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At least 307 records · Page 17

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↗

Optical Stark effect in the four-wave mixing and stimulated Raman spectra of N2

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.

Moosmuller, H.↗

Efficient vibrational Raman conversion in O2 and N2 cells by use of superfluorescence seeding

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.

Zhang, Barry↗

H irradiation effects on the GaAs-like Raman modes in GaAs{sub 1-x}N{sub x}/GaAs{sub 1-x}N{sub x}:H planar heterostructures

The GaAs-like longitudinal optical phonon frequency in two hydrogenated GaAs{sub 1-x}N{sub x}/GaAs{sub 1-x}N{sub x}:H microwire heterostructures—with similar N concentration, but different H dose and implantation conditions—has been investigated by micro-Raman mapping. In the case of GaAs{sub 0.991}N{sub 0.009} wires embedded in barriers where GaAs-like properties are recovered through H irradiation, the phonon frequency in the barriers undergoes a blue shift with respect to the wires. In GaAs{sub 0.992}N{sub 0.008} wires embedded in less hydrogenated barriers, the phonon frequency exhibits an opposite behavior (red shift). Strain, disorder, phonon localization effects induced by H-irradiation on the GaAs-like phonon frequency are discussed and related to different types of N-H complexes formed in the hydrogenated barriers. It is shown that the red (blue) character of the frequency shift is related to the dominant N-2H (N-3H) type of complexes. Moreover, for specific experimental conditions, an all-optical determination of the uniaxial strain field is obtained. This may improve the design of recently presented devices that exploit the correlation between uniaxial stress and the degree of polarization of photoluminescence.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Fe 2 O 3 -Au hybrid nanoparticles for sensing applications via SERS analysis

Multifunctional iron oxide-gold hybrid nanostructures have been produced via solution chemistries and investigated for analyte detection. Gold nanoparticles of various shapes have been used for probing surface-enhanced Raman scattering (SERS) effects as they display unique optical properties in the visible-near IR region of the spectrum. When coupled with other nanoparticles, namely iron oxide nanoparticles, hybrid structures with increased functionality were produced. By exploiting their magnetic properties, nanogaps or “hot spots” were rationally created and evaluated for SERS enhancement studies. The “hot spots” were created by using a seeded reaction to increase the gold loading on the iron oxide support by 43% by weight. SERS Nanomaterials were evaluated for their ability to promote surface-enhanced Raman scattering of a model analyte, 4-mercaptophenol. The data shows an enhancement effect of the model analyte on gold decorated iron oxide nanoparticles.

36 MATERIALS SCIENCE↗

Enhancement of Optical Nonlinearities in Composite Media and Structures via Local Fields and Electromagnetic Coupling Effects

This talk will review the linear and nonlinear optical properties of metal nanoparticles and dielectric microparticles, with an emphasis on local field effects, and whispering gallery modes (WGMs), as well as the conjunction of these two effects for enhanced Raman. In particular, enhanced optical properties that result from electromagnetic coupling effects will be discussed in the context of Mie scattering from concentric spheres and bispheres. Predictions of mode splitting and photonic bandgaps in micro-spheres will be presented and will be shown to be analogous to effects that occur in coupled resonator optical waveguides (CROW). Slow and fast light in SCISSOR / CROW configurations will also be discussed.

Smith, David D.↗

CALIPSO-Inferred Aerosol Direct Radiative Effects: Bias Estimates Using Ground-Based Raman Lidars

Observational constraints on the change in the radiative energy budget caused by the presence of aerosols, i.e. the aerosol direct radiative effect (DRE), have recently been made using observations from the Cloud- Aerosol Lidar and Infrared Pathfinder Satellite (CALIPSO). CALIPSO observations have the potential to provide improved global estimates of aerosol DRE compared to passive sensor-derived estimates due to CALIPSO's ability to perform vertically-resolved aerosol retrievals over all surface types and over cloud. In this study we estimate the uncertainties in CALIPSO-inferred aerosol DRE using multiple years of observations from the Atmospheric Radiation Measurement (ARM) program's Raman lidars (RL) at mid-latitude and tropical sites. Examined are assumptions about the ratio of extinction-to-backscatter (i.e. the lidar ratio) made by the CALIPSO retrievals, which are needed to retrieve the aerosol extinction profile. The lidar ratio is shown to introduce minimal error in the mean aerosol DRE at the top-of-atmosphere and surface. It is also shown that CALIPSO is unable to detect all radiatively-significant aerosol, resulting in an underestimate in the magnitude of the aerosol DRE by 30â€"50%. Therefore, global estimates of the aerosol DRE inferred from CALIPSO observations are likely too weak.

