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Accurate knowledge of post-detonation fireball temperatures is important for understanding device performance and for validation of numerical models. Such measurements are difficult to make even under controlled laboratory conditions. In this work temperature measurements were performed in the fireball of a commercial detonator (RP-80, Teledyne RISI). The explosion and fragments were contained in a plastic enclosure with glass windows for optical access. A hybrid femtosecond-picosecond (fs-ps) rotational coherent anti-Stokes Raman scattering (CARS) instrument was used to perform gas-phase thermometry along a one-dimensional measurement volume in a single laser shot. The 13-mm-thick windows on the explosive-containment housing introduced significant nonlinear chirp on the fs lasers pulses, which reduced the Raman excitation bandwidth and did not allow for efficient excitation of high-J Raman transitions populated at flame temperatures. To overcome this, distinct pump and Stokes pulses were used in conjunction with spectral focusing, achieved by varying the relative timing between the pump and Stokes pulses to preferentially excite Raman transitions relevant to flame thermometry. Light scattering from particulate matter and solid fragments was a significant challenge and was mitigated using a new polarization scheme to isolate the CARS signal. Fireball temperatures were measured 35–40 mm above the detonator, 12–25 mm radially outward from the detonator centerline, and at 18 and 28 µs after initiation. At these locations and times, significant mixing between the detonation products and ambient air had occurred thus increasing the nitrogen-based CARS thermometry signal. Initial measurements show a distribution of fireball temperatures in the range 300–2000 K with higher temperatures occurring 28 µs after detonation.

Width-increased dual-pump enhanced coherent anti-Stokes Raman spectroscopy (WIDECARS) measurements were used to determine the temperature and major species mole fractions in laminar, premixed, ethylene–air flames operating at atmospheric pressure. Conventional ultrabroadband dye lasers for WIDECARS, which use Pyrromethene dyes, have historically suffered from day-to-day wavelength shifting. To overcome this problem, a new ultrabroadband dye laser was developed in this study to provide a stable wavelength and power generation. A new dye laser pumping scheme and a mixture of Sulforhodamine 640, Kiton Red 620, and Rhodamine 640, was used to generate the desired FWHM ∼ 15 n m ( 410 c m − 1 ) bandwidth. The WIDECARS measured mole fraction ratios of C O 2 , CO, and H 2 with N 2 agreed well with chemical equilibrium calculations.

Digital holography is a three-dimensional (3D) measurement technique that can be used to quantitatively determine the size and 3D location of the objects inside a field-of-view. However, in systems where refractive index gradients are present, variations in optical phase due to high-speed shock-waves or low-speed thermal gradients can cause distortions that obscure objects. While techniques like phase-conjugate digital in-line holography and iterative phase measurement techniques have been developed in the past for phase removal or phase measurement, they require either nonlinear four-wave-mixing or iterative algorithms to operate. In this paper, we demonstrate a novel recalculated intensity propagation phase holography (RIPPH) method that captures distorted holograms using low-power continuous lasers, refocuses the hologram to the plane of the distortion, and cancels the phase distortion numerically in a single post-processing step. The resulting hologram can be numerically refocused to provide distortion-free 3D information describing objects that absorb or scatter light. In RIPPH, only the approximate z -locations of the phase distortions are needed, making this method significantly faster to compute than phase retrieval methods. Theoretical simulations are first used to describe and assess the distortion removal process. Experiments are then conducted to demonstrate at least 3 × lower edge distortion for RIPPH compared to traditional digital in-line holography. We demonstrate, for the first time, how phase distortions from supersonic air jets, particle-laden spherically expanding shock-waves, and convectively-driven thermal gradients are numerically cancelled and show how objects of interest are accurately recovered.

