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At least 109 records · Page 6

Evaluation of Raman scattering as a sensor of temperature and molecular density

The performance of the Raman scattering technique for the remote monitoring of temperature and molecular number density in various wind tunnel and engine testing facilities has been experimentally evaluated. Temperature measurements were made by monitoring the pure rotational spectrum of nitrogen and the rotational branch separations of nu2 of CF4 for temperatures in the range 300 to 1000 K. These measurements yielded an average error of 2.6 and 7.6%, respectively, for temperature measurements at pressures near 1 atm. Molecular number density measurements with 20% error could be made at densities as low as 3.5 times 10 to the 22-nd power per cu m by monitoring the 6 to 8 rotational transition of nitrogen, 3.5 times 10 to the 23-rd power per cu m by monitoring the Q-branch of the fundamental vibrational transition of nitrogen, and 7 times 10 to the 22-nd power per cu m by monitoring the nu1 fundamental vibrational transition of CF4.

Bandy, A. R.↗

Nonequilibrium vibrational population measurements in an expanding flow using spontaneous Raman scattering

Vibrational relaxation of nitrogen in a 2D nozzle flow is studied using spontaneous Raman scattering. An electric arc driven shock tube operating as a reflected shock tunnel produces stagnation conditions of 5600 K and 100 atm. A 248 nm KrF laser pulse is focused into the nozzle to produce spatially resolved spontaneous Raman spectra. Vibrational population distributions are derived from the spectra for the states v = 0 to v = 8. The experimental results are compared with two theoretical models: the Landau-Teller relaxation model and a numerical solution of the master equations using transition rates derived from SSH theory. The Landau-Teller correction factor has been measured at 1.0 - 1.5.

Sharma, Surendra P.↗

Spatio-Spectral Characterization of Multipolar Plasmonic Modes of Au Nanorods via Tip-Enhanced Raman Scattering

Tip-enhanced Raman (TER) spectral images of 4-thiobenzonitrile-coated Au nanorods map the spatial profiles and trace the resonances of dipolar and multipolar plasmonic modes that are characteristic of the imaged particles. For any particular rod, we observe sequential transitions between high-order modes at low frequency shifts and lower-order modes at higher frequencies. We also notice that higher-order modes (up to $m$ = 4) are generally observed for long rods as compared to their shorter analogues, where longitudinal dipolar resonances ($m$ = 1) are observable. In effect, this research adds a new dimension to local optical field mapping via TERS, which we have previously explored. Not only can the magnitudes, vector components, local/nonlocal characters of local optical fields be imaged through molecular TERS, but spatially varying local optical resonances are also direct observables.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Evaluation of turbulence induced noise in coherent anti-Stokes Raman scattering

The effect of turbulence in a transonic wind tunnel on coherent anti-Stokes Raman scattering is considered. The driving pump and Stokes waves are taken to be coaxially propagating Gaussian beam waves which are focused on the Raman active medium through the turbulent boundary layer of the flow tube. The random index of refraction variations in the layer are modeled as phase perturbations of the driving waves which cause a reduction of the mean on-axis field and an increase in the mean diameter of the beams. Effective Gaussian beam parameters are developed and the radiated anti-Stokes power calculated as a function of the phase screen parameters. A significant reduction in signal strength occurs for realistic estimates of the phase screen parameter appropriate to a confined transonic flow. A method for estimating the signal degradation which could be applied to other experimental situations is presented.

Elliott, R. A.↗

Attosecond impulsive stimulated X-ray Raman scattering in liquid water

We report the measurement of impulsive stimulated x-ray Raman scattering in neutral liquid water. An attosecond pulse drives the excitations of an electronic wavepacket in water molecules. The process comprises two steps: a transition to core-excited states near the oxygen atoms accompanied by transition to valence-excited states. Thus, the wavepacket is impulsively created at a specific atomic site within a few hundred attoseconds through a nonlinear interaction between the water and the x-ray pulse. We observe this nonlinear signature in an intensity-dependent Stokes Raman sideband at 526 eV. Our measurements are supported by our state-of-the-art calculations based on the polarization response of water dimers in bulk solvation and propagation of attosecond x-ray pulses at liquid density.

