Induction of the maximum Raman coherence in an extended medium through fractional adiabatic passage

The effect of fractional stimulated Raman adiabatic passage in an optically dense medium of three-level Λ atoms is shown to result in the maximum coherence on the Raman transition on a length of the medium that considerably exceeds the length of linear resonant absorption. The general case of unequal oscillator strengths of the adjacent transitions is analyzed. The results are of interest for coherent anti-Stokes Raman spectroscopy with delayed pulses.     

Theory of the resonance electronic Raman effect

The behaviour of electronic Raman scattering, excited under resonance conditions, is discussed in relation to molecular properties of the ground electronic state, the resonant excited state and the final electronic state. It is shown how the intensity distribution within vibronically structured electronic Raman bands depends on differences of molecular geometry and force field between these states.     

Multimode pumped continuous-wave solid-state Raman laser

We demonstrate the continuous-wave operation of a solid-state Raman laser containing a barium nitrate crystal as the Raman medium. The Raman laser, which has a singly resonant cavity, is pumped by multimode radiation. The Raman oscillation threshold is reached at approximately 2 W of pump power. As much as 500 kW/cm2 of Stokes power density at 60-kW/cm2 pump power density is obtained in the cavity.     

克尔介质中双原子与场拉曼作用系统的腔场谱

研究了含克尔介质腔中两个耦合二能级原子与双模光场拉曼相互作用过程的腔场谱。通过求解本征方程导出了腔场谱的计算公式,给出了双模初始光场均处于数态时的数值计算结果。发现在两模初始场均为弱场时,克尔效应不仅使峰位右移,还使峰的强度、个数和频率发生改变,破坏峰结构的对称性。在克尔效应较强时,原子之间的耦合对腔场的影响被抑制,谱结构主要由克尔效应决定。在强场条件下,无克尔介质加入时,原子间的耦合作用使各峰的强度都得到加强;随克尔效应的增强,靠近中心频率的主峰迅速增长并很快达到饱和,而远离中心频率的边峰则被抑制并产生劈裂。     

Lock-in stabilised externak cavity cw spin-flip Raman laser

A lock-in stabilised cw external-cavity spin-flip Raman laser has been operated in which a cavity mode resonant frequency is servo-controlled to the peak of the spontaneous gain as the magnetic field is swept. The design of the optical system eliminated additional undesired cavity interactions.     

CdSe量子点拉曼谱的共振效应研究

本文介绍了用共振拉曼光谱研究CdSe量子点材料的结果,认为拉曼峰是ZnSe和量子点界面模的叠加。指出当激发光能量逐渐离开ZnSe带隙时,共振减弱,ZnSe峰不再占主导,界面模的拉曼峰出现移动及变宽。     

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.     

Two-magnon Raman scattering in a spin density wave antiferromagnet

We present the results for a model calculation of resonant two-magnon Raman scattering in a spin density wave (SDW) antiferromagnet. The resonant enhancement of the two-magnon intensity is obtained from a microscopic analysis of the photon-magnon coupling vertex. By combining magnon-magnon interactions with ‘triple resonance’ phenomena in the vertex function the resulting intensity line shape is found to closely resemble the measured two-magnon Raman signal in antiferromagnetic cuprates. Both, resonant and non-resonant Raman scattering are discussed for the SDW antiferromagnet and a comparison is made to the conventional Loudon-Fleury theory of two-magnon light scattering.     

共焦腔增强的空气拉曼散射

拉曼光谱是一种无损、快速的物质成分分析和检测方法.由于拉曼信号强度微弱,使得拉曼光谱的检测应用受到极大的限制.针对增强拉曼散射信号强度、提高检测灵敏度这一问题,设计了一种用于自发拉曼散射信号增强的共焦腔样品池,开展了基于该共焦腔的空气拉曼散射信号增强研究.共焦腔的腔镜反射率为92%,这一设计在保证共焦腔通带宽度与激光器线宽匹配的同时能有效地降低共振调节难度.实验中采用0°探测构型收集拉曼信号,并由成像式拉曼光谱仪获取光谱信号.实验发现,在共振状态下,共焦腔的耦合效率达到87.5%,单向激光功率实现约11倍放大;与无共振腔相比,共焦腔对拉曼信号实现17倍放大,信噪比提高2倍.此外,空气中CO_2的3σ检测限达到200 ppm量级.结果表明,该系统对自发拉曼散射信号增强效果显著,并且有较高的检测灵敏度.     

