James R. Gord

Femtosecond coherent anti-Stokes Raman scattering measurement of gas temperatures from frequency-spread dephasing of the Raman coherence

Gas-phase temperatures and concentrations are measured from the magnitude and decay of the initial Raman coherence in femtosecond coherent anti-Stokes Raman scattering (CARS). A time-delayed probe beam is scattered from the Raman polarization induced by pump and Stokes beams to generate CARS signal; the dephasing rate of this initial coherence is determined by the temperature-sensitive frequency spread of the Raman transitions. Temperature is measured from the CARS signal decrease with increasing probe delay. Concentration is found from the ratio of the CARS and nonresonant background signals. Collision rates do not affect the determination of these quantities.

50-kHz-rate 2D imaging of temperature and H2O concentration at the exhaust plane of a J85 engine using hyperspectral tomography

This paper describes a novel laser diagnostic and its demonstration in a practical aero-propulsion engine (General Electric J85). The diagnostic technique, named hyperspectral tomography (HT), enables simultaneous 2-dimensional (2D) imaging of temperature and water-vapor concentration at 225 spatial grid points with a temporal response up to 50 kHz. To our knowledge, this is the first time that such sensing capabilities have been reported. This paper introduces the principles of the HT techniques, reports its operation and application in a J85 engine, and discusses its perspective for the study of high-speed reactive flows.

Gas-phase single-shot thermometry at 1 kHz using fs-CARS spectroscopy

Single-laser-shot temperature measurements at a data rate of 1 kHz employing femtosecond coherent anti-Stokes Raman scattering (fs-CARS) spectroscopy of N(2) are demonstrated. The measurements are performed using a chirped-probe pulse to map the time-dependent frequency-spread dephasing of the Raman coherence, which is created by approximately 80-fs pump and Stokes beams, into the spectrum of the coherent anti-Stokes Raman scattering signal pulse. Temperature is determined from the spectral shape of the fs-CARS signal for probe delays of approximately 2 ps with respect to the pump-Stokes excitation. The accuracy and precision of the measurements for the 300-2400 K range are found to be approximately 1%-6% and approximately 1.5%-3%, respectively.

Time-resolved dynamics of resonant and nonresonant broadband picosecond coherent anti-Stokes Raman scattering signals

The time-resolved dynamics of resonant and nonresonant broadband picosecond coherent anti-Stokes Raman scattering (CARS) signals in gas-phase media are investigated. For ∼135ps pump and probe beams and ∼106ps Stokes beams, the magnitude of the nonresonant signals are decreased by more than three orders of magnitude when the probe beam is delayed by ∼110ps, whereas the resonant nitrogen CARS signal is reduced only by a factor of 3. Investigation of these time dynamics is important for understanding the optimal time delay for nonresonant background suppression as well as for understanding the collisional and Doppler dependence of the resonant CARS signals.The time-resolved dynamics of resonant and nonresonant broadband picosecond coherent anti-Stokes Raman scattering (CARS) signals in gas-phase media are investigated. For ∼135ps pump and probe beams and ∼106ps Stokes beams, the magnitude of the nonresonant signals are decreased by more than three orders of magnitude when the probe beam is delayed by ∼110ps, whereas the resonant nitrogen CARS signal is reduced only by a factor of 3. Investigation of these time dynamics is important for understanding the optimal time delay for nonresonant background suppression as well as for understanding the collisional and Doppler dependence of the resonant CARS signals.

Hybrid femtosecond/picosecond coherent anti-Stokes Raman scattering for high-speed gas-phase thermometry

We demonstrate hybrid femtosecond/picosecond (fs/ps) coherent anti-Stokes Raman scattering for high-speed thermometry in unsteady high-temperature flames, including successful comparisons with a time- and frequency-resolved theoretical model. After excitation of the N(2) vibrational manifold with 100 fs broadband pump and Stokes beams, the Raman coherence is probed using a frequency-narrowed 2.5 ps probe beam that is time delayed to suppress the nonresonant background by 2 orders of magnitude. Experimental spectra were obtained at 500 Hz in steady and pulsed H(2)-air flames and exhibit a temperature precision of 2.2% and an accuracy of 3.3% up to 2400 K. Strategies for real-time gas-phase thermometry in high-temperature flames are also discussed, along with implications for kilohertz-rate measurements in practical combustion systems.

Theory of femtosecond coherent anti-Stokes Raman scattering spectroscopy of gas-phase transitions

A theoretical analysis of coherent anti-Stokes Raman scattering (CARS) spectroscopy of gas-phase resonances using femtosecond lasers is performed. The time-dependent density matrix equations for the femtosecond CARS process are formulated and manipulated into a form suitable for solution by direct numerical integration (DNI). The temporal shapes of the pump, Stokes, and probe laser pulses are specified as an input to the DNI calculations. It is assumed that the laser pulse shapes are 70 fs Gaussians and that the pulses are Fourier-transform limited. A single excited electronic level is defined as an effective intermediate level in the Raman process, and transition strengths are adjusted to match the experimental Raman polarizability. The excitation of the Raman coherence is investigated for different Q-branch rotational transitions in the fundamental 2330 cm(-1) band of diatomic nitrogen, assuming that the pump and Stokes pulses are temporally overlapped. The excitation process is shown to be virtually identical for transitions ranging from Q2 to Q20. The excitation of the Raman coherences is also very efficient; for laser irradiances of 5x10(17) W/m2, corresponding approximately to a 100 microJ, 70 fs pulse focused to 50 microm, approximately 10% of the population of the ground Raman level is pumped to the excited Raman level during the impulsive pump-Stokes excitation, and the magnitude of the induced Raman coherence reaches 40% of its maximum possible value. The theoretical results are compared with the results of experiments where the femtosecond CARS signal is recorded as a function of probe delay with respect to the impulsive pump-Stokes excitation.