Science & Technology - Other Topics↗

Raman scattering applied to gas mixing in the successive channel flow of two gases

The Raman scattering technique has been applied to investigate the effects of fluid undercutting in a simulation of the fluid-piston concept for wind-tunnel design. Measurements of the structure of the driver-driven gas interface and of the effect of undercutting on test duration were performed. Tests were conducted over a Froude number range of 0.0021 to 0.526 at driver-to-driven gas density ratios of 1.103 and 1.573. The effects of inlet design, test-channel inclination angle, and pretest pressurization were also examined. The results are compared with shadowgraph and pressure measurements to illustrate the characteristics of the Raman technique and to explain the discrepancy between the shadowgraph and pressure results.

Hillard, M. E., Jr.↗

Broadband coherent anti-Stokes Raman scattering (BCARS) microscopy for rapid, label-free biological imaging

Broadband coherent anti-Stokes Raman scattering (BCARS) microscopy is a label-free imaging approach that provides detailed chemical information at high spatial resolution in a sample through nonlinear, coherent excitation of molecular vibrations and detection of Raman spectra. While its utility for biological imaging has been demonstrated, many aspects of this technique must mature before it can be widely adopted. One of the areas of required improvement is imaging speed—most BCARS implementations involve sample rastering, which limits imaging speed. Beam scanning can provide faster BCARS imaging but presents some unique challenges. Here, we describe a beam-scanning BCARS microscopy system that improves spatial resolution twofold and imaging speed by fivefold over a previous beam-scanning implementation. These enhancements were enabled by an improvement in supercontinuum power and the use of a sCMOS camera for its high data transfer rate and low read noise. Implementation of the sCMOS camera required correction for the significant pixel-to-pixel background and photon response nonuniformity. Here, we report on the method that we implemented for calibrating and correcting the pixel-to-pixel differences in sCMOS camera noise.

Dixon, Jessica Z. [Georgia Institute of Technology↗

Direct evidence of the effect of a moderate external magnetic field on stimulated Raman scattering in the kinetic regime

We present results from an experiment carried out at the OMEGA-EP laser facility that investigated the effect of a perpendicular magnetic field on stimulated Raman scattering (SRS) and report the first direct measurement of magnetic mitigation of SRS. A 13-T magnetic field generated by pulsed-power coils was imposed on a gas jet plasma, and a novel three-picket interaction beam was used to explore SRS reflectivity for several plasma conditions within single shots. The time-resolved backscattered light shows that SRS was mitigated by the external 13-T magnetic field in the kinetic regime (kλ D ∼ 0.3, where k is the electron plasma wave's wavenumber and λ D is electron Debye length) and at a density of n e /n cr ∼ 0.10. On the other hand, we also measured an enhancement of SRS reflectivity at lower density (n e /n cr < 0.08). We discuss experimental results in the context of magnetohydrodynamic and particle-in-cell simulations that scan SRS dynamics for a variety of plasma conditions. While the experimental evidence of SRS mitigation validates prior work on the kinetic simulation of SRS in an external magnetic field, we also find that other mechanisms such as SRS rescatter can lead to an enhancement of measured SRS reflectivity in simulations of parameters relevant to our experiment.

