Forward picosecond Stokes-pulse generation in transient stimulated Raman scattering
Transient molecular vibration excitation by picosecond laser pulses found dependent on shape of Stokes pulses in Raman scattering study
Bloembergen, N.↗
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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.↗
Flow Visualization of Density in a Cryogenic Wind Tunnel Using Planar Rayleigh and Raman Scattering
Using a pulsed Nd:YAG laser (532 nm) and a gated, intensified charge-coupled device, planar Rayleigh and Raman scattering techniques have been used to visualize the unseeded Mach 0.2 flow density in a 0.3-meter transonic cryogenic wind tunnel. Detection limits are determined for density measurements by using both unseeded Rayleigh and Raman (N2 vibrational) methods. Seeding with CO2 improved the Rayleigh flow visualization at temperatures below 150 K. The seeded Rayleigh version was used to demonstrate the observation of transient flow features in a separated boundary layer region, which was excited with an oscillatory jet. Finally, a significant degradation of the laser light sheet, in this cryogenic facility, is discussed.
Herring, Gregory C.↗
Raman scattering from phonons and magnons in magnetic semiconductors, MnTe
Comparisons are made between theoretical and experimental data on laser Raman scattering by phonons and two-magnons in antiferromagnetic and paramagnetic phases of MnTe. The study was performed specifically to characterize the magnetic exchange coupling constants of the Mn ions in the samples. Crystal MnTe samples were bombarded with an Ar ion laser beam to obtain spectrometer and photon counter data. One E(2g) phonon with a room temperature energy of 178/cm and a two-magnon peak of 360/cm were observed in the Raman spectrum. A spin wave dispersion relation is presented for the spectrum. Finally, a Monte Carlo technique was used to calculate the two-magnon joint density of states that best fits the experimental data.
Mobasser, S. R.↗
Absolute intensity and polarization of rotational Raman scattering from N2, O2, and CO2
An experimental examination of the absolute intensity, polarization, and relative line intensities of rotational Raman scattering (RRS) from N2, O2, and CO2 is reported. The absolute scattering intensity for N2 is characterized by its differential cross section for backscattering of incident light at 647.1 nm, which is calculated from basic measured values. The ratio of the corresponding cross section for O2 to that for N2 is 2.50 plus or minus 5 percent. The intensity recent for N2, O2, and CO2 are shown to compare favorably to values calculated from recent measurements of the depolarization of Rayleigh scattering plus RRS. Measured depolarizations of various RRS lines agree to within a few percent with the theoretical value of 3/4. Detailed error analyses are presented for intensity and depolarization measurements. Finally, extensive RRS spectra at nominal gas temperatures of 23 C, 75 C, and 125 C are presented and shown to compare favorably to theoretical predictions.
Penney, C. M.↗
Dual-Pump Coherent Anti-Stokes Raman Scattering Temperature and CO2 Concentration Measurements
Measurements of temperature and CO2 concentration using dual-pump coherent anti-Stokes Raman scattering, (CARS) are described. The measurements were performed in laboratory flames,in a room-temperature gas cell, and on an engine test stand at the U.S. Air Force Research Laboratory, Wright-Patterson Air Force Base. A modeless dye laser, a single-mode Nd:YAG laser, and an unintensified back-illuminated charge-coupled device digital camera were used for these measurements. The CARS measurements were performed on a single-laser-shot basis. The standard deviations of the temperatures and CO2 mole fractions determined from single-shot dual-pump CARS spectra in steady laminar propane/air flames were approximately 2 and 10% of the mean values of approximately 2000 K and 0.10, respectively. The precision and accuracy of single-shot temperature measurements obtained from the nitrogen part of the dual-pump CARS system were investigated in detail in near-adiabatic hydrogen/air/CO2 flames. The precision of the CARS temperature measurements was found to be comparable to the best results reported in the literature for conventional two-laser, single-pump CARS. The application of dual-pump CARS for single-shot measurements in a swirl-stabilized combustor fueled with JP-8 was also demonstrated.
Lucht, Robert P.↗
Measurement of Off-Body Velocity, Pressure, and Temperature in an Unseeded Supersonic Air Vortex by Stimulated Raman Scattering
A noninvasive optical method is used to make time-averaged (30 sec) off-body measurements in a supersonic airflow. Seeding of tracer particles is not required. One spatial component of velocity, static pressure, and static temperature are measured with stimulated Raman scattering. The three flow parameters are determined simultaneously from a common sample volume (0.3 by 0.3 by 15 mm) using concurrent measurements of the forward and backward scattered line shapes of a N2 vibrational Raman transition. The capability of this technique is illustrated with laboratory and large-scale wind tunnel testing that demonstrate 5-10% measurement uncertainties. Because the spatial resolution of the present work was improved to 1.5 cm (compared to 20 cm in previous work), it was possible to demonstrate a modest one-dimensional profiling of cross-flow velocity, pressure, and translational temperature through the low-density core of a stream-wise vortex (delta-wing model at Mach 2.8 in NASA Langley's Unitary Plan Wind Tunnel).
