Frequency locking of dye lasers by intracavity stimulated Raman scattering

Intracavity stimulated Raman scattering gain is used to force spectral condensation of the dye laser emission to ～ 2 Å wide lines in an untuned dye oscillator longitudinally pumped by a repetitive N₂-laser. Several stimulated Stokes Raman frequencies of the solvents are observed. Interpretation is discussed in terms of spectro-temporal evolution of the dye intensity within an homogeneous band oscillator.     

Chaos in stimulated Raman scattering

Coherent state technique and maximal Lyapunov exponent method are used for the study of deterministic chaos in a system governing stimulated Raman scattering. The influence of the external pumping on dynamics of the system is investigated. Phase portraits and FFT spectra are presented.The author would like to express his sincere thanks to prof. J. Peina for his comments and stimulating discussions.     

Soliton experiments in stimulated Raman scattering

Experimental observations of solitons in stimulated Raman scattering are reported. Soliton formation resulted from the introduction of a phase shift in the incident Stokes beam as predicted by theory. Pulse sharpening and retardation on propagation in the Raman medium have been observed along with amplitude diminution. The first two features were predicted and the third was not. Spontaneous soliton formation has been observed in the absense of any amplitude modulation or apparent phase shift in the optical fields, indicating that additional sets of initial conditions may result in soliton formation.Work performed under the auspices of the U.S. Department of Energy.     

Efficient stimulated Raman scattering in silicon

Stimulated Raman scattering in silicon was investigated at liquid helium temperatures. A Q-switched single mode Nd: YAG laser was used to generate Stokes radiation at 1.127 μm. Time resolved measurements give a maximum power conversion efficiency of 20%. The effects of intensity induced losses are discussed.     

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.     

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.     

Single-pulse stimulated Raman scattering spectroscopy

We demonstrate the acquisition of stimulated Raman scattering spectra with the use of a single femtosecond pulse. High-resolution vibrational spectra are obtained by shifting the phase of a narrow band of frequencies within the input pulse spectrum, using spectral shaping. The vibrational lines are resolved via amplitude features formed in the spectrum after interaction with the sample. Using this technique, low-frequency Raman lines (<100 cm?1) are observed on both the Stokes and anti-Stokes sides.     

Studies of stimulated Raman scattering

The dependence of the excitation threshold and the intensity of the first Stokes component on the properties of the scattering material, the concentration of its molecules, and the exciting light intensity has been studied. It has been found that the intensity of stimulated Raman scattering lines depends exponentially on the intensity of the exciting light and the concentration of the scattering molecules. This dependence is in agreement with the theory developed.The author are gratful to P. A. Bazhuln, N. G. Basov, and A. M. Prokhorov for the present study.     

The buildup of stimulated Raman scattering from spontaneous Raman scattering

We present a quantum electrodynamic theory which shows for the first time how stimulated Raman scattering builds up, both spatially and temporally, from spontaneous Raman scattering. We analytically solve operator Maxwell-Bloch equations to find the Stokes field operator, and thus the Stokes intensity, for both monochromatic and broad-band (phase diffusion) pump lasers.     

Stokes-anti-Stokes entanglement in stimulated Raman scattering

A cavity model of Raman scattering from phonons by an undepleted laser field is considered. The fields in the interaction are coupled to the boson reservoir that produces the damping mechanism in the model. An analysis for the origination of quantum entanglement between the Stokes and anti-Stokes fields, depending on their coupling constants with the reservoir bosons and on the state of the reservoir, is performed under the assumption of the initial coherent state of phonons.     

水中受激拉曼散射的能量增强及受激布里渊散射的光学抑制

为提高液体介质中受激拉曼散射的输出能量,提出了通过温度调控来抑制受激布里渊散射的方法,设计了532 nm多纵模宽带脉冲激光泵浦的受激拉曼散射发生系统,测量了不同温度下水中前向受激拉曼散射及后向受激布里渊散射的输出能量,分析了水温、泵浦激光线宽及热散焦效应对受激拉曼散射输出能量影响的物理机制.实验结果表明:通过降低水温可实现对受激布里渊散射过程的有效抑制,同时减小热散焦效应带来的光束畸变,从而有效提高受激拉曼散射的输出能量.研究结果对液体介质中的受激拉曼散射多波长转换具有重要意义.     

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.     

Transient stimulated Raman scattering in gas mixtures

We studied, for the first time to our knowledge, transient stimulated Raman scattering in H(2)- D(2) and H(2)- CH(4) gas mixtures excited with 200-fs and 2-ps, 390-nm pulses. Depending on the composition and partial pressure, of those gases, we observed ~40 output lines simultaneously. Under optimum conditions a conversion efficiency of as much as 8% in the combination Raman line at 556 nm was obtained in the H(2)- CH(4) gas mixtures. The difference between picosecond and femtosecond pumping is due to self-phase modulation and to generation of a spectral continuum in the latter. Our calculation of the ratio of the partial pressures is in a good agreement with the experimental results. A new method for measuring the unknown Raman scattering cross section of gas molecules is suggested.     

Transient stimulated Raman scattering in binary mixed liquids

Stimulated Raman scattering (SRS) spectra in several mixed liquids with a large optical Kerr constant are studied with nanosecond and picosecond light pulses. These spectra show a dependence of the SRS intensity on the relaxation times T₂ of Raman active modes.