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At least 451 records · Page 25

Frequency Conversion of High-Power Gyrotron Radiation under Conditions of Raman Backscattering on an Auxiliary Electron Beam

The regime of Raman backscattering of a pumping wave that is cocurrent with an electron beam into the counterpropagating wave can be used for the radiation frequency conversion in high-power gyrotrons. The absolute instability developing in this system ensures generation of a scattered signal in the absence of external resonators, which allows the frequency of scattered radiation to be smoothly controlled within 20–40% by varying the electron energy in the case of high-power (megawatt) gyrotrons used as sources of pumping radiation.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Temperature measurements in metalized propellant combustion using hybrid fs/ps coherent anti-Stokes Raman scattering

We apply ultrafast pure-rotational coherent anti-Stokes Raman scattering (CARS) for temperature and relative oxygen concentration measurements in the plume emanating from a burning, aluminized ammonium-perchlorate propellant strand. Combustion of these metal-based propellants is a particularly hostile environment for laser-based diagnostics, with intense background luminosity and scattering from hot metal particles as large as several hundred micrometers in diameter. CARS spectra that were previously obtained using nanosecond pulsed lasers in an aluminum-particle-seeded flame are examined and are determined to be severely impacted by nonresonant background, presumably as a result of the plasma formed by particulate-enhanced laser-induced breakdown. Introduction of femtosecond/picosecond (fs/ps) laser pulses improves CARS detection by providing time-gated elimination of strong nonresonant background interference. Single-laser-shot fs/ps CARS spectra were acquired from the burning propellant plume, with picosecond probe-pulse delays of 0 and 16 ps from the femtosecond pump and Stokes pulses. At zero delay, nonresonant background overwhelms the Raman-resonant spectroscopic features. Time-delayed probing results in the acquisition of background-free spectra that were successfully fit for temperature and relative oxygen content. Temperature probability densities and temperature/oxygen correlations were constructed from ensembles of several thousand single-laser-shot measurements with the CARS measurement volume positioned within 3 mm or less of the burning propellant surface. Lastly, the results show that ultrafast CARS is a potentially enabling technology for probing harsh, particle-laden flame environments.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

A Monte Carlo study of flux ratios of raman scattered o vi features at 6825 and 7082 Å in symbiotic stars

Symbiotic stars are regarded as wide binary systems consisting of a hot white dwarf and a mass losing giant. They exhibit unique spectral features at 6825 and 7082 Å, which are formed via Raman scattering of O vi λλ 1032 and 1038 with atomic hydrogen. We adopt a Monte Carlo technique to generate the same number of O vi λ1032 and λ1038 line photons and compute the flux ratio F(6825)/F(7082) of these Raman scattered O vi features formed in neutral regions with a simple geometric shape as a function of H i column density N {sub H i}. In cylindrical and spherical neutral regions with the O vi source embedded inside, the flux ratio F(6825)/F(7082) shows an overall decrease from 3 to 1 as N {sub H i} increases in the range 10{sup 22--24} cm{sup −2}. In cases of slab geometry and other geometries with the O vi source outside the H i region, Rayleigh escape operates to lower the flux ratio considerably. For moderate values of N{sub HI}∼10{sup 23} cm{sup −2} the flux ratio behaves in a complicated way to exhibit a broad bump with a peak value of 3.5 in the case of a sphere geometry. We find that the ratio of Raman conversion efficiencies of O vi λλ 1032, 1038 ranges from 0.8 to 3.5. Our high resolution spectra of “D” type HM Sge and “S” type AG Dra obtained with the Canada–France–Hawaii Telescope show that the flux ratio F(6825)/F(7082) of AG Dra is significantly smaller than that of HM Sge, implying that “S” type symbiotics are characterized by higher N {sub H i} than “D” type symbiotics.

79 ASTRONOMY AND ASTROPHYSICS↗

How Does the Shape of the Stellar Spectrum Affect the Raman Scattering Features in the Albedo of Exoplanets?

