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Electric field enhanced Raman scattering and linear frequency shift of strontium titanate soft mode in random domain orientation and reorientation
Results and techniques for laboratory measurements of Raman scattering cross sections and depolarization ratios of atmospheric gases as a function of the incident photon energy are discussed. Referred to N2, the cross section of H2O changes by a factor of 2 as the incident photon energy is changed by 5%. Less striking results are obtained for SO2, NO and other atmospheric gases. Tentative results are given for spectral features of scattering from polluted air-water interfaces. Raman lidar is assessed as a potentially useful aid in remote sensing of atmospheric and water-borne pollution distributions at least in near-source concentrations.
On December 8 and 9, 1976, the 1024 channel Reticon silicon photodiode array detector in the coude spectrograph of a 2.7 m telescope was used to obtain spectra of Jupiter and the moon. Three separate data sets were obtained, including one of the Jovian equatorial region, one of the Jovian north polar cap, and one of Mare Serenetatis on the moon. A correlation analysis was conducted. The autocorrelation function of the Jovian spectrum was calculated and the autocorrelation function of the lunar spectrum was subtracted from it. The analysis made it possible to detect Raman scattering by H2 in the atmosphere of Jupiter. The pure rotational H2 S(0) and S(1) lines were detected. The ratio of the relative number of Raman scattered photons in the S(0) and S(1) features indicate that the H2 in the Jovian atmosphere is in the equilibrium, rather than the normal state. Therefore some sort of nonradiative process is responsible for transitions between the ortho and para states of H2.
Stimulated Raman scattering (SRS) from binary liquid mixture micrometer-sized droplets irradiated by nanosecond laser pulses exhibits previously unreported features. SRS emission at wavelength shifts corresponding to combination frequencies of the individual component Stokes shifts are observed in droplets but not in bulk mixtures. Furthermore, droplet SRS thresholds are determined by component refractive indices and concentrations, in contrast to bulk thresholds, for which self-focusing likely plays a dominant role.
The main thrust of the program was the study of stimulated Raman processes for application to atmospheric lidar measurements. This has involved the development of tunable lasers, the detailed study of stimulated Raman scattering, and the use of the Raman-shifted light for new measurements of molecular line strengths and line widths. The principal spectral region explored in this work was the visible and near-IR wavelengths between 500 nm and 1.5 microns. Recent alexandrite ring laser experiments are reported. The experiments involved diode injection-locking, Raman shifting, and frequency-doubling. The experiments succeeded in producing tunable light at 577 and 937 nm with line widths in the range 80-160 MHz.
We theoretically investigate quantum-enhanced coherent anti-Stokes Raman scattering (CARS) using squeezed light to amplify vibrational transition rates at low photon flux. Quantum sensing approaches are needed for nondestructive nanometrology such as in bioimaging where reduced photodamage is desired while retaining resolution and sensitivity. We analyze both single-mode squeezing applied to the pump field and two-mode squeezing between the pump and Stokes fields. We also show that the ordering of displacement and squeezing operations—whether displacement precedes squeezing or squeezing precedes displacement—has an impact on the resulting CARS transition amplitudes due to a difference in the photon number and the quantum-enhancement coefficients, with the latter offering a stronger enhancement in the case of two modes squeezing of the pump and Stokes under experimentally accessible conditions. Furthermore, our calculations capture these quantum enhancements through the intrinsic photon-number correlations of squeezed light, eliminating the need for interferometric detection or higher pump powers that are otherwise required to reach comparable sensitivities in classical CARS. Finally, we outline a quantum plasmonic extension of our model in which local field enhancements caused by surface plasmon excitation in metallic nanoparticles can be incorporated via mode-selective field amplification factors, offering a pathway toward combining squeezed-light quantum optics with surface-enhanced nanoscale spectroscopy and imaging.
Here, we explore the Fano resonance in ZrTe 5 , using terahertz Raman scattering measurements. We identified two closely spaced B 2g phonon modes, B 2g I and B 2g II, around 9 meV and 11 meV, respectively. Interestingly, only B 2g I exhibited the Fano resonance, an outcome of quantum interference between discrete phonon modes and continuous electronic excitations. This is consistent with the much stronger electron-phonon coupling of B 2g I mode demonstrated by first-principles calculations. Additionally, temperature-dependent measurements highlight an enhanced Fano asymmetry at elevated temperatures, contributed by the thermal renormalization of the band structure and electron-phonon coupling. This study offers insights into the complex interrelation of electron-phonon coupling, thermal effects, and Fano resonances in topological materials.
Spontaneous vibrational Raman scattering was used to measure temperature in an aviation combustor sector burning jet fuel. The inlet temperature ranged from 670 K (750 F) to 756 K (900 F) and pressures from 13 to 55 bar. With the exception of a discrepancy that we attribute to soot, good agreement was seen between the Raman-derived temperatures and the theoretical temperatures calculated from the inlet conditions. The technique used to obtain the temperature uses the relationship between the N2 anti-Stokes and Stokes signals, within a given Raman spectrum. The test was performed using a NASA-concept fuel injector and Jet-A fuel over a range of fuel/air ratios. This work represents the first such measurements in a high-pressure, research aero-combustor facility.
Raman scattering studies for a series of CVD-grown cubic SiC single-crystal films with film thickness from 600 A to 17 microns are discussed. The results suggest that the crystalline orientations of the Si substrate and the 3C-SiC film are the same. It is found that the Si 522/cm phonon from a Si wafer is enhanced in intensity by a factor of 2-3 due to a CVD overlayer of cubic SiC, and that the 3C-SiC longitudinal optical phonon at the Gamma point from SiC/Si samples is enhanced by a factor of two or three following the removal of the Si substrate. The variation of the Raman spectrum with incident power is investigated, and a method for determining the Raman cross section for 3 C-SiC is proposed.
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.
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.
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.
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.
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.
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.
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.
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.
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.