Coherent anti-Stoke Raman scattering thermometry in very-high-temperature systems.
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A nonintrusive diagnostic system is described which permits simultaneous measurement of temperature, nitrogen number density, and oxygen number density in hostile combustion environments. This system is pumped by a 10-Hz neodymium YAG laser, and signals are detected with an intensified photodiode array and dual photomultipliers. The system utilizes a folded BOXCARS beam arrangement, two probe dye lasers, dynamic range expansion, polarization rejection of nonresonant background, and multiplexing of the signal beams.
A system is provided. The system has a femtosecond oscillator to generate pulses used for pump and probe beams. A photonic crystal fiber is disposed in a path of the probe beam and produces pulses for a chirped probe beam. A high NA objective receives the pump and the chirped probe beam, redirects the received beams through a dielectric substrate towards an interface between a sample and the dielectric substrate to cause total internal reflection (TIR) at the sample-substrate interface, and produces corresponding evanescent waves in a portion of the sample adjacent to the sample-substrate interface, and collects a backward-propagating beam of pulses of responsive light. The portion of the sample illuminated by the evanescent waves emits responsive light. The dielectric substrate is transparent to the responsive light, the pump and the chirped probe beam. An image is produced having a specific image size using the received backward-propagating beam.
Impulsive stimulated Raman scattering (ISRS) using a single short femtosecond pump pulse to excite molecular vibrations offers an elegant pump-probe approach to perform vibrational imaging below 200 cm –1 . One shortcoming of ISRS is its inability to offer vibrational selectivity as all the vibrational bonds whose frequencies lie within the short pump-pulse bandwidth are excited. To date, several coherent control techniques have been explored to address this issue and selectively excite a specific molecular vibration by shaping the pump pulse. There has not been any systematic work that reports an analogous shaping of the probe pulse to implement preferential detection. In this work, we focus on vibrational imaging and report vibrational selective detection by shaping the probe pulse in time. Here, we demonstrate numerically and experimentally two pulse-shaping strategies with one functioning as a vibrational notch filter and the other functioning as a vibrational low-pass filter. This enables fast (25 μs/pixel) and selective hyperspectral imaging in the low-frequency regime (< 200 cm –1 ).
Plasma dynamics and chemistry have a broad range of timescales from picoseconds to milliseconds. In addition, it involves nonequilibrium energy transfer between electrons, ions, electronically and vibrationally excited states, radicals, intermediate species, and reactants and products as well as surface charges and chemistry. To understand plasma physics and chemistry, it is essential to conduct time and space resolved, quantitative detection of nonequilibrium temperature distributions, electron energy and number density, electric field, and species concentrations. There are enormous publications and review articles on this subject. The focus of this chapter is to be placed on the most recent progress in gas phase plasma properties and chemistry, especially on optical emission spectroscopy, laser absorption spectroscopy, Faraday rotational spectroscopy, Raman and Thompson scattering, femtosecond and picosecond (fs/ps) coherent anti-Stokes Raman scattering (CARS) spectroscopy, and electric field-induced second harmonic generation methods.
A method of examining a sample comprises exposing the sample to a pump pulse of electromagnetic radiation for a first period of time, exposing the sample to a stimulant pulse of electromagnetic radiation for a second period of time which overlaps in time with at least a portion of the first exposing, to produce a signal pulse of electromagnetic radiation for a third period of time, and interfering the signal pulse with a reference pulse of electromagnetic radiation, to determine which portions of the signal pulse were produced during the exposing of the sample to the stimulant pulse. The first and third periods of time are each greater than the second period of time.
The paper presents velocity measurements of shock-induced flow field, leading to vortex generation and plasma deformation in air. Femtosecond-laser electronic excitation tagging (FLEET) velocimetry was performed at the times Δt = 3, 20, 50, and 100 µs post laser-induced breakdown. Emissions over Δt = 3–10 µs showed the propagations of the initially elliptic shock, transitioning into a spherical front. The shock emanated along the laser axis causes the flow outward, and then the pressure gradient generated by the rarefaction wave drives the inward flow at later moments, with the velocity magnitude approaching a steady-state value of 40 m s -1 . Temporal velocity evolution was compared with non-self-similar solutions behind the propagating shock, which are sensitive to the size of the energy deposition, and the use of the measured initial plasma diameter reproduced the experiment. There establishes a region of uniform velocity around 35 m s -1 in the air-flow running through the plasma, which triggers the roll-up of the plasma surface by a large-scale vortex, providing the detail of flow field evolution from the shock propagation to the plasma deformation. A collective Thomson scattering and hybrid fs/ps pure rotational coherent anti-Stokes Raman scattering (CARS) were also performed to gain insight into the high-temperature plasma. An effective electron–ion recombination rate of 2 x 10 -12 cm 3 s -1 was measured at Δt = 0.5–10 µs, during a dynamic plasma expansion and compression. When the shock resides close to the plasma at Δt = 0.5–1 µs, the temperature distributions were found to follow the similarity law.