Two-photon resonant Raman and luminescence of excitonic molecules in CuCl

Two-photon resonant Raman scattering via excitonic molecule in CuCl is studied with using dye laser excitation of different band widths. The yield of the Raman scattering is found to drop remarkably at resonant excitation and luminescence line of 0.3 meV half-width comes out. The predominance of the Raman or luminescence or their coexistence depends on the intensity and energy band width of excitation light.     

Raman scattering in ferromagnetic semiconductors under crossed fields

The influence of crossed electric and magnetic fields on the intraband resonant contribution to Raman scattering is discussed. It is shown that in the presence of these fields, the Raman efficiency for one magnon process in ferromagnetic semiconductors exhibits two resonant peaks which are dependent on the ratio βE/Hβ.     

拉曼散射在共振及近共振时的条件：广义短时间近似

研究了频率失谐时共振拉曼散射的动力学过程．当入射光子能量远离共振吸收能量时,时域内的失相使散射过程变快．这使得频率失谐如同照相机的快门功能,具有规律的散射持续时间,为普通的稳态测量提供了控制散射时间的有效工具．基于这个理论对两个多模式模型系统以及反式-1,3,5-己三烯和鸟嘌呤-胞嘧啶Watson-Crick碱基对分子的共振拉曼光谱进行了研究．除了这些特殊的物理效应,快散射机制可以简化光谱,同时使散射理论得到简化．当入射光子频率在共振区域时,拉曼光谱中会出现较强的多倍频成分;当入射光子频率与第一共振吸收频率之间的失谐量为振动能量时,在快散射过程中,这些多倍频成分逐渐消失．因此,利用入射光子与共振频域的失谐可以明显地简化拉曼光谱,从复杂光谱中去除多倍频和软模的影响,并且可以避免共振态的解离和荧光衰减引起的干扰．     

Raman scattering and fluorescence emission in a single nanoaperture: Optimizing the local intensity enhancement

We investigate the potential of a single subwavelength aperture milled in an aluminium film to enhance the local electromagnetic field. We compare the Raman scattering of unadsorbed chlorobenzene molecules and the fluorescence emission of Cyanine-5 dyes, having the same excitation and collection setup for both experiments. For the optimal nanoaperture diameter, we report a clear enhancement factor of about 5 of the Raman scattering intensity per unit volume. Since Raman scattering probes the molecular vibrational levels and avoids the resonant pumping of a real excited state, the observed Raman enhancement is disconnected from the effects of the molecular energy levels alteration previously reported for fluorescent dyes. The observations are similar for both Raman and fluorescence experiments, and stand in good agreement with numerical electromagnetic computations of the excitation intensity inside the nanoaperture.     

Resonant Raman detection of macular pigment levels in the living human retina

We have used resonant Raman scattering as a novel, noninvasive in vivo optical technique to measure the concentration of macular carotenoid pigments in the living human retina. Using a backscattering geometry and resonant molecular excitation in the visible, we measure the Raman peaks that originate from the single- and double-bond stretch vibrations of the p -conjugated molecule's carbon backbone. The Raman signals scale linearly with carotenoid content, whereas the required laser excitation is well under safety limits for macular exposure. The Raman technique is objective and quantitative and may lead to a new method for rapid screening of carotenoid pigment levels in large human populations that are at risk for vision loss from age-related macular degeneration, the leading cause of blindness of the elderly in the United States.     

碳纳米管拉曼光谱研究新进展

本文介绍碳纳米管拉曼光谱研究的最新进展。重点介绍金属性和半导体性碳纳米管的共振拉曼效应、表面增强拉曼效应和偏振拉曼效应。同时也介绍了碳纳米管的温度效应、压力效应和杨氏模量的拉曼光谱研究     

Power resonances in a Raman gas laser

The observation of a new type of resonance due to double-quantum transitions in the standing-wave field of a Raman gas laser is reported. A resonance dip with a width equal to that of the optically forbidden transition was experimentally detected in the output-vs-timing curve of a Raman Ne laser (λ=1.15 m) upon pumping by radiation of a He−Ne laser at 1.52 m. The theory presented shows that the resonance arises in the third order of perturbation theory when in resonant SRS the line is inhomogeneously broadened. The resonance can be considered as resulting from the overlap of dips in the velocity distribution of the nonlinear polarization induced by the standing laser wave.     