Single-shot gas-phase thermometry using pure-rotational hybrid femtosecond/picosecond coherent anti-Stokes Raman scattering

High-repetition-rate, single-laser-shot measurements are important for the investigation of unsteady flows where temperature and species concentrations can vary significantly. Here, we demonstrate single-shot, pure-rotational, hybrid femtosecond/picosecond coherent anti-Stokes Raman scattering (fs/ps RCARS) thermometry based on a kHz-rate fs laser source. Interferences that can affect nanosecond (ns) and ps CARS, such as nonresonant background and collisional dephasing, are eliminated by selecting an appropriate time delay between the 100-fs pump/Stokes pulses and the pulse-shaped 8.4-ps probe. A time- and frequency-domain theoretical model is introduced to account for rotational-level dependent collisional dephasing and indicates that the optimal probe-pulse time delay is 13.5 ps to 30 ps. This time delay allows for uncorrected best-fit N2-RCARS temperature measurements with ~1% accuracy. Hence, the hybrid fs/ps RCARS approach can be performed with kHz-rate laser sources while avoiding corrections that can be difficult to predict in unsteady flows.

Interaction of a vortex with a flat flame formed between opposing jets of hydrogen and air

Studies on individual vortex-flame interactions constitute important elements for the understanding of the turbulent-flame structure. Vortices having sufficiently high normal velocity can pass through the flame by extinguishing it locally. In several circumstances they deform the flame surface significantly before attaining extinction conditions. The development of curvature on the flame surface, especially in hydrogen flames, could lead to different quenching patterns. An experimental/numerical investigation is performed to explore possible quenching patterns in opposing-jet diffusion flames. A diluted hydrogen-nitrogen mixture is used as the fuel. Vortices are driven toward the flame surface with different velocities from the air side. The changes in the structure of the flame during its interaction with the incoming vortex are recorded by measuring instantaneous OH-concentration field using the laser-induced fluorescence (LIF) technique. A time-dependent CFDC code that incorporates 13 species and 74 reactions is used for the simulation of these vortex-flame interactions. Both the experiments and calculations have identified two types of quenching patterns: namely, point and annular. It is found that when an air-side vortex is forced toward the flame at a relatively high speed, then the flame at the stagnation line quenches, resulting in a well-known point-quenching pattern. On the other hand, when the vortex is forced at a moderate speed, the flame surface deforms significantly, and quenching develops in an annular ring away from the stagnation line, resulting in an unusual annular-quenching pattern. Detailed analyses performed just before the development of annular quenching and 1 ms later suggest that this unusual annular quenching did not result from the strain rate. Based on the understanding gained from previous investigations on curvature effects in coaxial hydrogen jet flames and the findings made in the present study, it is argued that such quenching develops as a result of the combined effect of preferential diffusion and flame curvature.

Ultrahigh-frame-rate OH fluorescence imaging in turbulent flames using a burst-mode optical parametric oscillator

Burst-mode planar laser-induced fluorescence (PLIF) imaging of the OH radical is demonstrated in laminar and turbulent hydrogen-air diffusion flames with pulse repetition rates up to 50 kHz. Nearly 1 mJ/pulse at 313.526 nm is used to probe the OH P(2)(10) rotational transition in the (0,0) band of the A-X system. The UV radiation is generated by a high-speed-tunable, injection-seeded optical parametric oscillator pumped by a frequency-doubled megahertz-rate burst-mode Nd:YAG laser. Preliminary kilohertz-rate wavelength scanning of the temperature-broadened OH transition during PLIF imaging is also presented for the first time (to our knowledge), and possible strategies for spatiotemporally resolved planar OH spectroscopy are discussed.

Applications of Ultrafast Lasers for Optical Measurements in Combusting Flows

Optical measurement techniques are powerful tools for the detailed study of combustion chemistry and physics. Although traditional combustion diagnostics based on continuous-wave and nanosecond-pulsed lasers continue to dominate fundamental combustion studies and applications in reacting flows, revolutionary advances in the science and engineering of ultrafast (picosecond- and femtosecond-pulsed) lasers are driving the enhancement of existing diagnostic techniques and enabling the development of new measurement approaches. The ultrashort pulses afforded by these new laser systems provide unprecedented temporal resolution for studies of chemical kinetics and dynamics, freedom from collisional-quenching effects, and tremendous peak powers for broad spectral coverage and nonlinear signal generation. The high pulse-repetition rates of ultrafast oscillators and amplifiers allow previously unachievable data-acquisition bandwidths for the study of turbulence and combustion instabilities. We review applications of ultrafast lasers for optical measurements in combusting flows and sprays, emphasizing recent achievements and future opportunities.