We report pure-rotational N 2 –N 2 , N 2 –air, and O 2 –air S-branch linewidths for temperatures of 80–200 K by measuring the time-dependent decay of rotational Raman coherences in an isentropic free-jet expansion from a sonic nozzle. We recorded pure-rotational hybrid femtosecond/picosecond coherent anti-Stokes Raman scattering (fs/ps CARS) spectra along the axial centerline of the underexpanded jet, within the barrel shock region upstream of the Mach disk. The dephasing of the pure-rotational Raman coherence was monitored using probe-time-delay scans at different axial positions in the jet, corresponding to varying local temperatures and pressures. The local temperature was obtained by fitting CARS spectra acquired at zero probe time delay, where the impact of collisions was minimal. The measured decay of each available Raman transition was fit to a dephasing constant and corrected for the local pressure, which was obtained from the CARS-measured static temperature and thermodynamic relationships for isentropic expansion from the known stagnation state. Nitrogen self-broadened transitions decayed more rapidly than those broadened in air for all temperatures, corresponding to higher Raman linewidths. In general, the measured S-branch linewidths deviated significantly in absolute and relative magnitudes from those predicted by extrapolating the modified exponential gap model to low temperatures. The temperature dependence of the Raman linewidth for each measured rotational state of nitrogen (J ≤ 10) and oxygen (N ≤ 11) was fit to a temperature-dependent power law over the measurable temperature domain (80–200 K) and extrapolated to both higher rotational states and room temperature. Furthermore, the measured and modeled low-temperature linewidth data provided here will aid low temperature gas-phase pressure measurements with fs/ps CARS.
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.
Coherent anti Stokes Raman scattering (CARS) from the pure rotational Raman lines of N2 was employed to measure the instantaneous (10 nsec) rotational temperature of the gas at room temperature and below. An entire rotational CARS spectrum was generated by a single laser pulse using a broad bandwidth dye laser and was recorded on an optical multichannel analyzer. A best fit temperature obtained for individual experimental spectra by comparison with calculated spectra. Good agreement between CARS temperatures and thermocouple temperatures was observed.
This paper reports for the first time the combination of a dual-pump coherent anti-Stokes Raman scattering system with an interferometric Rayleigh scattering system (CARS - IRS) to provide time-resolved simultaneous measurement of multiple properties in combustion flows. The system uses spectrally narrow green (seeded Nd:YAG at 532 nm) and yellow (552.9 nm) pump beams and a spectrally-broad red (607 nm) beam as the Stokes beam. A spectrometer and a planar Fabry-Perot interferometer used in the imaging mode are used to record the spectrally broad CARS spectra and the spontaneous Rayleigh scattering spectra, respectively. Time-resolved simultaneous measurement of temperature, absolute mole fractions of N2, O2, and H2, and two components of velocity in a Hencken burner flame were performed to demonstrate the technique.
A computer calculation of the expected angular distribution of coherent anti-Stokes Raman scattering (CARS) from micrometer size polystyrene spheres based on a Mie-type model, and a pilot experiment to test the feasibility of measuring CARS angular distributions from micrometer size polystyrene spheres by simply suspending them in water are discussed. The computer calculations predict a very interesting structure in the angular distributions that depends strongly on the size and relative refractive index of the spheres.
A technique has been developed which allows the determination of a two-photon absorption cross-section to be made relative to the Raman scattering cross-section in nitrogen. Spatial and temporal effects associated with the lasers are ratioed out to give a result independent of laser parameters. The necessary theory to extract a cross-section from the measured ratio of a Coherent Anti-Stokes Raman Scattering (CARS) signal in N2 to a four-wave mixing signal in NO has been developed. The technique has been demonstrated on the R(22) + S(12) (J-double-prime = 9 1/2) line in NO and a cross-section of (2.9 + or - 1.8) x 10 to the -49th (cm to the 4th power)-s was determined. This technique appears to be applicable to a number of other diatomic molecules.
Coherent anti-Stokes Raman scattering (CARS) has long been the gold standard for non-intrusively measuring gas temperature in reacting flows such as flames and plasmas. Recently, the development of ultrafast hybrid fs/ps CARS has enabled the exploitation of coherence beating between neighboring spectral lines to simultaneously measure rotational and vibrational temperatures from a single pure rotational spectrum. However, the influence of non-Boltzmann vibrational state distributions and limitations due to collisional dephasing at pressures greater than 1 atm remains unclear. In this work, we use spectral simulations to investigate the effects of non-Boltzmann vibrational state distributions and the applicability of coherence beating at pressures up to 10 atm. We show that short probe pulses can be leveraged to quantify non-Boltzmann vibrational state distributions of N2. Furthermore, we demonstrate that fs/ps CARS coherence beating can simultaneously provide sensitive measurements of rotational and vibrational temperatures of both O2 and N2 in air. A sensitivity analysis was conducted to qualitatively explain the accuracy and precision comparisons between probe delays.