DFT study on the influence of electric field on surface‐enhanced Raman scattering from pyridine–metal complex

The influence of a static external electric field on surface‐enhanced Raman scattering is investigated by calculating the Raman spectra and excited state properties of pyridine–Au₂₀ complex with the density functional theory and time‐dependent density functional theory method. The external electric field with orientation parallel (positive) or antiparallel (negative) to the permanent dipole moment is respectively applied on the complex. This field slightly changes the equilibrium geometry and polarizabilities, which results in shifted vibration frequencies and selectively enhanced Raman intensities. The changes of charge transfer (CT) excited states in response to the electric field are visualized by employing the charge difference densities. Further, the energy of charge transfer transition is tuned by electric field to be resonant or not with the incident light, leading to the Raman intensities are enhanced or not enhanced. At the same time, the intensities of vibration modes are sensitive to the orientation of the field. The positive electric field enhances the totally symmetric ring breathing mode (~1009 cm⁻¹) but suppresses the trigonal ring breathing mode (~1051 cm⁻¹). On the contrary, the mode at 1051 cm⁻¹ is more enhanced than the mode at 1009 cm⁻¹ when the negative electric field is applied on the complex. The Raman spectra could be modulated by tuning the strength and direction of the electric field. Copyright © 2013 John Wiley & Sons, Ltd.     

Resonant Raman scattering from molecules adsorbed on non-metallic surfaces: An exact solution

A model of resonant Raman scattering of molecules weakly adsorbed on non-metallic surfaces is solved exactly. The model embodies the non-radiative electromagnetic interaction between molecule dipole transition and solid excitation, when the dominant screening effect is due to interband transitions or molecular excitons.The role of interband transitions in the resonant Raman response is also discussed by selected numerical examples in polaronic and non-polaronic regimes.     

Wave vector conservation in the first order resonant Raman scattering

The dependence of the shape and the intensity of the first order resonant Raman line 1LO on the direction and magnitude of phonon wave vector has been investigated in CdS crystals. Comparison of RRS in different orientations shows that in the most pure samples the phonon wave vector is determined, to a great extent, by the momentum conservation law. In Ni doped crystals one can observe violation of momentum conservation, resulting in a sharp increase of 1 LO intensity. The shape of the 1 LO line in such sample does not depend on the experimental orientation. For the first time the dependence of the Raman intensity on the scattering angle has been observed by the comparison of forward and backward scattering spectra. Observation of this dependence shows that the free excitons are the dominating intermediate states in the resonant Raman scattering in A₂B₆ compounds.     

Surface-enhanced Raman spectroscopy of semiconductor nanostructures

We review our recent results concerning surface-enhanced Raman scattering (SERS) by confined optical and surface optical phonons in semiconductor nanostructures including CdS, CuS, GaN, and ZnO nanocrystals, GaN and ZnO nanorods, and AlN nanowires. Enhancement of Raman scattering by confined optical phonons as well as appearance of new Raman modes with the frequencies different from those in ZnO bulk attributed to surface optical modes is observed in a series of nanostructures having different morphology located in the vicinity of metal nanoclusters (Ag, Au, and Pt). Assignment of surface optical modes is based on calculations performed in the frame of the dielectric continuum model. It is established that SERS by phonons has a resonant character. A maximal enhancement by optical phonons as high as 730 is achieved for CdS nanocrystals in double resonant conditions at the coincidence of laser energy with that of electronic transitions in semiconductor nanocrystals and localized surface plasmon resonance in metal nanoclusters. Even a higher enhancement is observed for SERS by surface optical modes in ZnO nanocrystals (above 10⁴). Surface enhanced Raman scattering is used for studying phonon spectrum in nanocrystal ensembles with an ultra-low areal density on metal plasmonic nanostructures.