The diagnostic potential of the spectral signatures of Raman scattering, imprinted in planetary albedo spectra at short optical wavelengths, has been demonstrated in research on planets in the solar system, and has recently been proposed as a probe of exoplanet atmospheres, complementary to albedo studies at longer wavelengths. Spectral features caused by Raman scattering offer insight into the properties of planetary atmospheres, such as the atmospheric depth, composition, and temperature, as well as the possibility of detecting and spectroscopically identifying spectrally inactive species, such as H{sub 2} and N{sub 2}, in the visible wavelength range. Raman albedo features, however, depend on both the properties of the atmosphere and the shape of the incident stellar spectrum. Identical planetary atmospheres can produce very different albedo spectra depending on the spectral properties of the host star. Here we present a set of geometric albedo spectra calculated for atmospheres with H{sub 2}/He, N{sub 2}, and CO{sub 2} composition, irradiated by different stellar types ranging from late A to late K stars. Prominent albedo features caused by Raman scattering appear at different wavelengths for different types of host stars. We investigate how absorption due to the alkali elements sodium and potassium may affect the intensity of Raman features, and we discuss the preferred strategies for detecting Raman features in future observations.

79 ASTRONOMY AND ASTROPHYSICS↗

THE DISCOVERY OF RAMAN SCATTERING IN H II REGIONS

We report here on the discovery of faint extended wings of H α observed out to an apparent velocity of ∼7600 km s{sup −1} in the Orion Nebula (M42) and in five H ii regions in the Large and the Small Magellanic Clouds. We show that these wings are caused by Raman scattering of both the O i and Si ii resonance lines and stellar continuum UV photons with H i followed by radiative decay to the H i n = 2 level. The broad wings also seen in H β and in H γ result from Raman scattering of the UV continuum in the H i n = 4 and n = 5 levels, respectively. The Raman scattering fluorescence is correlated with the intensity of the narrow permitted lines of O i and Si ii. In the case of Si ii, this is explained by radiative pumping of the same 1023.7 Å resonance line involved in the Raman scattering by the Ly β radiation field. The subsequent radiative cascade produces enhanced Si ii λλ 5978.9, 6347.1, and 6371.4 Å permitted transitions. Finally, we show that in O i, radiative pumping of the 1025.76 Å resonance line by the Lyman series radiation field is also the cause of the enhancement in the permitted lines of this species lying near H α in wavelength, but here the process is a little more complex. We argue that all these processes are active in the zone of the H ii region near the ionization front.

79 ASTRONOMY AND ASTROPHYSICS↗

High-yield entangled single photon source

The various technologies presented herein relate to utilizing photons at respective idler and signal frequencies to facilitate generation of photons at a pump frequency. A strong pump field can be applied at the .omega..sub.i and the .omega..sub.s frequencies, with the generated idler and signal pulses being utilized to generate a photon pair at the .omega..sub.p frequency. Further, the idler pump power can be increased relative to the signal pump power such that the pump power P.sub.i>pump power P.sub.s. Such reversed operation (e.g., .omega..sub.i+.omega..sub.s.fwdarw..omega..sub.p1+.omega..sub.p2) can minimize and/or negate Raman scattering effects. By complying with an energy conservation requirement, the .omega..sub.i and .omega..sub.s photons interacting with the material through the four-wave mixing process facilitates the entanglement of the .omega..sub.p1 and .omega..sub.p2 photons. The .omega..sub.i and .omega..sub.s photons can be respectively formed in different length waveguides with a delay utilized to facilitate common timing between the .omega..sub.i and .omega..sub.s photons.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Design and Preparation of SiC-ZrC Composite Coating Layers by FB-CVD Used in TRISO Coated Fuel Particles - 18417

Tri-structural-isotropic (TRISO) particle has been successful in high temperature gas cooled reactor (HTGR), but an improved design is required for future development. In this paper, two alternative designs of TRISO particle are proposed by introducing ZrC to the coating layers. One design is to add an individual ZrC layer between the inner PyC layer and the SiC layer. Another design is to construct a periodic coating layer with the repeated sequence of SiC/SiC-ZrC by doping pulsed ZrCl{sub 4} at proper time intervals during the SiC preparation process. The designed coating layers were successfully prepared on the ZrO{sub 2}/buffer/IPyC particles by the fluidized bed chemical vapor deposition (FB-CVD) method. Microstructures and characterizations of the composite coating layers were given based on XRD, SEM, EDX and Raman scattering analysis. By controlling the pulse parameter, the grain size of SiC is significantly decreased which means doping ZrCl{sub 4} can interrupt normal growth of SiC crystals. (authors)

21 SPECIFIC NUCLEAR REACTORS AND ASSOCIATED PLANTS↗

Assessment of mode-mixing and Herzberg-Teller effects on two-photon absorption and resonance hyper-Raman spectra from a time-dependent approach

