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At least 55 records · Page 3

Raman scattering as a probe of planetary atmospheres

The observable effects of Raman scattering on the spectra of the giant planets may provide new information on the composition and structure of these atmospheres. Satellite observations have already shown the influence of Raman scattering on the UV continuum albedo. A cross correlation technique is presented for detecting rotational and vibrational transitions of the Raman active gases in the atmosphere. This technique has been applied to ground-based visible spectra of Venus, Jupiter, Saturn and Uranus. Extension of this method into the UV would improve the detectability of the Raman lines because the ratio of Raman to Rayleigh cross section increases with decreasing wavelength. The technology currently exists to efficiently obtain high-signal-to-noise ratio UV spectra through the use of silicon diode array detectors. Application of the cross-correlation technique to UV spectra obtained from space vehicles would give a new important probe of the structure and composition of planetary atmospheres by enabling the use of the UV spectra of a planet to observe what would normally be an infrared molecular transition.

Cochran, W. D.↗

Signatures of non-Loudon-Fleury Raman scattering in the Kitaev magnet 𝛽−Li 2 ⁢IrO 3

We investigate the magnetic excitations of the hyperhoneycomb Kitaev magnet 𝛽−Li 2 ⁢IrO 3 by means of inelastic Raman scattering. The spectra exhibit the coexistence of a broad scattering continuum and two sharp low-energy peaks at 2.5 and 3 meV, with a distinctive polarization dependence. While the continuum is suggestive of fractional quasiparticles emerging from a proximate quantum spin liquid phase, the sharp peaks provide the first experimental signature of the “non-Loudon- Fleury” one-magnon scattering processes proposed recently. The corresponding microscopic mechanism is similar to the one leading to the symmetric off-diagonal exchange interaction Γ (because it involves a combination of both direct and ligand-mediated exchange paths) but is otherwise completely unexpected within the traditional Loudon-Fleury theory of Raman scattering. Furthermore, the present experimental verification therefore calls for a drastic reevaluation of Raman scattering in similar systems with strong spin-orbit coupling and multiple exchange paths.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Stimulated Raman scattering and the extreme high-velocity H2O maser features in W49

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.

Boyd, R. W.↗

Spontaneous Raman Scattering Diagnostics for High-pressure Gaseous Flames

A high-pressure (up to 60 atm) gaseous burner facility with optical access that provides steady, reproducible flames with high precision, and the ability to use multiple fuel/oxidizer combinations has been developed. In addition, a high-performance spontaneous Raman scattering system for use in the above facility has also been developed. Together, the two systems will be used to acquire and establish a comprehensive Raman scattering spectral database for use as a quantitative high-pressure calibration of single-shot Raman scattering measurements in high-pressure combustion systems. Using these facilities, the Raman spectra of H2-Air flames were successfully measured at pressures up to 20 atm. The spectra demonstrated clear rotational and ro-vibrational Raman features of H2, N2, and H2O. theoretical Raman spectra of pure rotational H2, vibrational H2, and vibrational N2 were calculated using a classical harmonic-oscillator model with pressure broadening effects and fitted to the data. At a gas temperature of 1889 K for a phi = 1.34 H2-Air flame, the model and the data showed good agreement, confirming a ro-vibrational equilibrium temperature.

Kojima, Jun↗

Analysis of Raman scattered Ly-alpha emissions from the atmosphere of Uranus

A line at 1280 A, due to Raman scattering of solar Lyman alpha (Ly-alpha) in the atmosphere of Uranus, has been detected by the Voyager Ultraviolet Spectrometer. The measured intensity of 40 + or - 20 R implies that 200 R to 500 R of the measured 1500 R Ly-alpha intensity at the subsolar point is due to Rayleigh scattering of the solar line. The presence of Rayleigh and Raman scattering at 1216 A suggests that the Uranian atmosphere is largely devoid of absorbing hydrocarbons above the 0.5 mbar level. The most natural explanation of this depletion is very weak vertical mixing equivalent to an eddy coefficient on the order of 200 sq cm/sec between 0.5 mbar and 100 mbar.

Yelle, R. V.↗

Raman scattering cross section for N2O4.

Measurement of the Raman scattering cross section for N2O4 at a Raman shift of 7.3 micron, using a Q-switched ruby laser as an excitation source. The cross section for N2 at a Raman shift of 4.3 micron was also measured and compared with the value given by Leonard (1970).

