Sukesh Roy

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.

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.

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.

Quasi-continuous burst-mode laser for high-speed planar imaging

The pulse-burst duration of a compact burst-mode Nd:YAG laser is extended by one order of magnitude compared to previous flashlamp-pumped designs by incorporating a fiber oscillator and diode-pumped solid-state amplifiers. The laser has a linewidth of <2 GHz at 1064.3 nm with 150 mJ per individual pulse at 10 kHz. The performance of the system is evaluated by using the third-harmonic output at 354.8 nm for high-speed planar laser-induced fluorescence of formaldehyde in a lifted methane-air diffusion flame. A total of 100 and 200 sequential images of unsteady fluid-flame interactions are acquired at repetition rates of 10 kHz and 20 kHz, respectively.

High-speed Intravascular Photoacoustic Imaging of Lipid-laden Atherosclerotic Plaque Enabled by a 2-kHz Barium Nitrite Raman Laser

Lipid deposition inside the arterial wall is a key indicator of plaque vulnerability. An intravascular photoacoustic (IVPA) catheter is considered a promising device for quantifying the amount of lipid inside the arterial wall. Thus far, IVPA systems suffered from slow imaging speed (~50 s per frame) due to the lack of a suitable laser source for high-speed excitation of molecular overtone vibrations. Here, we report an improvement in IVPA imaging speed by two orders of magnitude, to 1.0 s per frame, enabled by a custom-built, 2-kHz master oscillator power amplifier (MOPA)-pumped, barium nitrite [Ba(NO3)2] Raman laser. This advancement narrows the gap in translating the IVPA technology to the clinical setting.

Validation of temperature imaging by H2O absorption spectroscopy using hyperspectral tomography in controlled experiments.

This paper describes a preliminary demonstration and validation of temperature imaging using hyperspectral H2O absorption tomography in controlled experiments. Fifteen wavelengths are monitored on each of 30 laser beams to reconstruct the temperature image in a 381 mm × 381 mm square room-temperature plane that contains a 102 mm × 102 mm square zone of lower or higher temperature. The hyperspectral tomography technique attempts to leverage multispectral information to enhance measurement fidelity. The experimental temperature images exhibit average accuracies of 2.3% or better, with pixel-by-pixel standard deviations of less than 1%. In addition, even when the internal zone is only 4 K cooler than the surroundings, its presence is still detectable; statistical analysis of the associated experimental image reveals a 98% confidence that the internal zone is in fact cooler than the surroundings.