A time-dependent approach is presented to simulate the two-photon absorption (TPA) and resonance hyper-Raman scattering (RHRS) spectra including Duschinsky rotation (mode-mixing) and Herzberg-Teller (HT) vibronic coupling effects. The computational obstacles for the excited-state geometries, vibrational frequencies, and nuclear derivatives of transition dipole moments, which enter the expressions of TPA and RHRS cross sections, are further overcome by the recently developed analytical excited-state energy derivative approaches in the framework of time-dependent density functional theory. The excited-state potential curvatures are evaluated at different levels of approximation to inspect the effects of frequency differences, mode-mixing and HT on TPA and RHRS spectra. Two types of molecules, one with high symmetry (formaldehyde, p-difluorobenzene, and benzotrifluoride) and the other with non-centrosymmetry (cis-hydroxybenzylidene-2,3-dimethylimidazolinone in the deprotonated anion state (HDBI{sup −})), are used as test systems. The calculated results reveal that it is crucial to adopt the exact excited-state potential curvatures in the calculations of TPA and RHRS spectra even for the high-symmetric molecules, and that the vertical gradient approximation leads to a large deviation. Furthermore, it is found that the HT contribution is evident in the TPA and RHRS spectra of HDBI{sup −} although its one- and two-photon transitions are strongly allowed, and its effect results in an obvious blueshift of the TPA maximum with respect to the one-photon absorption maximum. With the HT and solvent effects getting involved, the simulated blueshift of 1291 cm{sup −1} agrees well with the experimental measurement.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Modeling of Raman-Scattering Signals in Biological Tissues by Direct and Two-Step Approaches

A search for an effective method of modelling of the Raman-spectroscopy problem in turbid (scattering) media has been performed taking into account the corresponding parameters of the detector and sample volume. A solution of the radiative-transfer equation by Monte-Carlo method underlies the proposed model. Two fundamental approaches to numerical modeling of Raman scattering are considered: the direct transport problem of Rayleigh and Raman photons at each point of the medium and the two-step model, in which a photon flux in the medium is calculated in the first stage, followed by generation of the corresponding number of Raman photons at each point.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Tuning the interaction between propagating and localized surface plasmons for surface enhanced Raman scattering in water for biomedical and environmental applications

With a view to biomedical and environmental applications, we investigate the plasmonic properties of a rectangular gold nanodisk array in water to boost surface enhanced Raman scattering (SERS) effects. To control the resonance wavelengths of the surface plasmon polariton and the localized surface plasmon, their dependence on the array period and diameter in water is studied in detail using a finite difference time domain method. A good agreement is obtained between calculated resonant wavelengths and those of gold nanodisk arrays fabricated using electron beam lithography. For the optimized structure, a SERS enhancement factor of 7.8 × 10{sup 7} is achieved in water experimentally.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Tip-enhanced near-field optical microscope with side-on and ATR-mode sample excitation for super-resolution Raman imaging of surfaces

A tip-enhanced near-field optical microscope with side-on and attenuated total reflectance (ATR) excitation and collection is described and used to demonstrate sub-diffraction-limited (super-resolution) optical and chemical characterization of surfaces. ATR illumination is combined with an Au optical antenna tip to show that (i) the tip can quantitatively transduce the optical near-field (evanescent waves) above the surface by scattering photons into the far-field, (ii) the ATR geometry enables excitation and characterization of surface plasmon polaritons (SPPs), whose associated optical fields are shown to enhance Raman scattering from a thin layer of copper phthalocyanine (CuPc), and (iii) SPPs can be used to plasmonically excite the tip for super-resolution chemical imaging of patterned CuPc via tip-enhanced Raman spectroscopy (TERS). ATR-illumination TERS is also quantitatively compared with the more conventional side-on illumination scheme. In both cases, spatial resolution was better than 40 nm and tip on/tip off Raman enhancement factors were >6500. Furthermore, ATR illumination was shown to provide similar Raman signal levels at lower “effective” pump powers due to additional optical energy delivered by SPPs to the active region in the tip-surface gap.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Effect of the magnetic field on coexisting stimulated Raman and Brillouin backscattering of an extraordinary mode

