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The conversion efficiency of the first Stokes radiation generated by backward stimulated Raman scattering is measured in CH4 and H2 that are pumped by a third harmonic of a Nd:YAG laser in the 12-55-mJ energy range and in the 0.86-6.00-MPa pressure range. Our experimental results show that CH4 is a better Raman medium than H2 at moderate pressures (a few megapascals) to efficiently generate backward Raman lines.
Technique for measuring velocity, static pressure, and translational temperature of flowing molecules by use of stimulated Raman spectroscopy demonstrated in supersonic wind tunnel at NASA Langley Research Center. Nonintrusive, accurate wind-tunnel measurements obtained without seeding flows. Optical equipment for vibration-free Raman doppler velocimetry in wind tunnel includes specially designed retrometer that reduces sensitivity of system to vibrations. This capability very valuable in aerodynamic testing and proves useful in wide variety of laboratory, industrial, and engineering applications.
Here, we use a subignition scale laser, the 30 kJ Omega, and a novel shallow-cone target to study laser-plasma interactions at the ablation-plasma density scale lengths and laser intensities anticipated for direct drive shock-ignition implosions at National Ignition Facility scale. Our results show that, under these conditions, the dominant instability is convective stimulated Raman scatter with experimental evidence of two plasmon decay (TPD) only when the density scale length is reduced. Particle-in-cell simulations indicate this is due to TPD being shifted to lower densities, removing the experimental back-scatter signature and reducing the hot-electron temperature. The experimental laser energy-coupling to hot electrons was found to be 1%–2.5%, with electron temperatures between 35 and 45 keV. Radiation-hydrodynamics simulations employing these hot-electron characteristics indicate that they should not preheat the fuel in MJ-scale shock ignition experiments.
We report first-Stokes vibrational conversion efficiency of 21 percent and 35 percent, respectively, in high-pressure O2- and N2-stimulated Raman cells. Broadband superfluorescence is employed to seed these Raman cells, significantly increasing the conversion efficiences with no measured effect on the Raman spectrum. The addition of helium buffer gas reduces competition from stimulated Brillouin scattering and improves the pulse-to-pulse stability and spatial mode quality by increasing the thermal conductivity. Further improvement of the spatial mode quality is achieved by use of gentle heating on the bottom of the cell to induce convection.
Optical components for laser beams with high peak and averaged powers are being developed worldwide using stimulated plasma scattering that occurs when plasmas interact with intense, coherent light. After decades of pursuit of pulse compressors, mirrors, and other plasma based components that can be created by stimulated scattering from electron density perturbations forming on ultra-short time scales (e.g., via Stimulated Raman Scattering), more recent work has produced optical components on longer time scales allowing ion motion as well [via Stimulated Brillouin Scattering (SBS)]. In the most recent work, ion wave plasma optics have had success in producing pulses of focusable coherent light with high energy and fluence by operating on ns time scales and now promise to enable numerous applications. Experiments have further shown that in some parameter regimes, even simple plasma response models can describe the output of such optics with sufficient accuracy that they can be used as engineering tools to design plasma optics for future applications, as is already being done to control power deposition in fusion targets. In addition, the development of more sophisticated models promises to enable still higher performance from SBS driven plasma optical components under a wider range of conditions. The present status and most promising directions for future development of ion wave plasma optic techniques are discussed here.
As an alternative inertial confinement fusion scheme, shock ignition requires a strong converging shock driven by a high-intensity laser pulse to ignite a pre-compressed fusion capsule. Understanding nonlinear laser-plasma instabilities is crucial to assess and improve the laser-shock energy coupling. Recent experiments conducted on the OMEGA EP laser facility have for the first time demonstrated that such instabilities can 100% deplete the first 0.5 ns of the high-intensity laser. Here, analyses of the observed laser-generated blast wave suggest that this pump-depletion starts at 0.02 critical density and progresses to 0.1-0.2 critical density, which is also confirmed by the time-resolved stimulated Raman backscattering spectra. The pump-depletion dynamics can be explained by the breaking of ion-acoustic waves in stimulated Brillouin scattering. Such pump-depletion would inhibit the collisional laser energy absorption but may benefit the generation of hot electrons with moderate temperatures for electron shock ignition.
