Study of second-order nonlinear hyperpolarisability of all-trans-β-carotene in solutions by linear spectroscopic technique

This paper demonstrates the second-order nonlinear hyperpolarisability \gamma of all-trans-β-carotene in different solvents by linear spectroscopic technique that is based on resonance Raman scattering and UV--VIS (Ultraviolet-visible) absorption spectroscopy. Owing to the two-level model well describing the link that exists between the resonance Raman scattering and stimulated Raman scattering, the stimulated Raman polarisability α_{\rm R} can be calculated through the two-photon resonance system. The value of \gamma of all-trans-β-carotene in carbon bisulfide solution is 6.435\times 10^{-33} esu (1~esu of resistance =8.98755\times10^{11}~\Omega) that is close to the true value, because the solution of all-trans-β-carotene in carbon bisulfide satisfies the rigid resonance Raman scattering condition. This method is expected to be worthy of applications to measure the second-order nonlinear hyperpolarisability of a conjugate organic molecule.     

Time—dependent Theory of Raman Scattering with Pulses—Application to Continuum Raman Spectroscopy

A theory of real-time dependence of Raman scattering for a pulse-mode laser is developed within second-order perturbation theory and using the wavepacket terminology.We apply the theory to continuum Raman scattering for short and long pulses and varying pulse carrier frequency,For an initial ground virational state,it is shown that the rate of Raman emission as a funcition of time and pulse carrier frequency is structureless for all pulses,and for pulses that are longer than the dissociation time the rate also decays with the pulses.This is contrary to recently reported resonance fluorescence type structures at long times (M.Shapiro,J.Chem.Phys.99,2453(1993),We explain why such structures are unphysical for continuum Raman scattering.     

Stimulated resonance Raman scattering

A quantum mechanical theory of stimulated resonance Raman scattering taking full account of the effects of the incident and scattered radiation on the state and properties of the molecules is developed. The resulting formulas enable the amplification of the scattered radiation and the attenuation of the incident flux to be determined. The conditions under which stimulated Raman scattering produces amplification of radiation are formulated. The range of applicability of the theory, not taking account of the effects of radiation on the properties of the material is discussed.     

Determination of resonance frequencies in silica fiber using SRS gain

In this paper, a new approach for the determination of resonance frequencies of a material using stimulated Raman scattering is reported. A numerical model for nonlinear composite Raman susceptibility (CRS) is proposed considering the effect of molecular vibrations. The model considers four parameters for each molecular vibration, termed as quadruplets. Based on this CRS, the theoretical Raman gain in silica fiber is estimated. Genetic algorithm technique is used to find out the quadruplets, resonance frequencies in particular, by matching the estimated Raman gain with its experimental value. Eight optimized resonance frequencies are obtained for silica material.     

Frequency shifts in stimulated Raman scattering

The nonresonant contributions to the nonlinear susceptibility χ⁽³⁾ produce a frequency chirp during stimulated Raman scattering. In the case of transient stimulated Raman scattering, the spectrum of the generated Stokes pulse is found at higher frequencies than expected from spontaneous Raman data. The frequency difference can be calculated from the theory of stimulated Raman scattering.     

Effect of stimulated raman scattering on the formation of the random lasing spectrum of dyes

The nature of the line structure of the random lasing spectrum of vesicular films activated by dyes (rhodamine 6G, pyrromethene 597) has been analyzed. The spectral lines appear above the random lasing threshold and are manifested only within the spectrum of the amplified spontaneous radiation of dye molecules against the continuous-pedestal background. Their intensities are proportional to the product of the intensities of the pump and continuous spectrum at the frequencies of these lines, and the frequencies are exactly reproduced from pulse to pulse. The shifts of the lines are strongly correlated with the pump frequency and the frequencies of these lines coincide with the frequencies of the Raman scattering lines of dye molecules. Using these properties, it has been shown that the observed lines are due to stimulated resonant Raman scattering by dye molecules, which occurs simultaneously with the stimulated emission of these molecules. These two processes affect each other and jointly form a united nonlinear process where all of the oscillations active in Raman scattering are manifested.     