Herring, Gregory C.↗
Quantitative Analysis of Spectral Interference of Spontaneous Raman Scattering in High-Pressure Fuel-Rich H2-Air Combustion
We present a theoretical study of the spectral interferences in the spontaneous Raman scattering spectra of major combustion products in 30-atm fuel-rich hydrogen-air flames. An effective methodology is introduced to choose an appropriate line-shape model for simulating Raman spectra in high-pressure combustion environments. The Voigt profile with the additive approximation assumption was found to provide a reasonable model of the spectral line shape for the present analysis. The rotational/vibrational Raman spectra of H2, N2, and H2O were calculated using an anharmonic-oscillator model using the latest collisional broadening coefficients. The calculated spectra were validated with data obtained in a 10-atm fuel-rich H2-air flame and showed excellent agreement. Our quantitative spectral analysis for equivalence ratios ranging from 1.5 to 5.0 revealed substantial amounts of spectral cross-talk between the rotational H2 lines and the N2 O-/Q-branch; and between the vibrational H2O(0,3) line and the vibrational H2O spectrum. We also address the temperature dependence of the spectral cross-talk and extend our analysis to include a cross-talk compensation technique that removes the nterference arising from the H2 Raman spectra onto the N2, or H2O spectra.
Kojima, Jun↗
Quantitative Multi-Scalar Raman Scattering Diagnostics in High-Pressure Flames
This poster presentation contains viewgraphs which summarize the design, operation, and resulting data of a Raman scattering diagnostic system for spectroscopy of high pressure flames.
Nguyen, Quang-Viet↗
Raman scattering measurements in flames using a tunable KrF excimer laser
A narrow-band tunable KrF excimer laser is used as a spontaneous vibrational Raman scattering source to demonstrate that single-pulse concentration and temperature measurements, with only minimal fluorescence interference, are possible for all major species (O2, N2, H2O, and H2) at all stoichiometries (fuel-lean to fuel rich) of H2-air flames. Photon-statistics-limited precisions in these instantaneous and spatially resolved single-pulse measurements are typically 5 percent, which are based on the relative standard deviations of single-pulse probability distributions. In addition to the single-pulse N2 Stokes/anti-Stokes ratio temperature measurement technique, a time-averaged temperature measurement technique is presented that matches the N2 Stokes Raman spectrum to theoretical spectra by using a single intermediate state frequency to account for near-resonance enhancement. Raman flame spectra in CH4-air flames are presented that have good signal-to-noise characteristics and show promise for single-pulse UV Raman measurements in hydrocarbon flames.
Wehrmeyer, Joseph A.↗
Raman scattering characterization of space solar cell structures
A contactless method for the determination of the free-carrier density and the composition distribution across the thickness of 3-5 multi-layer solar cell structures, using the Raman scattering method, is developed. The method includes a step analysis of Raman spectra from optical phonons and phonon-plasmon modes of different layers. The method provides simultaneous measurements of the element composition and the thickness of the structure's layers together with the free-carrier density. The results of measurements of the free-carrier density composition distributions of the liquid phase epitaxy grown AlGaAs/GaAs and GaSb solar cell structures are presented and discussed.
Mintairov, Alexander M.↗
Enhanced Raman scattering from cesium suboxides on silver particles and the structure of S-1 photocathodes
An explanation is given for the results of recent enhanced Raman scattering studies of photomultiplier tubes with S-1 photocathode surfaces which indicated the presence of Cs11O3 but not Cs2O. The reason for the discrepancy between the currently accepted model of the S-1 and this recent result is discussed.
Bates, C. W., Jr.↗
Stimulated Raman scattering seeded by a fibre continuum
A broadband continuum generated in a germanosilicate optical fiber has been used as a coherent seed to initiate stimulated Raman scattering in gases. The technique used is described. The results show a fivefold increase in conversion efficiency and a similar reduction in the requisite pump power.