Gas jet↗

First Results from the OMI Rotational Raman Scattering Cloud Pressure Algorithm

We have developed an algorithm to retrieve scattering cloud pressures and other cloud properties with the Aura Ozone Monitoring Instrument (OMI). The scattering cloud pressure is retrieved using the effects of rotational Raman scattering (RRS). It is defined as the pressure of a Lambertian surface that would produce the observed amount of RRS consistent with the derived reflectivity of that surface. The independent pixel approximation is used in conjunction with the Lambertian-equivalent reflectivity model to provide an effective radiative cloud fraction and scattering pressure in the presence of broken or thin cloud. The derived cloud pressures will enable accurate retrievals of trace gas mixing ratios, including ozone, in the troposphere within and above clouds. We describe details of the algorithm that will be used for the first release of these products. We compare our scattering cloud pressures with cloud-top pressures and other cloud properties from the Aqua Moderate-Resolution Imaging Spectroradiometer (MODIS) instrument. OMI and MODIS are part of the so-called A-train satellites flying in formation within 30 min of each other. Differences between OMI and MODIS are expected because the MODIS observations in the thermal infrared are more sensitive to the cloud top whereas the backscattered photons in the ultraviolet can penetrate deeper into clouds. Radiative transfer calculations are consistent with the observed differences. The OMI cloud pressures are shown to be correlated with the cirrus reflectance. This relationship indicates that OMI can probe through thin or moderately thick cirrus to lower lying water clouds.

Joiner, Joanna↗

Single pulse vibrational Raman scattering by a broadband KrF excimer laser in a hydrogen-air flame

Spontaneous vibrational Raman scattering (VRS) is produced by a broadband excimer laser at 248 nm (KrF) in a H2-air flame, and VRS spectra are recorded for lean, stoichiometric, and rich flames. Except at very lean flame conditions, laser-induced fluorescence (LIF) processes interfere with VRS Stokes lines from H2, H2O, and O2. No interference is found for the N2 Stokes and N2 anti-Stokes lines. In a stoichiometric H2/air flame, single-pulse measurements of N2 concentration and temperature (by the VRS Stokes to anti-Stokes ratio) have a relative standard deviation of 7.7 and 10 percent, respectively. These single pulse measurement errors compare well with photon statistics calculations using measured Raman cross sections.

Pitz, Robert W.↗

Longitudinal Single‐Cell Imaging of Engineered Strains with Stimulated Raman Scattering to Characterize Heterogeneity in Fatty Acid Production

Abstract Understanding metabolic heterogeneity is critical for optimizing microbial production of valuable chemicals, but requires tools that can quantify metabolites at the single‐cell level over time. Here, longitudinal hyperspectral stimulated Raman scattering (SRS) chemical imaging is developed to directly visualize free fatty acids in engineered Escherichia coli over many cell cycles. Compositional analysis is also developed to estimate the chain length and unsaturation of the fatty acids in living cells. This method reveals substantial heterogeneity in fatty acid production among and within colonies that emerges over the course of many generations. Interestingly, the strains display distinct types of production heterogeneity in an enzyme‐dependent manner. By pairing time‐lapse and SRS imaging, the relationship between growth and production at the single‐cell level are examined. The results demonstrate that cell‐to‐cell production heterogeneity is pervasive and provides a means to link single‐cell and population‐level production.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Spatially Resolved Mapping of Three-Dimensional Molecular Orientations with ~2 nm Spatial Resolution through Tip-Enhanced Raman Scattering

We record local optical field images of silver nanocubes (75 nm) using tip-enhanced Raman (TER) spectral imaging. The images that we observe are consistent with several recent reports from our group, but here, we demonstrate sub-2 nm spatial resolution in local optical field nanoimaging under ambient laboratory conditions. This is achieved by scanning the substrate (nanocube on Si) relative to a 4-thiobenzonitrile (TBN)-functionalized Ag-coated TER probe. The spatial resolution that we obtain necessitates that only a few molecules govern the recorded optical response; molecular orientation becomes an important consideration in such measurements. We model the orientation through geometry optimization of a TBN molecule chemisorbed onto an Ag79 cluster (sphere with a ~1 nm diameter). Using the computed orientation of the cluster-bound molecule, we then model the optical response using formalism that accounts for the orientation of the molecule relative to vector components of the local optical fields. We find optimal agreement between experiment and theory. In effect, this work reveals the parallels between single-molecule Raman scattering and high-spatial-resolution TER spectroscopy, even when the images themselves cannot be used to visualize a single molecule in real space.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Time-domain modelling and thermometry of the CH 4 v 1 Q-branch using hybrid femtosecond/picosecond coherent anti-Stokes Raman scattering