Nonlinear-laser effects in χ(<Superscript>3</Superscript>)-and χ(<Superscript>2</Superscript>)-active organic single crystals

The process of stimulated Raman scattering (SRS) allows one to convert laser emission wavelength of crystals, providing suitable molecular or lattice modes which contribute to third-order nonlinear optical susceptibility. Renewed interest in this field emerged because of the discovery of SRS in crystals that contain molecular units exhibiting Raman active modes. Particularly, organic nonlinear optical crystals used so far for frequency doubling and third harmonic generation seem to have a great potential for SRS application. This review paper reported same results on efficient SRS lasing effects that were discovered recently in organic crystals.     

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.     

超短超强激光与气体靶相互作用中的背向受激Raman散射

 实验诊断测量了超短超强激光与气体靶相互作用产生的背向受激Raman散射,在实验条件下呈现强耦合模式,背向受激Raman散射出现非线性Stokes多峰伴线结构,峰值的频率间隔小于等离子体波的频率,可以大致地推断出激光打靶过程中产生的等离子体密度偏低,其结果与等离子体强耦合理论计算结果一致。     

Multimodal nonlinear optical microscopy

Because each nonlinear optical (NLO) imaging modality is sensitive to specific molecules or structures, multimodal NLO imaging capitalizes the potential of NLO microscopy for studies of complex biological tissues. The coupling of multiphoton fluorescence, second‐harmonic generation, and coherent anti‐Stokes Raman scattering (CARS) has allowed investigation of a broad range of biological questions concerning lipid metabolism, cancer development, cardiovascular disease, and skin biology. Moreover, recent research shows the great potential of using a CARS microscope as a platform to develop more advanced NLO modalities such as electronic‐resonance‐enhanced four‐wave mixing, stimulated Raman scattering, and pump‐probe microscopy. This article reviews the various approaches developed for realization of multimodal NLO imaging as well as developments of new NLO modalities on a CARS microscope. Applications to various aspects of biological and biomedical research are discussed.     

Raman effect in the x-ray region

This paper presents a brief review of x-ray Raman scattering and some of our calculations on Raman scattered line shapes from light elements. We summarise the history of the Raman process in the x-ray region and present a detailed theory of the Raman scattering from an atomic many-electron system. Actual calculations of the Raman cross-section using this theory in single-particle approximation are given. The process of internal resonance Raman scattering is also discussed in the same formulation. The Raman cross-section is compared with the cross-sections of other x-ray scattering processes.     

Stimulated raman scattering of rapidly amplified short laser pulses

The theory of transient forward stimulated Raman scattering (FSRS) of rapidly amplified short laser pulses is put forth to complement the classical theory for FSRS of stationary pulses. Quantitative conditions for FSRS suppression are identified. In particular, it is shown quantitatively how the limitation imposed by pumped pulse FSRS on the output laser intensity in plasma-based ultrapowerful backward Raman amplifiers can be overcome through a selective detuning of the Stokes resonance.     

Influence of parametric four-wave mixing effects on stimulated Raman scattering in bimodal optical fibers

We analyze stimulated Raman scattering in normally dispersive bimodal fibers under single-frequency pumping conditions. Experiments show that whenever the interacting nonlinear waves propagate in the LP(01) and LP(11) modes, a parametric four-wave mixing enters unavoidably into play in the wave-coupling behavior, which causes qualitatively different phenomena compared with the ordinary process of Raman scattering, such as the parametric suppression of the first-order Raman Stokes radiation.     

The generation of stimulated resonance Raman scattering using external dye fluorescence

Different dyes in locally separated cells have been investigated in order to obtain information about the mechanisms responsible for the generation of stimulated resonance Raman scattering. The experiments show in agreement with the theoretical results that the appearance of initial signals as well as the effect of dye amplification influences the behaviour of stimulated resonance Raman scattering.     

表面等离子激元非线性表面增强拉曼散射效应

本文采用热蒸发法制备得到纳米Ag颗粒作为增强拉曼衬底, 利用入射光子与纳米颗粒表面价电子的相互作用机理, 激发出高能表面等离子激元, 其表面等离子形成的高能"热点"起到表面增强拉曼散射效果. 通过比较不同入射光强下的拉曼峰强, 指出纳米Ag颗粒的增强拉曼散射效果可以实现低探测光强下的高散射强度, 即纳米Ag颗粒的表面等离子激元具有非线性的表面增强拉曼散射效果, 可降低对样品的光、热损伤, 以利于拓展拉曼散射光谱的应用范围. 同时比较不同纳米Ag颗粒衬底的表面增强拉曼散射效果表明, 采用的热蒸发工艺具有较大的工艺域度, 具有较强的工艺兼容性.     