This paper presents a model to study the interplay between the stimulated Raman scattering (SRS) and stimulated Brillouin scattering (SBS) in the presence of background magnetic field. This formalism is applicable to laser produced plasma as well as to heating mechanism in toroidal system by an extraordinary electromagnetic wave. In the former case, the magnetic field is self-generated, while in the latter case (toroidal plasmas) magnetic field is applied externally. The behavior of one scattering process is explicitly dependent on the coexisting scattering process as well as on the magnetic field. Explicit expressions for the back-reflectivity of scattered beams (SRS and SBS) are presented. It has been demonstrated that due to the magnetic field and coexistence of the scattering processes (SRS and SBS) the back-reflectivity gets modified significantly. Results are also compared with the three wave interaction case (isolated SRS or SBS case)

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Effect of laser beam filamentation on coexisting stimulated Raman and Brillouin scattering

This paper presents the study of stimulated Raman scattering (SRS) and stimulated Brillouin scattering (SBS) when both of these processes are coexisting and pump laser beam initial power is more than filamentation threshold. On account of the ponderomotive nonlinearity, the pump laser beam gets filamented, and both the scattering processes (SRS and SBS) get affected. Simultaneous presence of SRS and SBS (five wave interaction case) also affect the pump filamentation process due to pump depletion. Both the scattering processes (SRS and SBS) are enhanced due to filamentation of laser beam. Results are also compared with the three wave interaction case (either SRS or SBS) with and without filamentation.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Control of Brillouin short-pulse seed amplification by chirping the pump pulse

Seed amplification via Brillouin backscattering of a long pump pulse is considered. Similar to Raman amplification, several obstructive effects may occur during short-pulse Brillouin amplification. One is the spontaneous Raman backscattering of the pump before interacting with the seed. Preforming the plasma and/or chirping the pump will reduce unwanted pump backscattering. Optimized regions for low-loss pump propagation were proposed already in conjunction with Raman seed amplification. Hence, the influence of the chirp of the pump during Brillouin interaction with the seed becomes important and will be considered here. Both, the linear as well as the nonlinear evolution phases of the seed caused by Brillouin amplification under the action of a chirped pump are investigated. The amplification rate as well as the seed profiles are presented as function of the chirping rate. Also the dependence of superradiant scaling rates on the chirp parameter is discussed.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Effect of an Optical Breakdown on the Stimulated Raman Scattering in Water in the Field of Picosecond Laser Pulses

Experiments on nonstationary stimulated Raman scattering (SRS) of laser pulses and an optical breakdown are performed to study water samples with gas nanobubbles (bubstons) and without the bubston phase. The SRS excitation threshold in water with the bubston phase turns out to be higher than that in bubston-free water, and the optical breakdown threshold in bubston-containing water is lower than that in bubston-free water. The spectral composition of the SRS signal from bubston-free water samples is found to differ from that of bubston-containing water samples. This effect is caused by the formation of long-lived high-molecular H{sub 2}O complexes near the bubston surface, which are stabilized by the dispersion forces acting from this surface. Since these complexes are located inside 1–2 monolayers adjacent to the surface, the volume density of these complexes is negligibly small as compared to the density of “free” (not bound to bubstons) molecules. To interpret the experimental results, we advance a hypothesis that the detected effect is related to the giant enhancement caused by the generation of a resonance plasmon inside a bubston during an optical breakdown. As follows from our estimates, the bubston-related plasma frequency falls in the range 2600–3200 cm{sup –1}; it is this range that contains the SRS spectral lines of water containing the bubston phase.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Synthesis of silver particles on copper substrates using ethanol-based solution for surface-enhanced Raman spectroscopy

The displacement reaction of AgNO{sub 3} and copper metal is an effective and economical way to fabricate Ag-Cu surface enhanced Raman scattering (SERS) substrates. Aqueous solutions of AgNO{sub 3} are usually used for substrate preparation. In this work, a new method for Ag-Cu SERS substrate preparation is proposed, which uses an ethanol solution rather than an aqueous AgNO{sub 3} solution. Analysis of the surface morphologies of sample substrates by field emission scanning electron microscopy (FESEM) showed that the silver nanoparticles prepared by this new method were more regular than those prepared in the traditional aqueous solution. The SERS spectra of Rhodamine 6G (R6G) adsorbed on these Ag-Cu substrates were then investigated and compared. It was found that the Ag-Cu substrates prepared by this method provide significant improvements in Raman signal sensitivity and large-area uniformity. The enhancement factor of this new substrate is about 330 times higher than that prepared using an aqueous AgNO{sub 3} solution under identical experimental conditions. It was also found that 70% of the original sensitivity of the substrate remains after 15 days of exposure to air.

36 MATERIALS SCIENCE↗