超衍射极限相干反斯托克斯拉曼散射显微成像技术及其探测极限分析

理论上提出一种突破衍射极限限制的相干反斯托克斯拉曼散射显微成像方法, 并对其探测极限进行分析.通过引入环形附加探测光与艾里斑周边的声子作用, 实现点扩展函数的改造, 提高相干反斯托克斯拉曼散射显微成像系统的横向空间分辨率. 随着分辨率的提高, 信号强度也随之降低, 尤其当应用于生物学、医学研究时, 样品分子数密度通常很低, 这将导致信号探测更加困难. 因此分析系统的探测极限, 确定超分辨体积元内的最小可探测分子数是展开超衍射极限相干反斯 托克斯拉曼散射显微成像实验研究的重要前提. 当泵浦光、斯托克斯光、探测光光强均达到极大值, 分辨率约40 nm三维空间内, 超衍射极限相干反斯托克斯拉曼散射显微成像系统的散粒噪声信噪比由曝 光时间与样品分子数密度决定. 曝光时间若取20 ms, 探测极限约为10³, 样品分子数目只有大于探测极限, 才能保证信号可以从噪声背景中提取出来. 关键词： 突破衍射极限 相干反斯托克斯拉曼散射 非线性光学 探测极限     

Nonlinear interferometric vibrational imaging

Coherent anti-Stokes Raman scattering (CARS) processes are "coherent," but the phase of the anti-Stokes radiation is lost by most incoherent spectroscopic CARS measurements. We propose a Raman microscopy imaging method called nonlinear interferometric vibrational imaging, which measures Raman spectra by obtaining the temporal anti-Stokes signal through nonlinear interferometry. With a more complete knowledge of the anti-Stokes signal, we show through simulations that a high-resolution Raman spectrum can be obtained of a molecule in a single pulse using broad band radiation. This could be useful for identifying the three-dimensional spatial distribution of molecular species in tissue.     

Femtosecond spectroscopy of coherent anti-Stokes Raman scattering with frequency-tunable chirped pulses generated in a microstructure fiber

A new scheme of chirped-pulse femtosecond coherent anti-Stokes Raman scattering spectroscopy is proposed and experimentally implemented. A theory of this modification of coherent nonlinear spectroscopy is developed. We use this approach to show that a linear time-frequency mapping defined by linearly chirped pulses allows the spectra of nonlinear response of a medium to be measured by varying the delay time between the pump pulses. Microstructure fibers with a special dispersion profile are at the heart of the experimental implementation of this technique. Such fibers are ideally suited for the generation of frequency-tunable pulses with a smooth envelope and a controlled chirp. We present the results of experimental characterization of the envelope, spectrum, and chirp of anti-Stokes pulses generated in microstructure fibers by femtosecond Cr:forsterite-laser pulses. These frequency-tunable anti-Stokes pulses produced and shaped in microstructure fibers are then employed for coherent anti-Stokes Raman scattering spectroscopy of toluene solution.     

超衍射极限相干反斯托克斯拉曼散射显微成像技术中空心光束的形成

空心光束的质量是超衍射极限相干反斯托克斯拉曼散射显微成像技术中决定成像质量的一个至关重要的因素. 本文基于菲涅耳衍射理论,分析了螺旋相位片法产生空心光束的物理机理,并且模拟了不同的入射条件对产生的空心光束的影响. 模拟结果表明:波长与相位片中心波长匹配且光强呈圆对称分布的高斯光垂直入射到相位片上,当高斯光束中心与相位片中心完全对准时,可获得较理想的空心光束;入射光光强分布的圆对称性以及入射光中心与相位片中心的对准程度都会影响产生的空心光束的强度分布;同时,高斯光束小角度倾斜入射时,空心光的强度分布仍呈圆对称,却在观察面发生一定的位移;此外,入射光中心波长偏离相位片中心波长不大时,对产生的空心光束的强度分布几乎没有影响. 上述分析结果对用于超衍射相干反斯托克斯拉曼散射显微成像技术中理想空心光束的获取具有重要的指导意义. 关键词： 空心光束 超衍射极限 相干反斯托克斯拉曼散射 螺旋相位片     

Pulse shaping by modulation instability in a photonic-crystal fiber for coherence control and single-beam coherent anti-Stokes Raman-scattering microspectroscopy

Modulation instability in a highly nonlinear photonic-crystal fiber is shown to allow the generation of optimally pulse-shaped field waveforms that are ideally suited for coherence-controlled nonlinear Raman scattering, including single-beam coherent anti-Stokes Raman-scattering microspectroscopy. This approach enables the integration of the efficient spectral transformation and pulse-shaping operations needed for the realization of nonlinear Raman techniques in a single fiber-format component.     

