Publications

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In many fields of study, from coherent Raman microscopy on living cells to time-resolved coherent Raman spectroscopy of gas-phase turbulence and combustion reaction dynamics, the need for the capability to time-resolve fast dynamical and nonrepetitive processes has led to the continued development of high-speed coherent Raman methods and new high-repetition rate laser sources, such as pulse-burst laser systems. However, much less emphasis has been placed on our ability to detect shot to shot coherent Raman spectra at equivalently high scan rates, across the kilohertz to megahertz regime. This is beyond the capability of modern scientific charge coupled device (CCD) cameras, for instance, as would be employed with a Czerny-Turner type spectrograph. As an alternative detection strategy with megahertz spectral detection rate, we demonstrate dispersive Fourier transformation detection of pulsed (~90 ps) coherent Raman signals in the time-domain. Instead of reading the frequency domain signal out using a spectrometer and CCD, the signal is transformed into a time-domain waveform through dispersive Fourier transformation in a long single-mode fiber and read-out with a fast sampling photodiode and oscilloscope. Molecular O- and S-branch rotational sideband spectra from both N2 and H2 were acquired employing this scheme, and the waveform is fitted to show highly quantitative agreement with a molecular model. The total detection time for the rotational spectrum was 20 ns, indicating an upper limit to the detection frequency of ~50 MHz, significantly faster than any other reported spectrally-resolved coherent anti-Stokes Raman detection strategy to date.

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Coherent anti-Stokes Raman spectroscopy (CARS) is a sensitive technique for probing highly luminous flames in combustion applications to determine temperatures and species concentrations. CARS thermometry has been demonstrated for the vibrational Q-branch and pure-rotational S-branch of several small molecules. Practical advantages of pure-rotational CARS, such as multi-species detection, reduction of coherent line mixing and collisional narrowing even at high pressures, and the potential for more precise thermometry, have motivated experimental and theoretical advances in S-branch CARS of nitrogen (N2), for example, which is a dominant species in air-fed combustion processes. Although hydrogen (H2) is of interest given its prevalence as a reactant and product in many gas-phase reactions, laser bandwidth limitations have precluded the extension of CARS thermometry to the H2 S-branch. We demonstrate H2 thermometry using hybrid femtosecond/picosecond pure-rotational CARS, in which a broadband pump/Stokes pulse enables simultaneous excitation of the set of H2 S-branch transitions populated at flame temperatures over the spectral region of 0-2200 cm-1. We present a pure-rotational H2 CARS spectral model for data fitting and compare extracted temperatures to those from simultaneously collected N2 spectra in two systems of study: a heated flow and a diffusion flame on a Wolfhard-Parker slot burner. From 300 to 650 K in the heated flow, the H2 and N2 CARS extracted temperatures are, on average, within 2% of the set temperature. For flame measurements, the fitted H2 and N2 temperatures are, on average, within 5% of each other from 300 to 1600 K. Our results confirm the viability of pure-rotational H2 CARS thermometry for probing combustion reactions.

Ultrabroadband coherent anti-Stokes Raman spectroscopy (CARS) was employed for one-dimensional imaging of temperature and major species distributions simultaneously in the near-wall region of a CH4/air flame supported on a side-wall-quenching burner. Automatic temporal and spatial overlap of the approximetaly 7 fs pump and Stokes pulses was achieved through a two-beam CARS phase-matching scheme and the crossed approximately 75 ps probe beam provides excellent spatial sectioning of the probed location. Concurrent detection of N2 O2 H2 CO CO2 and CH4 was performed. A CH4/air premixed flame at lean stoichiometric and rich conditions and Reynolds number = 5000 was probed as it quenches against a cooled steel side-wall parallel to the flow providing a persistent flame-wall interaction. An imaging resolution of better than 40 μm was achieved across the field-of-view allowing thermochemical states of the thermal boundary layer to be resolved to within approximately 30 μm of the interface.

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In this LDRD project, we developed a capability for quantitative high - speed imaging measurements of high - pressure fuel injection dynamics to advance understanding of turbulent mixing in transcritical flows, ignition, and flame stabilization mechanisms, and to provide e ssential validation data for developing predictive tools for engine combustion simulations. Advanced, fuel - efficient engine technologies rely on fuel injection into a high - pressure, high - temperature environment for mixture preparation and com bustion. Howe ver, the dynamics of fuel injection are not well understood and pose significant experimental and modeling challenges. To address the need for quantitative high - speed measurements, we developed a Nd:YAG laser that provides a 5ms burst of pulses at 100 kHz o n a robust mobile platform . Using this laser, we demonstrated s patially and temporally resolved Rayleigh scattering imaging and particle image velocimetry measurements of turbulent mixing in high - pressure gas - phase flows and vaporizing sprays . Quantitativ e interpretation of high - pressure measurements was advanced by reducing and correcting interferences and imaging artifacts.

