Determination of gas temperatures from laser Raman scattering
Determination of gas temperature from laser-Raman scattering
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Determination of gas temperature from laser-Raman scattering
The efficiency of coherent anti-Stokes Raman scattering (CARS) is calculated as a function of the input beam sizes of the Stokes and pump laser beams. A Green's function formalism is used to show that maximum efficiency occurs when the confocal parameters of the two input beams are unequal and when the phase mismatch between the anti-Stokes field and the nonlinear polarization is nonzero.
A novel technique for extracting Q-branch Raman signals scattered by a diatomic species from the emission spectrum resulting from the irradiation of combustion products using a broadband excimer laser has been developed. This technique is based on the polarization characteristics of vibrational Raman scattering and can be used for both single-shot Raman extraction and time-averaged data collection. The Q-branch Raman signal has a unique set of polarization characteristics which depend on the direction of the scattering while fluorescence signals are unpolarized. For the present work, a calcite crystal is used to separate the horizonal component of a collected signal from the vertical component. The two components are then sent through a UV spectrometer and imaged onto an intensified CCD camera separately. The vertical component contains both the Raman signal and the interfering fluorescence signal. The horizontal component contains the fluorescence signal and a very weak component of the Raman signal; hence, the Raman scatter can be extracted by taking the difference between the two signals. The separation of the Raman scatter from interfering fluorescence signals is critically important to the interpretation of the Raman for cases in which a broadband ultraviolet (UV) laser is used as an excitation source in a hydrogen-oxygen flame and in all hydrocarbon flames. The present work provides a demonstration of the separation of the Raman scatter from the fluorescence background in real time.
Stimulated Raman scattering in IR active nontotally symmetric vibration of alpha quartz crystal, noting parametric oscillation
Raman scattering is a powerful technique for quantitatively probing high temperature and high speed flows. However, this technique has typically been limited to clean hydrogen flames because of the broadband fluorescence interference which occurs in hydrocarbon flames. Fluorescence can also interfere with the Raman signal in clean hydrogen flames when broadband UV lasers are used as the scattering source. A solution to this problem has been demonstrated. The solution to the fluorescence interference lies in the fact that the vibrational Q-branch Raman signal is highly polarized for 90 deg. signal collection and the fluorescence background is essentially unpolarized. Two basic schemes are available for separating the Raman from the background. One scheme involves using a polarized laser and collecting a signal with both horizontal and vertical laser polarizations separately. The signal with the vertical polarization will contain both the Raman and the fluorescence while the signal with the horizontal polarization will contain only the fluorescence. The second scheme involves polarization discrimination on the collection side of the optical setup. For vertical laser polarization, the scattered Q-branch Raman signal will be vertically polarized; hence the two polarizations can be collected separately and the difference between the two is the Raman signal. This approach has been used for the work found herein and has the advantage of allowing the data to be collected from the same laser shot(s). This makes it possible to collect quantitative Raman data with single shot resolution in conditions where interference cannot otherwise be eliminated.
Much interest in our laboratory has focused on aggregation of organic compounds, particularly cyanine dyes and porphyrins. For this discussion we have applied absorption and Raman scattering spectroscopies to characterize aggregated TSPP (tetrakis-(p-sulfonatophynyl) porphyrin) in aqueous solution. Based on concentration, pH and ionic strength dependence of TSPP absorption, we deduce that aggregation evolves through the formation of TSPP diacid and that the diacid is the repeating unit in the aggregate. The Raman bands of TSPP in strongly acidic solution lead us further to conclude that vibrations of adjacent molecules are perturbed in a fashion that is consistent with the pyrrolic ring in the porphinato macrocycle being ruffled, and that two aggregate arrangements occur: specifically J- and H-type aggregates. Furthermore, aggregation enhancement is advanced as a viable mechanism to explain enhanced Raman Scattering for homogeneous aqueous phase TSPP, where the surface-enhancement mechanism is not applicable.
Using a frequency-doubled Nd-YAG pulsed laser and a single-intensified CCD camera, Rayleigh scattering measurements have been performed to study the cluster formation in a Mach 6 wind tunnel at NASA Langley Research Center. These studies were conducted both in the free stream and in a model flow field for various flow conditions to gain an understanding of the dependence of the Rayleigh scattering (by clusters) on the local pressures and temperatures in the facility. Using the same laser system, simultaneous measurements of the local temperature have also been performed using the rotational Raman scattering of molecular nitrogen and determined the densities of molecular oxygen and nitrogen by using the vibrational Raman scattering from these species. Quantitative results are presented in detail with emphasis on the applicability of the Rayleigh scattering for obtaining quantitative measurements of molecular densities both in the free stream and in the model flow field.
Using a frequency-doubled Nd-YAG pulsed laser and a single-intensified CCD camera, Rayleigh scattering measurements have been performed to study the cluster formation in a Mach 6 wind tunnel at NASA Langley Research Center. These studies were conducted both in the free stream and in a model flow field for various flow conditions to gain an understanding of the dependence of the Rayleigh scattering (by clusters) on the local pressures and temperatures in the facility. Using the same laser system, we have also performed simultaneous measurements of the local temperature using the rotational Raman scattering of molecular nitrogen and determined the densities of molecular oxygen and nitrogen by using the vibrational Raman scattering from these species. Quantitative results will be presented in detail with emphasis on the applicability of the Rayleigh scattering for obtaining quantitative measurements of molecular densities both in the free stream and in the model flow field.
Raman scattering by SO2 in an electrical generating plant stack plume has been observed using an optical radar system. Good qualitative agreement is evident between SO2 backscatter intensity and the plant's electrical power output.
A modification of the standard theory of stimulated Raman scattering (SRS) first proposed by Sparks (1974, 1975) is analyzed and shown to incorporate a possibly important physical effect; however, its original formulation is incorrect. The analysis is based on an exact numerical integration of the coupled equations of the modified theory, the results of which are compared with both the conventional theory of SRS and with one set of experimental data. A reformulation of the modified theory is suggested that leads to a gain which is in somewhat better agreement with the data than is the conventional theory.
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.
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.