Beam propagation method for wide-field nonlinear wave mixing microscope

We develop a nonlinear beam propagation method for signal generation in inhomogeneous medium for wide-field nonlinear wave mixing microscope. Experimental results performed in wide-field coherent anti-Stokes Raman imaging have shown good agreement with the developed theory.     

混合溶液中CARS过程的非共振信号实验研究

相干反斯托克斯拉曼散射是一种非线性四波混频效应,但是通过探测共振信号不易进行物质成分的定量光谱分析。本文利用单频相干反斯托克斯拉曼散射光谱分析法,对不同体积比混合的乙醇溶液在远离双光子共振跃迁及其远离溶质与溶剂的特征拉曼共振态位置进行了光谱探测。通过对实验结果进行分析发现,在共振位置2 876 cm-1的信号强度随混合溶液中的乙醇的体积比增加而增加,呈二次方关系。而在远离共振态位置的非共振信号强度随混合溶液中乙醇的体积比增加而增加,且呈线性关系,进而说明了非共振信号强度随着分子数浓度N呈线性变化关系。因此,通过探测非共振信号强度与分子数浓度关系可以为混合物中特定成分的定量光谱分析提供一种研究途径。     

铷原子热蒸气中强非线性效应产生激光模式图样的实验研究

研究了具有高斯横向分布的连续激光束单次通过铷原子蒸气后,在近共振附近铷原子蒸气中,由强的非线性克尔效应导致激光分裂成细丝的现象,并且这些细丝的衍射图样在远场通过相干叠加,可以形成具有规则结构的斑图模式.实验上研究了输入光功率,铷泡温度和抽运激光频率相对于⁸⁵Rb原子D₂线的不同失谐位置等因素对斑图模式的影响.由于铷原子的超精细能级结构,在铷原子蒸气中同时存在与三阶非线性效应相关的四波混频现象,通过扫描探测光的频率同时观察到具有斯托克斯和反斯托克斯光子的拉曼增益现象. 关键词： 铷原子蒸气 克尔效应 自聚焦 斑图     

Femtosecond phase-and-polarization control for background-free coherent anti-Stokes Raman spectroscopy

Phase-and-polarization coherent control is applied to control the nonlinear response of a quantum system. We use it to obtain high-resolution background-free single-pulse coherent anti-Stokes Raman spectra. The ability to control both the spectral phase and the spectral polarization enables measurement of a specific off-diagonal susceptibility tensor element while exploiting the different spectral response of the resonant Raman signal and the nonresonant background to achieve maximal background suppression.     

Epitaxial growth of Ge1-xSnx films with x up to 0.14 grown on Ge （001） at low temperature

We characterize the structures of Ge1-xSnx films with x up to 0.14 grown on Ge （001） by molecular-beam epitaxy at low temperature. The results show that Ge1-xSnx films are fully strained even at high Sn composition. The in-plane lattice parameters remain exactly the same as that of the substrate. Depth sensitivity analysis of the lattice parameters indicates that the strains of the epitaxial films are all in homogeneity. The films are fully strained. Poisson ratios, the force constants for the bonds between Ge and Sn are estimated and discussed in the present paper. Raman results show Ge-Ge, Ge-Sn, Sn-Sn vibrational modes. The Sn-Sn bond aggregation may respond to the high quality of our films. The fully strained epitaxy films with high content of Sn may be useful in designing the high quality GeSn films.     

Coherent anti-Stokes Raman scattering microscopy with a photonic crystal fiber based light source

A coherent anti-Stokes Raman scattering microscope based on a Ti:sapphire femtosecond oscillator and a photonic crystal fiber is demonstrated. The nonlinear response of the fiber is used to generate the additional wavelength needed in the Raman process. The applicability of the setup is demonstrated by imaging of micrometer-sized polystyrene beads.     

Applications of stimulated Raman scattering

The applications of stimulated Raman scattering reviewed in this paper include: determination of spontaneous Raman parameters and nonlinear susceptibilities by gain measurements and coherent anti-Stokes Raman spectroscopy, excitation of molecular vibrations and lattice waves and measurement of their relaxation times, generation of intense tunable light in the infrared region of the spectrum. The main results of the theory of stimulated Raman scattering relevant to the understanding of these applications are discussed.     