Thorsen, Tyler↗

CALIPSO-Inferred Aerosol Direct Radiative Effects: Bias Estimates Using Ground-Based Raman Lidars

Observational constraints on the change in the radiative energy budget caused by the presence of aerosols, i.e. the aerosol direct radiative effect (DRE), have recently been made using observations from the Cloud- Aerosol Lidar and Infrared Pathfinder Satellite (CALIPSO). CALIPSO observations have the potential to provide improved global estimates of aerosol DRE compared to passive sensor-derived estimates due to CALIPSO's ability to perform vertically-resolved aerosol retrievals over all surface types and over cloud. In this study we estimate the uncertainties in CALIPSO-inferred aerosol DRE using multiple years of observations from the Atmospheric Radiation Measurement (ARM) program's Raman lidars (RL) at midlatitude and tropical sites. Examined are assumptions about the ratio of extinction-to-backscatter (i.e. the lidar ratio) made by the CALIPSO retrievals, which are needed to retrieve the aerosol extinction profile. The lidar ratio is shown to introduce minimal error in the mean aerosol DRE at the top-of-atmosphere and surface. It is also shown that CALIPSO is unable to detect all radiatively-significant aerosol, resulting in an underestimate in the magnitude of the aerosol DRE by 30-50%. Therefore, global estimates of the aerosol DRE inferred from CALIPSO observations are likely too weak.

Thorsen, Tyler↗

Effect of ion interactions on the Raman spectrum of NO 3 − : Toward monitoring of low-activity nuclear waste at Hanford

Raman spectroscopy is a valuable in-situ technique for many applications. The concentrations of species in complex ionic mixtures of nuclear waste can be estimated using Raman measurements. However, it has been experimentally observed that ion interactions can cause a modification of Raman peak intensities and positions. The present work explores the nonlinear behavior associated with the nitrate anion, NO 3 − , which is present in abundance in low activity nuclear waste. We examine changes in the main Raman peak of the nitrate anion in the presence of other ions. A wide range of concentrations are covered, including those expected during direct-feed low-activity waste (DFLAW) processing at the Hanford site in the State of Washington. The experiments showed that the ions interact and associate to form ion pairs, which results in a blue shift (i.e., a shift towards higher wavenumbers) in the main Raman peak of nitrate. The results indicate that cation concentration is a better predictor of the peak shift, compared to ionic strength, both for binary and multicomponent mixtures. These findings have direct implications on the development of spectra-to-composition models for the DFLAW system, since they show deviations from the linearity assumptions used in common chemometric models.

42 ENGINEERING↗

Conversion of ultrashort laser pulses to wavelengths above 3 mm in tapered germanate fibres

Tapered germanate fibres are proposed for effective adiabatic conversion of Raman soliton pulses to the mid-IR region. A theoretical analysis demonstrates that, in fibres with anomalous group velocity dispersion decreasing along their length, wavelengths of up to 3.5 μm can be reached, which are unattainable in fibres with a constant core diameter at the same parameters of a 2-μm input signal. The analysis relies on a one-way wave equation that takes into account the combined effect of dispersion, Kerr and Raman nonlinearities, nonlinear dispersion and optical losses and the frequency dependence of the effective fundamental transverse mode size. (extreme light fields and their applications)

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Liquid Water Cloud Measurements Using the Raman Lidar Technique: Current Understanding and Future Research Needs