Raman Excitation + Laser Induced Electronic Fluorescence (RELIEF) is a double resonance velocimetry technique in which oxygen molecules are vibrationally excited via stimulated Raman scattering at a specific location within a flow field. After suitable time delay, typically 1-10 microseconds, the displacement of the tagged molecules is determined by laser induced fluorescence imaging. Providing support for the installation of simplified RELIEF flow tagging instrumentation at NASA LaRC was the principal goal of this research.
Frequency upconversion by means of stimulated Raman scattering is examined. A monochromatic beam is scattered into the anti-Stokes wave in a medium with an inverted population of the pair of energy levels involved. A method is proposed in which the beam from a laser tuned to the desired anti-Stokes frequency provides an initial stimulating wave of sufficient intensity to ensure the desired Raman scattering dominates competitive processes.
Effects of quantum mechanical interferences on third-order susceptibilities in molecules are studied. First principle calculations for molecular hydrogen are presented and shown to agree with results derived from experimental stimulated Raman gain and spontaneous Raman cross-section data. 10 percent third-harmonic conversion efficiency in H2 at 1 atm without phase matching should require a 150 MW per sq cm at 4.81 microns. As little as 5.9-MW power is sufficient when the beam is properly focused. Resonance Raman scattering (RRS) is proposed for experimentally investigating the interference effects, which tend to reduce the strength of third-order nonlinear susceptibilities.
For improved DIAL measurements of water vapor in the upper troposphere or lower stratosphere, narrowband (about 0.03/cm) laser radiation at 720- and 940-nm wavelengths was generated by stimulated Raman scattering (SRS), using the narrow linewidth (about 0.02/cm) output of a Nd:YAG-pumped dye laser. For a hydrogen pressure of 350 psi, the first Stokes conversion efficiencies to 940 nm were 20 percent and 35 percent, when using a conventional and waveguide Raman cell, respectively. The linewidth of the first Stokes line at high cell pressures, and the inferred collisional broadening coefficients, agree well with those previously measured in spontaneous Raman scattering.
Laser-plasma instabilities under ignition conditions for direct-drive inertial confinement fusion are studied using two-dimensional Particle-in-Cell simulations with a combination of in-plane (PP) and out-of-the-plane (SP) lasers. The results show that stimulated Raman side scattering can induce significant pump depletion and form a gap in the Raman scattered light spectra that have been observed in experiments.
The differential absorption lidar (DIAL) measurement of tropospheric ozone requires use of high average power UV lasers operating at two appropriate DIAL wavelengths. Laboratory experiments have demonstrated that a KrF excimer laser can be used to generate several wavelengths with good energy conversion efficiencies by stimulated Raman shifting using hydrogen (H2) and deuterium (D2). Computer simulations for an airborne lidar have shown that these laser emissions can be used for the less than 5 percent random error, high resolution measuremment of ozone across the troposphere using the DIAL technique. In the region of strong ozone absorption, laser wavelengths of 277.0 and 291.7 nm were generated using H2 and D2, respectively. In addition, a laser wavelength at 302.0 nm was generated using two cells in series, with the first containing D2 and the second containing H2. The energy conversion efficiency for each wavelength was between 14 and 27 percent.
Phase matching of diverse electromagnetic modes (specifically, coexisting optical and microwave modes) in a whispering-gallery-mode (WGM) resonator has been predicted theoretically and verified experimentally. Such phase matching is necessary for storage of microwave/terahertz and optical electromagnetic energy in the same resonator, as needed for exploitation of nonlinear optical phenomena. WGM resonators are used in research on nonlinear optical phenomena at low optical intensities and as a basis for design and fabrication of novel optical devices. Examples of nonlinear optical phenomena recently demonstrated in WGM resonators include low-threshold Raman lasing, optomechanical oscillations, frequency doubling, and hyperparametric oscillations. The present findings regarding phase matching were made in research on low-threshold, strongly nondegenerate parametric oscillations in lithium niobate WGM resonators. The principle of operation of such an oscillator is rooted in two previously observed phenomena: (1) stimulated Raman scattering by polaritons in lithium niobate and (2) phase matching of nonlinear optical processes via geometrical confinement of light. The oscillator is partly similar to terahertz oscillators based on lithium niobate crystals, the key difference being that a novel geometrical configuration of this oscillator supports oscillation in the regime. The high resonance quality factors (Q values) typical of WGM resonators make it possible to achieve oscillation at a threshold signal level much lower than that in a non-WGM-resonator lithium niobate crystal.