Molecular discrimination and contrast enhancement using a scanning coherent anti-stokes Raman microscope

New applications of a nonlinear optical microscope using coherent anti-Stokes Raman scattering (CARS) are presented. Excellent molecular discrimination using chemically similar molecular species and signal contrast enhancement using digital image processing are demonstrated. Limitations of the technique and future applications are discussed.     

Generation of three-primary-color Raman comb in the continuous-wave regime

We demonstrate the generation of continuous-wave Stokes and anti-Stokes Raman sidebands including the three-primary-color (683, 532, and 436 nm) components. The Raman sidebands are generated through both stimulated and coherent anti-Stokes Raman scattering in a broadband high-finesse optical cavity filled with gas-phase hydrogen as a Raman-active medium and covering the entire visible spectral range (420–680 nm). The blue emission is considerably enhanced by matching the frequency with one of the longitudinal modes of the optical cavity, and high conversion efficiencies are observed when the coherent length corresponds to an integral multiple of the round-trip length of the optical cavity. This indicates that phase-matching plays a critical role in determining the efficiency of the Raman comb generation.     

Raman lasing and cascaded coherent anti-Stokes Raman scattering of a two-phonon Raman band

Raman lasing of a two-phonon Raman band in the anti-Stokes side is demonstrated. Two femtosecond light pulses with identical wavelengths are irradiated onto a SrTiO3 crystal in a cross-beam configuration. Under low excitation power, several wave-mixing signals with identical wavelengths are emitted. When the power exceeds a critical value, cascaded coherent anti-Stokes Raman scattering (CARS) signals are emitted, the frequency step of which is coincident with that of the strongest two-phonon Raman band of 2TO2.     

Temperature dependence of longitudinal optical phonon lifetimes in GaP

The decay of coherently excited longitudinal optical phonons in GaP has been observed through time delayed coherent anti-Stokes Raman scattering measurements with picosecond light pulses. The temperature dependence of the decay is compared to that observed through Raman linewidth measurements and to that predicted theoretically for spontaneous three-phonon decay processes.     

Rotational temperature and density measurements in a hypersonic flow by dual-line CARS

Rotational temperature and nitrogen number density are measured in the shock wave/boundary layer interaction region in the vicinity of a two-dimensional compression corner disposed in a low pressure, 55 K, Mach 10 hypersonic air flow. Spatially-resolved data are recorded using a nonlinear optical technique named dual-line coherent anti-Stokes Raman scattering (DLCARS). Averaged temperature and density profiles are compared with those predicted by a Navier-Stokes solver. Good agreement is found.     

Dual-broadband rotational CARS modelling of nitrogen at pressures up to 9 MPa. I. Inter-branch interference effect

An improved model for pure rotational coherent anti-Stokes Raman scattering (CARS) has been developed for the dual-broadband approach. This model takes into account the fact that coherent anti-Stokes as well as Stokes radiation are generated simultaneously, and these two branches overlap and interact at high pressures giving rise to an inter-branch interference effect. In combustion studies, the anti-Stokes branch is used to determine temperature and concentrations of key species, of which nitrogen is the most widely used, and we have found that the interference effect on the anti-Stokes side is of such magnitude that it clearly needs to be taken into account at pressures of a few MPa. The necessary modifications to the total third-order susceptibility are presented and a derivation of the convolution integral for a finite-bandwidth pump source is given. Received: 18 February 2002 / Revised version: 9 July 2002 / Published online: 22 November 2002 RID="*" ID="*"Corresponding author. Fax: +46-46/2224542, E-mail: mikael.afzelius@forbrf.lth.se     

在单模光纤中放大的反斯托克斯拉曼背向自发散射的温度效应

在单模光纤中,输入的激光功率大于阈值时．出现放大的反斯托克斯拉曼背向自发散射现象。实验发现：放大的反斯托克斯拉曼背向自发散射具有温度效应．与反斯托克斯拉曼背向自发散射一样,放大的拉曼散射光的光子通量受到光纤温度的调制。反斯托克斯拉曼背向白发散射的放大效应抑制了单模光纤中的相干噪声,改善了系统的信噪比。实验还发现．放大的反斯托克斯扎曼背向自发散射空域曲线上放大的端点位置随激发功率的增高前移并具有一定的规律性。放大的反斯托克斯拉曼背向自发散射的温度效应作为一种新的测温原理,已应用于远程30km分布光纤温度传感器系统。