Here, we present time-domain measurements and modelling of the CH 4 v 1 vibrational Q-branch, as well as simultaneous temperature acquisition from the CH 4 and N 2 vibrational Q-branches using broadband hybrid femtosecond/picosecond coherent anti-Stokes Raman scattering (fs/ps CARS). Accurate measurements with fs/ps CARS require knowledge of the time-domain response of the probed molecule at different temperatures and pressures. In this work, a fs/ps CARS model was developed for theCH 4 v 1 Q-branch and validated using time-resolved probe delay scans at pressures between 70 and 600 Torr and temperatures between 295 and 1000 K. A simplified modified exponential energy gap model was used to determine the linewidths of the Raman transitions within the Q-branch. Total Q-branch linewidths for the entire explored parameter space were also determined from the probe delay scans. This enabled quantitative measurements of CH 4 with fs/ps CARS as well as the temperature through the hot bands of the CH 4 v 1 Q-branch. With a broadband fs laser pulse in a two-beam phase matching scheme, the N 2 Q-branch and CH 4 v 1 Q-branch were simultaneously measured in a heated cell, and the temperatures from each molecule's spectra was evaluated. Here, the fitted temperatures corresponded well with differences ranging from 4 to 17%. It was also shown that exchanging 90% of CH 4 for N 2 or Ar at 295 K and 500 Torr did not significantly impact the normalized time-domain signal prior to a 100 picosecond probe delay. Spatially resolved one-dimensional (1-D) thermometry using the CH 4 Q-branch was also demonstrated with an imaged spatial resolution of 40 µm. With the developed model, 1-D quantitative measurements of CH 4 concentration and temperature can be measured with time resolution of tens of picoseconds.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Using Raman scattering to study reacting gas flow over a catalyst

l present a series of computational methods for analyzing and correcting Raman scattering from a reacting gas flow. My work focused on the laser diagnostic measurements of formaldehyde production over a silver catalyst, specifically the Raman spectroscopy component. This technique offers a non-intrusive, in situ way to measure the coupling between the gas phase and surface activity of a catalytic reaction at relevant industrial conditions. This report outlines the steps followed for correcting the non-idealities in the data due to both the detection optics and scattering mechanics. By implementing such refinement steps, l can generate an accurate 2D spatial map of the temperature profile, number densities for major species, and relative consumption of reactants throughout the reactor cell.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Stimulated Raman scattering mechanisms and scaling behavior in planar direct-drive experiments at the National Ignition Facility

Stimulated Raman scattering (SRS) has been investigated comprehensively in planar-geometry experiments at the National Ignition Facility at conditions relevant to the corona of inertial con finement fusion (ICF) ignition-scale direct-drive targets. These experiments at measured electron temperatures of 4 to 5 keV, simulated density scale lengths Ln of 400 to 700 um, and laser intensities at the quarter-critical density of up to 1.5 x 10 15 W/cm 2 have determined SRS thresholds and the scaling behavior of SRS for various beam geometries. Several SRS mechanisms, including saturated absolute SRS near the quarter-critical density and additional SRS, including near-backscatter or sidescatter at lower densities, have been identi fied. Correlation of time-dependent SRS at densities ~0.15 to 0.21 of the critical density with hot-electron signatures, as well as the magnitudes of these signatures across different experiments, is observed. Additional modeling work is needed to de nitively identify the density region in which hot electrons are generated, and will guide SRS and hot-electron preheat mitigation strategies for direct-drive-ignition designs.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

Spatially and spectrally resolved multipoint coherent anti-Stokes Raman scattering from N2 and O2 flows

Single-shot spectrally resolved broadband rotational coherent anti-Stokes Raman scattering (CARS) from multiple points along a line intersecting a flow has been observed for N2 and O2. A large-angle phase-matching configuration was used to achieve spatial resolution of 0.1 mm x 0.1 mm x 0.1 mm for each of 20 points in the interaction volume. Single-shot multipoint CARS of N2 at different temperatures and of several species in a coflowing jet was observed.

Snow, J. B.↗