A high-speed temperature diagnostic based on spontaneous Raman scattering (SRS) was demonstrated using a pulse-burst laser. The technique was first benchmarked in near-adiabatic H 2 - a i r flames at a data-acquisition rate of 5 kHz using an integrated pulse energy of 1.0 J per realization. Both the measurement precision and accuracy in the flame were within 3% of adiabatic predictions. This technique was then evaluated in a challenging free-piston shock tube environment operated at a shock Mach number of 3.5. SRS thermometry resolved the temperature in post-incident and post-reflected shock flows at a repetition rate of 3 kHz and clearly showed cooling associated with driver expansion waves. Collectively, this Letter represents a major advancement for SRS in impulsive facilities, which had previously been limited to steady state regions or single-shot acquisition.

Three-beam rotational coherent anti-Stokes Raman scattering (CARS) measurements performed in highly scattering environments are susceptible to contamination by two-beam CARS signals generated by the pump–probe and Stokes–probe interactions at the measurement volume. If this occurs, differences in the Raman excitation bandwidth between the two-beam and three-beam CARS signals can add significant errors to the spectral analysis. This interference to the best of our knowledge has not been acknowledged in previous three-beam rotational CARS experiments, but may introduce measurement errors up to 25% depending on the temperature, amount of scattering, and differences between the two-beam and three-beam Raman excitation bandwidths. In this work, the presence of two-beam CARS signal contamination was experimentally verified using a femtosecond–picosecond rotational CARS instrument in two scattering environments: (1) a fireball generated by a laboratory-scale explosion that contained particulate matter, metal fragments, and soot, and (2) a flow of air and small liquid droplets. A polarization scheme is presented to overcome this interference. By rotating the pump and Stokes polarizations + 55 ∘ and − 55 ∘ from the probe, respectively, the two-beam and three-beam CARS signals are orthogonally polarized and can be separated using a polarization analyzer. Using this polarization arrangement, the Raman-resonant three-beam CARS signal amplitude is reduced by a factor of 2.3 compared to the case where all polarizations are parallel. This method is successfully demonstrated in both scattering environments. A theoretical model is presented, and the temperature measurement error is studied for different experimental conditions. The criteria for when this interference may be present are discussed.

Knowledge of soot particle sizes is important for understanding soot formation and heat transfer in combustion environments. Soot primary particle sizes can be estimated by measuring the decay of time-resolved laser-induced incandescence (TiRe-LII) signals. Existing methods for making planar TiRe-LII measurements require either multiple cameras or time-gate sweeping with multiple laser pulses, making these techniques difficult to apply in turbulent or unsteady combustion environments. Here, we report a technique for planar soot particle sizing using a single high-sensitivity, ultra-high-speed 10 MHz camera with a 50 ns gate and no intensifier. With this method, we demonstrate measurements of background flame luminosity, prompt LII, and TiRe-LII decay signals for particle sizing in a single laser shot. The particle sizing technique is first validated in a laminar non-premixed ethylene flame. Then, the method is applied to measurements in a turbulent ethylene jet flame.

Digital inline holography (DIH) provides instantaneous three-dimensional (3D) measurements of diffracting objects; however, phase disturbances in the beam path can distort the imaging. In this Letter, a phase conjugate digital inline holography (PCDIH) configuration is proposed for removal of phase disturbances. Brillouin-enhanced four-wave mixing produces a phase conjugate signal that back propagates along the DIH beam path. The results demonstrate the removal of distortions caused by gas-phase shocks to recover 3D images of diffracting objects.

Femtosecond, two-photon-absorption laser-induced-fluorescence (TALIF) imaging measurements of krypton (Kr) are demonstrated to study mixing in gaseous flows. A measurement approach is presented in which observed Kr TALIF signals are 7 times stronger than the current state-of-the-art methodology. Fluorescence emission is compared for different gas pressures and excitation wavelengths, and the strongest fluorescence signals were observed when the excitation wavelength was tuned to 212.56 nm. Using this optimized excitation scheme, 1-kHz, single-laser-shot visualizations of unsteady flows and two-dimensional measurements of mixture fraction and scalar dissipation rate of a Kr-seeded jet are demonstrated.