Chen, C. J.↗

Evidence for Trapping-Induced Nonlinear Frequency Shifts in Langmuir Waves Driven via Stimulated Raman Scattering

Thomson scattering is used to detect the spectra of Langmuir waves driven through the backward stimulated Raman scattering process in a diffraction limited laser focal spot. Measured Langmuir wave spectral frequencies are found to vary in time and have broadened spectral power, consistent with a nonlinear frequency shift of the driven Langmuir wave due to electron-trapping. Broadening of the Langmuir wave spectral power is observed to decrease in time, consistent with measured variations in the frequency shift of the driven Langmuir waves. Furthermore, the observed spectral broadening is consistent with the temporally short (ps), bursty nature of backward stimulated Raman scattered light observed in simulations that cannot be resolved by the Thomson scattering diagnostic. Comparison of the broadened spectrum with time integrated spectra from two-dimensional particle-in-cell simulations shows favorable comparison in the broadened spectral widths, supporting the supposition of electron-trapping induced, nonlinear shifting of daughter Langmuir wave frequencies.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Raman scattering from rapid thermally annealed tungsten silicide

Raman scattering as a technique for studying the formation of tungsten silicide is presented. The tungsten silicide films have been formed by rapid thermal annealing of thin tungsten films sputter deposited on silicon substrates. The Raman data are interpreted by using data from resistivity measurements, Auger and Rutherford backscattering measurements, and scanning electron microscopy.

Kumar, Sandeep↗

A study of transient stimulated Raman scattering and self-focusing in the picosecond time regime

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.

Reintjes, J. F.↗

Boosting the performance of Brillouin amplification at sub-quarter-critical densities via reduction of parasitic Raman scattering

Brillouin amplification of laser pulses in plasma has been shown to be a promising approach to produce picosecond pulses of petawatt power. A key challenge is preservation of the quality of the amplified pulse, which requires control of parasitic instabilities that accompany the amplification process. At high plasma densities (> cr /4), ponderomotive filamentation has been identified as the biggest threat to the integrity of the amplifying pulse. It has therefore been proposed to perform Brillouin scattering at densities below n cr /4 to reduce the influence of filamentation. However, parasitic Raman scattering can become a problem at such densities, contrary to densities above n cr /4 where it is forbidden. In this paper, we investigate the influence of parasitic Raman scattering on Brillouin amplification at densities below n cr /4. We expose the specific problems posed by both Raman backward and forward scattering, and how both types of scattering can be mitigated, leading to an increased performance of the Brillouin amplification process.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

High-energy, low-jitter, narrowband ps probe laser for kHz-rate fs/ps coherent anti-Stokes Raman scattering

Hybrid fs/ps coherent anti-Stokes Raman scattering (CARS) thermometry often utilizes ps probe pulses derived from pulse shaping or spectrally filtering the primary laser source or by synchronization with a low repetition rate external laser. This results in limited energy, spectral resolution, and/or repetition rate of the ps probe. In this work, a master-oscillator power-amplifier (MOPA) laser was synchronized to the oscillator of a Ti:sapphire regenerative amplifier to achieve high-energy (600 µJ), narrowband (58 ps) probe pulses at kHz repetition rates. Furthermore, temporal filtering allows the pulse characteristics to be adjusted for each application. At 25 Torr, relevant to high-speed flows, the kHz-rate MOPA system generated signal-to-noise ratios 3× higher in nitrogen and had improved precision relative to a 10 ps probe derived from spectral filtering and the power-amplifier. The MOPA system also enabled single-shot ro-vibrational hybrid fs/ps CARS thermometry in 650 K heated air.

47 OTHER INSTRUMENTATION↗

Improved Raman-Scattering Gas-Species Monitor

Improved Raman-scattering instrument provides real-time measurements of concentration of gas species of interest mixed with other gases. High efficiency achieved by multiple passes of laser beam, fast collection optics. Costs less, weighs less, and operates more easily. In original application, instrument used to determine whether flammable or explosive concentration of leaking hydrogen present in atmosphere that contains varying concentrations of helium, air, and possibly other gases in addition to hydrogen.

Adler-Golden, Steven↗

UV Raman scattering measurements in a Mach 2 H2-air flame for assessment of CFD models

An UV narrowband tunable excimer laser is used for spontaneous Raman scattering measurements in hydrogen diffusion flames. The UV Raman system is characterized by a repetition rate of about 100 Hz, a temporal resolution of about 20 ns, and a spatial resolution of about 0.4 mm. It is concluded that a single KrF excimer laser based on spontaneous Raman scattering in conjunction with laser-induced predissociative fluorescence is capable of measuring instantaneously and simultaneously major species (H2, O2, N2, H2O), minor species (OH), and temperature.

Cheng, T. S.↗

Stimulated Raman scattering of light absorbing media excited by ultrashort laser pulses

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.