The vibrational dephasing of the 656/cm mode (nu1, a1g) of CS2 and the 991/cm mode (nu2, a1g) of benzene have been studied as a function of concentration in mixtures with a number of solvents using a ps time-resolved CARS technique. This technique employs two tunable synchronously-pumped mode-locked dye lasers in a stimulated Raman pump, coherent anti-Stokes Raman probe time-resolved experiment. Results are obtained for CS2 in carbon tetrachloride, benzene, nitrobenzene, and ethanol and for benzene nu2 in CS2. The dephasing rates of CS2 nu1 increase on dilution with the polar solvents and decrease or remain constant on dilution with the nonpolar solvents. The CS2/benzene solutions show a contrasting behavior, with the CS2 nu1 dephasing rate being nearly independent of concentration whereas the benzene nu2 dephasing rate decreases on dilution. These results are compared to theoretical models for vibrational dephasing of polyatomic molecules in solution.
The use of an O2:He stimulated Raman cell to generate the Stokes beam for the Raman vibrational pumping step of the RELIEF (Raman Excitation plus Laser-Induced Electronic Fluorescence) flow tagging method is reported. Use of the Raman cell rather than a dye laser provides pump and Stokes beams which are automatically frequency matched and temporally and spatially overlapped. The Nd:YAG pump laser is operated multilongitudinal mode, which eliminates the need for injection seeding, resulting in decreased operation complexity and improved stability with respect to acoustic noise. Results are presented for 1st Stokes conversion efficiency and stimulated Brillouin backscattering loss and are compared to the case of pure O2. Scanning CARS measurements of the Q-branch lineshape for both pure O2 and the O2:He mixture are also presented.
Since the XeCl excimer laser (308 nm) was first used in Differential Absorption Lidar (DIAL) for stratospheric ozone detection, the XeCl ozone lidar became a useful tool for the monitoring of the stratospheric ozone concentration. Shorter wavelength lasers are needed for the observation of ozone in the troposphere where the ozone concentration is about one order of magnitude smaller than in the stratosphere. In 1983, tropospheric ozone was observed with the combination of the second Stokes line (290.4 nm) of stimulated Raman scattering from methane pumped by a KrF laser and the XeCl laser line. The measurement of the ozone distribution from ground to 30 km was reported, using three Stokes lines of Raman lasers pumped by a KrF laser. At wavelengths shorter than 295 nm, the background solar radiation is effectively suppressed by atmospheric ozone. Such a solar-blind effect can be expected when two wavelengths 277 and 290.4 nm are used for DIAL ozone detection. A preliminary measurement of the day time ozone distribution in the troposphere is presented using these wavelengths generated by a KrF laser with a Raman shifter. Analysis using the lidar equation predicts the maximum detectable range is 7 km.
Existing DIAL systems for water vapor measurements in the troposphere operate at wavelengths near 720 nm. The use of stronger water vapor absorption lines in the range 930 to 960 nm will significantly improve DIAL measurements in the upper troposphere and lower stratosphere where water vapor concentrations are low. The generation of light at 940 nm using a frequency doubled Nd:YAG pumped dye laser is inefficient due to the small absorption if infrared dyes at the pump wavelength. However, 940 nm generation utilizing stimulated Raman scattering of dye lasers is attractive because of a potentially high conversion efficiency plus the possibility of retaining the narrow linewidth available from some dye lasers. The Raman conversion efficiency and line broadening are presented for first Stokes operation at 720 and 940 nm using hydrogen and deuterium as the Raman media.
Important advances is recently made in the search for materials with complex multi-phase landscapes that host photoinduced metastable collective states with exotic functionalities. In almost all cases so far, the desired phases are accessed by exploiting light–matter interactions via the imaginary part of the dielectric function through above-bandgap or resonant mode excitation. Nonresonant Raman excitation of coherent modes is experimentally observed and proposed for dynamic material control, but the resulting atomic excursion is limited to perturbative levels. Here, in this study, this challenge is overcome by employing nonresonant ultrashort pulses with low photon energies well below the bandgap. Using mid-infrared pulses, ferroelectric reversal is induced in lithium niobate, and the large-amplitude mode displacements are characterized through femtosecond stimulated Raman scattering and second harmonic generation. This approach, validated by first-principle calculations, defines a novel method for synthesizing hidden phases with unique functional properties and manipulating complex energy landscapes at reduced energy consumption and ultrafast speeds.