Single-laser-shot femtosecond rotational coherent anti-Stokes Raman scattering (fs-RCARS) temperature measurements are performed across a 6-mm line in a turbulent, sooting ethylene jet flame to characterize temperature gradients. A 60- fs pulse is used to excite many rotational Raman transitions in N 2 , and a 160-ps pulse is used to probe the Raman coherence. The spatial resolution of the measurements is 500 μm in the direction of beam propagation and 50 μm in the transverse directions. Measurements have been performed at multiple locations in the jet flame, and the measured temperature are similar to previously recorded point measurements. Future work will include performing simultaneous laser-induced incandescence (LII) measurements to measure soot volume fraction to perform joint statistical analysis of the sooting turbulent flame.

Currently there is a substantial lack of data for interactions of shock waves with particle fields having volume fractions residing between the dilute and granular regimes. To close this gap, a novel multiphase shock tube has been constructed to drive a planar shock wave into a dense gas–solid field of particles. A nearly spatially isotropic field of particles is generated in the test section by a gravity-fed method that results in a spanwise curtain of spherical 100-micron particles having a volume fraction of about 20%. Interactions with incident shock Mach numbers of 1.66, 1.92, and 2.02 are reported. High-speed schlieren imaging simultaneous with high-frequency wall pressure measurements are used to reveal the complex wave structure associated with the interaction. Following incident shock impingement, transmitted and reflected shocks are observed, which lead to differences in particle drag across the streamwise dimension of the curtain. Shortly thereafter, the particle field begins to propagate downstream and spread. For all three Mach numbers tested, the energy and momentum fluxes in the induced flow far downstream are reduced about 30–40% by the presence of the particle field.

We present a dual-pump coherent anti-Stokes Raman scattering (CARS) instrument, which has been constructed for the probing of temperature fluctuations in turbulent pool fires of meter-scale. The measurements were performed at the Fire Laboratory for Accreditation of Models and Experiments (FLAME) facility at Sandia National Laboratories, which provides a canonical fire plume in quiescent wind conditions, with well-characterized boundary conditions and access for modern laser-diagnostic probes. The details of the dual-pump CARS experimental facility for the fire-science application are presented, and single-laser-shot CARS spectra containing information from in-fire N2, O2, H2, and CO2 are provided. Single-shot temperatures are obtained from spectral fitting of the Raman Q-branch signature of N2, from which histograms that estimate the pdf of the enthalpy-averaged temperature fluctuations at the center of the fire plume are presented. Results from two different sooting fire experiments reveal excellent test-to-test repeatability of the fire plume provided by FLAME, as well as the CARS-measured temperatures. The accuracy and precision of the CARS temperatures is assessed from measurements in furnace-heated air, where the temperature can be accurately determined by a thermocouple. At temperatures in excess of 500 K, the furnace results show that the CARS measurements are accurate to within 2–3% and precise to within ±3–5% of the measured absolute temperature.

We investigate the utility of dual-pump coherent anti-Stokes Raman scattering of N 2 for the probing of rich acetylene- and ethylene-fueled flames with soot volume fractions upwards of 2 ppm, which is well in excess of recent reports of sooting flame measurements with the dual-pump approach. A substantial level of interference in the coherent-Raman spectra is observed when the N 2 (3-branch signature is positioned in spectral regions that have been reported to be interference-free and are removed from the peaks of the C 2 Swan system that are the chief obstacle to thermometry in sooting flames. This interference is attributed to coherent-Raman processes in laser-produced C2 and in olefinic hydrocarbons, which exhibit Raman frequencies that are resonant with the pump-2/Stokes frequency difference. A second source of coherent interference is also discussed, in which a significant nonresonant pedestal is added to the coherent-Raman signal, presumably as a result of laser-induced breakdown in the presence of only the highest soot loadings probed here. Two "spectrally quiet" regions for the coherent-Raman signal near 483 and 496 nm are identified, and temperature profiles from an array of heavily sooting acetylene-fueled nonpremixed flames and a premixed ethylene/air flame are provided using a N 2 Q-branch signature positioned near 483 nm. The results show that dual-pump coherent anti-Stokes Raman scattering of N 2 is a viable thermometer at soot loadings at least as high as 2 ppm, albeit with more restrictions on the spectral position of the signal than previously thought.