Selker, M. D.↗
Imaging Hydrogen Leaks With Raman Scattering
Proposed spectral imaging system used to detect leaking hydrogen from distance of 100 ft or more. Video cameras form images of leaking hydrogen by use of Raman scattering of laser beam from hydrogen. By indicating potentially explosive concentrations of hydrogen in air, system contributes to safety at facilities producing and handling hydrogen, such as fueling stations for hydrogen-burning automobiles of near future.
Mcdermid, Iain S.↗
Surface-Enhanced Raman Scattering Using Silica Whispering-Gallery Mode Resonators
The motivation of this work was to have robust spectroscopic sensors for sensitive detection and chemical analysis of organic and molecular compounds. The solution is to use silica sphere optical resonators to provide surface-enhanced spectroscopic signal. Whispering-gallery mode (WGM) resonators made from silica microspheres were used for surface-enhanced Raman scattering (SERS) without coupling to a plasmonic mechanism. Large Raman signal enhancement is observed by exclusively using 5.08-micron silica spheres with 785-nm laser excitation. The advantage of this non-plasmonic approach is that the active substrate is chemically inert silica, thermally stable, and relatively simple to fabricate. The Raman signal enhancement is broadly applicable to a wide range of molecular functional groups including aliphatic hydrocarbons, siloxanes, and esters. Applications include trace organic analysis, particularly for in situ planetary instruments that require robust sensors with consistent response.
Anderson, Mark S.↗
Three-beam hybrid fs/ps coherent anti-Stokes Raman scattering of rotation–vibration non-equilibrium
In this work, we demonstrate time-resolved rotational and vibrational temperature measurements to probe plasma non-equilibrium through a simple three-beam hybrid femtosecond/picosecond coherent anti-Stokes Raman scattering (fs/ps CARS) system. A single pump/Stokes pair is employed to generate both the pure-rotational and ro-vibrational Raman coherence. A novel phase-matching scheme, to our knowledge, is employed to spatially overlap the two CARS signals, simplifying the optical design and allowing signal selection by tuning a single spectrometer grating. Measurements were performed near the electrodes in a N 2 DC glow discharge. Both the rotational temperature and the vibrational populations up to $v$ = 8 were calculated from the separately measured single-shot pure-rotational and ro-vibrational CARS spectra. Strong rotation–vibration non-equilibrium was observed at both electrodes, with the cathode showing higher vibrational and rotational temperatures. In addition, non-Boltzmann behaviors were observed at both electrodes. This simplified approach enables measurements of rotational and vibrational temperatures with high spatial resolution in non-equilibrium flows.
42 ENGINEERING↗
Observations of stimulated Raman scattering and laser-induced breakdown in millimeter-sized droplets
We report the first observations, to our knowledge, of nonlinear optical effects in large (millimeter-sized) droplets. Stimulated Raman scattering (SRS) and laser-induced breakdown (LIB) are simultaneously observed in acoustically levitated millimeter-sized glycerol droplets irradiated by either a frequency-doubled (532-nm) or a frequency-tripled (355-nm) Nd:YAG laser. The two processes, which occur above a nearby coincident irradiation threshold, are conjectured to arise from a common initiation mechanism: self-focusing. LIB generates vapor bubbles within the droplet, resulting in the quenching of SRS emission.
Biswas, A.↗
Label-free nanoscopy of cell metabolism by ultrasensitive reweighted visible stimulated Raman scattering
Nanoscopic imaging of cell metabolism is hindered by the incompatibility of small metabolites with fluorescent dyes and the limited resolution of imaging mass spectrometry. We present ultrasensitive reweighted visible stimulated Raman scattering (URV-SRS), a label-free vibrational nanoscopy technique that enables multiplexed detection of metabolic nanostructures within cells. We developed an extensively chirped spectral focusing visible SRS microscope that achieves a detection limit of 4,000 molecules and introduced a self-supervised learning-based denoiser to robustly suppress non-independent SRS noise by over 7.2 dB. The instrumentation-based signal enhancement and computation-based noise suppression synergistically improved the detection sensitivity by 50 times over near-infrared SRS. Leveraging this enhanced sensitivity, we further pushed the resolution to nanoscopic levels by introducing Fourier reweighting to amplify sub-100 nm spatial frequencies previously overwhelmed by noise. Validated by Fourier ring correlation, URV-SRS achieves a lateral resolution of 86 nm in cellular imaging. Here, we applied URV-SRS to elucidate the reprogramming of metabolic nanostructures associated with virus replication in Vero E6 host cells and to compositionally delineate subcellular fatty acid synthesis in engineered Escherichia coli, demonstrating its capability towards nanoscopic spatial metabolomics.
59 BASIC BIOLOGICAL SCIENCES↗