Some new aspects in stimulated raman scattering from hydrogen gas.
Stimulated Raman scattering from hydrogen gas, discussing simultaneous SRS of harmonic ruby radiation and vibrational rotational lines
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Stimulated Raman scattering from hydrogen gas, discussing simultaneous SRS of harmonic ruby radiation and vibrational rotational lines
Stimulated Raman effects in anisotropic crystal potassium dihydrogen phosphate with Stokes generations
The influence of the optical Stark effect on spectral line shapes in four-wave-mixing Raman spectroscopy (FWMRS) and stimulated Raman spectroscopy (SRS) is investigated experimentally and theoretically. Using an experimental setup capable of rapid alternation between the simultaneous measurement of coherent Stokes Raman spectroscopy and inverse Raman spectroscopy at low and high intensities, together with a sophisticated frequency reference scheme, it was possible to perform a rather direct comparison between Stark-broadened and non-Stark-broadened spectra of both classes of Raman spectroscopies. The results demonstrate that SRS spectra show more Stark shift and broadening than their FWMRS counterparts. A discrepancy with theoretical results is pointed out, and an attempt is made to explain it.
Two third order processes, stimulated Raman scattering and self-focusing, with picosecond pulses are studied. In the case of transient stimulated scattering, the gain is reduced from the steady state value, and qualitatively new features, such as shortening and delay of the Stokes pulse relative to the laser pulse, appear. These predictions are extended to realistic laser pulses, and experiments confirm all of the theoretical predictions. The self-focusing and frequency broadening of picosecond pulses is studied in the absence of stimulated Raman scattering in several materials with large orientational Kerr constants. Measurements of the relaxation time indicate that the orientational Kerr effect is important in the self-focusing of picosecond pulses. Self-focused filaments are observed to propagate with constant diameters over a distance greater than 10 cm, but disappear before the end of a 20 cm cell. The filaments radiate light continuously along their path and the spectrum of the light shows that the frequency content extends symmetrically for several hundred wave numbers on either side of the laser frequency.
Angular emission properties of stimulated Raman radiation from liquids, noting two classes of radiation
The main thrust of the program was the study of stimulated Raman processes for application to atmospheric lidar measurements. This has involved the development of tunable lasers, the detailed study of stimulated Raman scattering, and the use of the Raman-shifted light for new measurements of molecular line strengths and line widths. The principal spectral region explored in this work was the visible and near-IR wavelengths between 500 nm and 1.5 microns. Recent alexandrite ring laser experiments are reported. The experiments involved diode injection-locking, Raman shifting, and frequency-doubling. The experiments succeeded in producing tunable light at 577 and 937 nm with line widths in the range 80-160 MHz.
The dependence of the first Stokes stimulated Raman conversion efficiency of fourth-harmonic radiation from a Nd:YAG laser at 266 nm has been studied for the isotopic species H2, HD, and D2 as a function of gas pressure and laser energy using a low numerical aperture (about 0.0045) pumping geometry. While the laser energy threshold for first Stokes conversion varies significantly among the species, photon conversion efficiencies of at least 50 percent can be achieved for all of them for laser pump energies at 266 nm of 50 mJ/pulse or less. This study provides a new measurement of the differential cross section for stimulated Raman scattering in HD of 8.1 + or - 2.4 x 10 to the -29th sq cm/sr at 266 nm and at high pressures, and agreement is found with previous measurements of the cross sections for H2 and D2. The results have been used to optimize the laser transmitter system for a differential-absorption lidar to measure tropospheric ozone concentration profiles.
Ultrashort pulse formation in short pulse stimulated Raman oscillator, achieving partial group velocity matching
A modification of the standard theory of stimulated Raman scattering (SRS) first proposed by Sparks (1974, 1975) is analyzed and shown to incorporate a possibly important physical effect; however, its original formulation is incorrect. The analysis is based on an exact numerical integration of the coupled equations of the modified theory, the results of which are compared with both the conventional theory of SRS and with one set of experimental data. A reformulation of the modified theory is suggested that leads to a gain which is in somewhat better agreement with the data than is the conventional theory.