This paper describes recent work in the Raman lidar liquid water cloud measurement technique. The range-resolved spectral measurements at the National Aeronautics and Space Administration Goddard Space Flight Center indicate that the Raman backscattering spectra measured in and below low clouds agree well with theoretical spectra for vapor and liquid water. The calibration coefficients of the liquid water measurement for the Raman lidar at the Atmospheric Radiation Measurement Program Southern Great Plains site of the U.S. Department of Energy were determined by comparison with the liquid water path (LWP) obtained with Atmospheric Emitted Radiance Interferometer (AERI) and the liquid water content (LWC) obtained with the millimeter wavelength cloud radar and water vapor radiometer (MMCR-WVR) together. These comparisons were used to estimate the Raman liquid water cross-sectional value. The results indicate a bias consistent with an effective liquid water Raman cross-sectional value that is 28%-46% lower than published, which may be explained by the fact that the difference in the detectors' sensitivity has not been accounted for. The LWP of a thin altostratus cloud showed good qualitative agreement between lidar retrievals and AERI. However, the overall ensemble of comparisons of LWP showed considerable scatter, possibly because of the different fields of view of the instruments, the 350-m distance between the instruments, and the horizontal inhomogeneity of the clouds. The LWC profiles for a thick stratus cloud showed agreement between lidar retrievals andMMCR-WVR between the cloud base and 150m above that where the optical depth was less than 3. Areas requiring further research in this technique are discussed.

vapor and liquid water↗

Laser radar studies: A study of the feasibility of remote measurement of atmospheric density and turbidity by means of rotational Raman scattering of laser light

A remote sensing technique is described which utilizes elastic scattering and rotational Raman scattering of laser light in the atmosphere to obtain soundings of turbidity, transmissivity and density. A scheme is devised whereby, through selective weighting of the rotational Raman lines, the effect of atmospheric temperature structure may be eliminated. The close spectral proximity of the elastic and Raman-scattered signals, combined with the fact that the Raman scattering is quite weak, produces special requirements for the spectroscopic and light-gathering components of a rotational Raman laser radar system. These requirements are investigated. A computation of typical signal-to-noise ratios is made. It is shown that daytime signal-to-noise ratios greater than 10 db are to be expected for observation heights of 5 km and below. For nighttime work, 10 db signal-to-noise ratios are achievable to altitudes as high as 15 km.

Reiss, N.↗

Ring Effect Studies: Rayleigh Scattering, including Molecular Parameters for Rotational Raman Scattering, and the Faunhofer Spectrum

Improved parameters for the description of Rayleigh scattering in air and for the detailed rotational Raman scattering component for scattering by O2 and N2 are presented for the wavelength range 200-1000 nm. These parameters enable more accurate calculations of bulk molecular scattering and of the 'Ring effect' for a variety of atmospheric radiative transfer and constituent retrieval applications. A solar reference spectrum with accurate absolute vacuum wavelength calibration, suitable for convolution with the rotational Raman spectrum for Ring effect calculations, has been produced and is briefly described. The solar-rotational Raman convolved product is available for fitting of atmospheric spectra.

Chance, K. V.↗

Impact of moderate pump–Stokes chirp on femtosecond coherent anti-Stokes Raman scattering spectra

The effects of inducing moderate chirp in the pump and Stokes beams in chirped-probe-pulse femtosecond coherent anti-Stokes Raman scattering (CARS) spectroscopy are discussed. This is an important issue for measurements in high-pressure systems where the CARS beams must be transmitted through glass of significant thickness to reach the probe volume of interest. The effects were investigated both experimentally, by inserting disks of SF-11 glass into the pump and Stokes beam paths, and theoretically, by incorporating pulse chirp into our time-dependent density matrix (TDDM) simulations. Experimentally, we found that inducing moderate pump and Stokes chirp produced significant spectral narrowing of the nonresonant four-wave mixing contribution to the CARS signal, and this allowed us to control the resonant excitation bandwidth to eliminate interferences from neighboring species. The temperature measurement accuracy and precision were essentially unchanged with respect to the unchirped pump and Stokes case. The effect of moderate pump and Stokes chirp on the narrowing of the Raman excitation efficiency envelope was investigated by solving the full set of TDDM through direct numerical integration. The numerical efficiency of the solutions was enhanced dramatically by developing a parallel version of the TDDM code. The calculated Raman excitation efficiency profile was incorporated in our phenomenological spectral fitting codes.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Influence of the nanoparticles agglomeration state in the quantum-confinement effects: Experimental evidences

The agglomeration state facilitates particle-particle interaction which produces important effects in the phonon confinement effects at the nanoscale. A partial phonon transmission between close nanoparticles yields a lower momentum conservation relaxation than in a single isolated nanoparticle. It means a larger red shift and broadening of the Raman modes than the expected ones for Raman quantum confinement effects. This particle-particle interaction can drive to error when Raman responses are used to estimate the size of the nanoscaled materials. In this work different corrections are suggested to overtake this source of error.

36 MATERIALS SCIENCE↗