The interaction of a Mach 1.67 shock wave with a dense particle curtain is quantified using flash radiography. These new data provide a view of particle transport inside a compressible, dense gas–solid flow of high optical opacity. The curtain, composed of 115-µm glass spheres, initially spans 87 % of the test section width and has a streamwise thickness of about 2 mm. Radiograph intensities are converted to particle volume fraction distributions using the Beer–Lambert law. The mass in the particle curtain, as determined from the X-ray data, is in reasonable agreement with that given from a simpler method using a load cell and particle imaging. Following shock impingement, the curtain propagates downstream and the peak volume fraction decreases from about 23 to about 4 % over a time of 340 µs. The propagation occurs asymmetrically, with the downstream side of the particle curtain experiencing a greater volume fraction gradient than the upstream side, attributable to the dependence of particle drag on volume fraction. Bulk particle transport is quantified from the time-dependent center of mass of the curtain. The bulk acceleration of the curtain is shown to be greater than that predicted for a single 115-µm particle in a Mach 1.67 shock-induced flow.

We investigate the feasibility of gas-phase pressure measurements using fs/ps rotational CARS. Femtosecond pump and Stokes pulses impulsively prepare a rotational Raman coherence, which is probed by a high-energy 5-ps pulse introduced at a time delay from the Raman preparation. These ultrafast laser pulses are shorter than collisional-dephasing time scales, enabling a new hybrid time- and frequency-domain detection scheme for pressure. Single-laser-shot rotational CARS spectra were recorded from N2 contained in a room-temperature gas cell for pressures from 0.4 to 3 atm and probe delays ranging from 16 to 298 ps. Sensitivity of the accuracy and precision of the pressure data to probe delay was investigated. The technique exhibits superior precision and comparable accuracy to previous laser-diagnostic pressure measurements.

We investigate the feasibility of gas-phase pressure measurements at kHz-rates using fs/ps rotational CARS. Femtosecond pump and Stokes pulses impulsively prepare a rotational Raman coherence, which is then probed by a high-energy 6-ps pulse introduced at a time delay from the Raman preparation. Rotational CARS spectra were recorded in N2 contained in a room-temperature gas cell for pressures from 0.1 to 3 atm and probe delays ranging from 10-330 ps. Using published self-broadened collisional linewidth data for N2, both the spectrally integrated coherence decay rate and the spectrally resolved decay were investigated as means for detecting pressure. Shot-averaged and single-laser-shot spectra were interrogated for pressure and the accuracy and precision as a function of probe delay and cell pressure are discussed. Single-shot measurement accuracies were within 0.1 to 6.5% when compared to a transducer values, while the precision was generally between 1% and 6% of measured pressure for probe delays of 200 ps or more, and better than 2% as the delay approached 300 ps. A byproduct of the pressure measurement is an independent but simultaneous measurement of the gas temperature.

In recent years, time-resolved particle image velocimetry (TR-PIV) has evolved as a means of measuring temporally correlated velocity fields, allowing the acquisition of PIV movies. Extension beyond roughly 10 kHz is not yet feasible with the diode-pumped solid-state lasers that typically are used in lower speed regimes. Instead, TR-PIV in high-speed flows is best accomplished using a pulse-burst laser, as this is the only light source capable of producing sufficient energy at the necessary pulse rates. Furthermore, it can produce pairs of pulses at arbitrary separation times, which allows the very short times between paired exposures compatible with high-speed flow, in contrast with the long time between exposures using a single kHz-rate laser. Simultaneous with the maturation of pulse-burst laser technology, quality high-speed cameras have begun to achieve desirable framing rates without excessive sacrifice of the size of the spatial array.

