‐excitation fluorescence (TPEF) signal which should be effectively suppressed during the CARS experiment. Using an energetically balanced duel‐wavelength excitation scheme and spectral purification of detecting signal, the TPEF was completely blocked providing a possibility to probe microalgae and cyanobacteria in a fingerprint region of the CARS spectrum. Microspectroscopy experiments were carried out with three species ‐ cyanobacteria Nostoc Commune, Nostoc sp. and Chlorella sp. Distinct bands obtained in CARS spectra of such species were assigned to carotenoids and were taken as spectral markers in the imaging experiment. CARS imaging known as a chemical selective and label‐free technique allows non‐invasion monitoring of accumulation and movement of chemical compound at the subcellular level. Obtained high‐resolution images of carotenoid distribution in algae and cyanobacteria clearly demonstrate the potential of CARS microscopy for spatially resolved analysis of the natural products stored in the microalgae and cyanobacteria cell. Copyright © 2013 John Wiley & Sons, Ltd.     

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%。     

基于高光谱成像技术的脐橙叶片的叶绿素含量及其分布测量

为实现脐橙叶片叶绿素含量无损检测及其分布可视化表征,采用高光谱成像技术,结合自适应重加权算法(CARS)和连续投影算法(SPA),筛选特征光谱变量,进行脐橙叶片叶绿素含量及可视化分布研究。选取叶绿素测量位置的7×7矩形感兴趣区域,提取并计算脐橙叶片平均光谱。基于Kennard-ston方法,将148个脐橙叶片样品划分成建模集和预测集(111∶37)。采用CARS和SPA算法分别筛选出了32个和6个叶绿素特征光谱变量,用于建立偏最小二乘(PLS)回归模型。采用37个未参与建模的脐橙叶片样品评价模型的预测能力,经比较,CARS-PLS和SPA-PLS模型均优于变量筛选前的PLS模型,且CARS-PLS和SPA-PLS模型的预测能力几乎相同,其预测集相关系数分别为0.90和0.91,均方根误差分别为1.53和1.60。SPA-PLS模型计算脐橙叶片每个像素点的叶绿素含量,经伪彩色变换,绘制了脐橙叶片叶绿素含量可视化分布图。实验结果表明:变量筛选方法结合高光谱成像技术,能够实现脐橙叶片叶绿素含量无损检测及叶绿素分布可视化表达,并简化了数学模型。     

Coherent Raman spectra of the ν1 mode of BF3 and BF3

High resolution (0.001 cm⁻¹) coherent anti-Stokes Raman spectroscopy (CARS) was used to directly examine the ν₁ symmetric stretching mode of the planar symmetric D_3h molecules ¹⁰BF₃ and ¹¹BF₃. Simulations of the spectra were done using ν₁ rovibrational parameters deduced from published infrared hot-band and difference-band studies and the close similarity to the observed CARS spectra confirms the validity of the infrared constants. No significant perturbations by Fermi resonance or Coriolis interactions with nearby states are observed, in marked contrast to the case of sulfur trioxide, a similar D_3h molecule recently studied. In the harmonic approximation, the ¹⁰BF₃ and ¹¹BF₃ν₁ Q-branches would be identical since the isotopic substitution is at the center of mass but, interestingly, the ν₁ stretching frequency for ¹¹BF₃ is found to be 0.198 cm⁻¹higher than for the lighter ¹⁰BF₃ isotopomer. This counterintuitive result is reproduced almost exactly (0.200 cm⁻¹) by ab initio calculations (B3LYP/cc-pVTZ) that included evaluation of cubic and quartic force constants and x_ij anharmonicity constants. The ab initio computations also predict to within 1% the ΔB, ΔC changes in the rotational constants in going from the ground state to the v₁ = 1 vibrational level. The results illustrate nicely the complementary interplay of modern infrared, Raman, and ab initio methods in obtaining and analyzing rovibrational spectra.     

Four-wave mixing in OH: comparison between CARS and DFWM

Summary A comparison between CARS and Degenerate Four-Wave Mixing experiments on OH is performed in a premixed CH₄-air flame. Both optical phase conjugation and forward BOXCARS geometries are studied in DFWM. The relative properties of these two configurations are experimentally investigated from the study of theP andQ branches of the (O−O) band. Paper presented at the ?XI European CARS Workshop?, Florence, Italy, 23–25 March, 1992.     

Validation experiments for spatially resolved one-dimensional emission spectroscopy temperature measurements by dual-pump CARS in a sooting flame

In this work, an emission spectroscopic (ES) technique for the determination of soot temperatures in an axisymmetric flame is validated against coherent anti-Stokes Raman spectroscopy (CARS) as preparation for a zero gravity measurement campaign. In order to reduce valuable measurement times during the parabolic flights, a setup for spatially resolved one-dimensional measurements along a line has been built up using an imaging spectrometer and a CCD-camera for data acquisition.In order to assess the performance of the ES technique, accurate coherent anti-Stokes Raman scattering (CARS) measurements have been performed at the same conditions. Hereby, great care has to be taken to minimize the known interferences in sooting flames. The non-resonant signal contribution was suppressed by a polarization technique and the signal wavelength was shifted to an interference free region. These modifications are discussed in detail. The temperatures obtained by both methods are in good agreement in most regions of the flame. It turned out that the described approach for ES is an appropriate and robust alternative for measuring temperatures in sooting axisymmetric flames, if more accurate techniques cannot be applied, e.g., during investigations in zero-g parabolic flight experiments.     

CARS temperature measurement in a LOX/CH4 spray flame

Coherent anti‐Stokes Raman scattering (CARS) spectroscopy has been used to investigate cryogenic liquid oxygen/gaseous methane (LOX/CH₄) flames on a medium‐size test facility at a pressure of 0.24 MPa and mass flow of 0.025 kg/s. Single‐shot, broadband CARS spectra with simultaneous detection of the Q‐branches of hydrogen and water molecules were recorded with good signal‐to‐noise ratio. Temperature was deduced from the H₂ and H₂O CARS profiles. The spatial temperature distribution in a comparatively harsh environment has been measured successfully. The measurements took place in the windowed combustion chamber of the DLR M3 test facility, aiming to provide data for validation of rocket combustor modeling. Copyright © 2010 John Wiley & Sons, Ltd.