Marchevskiy, F. N.↗

Detection of atomic oxygen and its electronic coherence decays using time-resolved ultrafast coherent Raman scattering

We report the detection of atomic oxygen and quantitative measurements of its electronic Raman coherence decays in flames and low-temperature plasmas using time-resolved hybrid femtosecond/picosecond coherent anti-Stokes Raman scattering (CARS). Atomic oxygen was detected using the Raman transitions between the spin–orbit coupled triplet ground states. Atomic oxygen was generated in an H 2 /O 2 /Ar diffusion flame and an O 2 /Ar pulsed plasma discharge. Single exponential decays were observed for the O( 3 P 2 )–O( 3 P 1 ) Raman transition at 158.3 cm −1 and the O( 3 P 2 )–O( 3 P 0 ) Raman transition at 227 cm −1 . From the decay measurements, the atomic O Raman linewidths were obtained from 25 to 150 Torr in non-equilibrium plasma and at 760 Torr in a flame. Enhanced signal-to-noise ratios (SNRs) of atomic oxygen and atomic to molecular oxygen signal contrasts were obtained by taking advantage of electronic triplet coherence beating. Enhancement of up to seven times in the atomic O SNR was observed. Furthermore, we also found that the dephasing rates of O 2 (v = 0–3, N = 37) were similar, which provides evidence for the assumption that vibrational excitation does not influence the dephasing of diatomic molecular rotational CARS transitions.

Atomic and molecular spectroscopy↗

Modeling Surface-Enhanced Raman Scattering of Au-Pyrazine and Au-Pyrazine-Au Nanorod Dimer Systems with the TD-DFTB Method

This study investigates Raman scattering from a pyrazine molecule adsorbed on gold nanorod surfaces using the time-dependent density functional tight-binding (TD-DFTB) method. We analyze surface enhanced Raman scattering (SERS) of the molecule for two configurations: one where the molecule is adsorbed on a single gold nanorod forming Au-pyrazine complex, and another where it forms a nano-junction Au-pyrazine-Au dimer system. These two configurations offer distinct chemical environments for the molecule and different local field enhancements, with the dimer systems generating enhanced hotspot regions at the junctions. We present results for nanojunction, Au-pyrazine-Au dimer structures, for variable nanogap sizes that lead to shift in the plasmon energy. The study identifies contributions to the SERS enhancements from chemical, electromagnetic, and resonance charge transfer mechanisms. Our results show that the chemical mechanism provides enhancement factors in the range of 10 2 –10 3 , while the electromagnetic enhancements are on the order of 10 3 –10 5 for monomer systems and 10 6 –10 8 for dimer structures. We present results for a nanorod with a length of 5.3 nm and a width of 0.52 nm, consisting of 121 gold atoms.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Stimulated Raman Scattering Microscopy: Real-Time In-Situ Physical and Chemical Characterization of Reverse Osmosis Desalination Membrane Scaling

We introduce a stimulated Raman scattering (SRS) methodology designed for rapid, real-time, and in situ monitoring of RO membrane scaling adapted for bench-scale desalination flow cells. The methodology can provide new insights into membrane scaling dynamics by offering time-resolved reflection imaging of inorganic crystal growth, coupled with chemical identification from Raman spectral data. These capabilities allow for direct local measurement of the membrane surface area covered by different scalants as well as an approximation of the scalant volume using three-dimensional, integrated Raman intensity. The 2D and 3D SRS results obtained from CaSO 4 scaling experiments are compared to and are in reasonable agreement with those provided by confocal microscopy. The real-time physical and chemical characterization capabilities presented here could be extended to study combinations of inorganic, organic, and biological fouling. Overall, the SRS methodology represents an advancement in real-time sensing of membrane fouling that offers the potential for improved operation, lower cost, and more resilient RO membrane systems for sustainable water management.

42 ENGINEERING↗

Electron acceleration at oblique angles via stimulated Raman scattering at laser irradiance >10 16 W cm –2 μm 2

The generation of hot, directional electrons via laser-driven stimulated Raman scattering (SRS) is a topic of great importance in inertial confinement fusion (ICF) schemes. Little recent research has been dedicated to this process at high laser intensity, in which back, side, and forward scatter simultaneously occur in high energy density plasmas, of relevance to, for example, shock ignition ICF. In this paper, we present an experimental and particle-in-cell (PIC) investigation of hot electron production from SRS in the forward and near-forward directions from a single speckle laser of wavelength λ 0 = 1.053μm, peak laser intensities in the range I 0 = 0.2–1.0×10 17 Wcm –2 and target electron densities between ne = 0.3–1.6% n c , where n c is the plasma critical density. As the intensity and density are increased, the hot electron spectrum changes from a sharp cutoff to an extended spectrum with a slope temperature T = 34 ± 1 keV and maximum measured energy of 350 keV experimentally. Multidimensional PIC simulations indicate that the high energy electrons are primarily generated from SRS-driven electron plasma wave phase fronts with k vectors angled ~50° with respect to the laser axis. These results are consistent with analytical arguments that the spatial gain is maximized at an angle which balances the tendency for the growth rate to be larger for larger scattered light wave angles until the kinetic damping of the plasma wave becomes important. The efficiency of generated high energy electrons drops significantly with a reduction in either laser intensity or target electron density, which is a result of the rapid drop in growth rate of Raman scattering at angles in the forward direction.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