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.     

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.     

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.     

Sättigungseffekte und Linienaufspaltung bei der stimulierten Resonanz-Raman-Streuung

Saturation Effects and Line Splitting of the Stimulated Resonance Raman Scattering The gain of the stimulated resonance Raman scattering (SRRS) is calculated for the case of any sharp resonance. It is shown that under steady-state conditions for longitudinal excitation in direction of the cell the saturation of the absorption is a necessary condition to find a sufficient large gain. Therefore, in the case of a Franck-Condon excitation the SRRS with an excited initial level is only possible, whereas for a O—O-excitation the SRRS with the ground or an excited state as initial state is equally probable. Changing of the population by stimulated fluorescence does not influence this assertion.     

Theoretical investigation on the pumping effect of stimulated Brillouin scattering on stimulated Raman scattering in water

The pumping effect of stimulated Brillouin scattering on stimulated Raman scattering is investigated theoretically through the coupled wave equations of stimulated Brillouin scattering and stimulated Raman scattering. The numerical simulations are in agreement with the experimental results. They indicate that the backward stimulated Raman scattering is excited and amplified collectively by both pump laser and stimulated Brillouin scattering.     

Analysis and simulation of single-frequency Raman fiber amplifiers

High power operation of single-frequency Raman fiber amplifiers is usually limited by the onset of stimulated Brillouin scattering. A theoretical investigation on single-frequency Raman fiber amplifier limited by stimulated Brillouin scattering is presented in this paper, based on the intensity equations combining stimulated Brillouin scattering and stimulated Raman scattering. A combination of methods is proposed to increase the output power of single-frequency Raman fiber amplifier. These methods include applying a suitable pump scheme according to the fiber length and seed signal power, using short gain fibers, utilizing a multiple-stage scheme and providing suppression of stimulated Brillouin scattering.     

Non‐degenerate second‐order scattering and difference combination bands in infrared‐pump/anti‐Stokes resonance Raman‐probe experiments

Non‐degenerate second‐order scattering due to interaction of infrared and ultraviolet pulses is observed in picosecond infrared‐pump/anti‐Stokes Raman‐probe experiments under electronic resonance conditions. We detected resonance hyper‐Rayleigh scattering at the sum frequency of the pulses as well as the corresponding frequency‐down‐shifted resonance hyper‐Raman lines. Nearly coinciding resonance hyper‐Raman and one‐photon resonance Raman spectra indicate conditions of A‐term resonance Raman scattering. Second‐order scattering is distinguished from transient anti‐Stokes Raman scattering of v = 1 to v = 0 transitions and v = 1 to v′ = 1 combination transitions by taking into account their different spectral and temporal behaviour. Separating these processes is essential for a proper analysis of transient vibrational populations. Copyright © 2007 John Wiley & Sons, Ltd.     

Spatio-temporal dynamics of multicolor spatial Kerr solitons

We present numerical and experimental results showing the rich and complex spatio-temporal dynamics of multicolor spatial vector soliton generated by stimulated Raman scattering in a Kerr planar waveguide. By taking into account their temporal dimension, we found the precise domain of existence of multicolor soliton whose components are mutually guided and spatio-temporally superimposed. In addition, we observe the Raman Stokes component in the trailing edge of the pump pulse and show that it is associated with the slow-light process induced by the sharp resonance of the Raman gain medium.     

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.     

Double resonance Raman scattering of second-order Raman modes from an individual graphite whisker

Resonant Raman scattering of second-order Raman modes from an individual graphite whisker synthesized by a high-temperature heat-treatment method at a special pressure was discussed here. The dependence of phonon frequencies on the incoming laser light and the frequency difference between Stokes and anti-Stokes scattering show their origin from double resonance Raman scattering. Our results show that all the experimental results of second-order Raman modes in graphite whiskers, such as the excitation-energy dependence on the mode frequency, the frequency shift between a second-order Raman mode and its fundamentals, and the frequency discrepancy between Stokes and anti-Stokes components of a second-order Raman mode can be well understood by double resonance Raman scattering.     

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.     