It is proposed to use high-resolution stimulated Raman spectroscopy to directly measure high-speed molecular flow velocities in wind tunnels and in combustive chambers. A feasibility study indicates that flow speeds from Mach 0.04 up may be measured with the proposed method using available laser systems. It is pointed out that the success of the proposed technique will make it possible to measure all interesting flow parameters, i.e., species concentration, temperature, and velocity, in a time of less than 1 microsecond at a repetition rate of 10,000/s using a single experimental arrangement.
Stimulated Raman scattering in IR active nontotally symmetric vibration of alpha quartz crystal, noting parametric oscillation
The observation and measurement of frequency shifts in stimulated Raman gain spectroscopy resulting from subsonic molecular nitrogen flows emerging from a simple nozzle are reported. The flow velocity in the region of the measurement was determined to be 145 m/s with an accuracy of plus or minus 30 m/s. It is expected that significantly better flow-velocity resolution will be obtained in future experiments using inverse Raman scattering.
Stimulated Raman scattering of the intense 22.2-GHz water-vapor maser radiation within W49 is examined as a possible explanation of the extremely broad spectrum of W49 extending to + or - 200 km/sec apparent Doppler velocity. Under the most favorable conditions, Raman scattering from ammonia molecules is calculated to be observable. It is unlikely that the Raman process contributes appreciably in the case of W49, as it fails to predict the observed spatial and spectral distribution of the radiation.
The results of numerical calculations of the transient stimulated Raman scattering reported previously have been verified experimentally under conditions where both linear dispersion and self-focusing effects were negligible. The existence of a delay between maxima of the laser and Stokes pulses is experimentally demonstrated for the first time, while the pulse shortening in time via Raman scattering is established more firmly than in previous work. The incident-laser-pulse duration, generated-Stokes-pulse duration, and delay between intensity maxima for the laser and Stokes pulses were measured with the two-photon absorption-fluorescence technique. The effective phonon-dephasing time is determined via spontaneous Raman scattering. By using these measured quantities, inferences are made as to the magnitude of the transient gain and the shape of the exciting picosecond laser pulse.
The fluctuation-dissipation theory of spontaneous and stimulated vibration Raman scattering is worked out taking into account the dissipation losses at frequencies of laser pump and scattering radiation. General expressions are found, which describe the absolute intensities and shape, energy and duration of scattered pulses in terms of the parameters of the medium and the the input laser pulses. The general regularities are analyzed in detail. Conditions are found for the realization of spontaneous or stimulated Raman scattering and its dependence on absorption, pulse duration and other parameters of the problem.
A broadband continuum generated in a germanosilicate optical fiber has been used as a coherent seed to initiate stimulated Raman scattering in gases. The technique used is described. The results show a fivefold increase in conversion efficiency and a similar reduction in the requisite pump power.
We report the first observations, to our knowledge, of nonlinear optical effects in large (millimeter-sized) droplets. Stimulated Raman scattering (SRS) and laser-induced breakdown (LIB) are simultaneously observed in acoustically levitated millimeter-sized glycerol droplets irradiated by either a frequency-doubled (532-nm) or a frequency-tripled (355-nm) Nd:YAG laser. The two processes, which occur above a nearby coincident irradiation threshold, are conjectured to arise from a common initiation mechanism: self-focusing. LIB generates vapor bubbles within the droplet, resulting in the quenching of SRS emission.
Self-, argon-, and helium-broadening coefficients have been measured for 13 lines in the 2nu2 Raman Q branch of CH4 using stimulated inverse Raman spectroscopy. The linewidths clearly show the symmetry-state dependence characteristic of pressure broadening, and inelastic processes in general, involving spherical-top molecules. Pressure-induced line shifts have also been measured for these features in pure methane. The pressure-shift coefficients do not display the symmetry-state dependence found for the linewidths. By applying the Rosenkranz perturbation treatment to a pair of collisionally mixed lines, an estimate of individual state-to-state contributions to the overall linewidth has been obtained.