In this work, the use of Raman Stokes peak location and linewidth broadening methods were evaluated for thermometry applications of polysilicon microheaters subjected to evolving thermal stresses. Calibrations were performed using the temperature dependence of each spectral characteristic separately, and the uncertainty of each method quantified. It was determined that the Stokes linewidth was independent of stress variation allowing for temperature determination, irrespective of stress state. However, the linewidth method is subject to greater uncertainty than the Stokes shift determination. The uncertainties for each method are observed to decrease with decreasing temperature and increasing integration times. The techniques were applied to mechanically constrained electrically active polysilicon microheaters. Results revealed temperatures in excess of 500°C could be achieved in these devices. Using the peak location method resulted in an underprediction of temperature due to the development of a relative compressive thermal stress with increasing power dissipation.

Micro-Raman spectroscopy has proven to be a valuable tool for obtaining temperature measurements in active semiconductor and MEMS devices. By using the temperature-calibrated response of the polysilicon Raman signature, we have obtained spatially resolved temperature measurements of U-shaped electro-thermal actuators. Both the peak position and the line width of the characteristic Raman peak have been used as temperature metrics. The measured thermal profiles are further compared to numerical models of the electro-thermal response of the devices as designed and fabricated. The obtained thermal profiles are in qualitative agreement with published modeled thermal profiles of similar devices and are within 15 °C of our modeled profiles. These measurements represent the first reported experimental temperature profile measurements for flexure type actuators and can be used to validate the existing models. Moreover, the comparison of line width and position-based temperatures are in good agreement, differing slightly over the flexure regions of the device.

In this paper, we report spatially resolved temperature profiles along the legs of working V-shaped electrothermal (ET) actuators using a surface Raman scattering technique. The Raman probe provides nonperturbing optical data with a spatial resolution of 1.2 /spl mu/m, which is required to observe the 3-/spl mu/m-wide actuator beams. A detailed uncertainty analysis reveals that our Raman thermometry of polycrystalline silicon is performed with fidelity of /spl plusmn/10 to 11 K when the peak location of the Stokes-shifted optical phonon signature is used as an indicator of temperature. This level of uncertainty is sufficient for temperature mapping of many working thermal MEMS devices which exhibit characteristic temperature differences of several hundred Kelvins. To our knowledge, these are the first quantitative and spatially resolved temperature data available for thermal actuator structures. This new temperature data set can be used for validation of actuator thermal design models and these new results are compared with finite-difference simulations of actuator thermal performance.

In this paper, an acetone planar laser-induced fluorescence (PLIF) technique for nonintrusive temperature imaging is demonstrated in gas-phase (Pr = 0.72) turbulent Rayleigh–Benard convection at Rayleigh number Ra = 1.3×105. The PLIF technique provides quantitative spatially correlated temperature data without the flow intrusion or time lag associated with physical probes, and without the significant path averaging that plagues most optical heat-transfer diagnostic tools, such as the Mach–Zehnder interferometer, thus making PLIF an attractive choice for quantitative thermal imaging in easily perturbed, complex three-dimensional flow fields. The "instantaneous" (20-ns integration time) thermal images presented have a spatial resolution of 176×176×500 µm and a single-pulse temperature measurement precision of ± 2.5 K, or 2.5% of the total temperature difference. These images represent a two-dimensional slice through a complex three-dimensional flow, allowing for thermal structure of the turbulence to be quantified. Statistics such as the horizontally averaged temperature profile, root-mean square (rms) temperature fluctuation, two-point spatial correlations, and conditionally averaged plume structures are computed from an ensemble of 100 temperature images. The profiles of the mean temperature and rms temperature fluctuation are in good agreement with previously published data, and the results obtained from the two-point spatial correlations and conditionally averaged temperature fields show the importance of large-scale coherent structures in this turbulent flow.