Parameter identification and synchronization between uncertain stimulated Raman scattering and NH3 laser

The parameter identifiers and synchronization controllers are designed based on stability theory in order to realize the synchronization of two chaotic systems with diverse structures and the parameter identification of the uncertain system. The stimulated Raman scattering and NH₃ laser are taken as examples. The simulation results show that the global synchronization between the uncertain stimulated Raman scattering and the NH₃ laser can be achieved, and all the parameters in the stimulated Raman scattering system can be identified simultaneously. The method is proved effective and feasible.     

Multifrequency stimulated Raman scattering of light in liquid nitrogen infiltrated into 3D photonic crystals

Spectral characteristics of stimulated Raman scattering at least in synthetic opal matrices infiltrated with liquid nitrogen upon excitation by nanosecond laser pulses are studied. The effect of the stop band position on the generation efficiency of anti-Stokes components of stimulated Raman scattering up to the third order is demonstrated. The excitation threshold of stimulated Raman scattering in liquid nitrogen infiltrated into opals is significantly lower in comparison with the generation in bulk samples.     

ICF驱动器长脉冲下三倍频晶体中的横向受激拉曼散射

 ICF驱动器在脉宽为3ns的长脉冲条件下运行时，三倍频晶体中的横向受激拉曼散射效应将比短脉冲条件下的效应更为显著。针对长脉冲运行时，KDP晶体和KD*P晶体产生的横向受激拉曼散射光对晶体的危害性作了对比分析，并研究了横向受激拉曼散射效应与增益系数之间的关系，为选择何种晶体作为三倍频晶体提供了理论依据。     

Picosecond stimulated Raman scattering in crystals

The comparative values of the peak and integral cross sections of spontaneous Raman scattering and the optical dephasing time of molecular vibrations were determined for several oxide crystals by spontaneous Raman spectroscopy. The spectral, time, and energy parameters of stimulated Raman scattering (SRS) were measured for ten crystals using picosecond YLF: Nd laser pumping with a radiation wavelength of 1047 nm. An analysis of the experimental dependence of the threshold energy of pumping SRS on the integral and peak cross sections of spontaneous Raman scattering showed that the SRS gain increment explicitly depended on the integral cross section and was independent of the peak cross section of spontaneous Raman scattering as the ratio between the pumping pulse width (11 ps) and the time of optical dephasing of molecular vibrations changed from 0.42 to 9.3. The gain coefficients of steady-state stimulated Raman scattering under threshold stimulated Raman scattering conditions were determined for all the crystals studied on the basis of the measured threshold SRS pumping energies, the duration and width of the spectrum of pulses, the nonlinear interaction length, the intensity of pumping, and the theoretical dependences that relate the steady-state and transient SRS gain increments. The steady-state SRS gain coefficients obtained in this work fitted well a linear dependence on the peak cross sections of spontaneous Raman scattering, which substantiated the correctness of our analysis and measurements.     

Stimulated Raman scattering in light and heavy water under picosecond laser excitation

The spectra of stimulated Raman scattering in ordinary and heavy water under excitation by second harmonic of a picosecond Nd:YAG laser were compared. It was shown that when stimulated Raman scattering is excited in water in cavities of a photonic crystal (synthetic opal matrix constructed of silica nanoglobules) or a photonic glass in the form of close-packed monodimensional millimeter-size amorphous-quartz balls, the efficiency of stimulated Raman scattering increases significantly compared to a uniform liquid medium.     

Theory of stimulated resonance raman scattering in dyes with ground or excited initial state

The theory of stimulated resonance Raman scattering (SRRS) in dyes with ground or excited initial state (up-down or down-up mechanism) is investigated. The gains for these processes are obtained by means of an analytical solution of the rate equation. It is shown that under pumping conditions the down-up SRRS is more probable than the up-down SRRS.     

Double line stimulated Raman scattering in benzene

Simultaneous stimulated Raman scattering at the 992 cm^–1 and the 3063 cm^–1 line of benzene is observed by mode-locked ruby laser pulse excitation. The double line stimulated Raman scattering is initiated by self-focusing. The influence of small-scale self-focusing, self-phase modulation, and cross-phase modulation on the double line stimulated Raman scattering is discussed. At low pump pulse intensities, before the onset of small-scale self-focusing, the steady-state Raman gain factors of both Raman lines are determined by Raman energy conversion efficiency measurements.