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Hybrid femtosecond/picosecond rotational coherent anti-Stokes Raman spectroscopy (CARS) is developed utilizing a two-beam phase-matching approach for one-dimensional (1D) measurements demonstrated in an impinging jet burner to probe time-resolved head on quenching (HOQ) of a methane/air premixed flame at Φ = 1.0 and Reynolds number = 5000. Single-laser-shot 1D temperature profiles are obtained over a distance of at least 4 mm by fitting the pure-rotational N2 CARS spectra to a spectral library calculated from a time-domain CARS code. An imaging resolution of ∼61 μm is obtained in the 1D-CARS measurements. The acquisition of single-shot 1D CARS measurements, as opposed to traditional point-wise CARS techniques, enables new spatially correlated conditional statistics to be determined, such as the position, magnitude, and fluctuations of the instantaneous temperature gradient. The temperature gradient increases as the flame approaches the metal surface, and decreases during quenching. The standard deviation of the temperature gradient follows the same trend as the temperature gradient, increasing as the flame front approaches the surface, and decreasing after quenching.

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A novel fast method to update the object texture of the triangular mesh hologram is proposed. The angular spectrum of the three-dimensional object represented in triangular meshes is calculated with various pre-defined spectrum shifts. These shifted angular spectrums are added with appropriate coefficients to synthesize the hologram with arbitrary texture on the three-dimensional object in an enhanced speed. © 2013 Optical Society of America.

We report a passively Q-switched all-fiber laser using a large mode area (LMA) Yb3+-doped fiber cladding-pumped at 915 nm and an unpumped single-mode Yb3+-doped fiber as the saturable absorber (SA). The saturable absorber and gain fibers were first coupled with a free-space telescope to better study the composite system, and then fusion spliced with fiber tapers to match the mode field diameters. ASE generated in the LMA gain fiber preferentially bleaches the SA fiber before depleting the gain, thereby causing the SA fiber to act as a passive saturable absorber. Using this scheme we first demonstrate a Q-switched oscillator with 40 μJ 79 ns pulses at 1026 nm using a free-space taper, and show that pulses can be generated from 1020 nm to 1040 nm. We scale the pulse energy to 0.40 mJ using an Yb3+-doped cladding pumped fiber amplifier. Experimental studies in which the saturable absorber length, pump times, and wavelengths are independently varied reveal the impact of these parameters on laser performance. Finally, we demonstrate 60 μJ 81 ns pulses at 1030 nm in an all fiber architecture using tapered mode field adaptors to match the mode filed diameters of the gain and SA fibers. © 2013 Copyright SPIE.

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Time-resolved picosecond pure-rotational coherent anti-Stokes Raman spectroscopy is demonstrated for thermometry and species concentration determination in flames. Time-delaying the probe pulse enables successful suppression of unwanted signals. A theoretical model is under development. ©2010 Optical Society of America.

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Two-photon laser-induced fluorescence (TP-LIF) line imaging of atomic hydrogen was investigated in a series of premixed CH4/O 2/N2, H2/O2, and H 2/O2/N2 flames using excitation with either picosecond or nanosecond pulsed lasers operating at 205 nm. Radial TP-LIF profiles were measured for a range of pulse fluences to determine the maximum interference-free signal levels and the corresponding picosecond and nanosecond laser fluences in each of 12 flames. For an interference-free measurement, the shape of the TP-LIF profile is independent of laser fluence. For larger fluences, distortions in the profile are attributed to photodissociation of H2O, CH3, and/or other combustion intermediates, and stimulated emission. In comparison with the nanosecond laser, excitation with the picosecond laser can effectively reduce the photolytic interference and produces approximately an order of magnitude larger interference-free signal in CH4/O2/N2 flames with equivalence ratios in the range of 0.5 ≤ Φ ≤ 1.4, and in H2/O2 flames with 0.3 ≤ Φ ≤ 1.2. Although photolytic interference limits the nanosecond laser fluence in all flames, stimulated emission, occurring between the laser-excited level, H(n = 3), and H(n = 2), is the limiting factor for picosecond excitation in the flames with the highest H atom concentration. Nanosecond excitation is advantageous in the richest (Φ = 1.64) CH 4/O2/N2 flame and in H2/O 2/N2 flames. The optimal excitation pulse width for interference-free H atom detection depends on the relative concentrations of hydrogen atoms and photolytic precursors, the flame temperature, and the laser path length within the flame. © 2008 Optical Society of America.

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We report improved measurements of the temperature-dependent cross sections for the quenching of fluorescence from the A +2 (v′ =0) state of NO. Cross sections were measured for gas temperatures ranging from 294 to 1300 K for quenching by NO (X Π2), H2 O, CO2, O2, CO, N2, and C2 H2. The A +2 (v′ =0) state was populated via two-photon excitation with a picosecond laser at 454 nm, and the decay rate of the fluorescence originating from A +2 (v′ =0) was measured directly. Thermally averaged quenching cross sections were determined from the dependence of the fluorescence decay rate on the quencher gas pressure. Our measurements are compared to previous measurements and models of the quenching cross sections, and new empirical fits to the data are presented. Our new cross-section data enable predictions in excellent agreement with prior measurements of the fluorescence lifetime in an atmospheric-pressure methane-air diffusion flame. The agreement resolves discrepancies between the lifetime measurements and predictions based on the previous quenching models, primarily through improved models for the quenching by H2 O, CO2, and O2 at temperatures less than 1300 K. © 2006 American Institute of Physics.

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