We present the results of an LDRD project to develop diagnostics to perform fundamental measurements of material properties during shock compression of condensed phase materials at micron spatial scales and picosecond time scales. The report is structured into three main chapters, which each focus on a different diagnostic devel opment effort. Direct picosecond laser drive is used to introduce shock waves into thin films of energetic and inert materials. The resulting laser - driven shock properties are probed via Ultrafast Time Domain Interferometry (UTDI), which can additionally be used to generate shock Hugoniot data in tabletop experiments. Stimulated Raman scattering (SRS) is developed as a temperature diagnostic. A transient absorption spectroscopy setup has been developed to probe shock - induced changes during shock compressio n. UTDI results are presented under dynamic, direct - laser - drive conditions and shock Hugoniots are estimated for inert polystyrene samples and for the explosive hexanitroazobenzene, with results from both Sandia and Lawrence Livermore presented here. SRS a nd transient absorption diagnostics are demonstrated on static thin - film samples, and paths forward to dynamic experiments are presented.

1 Figure 1. Energy level diagram for the fs/ps rotational CARS process: broadband femtosecond preparation pulses centered near 800 nm, and represented by thick red lines, prepare a Raman coherence at time t = 0. A frequency-narrow picosecond probe centered near 400 nm, and shown as a narrow blue line, probes the coherence at time delay t = , to yield CARS/CSRS signal shown as a thick blue line. Pure-Rotational fs/ps CARS Measurements of Temperature and Concentration using a Second-Harmonic BandwidthCompressed Probe

This paper describes the use of dual-broadband, pure-rotational coherent anti-Strokes Raman spectroscopy (CARS) as a non-intrusive temperature diagnostic for convective-heat-transfer flows. The characteristics of the dual-broadband, pure-rotational CARS technique are discussed, and the technique is compared to other temperature measurement methods. Dual-broadband, pure-rotational CARS was used to measure mean temperature profiles in a low-Reynolds-number, turbulent boundary layer. The results are presented in wall units and compared to the thermal law of the wall for zero-pressure-gradient boundary layers. Temperature data were acquired as close as 50 μm (±25 μm) to the wall, with a spatial resolution of 50 μm normal to the heat transfer surface, and a 2 σ precision limit of ±4 K. The spatial resolution of this experimental method provides detailed information in complex thermal boundary layers and allows for an estimation of the convective heat flux to within an estimated uncertainty of −5% to +25%. Single-laser-shot temperature data were acquired in a gas cell, and the potential for measurement of rms temperature fluctuations is discussed in terms of the resulting probability density functions.

We present the results of a two year early career LDRD project, which has focused on the development of ultrafast diagnostics to measure temperature, pressure and chemical change during the shock initiation of energetic materials. We compare two single-shot versions of femtosecond rotational CARS to measure nitrogen temperature: chirped-probe-pulse and ps/fs hybrid CARS thermometry. The applicability of measurements to the combustion of energetic materials will be discussed. We have also demonstrated laser shock and particle velocity measurements in thin film explosives using stretched femtosecond laser pulses. We will discuss preliminary results from Al and PETN thin films. Agreement between our results and previous work will be discussed.

A hybrid fs/ps pure-rotational CARS scheme is characterized in furnace-heated air at temperatures from 290 to 800 K. Impulsive femtosecond excitation is used to prepare a rotational Raman coherence that is probed with a ps-duration beam generated from an initially broadband fs pulse that is bandwidth limited using air-spaced Fabry-Perot etalons. CARS spectra are generated using 1.5- and 7.0-ps duration probe beams with corresponding coarse and narrow spectral widths. The spectra are fitted using a simple phenomenological model for both shot-averaged and single-shot measurements of temperature and oxygen mole fraction. Our single-shot temperature measurements exhibit high levels of precision and accuracy when the spectrally coarse 1.5-ps probe beam is used, demonstrating that high spectral resolution is not required for thermometry. An initial assessment of concentration measurements in air is also provided, with best results obtained using the higher resolution 7.0-ps probe. This systematic assessment of the hybrid CARS technique demonstrates its utility for practical application in low-temperature gas-phase systems.