Generation of a continuum and stimulated Raman scattering harmonics during scattering of electromagnetic radiation of relativistic intensity

A theory of the propagation instability of plane, monochromatic, circularly polarized electromagnetic waves of relativistic intensity in matter is developed for a spatially three-dimensional geometry including arbitrary polarization of the scattered radiation. Harmonic generation owing to striction and relativistic nonlinearity is examined, as well as scattering owing to electron recoil, the decay instability of the harmonics with formation of scattered electromagnetic waves (Stokes components of the stimulated Raman scattering and plasmons), the interaction of electromagnetic waves in the plasma (antistokes stimulated Raman scattering), and the generation of a radiative continuum. The transition of the three-dimensional theory to a one-dimensional problem in the nonrelativistic limit is discussed. Zh. éksp. Teor. Fiz. 113, 2034–2046 (June 1998)     

Bubble nonlinear dynamics and stimulated scattering process

A complete understanding of the bubble dynamics is deemed necessary in order to achieve their full potential applications in industry and medicine. For this purpose it is first needed to expand our knowledge of a single bubble behavior under different possible conditions including the frequency and pressure variations of the sound field. In addition, stimulated scattering of sound on a bubble is a special effect in sound field, and its characteristics are associated with bubble oscillation mode. A bubble in liquid can be considered as a representative example of nonlinear dynamical system theory with its resonance, and its dynamics characteristics can be described by the Keller–Miksis equation. The nonlinear dynamics of an acoustically excited gas bubble in water is investigated by using theoretical and numerical analysis methods. Our results show its strongly nonlinear behavior with respect to the pressure amplitude and excitation frequency as the control parameters, and give an intuitive insight into stimulated sound scattering on a bubble. It is seen that the stimulated sound scattering is different from common dynamical behaviors, such as bifurcation and chaos, which is the result of the nonlinear resonance of a bubble under the excitation of a high amplitude acoustic sound wave essentially. The numerical analysis results show that the threshold of stimulated sound scattering is smaller than those of bifurcation and chaos in the common condition.     

Theorie des stimulierten Raman-Effekts

We consider stimulated Raman emission in solids, placed in a plane laser beam external to the cavity. The Hamiltonian of the system of phonons, electrons and electromagnetic fields is derived within the framework of a generalized adiabatic approximation for electrons and nuclei. It contains terms due to nonlinear interactions between electrons and phonons. Because the usual time-dependent perturbation theory cannot describe coherence effects properly we turn toHeisenberg's equations of motion for the operators of photons, phonons and electron excitations. In order to solve these equations in the steady state we apply an iteration procedure. We start with the light waves which give rise to electron transitions. The electrons such excited create phonons which then react on the electrons. Finally the electrons are coupled again to the lightfield. This procedure yields besides the usual wellknown Raman process two main processes occurring in stimulated Raman emission: a coupled two step Raman process and a parametric process. In the first one two phonons are involved. If the linewidth of phonons is comparable to the phonon frequencies the non-resonant parts of the above processes also become important. In solving the set of coupled equations for the light amplitudes, obtained from the iteration procedure, we only consider terms due to the first Stokes, the first anti-Stokes and the laser line. We then find frequency shifts of these lines due to the stimulated emission which are of the order of the linewidth of photons if this linewidth is very much smaller than that of phonons as it is the case in solids. This means that the coupled two step Raman process is dominant, in good agreement with measurements ofChiao andStoicheff in calcite.     

Calculation of the stationary generation power of a solid-state raman laser with intracavity second harmonic generation and sum frequency mixing

Analytical equations for the power of second-harmonic stationary generation or sum frequency mixing in a Raman laser with an intracavity nonlinear medium are developed and analyzed as functions of pumping mode and other parameters of the laser system. Parameter relationships providing the maximum output power and conditions for suppression of both stimulated Raman scattering by sum frequency mixing and; consequently, of sum frequency mixing itself are found.