We demonstrate an approach for picosecond probe-beam generation that enables hybrid femtosecond/picosecond pure-rotational coherent anti-Stokes Raman scattering (CARS) measurements in flames. Sum-frequency generation of bandwidth-compressed picosecond radiation from femtosecond pumps with phase-conjugate chirps provides probe pulses with energies in excess of 1 mJ that are temporally locked to the femtosecond pump/Stokes preparation. This method overcomes previous limitations on hybrid femtosecond/picosecond rotational CARS techniques, which have relied upon less efficient bandwidth-reduction processes that have generally resulted in prohibitively low probe energy for flame measurements. We provide the details of the second-harmonic approach and demonstrate the technique in near-adiabatic hydrogen/air flames.

A hybrid fs/ps pure-rotational CARS scheme is characterized for thermometry in furnace-heated air at temperatures from 290 to 800 K. Impulsive femtosecond excitation is used to prepare a rotational Raman coherence that is probed with a ps-duration beam generated from an initially broadband fs pulse that is bandwidth limited using air-spaced Fabry-Perot etalons. CARS spectra are generated using 1.5- and 7-ps duration probe beams with corresponding coarse and narrow spectral widths. The spectra are fitted using a simple phenomenological model for both shot-averaged and single-shot measurements of temperature and oxygen mole fraction. Our single-shot measurements exhibit high levels of precision when the spectrally coarse 1.5-ps probe beam is used. This systematic assessment of the hybrid CARS technique demonstrates its utility for practical application in moderatetemperature gas-phase systems.

We apply ultrafast pure-rotational coherent anti-Stokes Raman scattering (CARS) for temperature and relative oxygen concentration measurements in the plume emanating from a burning, aluminized ammonium-perchlorate propellant strand. Combustion of these metal-based propellants is a particularly hostile environment for laser-based diagnostics, with intense background luminosity and scattering from hot metal particles as large as several hundred micrometers in diameter. CARS spectra that were previously obtained using nanosecond pulsed lasers in an aluminum-particle-seeded flame are examined and are determined to be severely impacted by nonresonant background, presumably as a result of the plasma formed by particulate-enhanced laser-induced breakdown. Introduction of femtosecond/picosecond (fs/ps) laser pulses improves CARS detection by providing time-gated elimination of strong nonresonant background interference. Single-laser-shot fs/ps CARS spectra were acquired from the burning propellant plume, with picosecond probe-pulse delays of 0 and 16 ps from the femtosecond pump and Stokes pulses. At zero delay, nonresonant background overwhelms the Raman-resonant spectroscopic features. Time-delayed probing results in the acquisition of background-free spectra that were successfully fit for temperature and relative oxygen content. Temperature probability densities and temperature/oxygen correlations were constructed from ensembles of several thousand single-laser-shot measurements with the CARS measurement volume positioned within 3 mm or less of the burning propellant surface. The results show that ultrafast CARS is a potentially enabling technology for probing harsh, particle-laden flame environments.

We discuss recent experiments and modeling for the chirped-probe-pulse generation of single-laser-shot femtosecond pure-rotational CARS/CSRS spectra from room-temperature gases. A pure-rotational Raman coherence is impulsively generated using near-transformlimited femtosecond pump/Stokes excitation, and the coherence is probed by stretching a nominally 100-fs near-transform-limited probe beam to approximately 1.7 ps via the refractive-index dispersion in a 30-cm long flint-glass rod. The linearly chirped probe spectrum and phase beat against the time-dependent Raman polarization to generate complex spectra. Chirped-probe-pulse rotational CARS/CSRS offers an interesting alternative to hybrid fs/ps rotational CARS, in which a band-limited pulse of limited energy is used, because all of the available probe pulse energy can be retained in a chirped-probepulse experiment. Our early chirped-probe spectra are presented and the details of our initial model calculations are provided. The temperature sensitivity of the chirped-probe results is illustrated using calculated spectra.

Understanding the particle-particle and shock-particle interactions that occur in dense gas-solid flows is limited by a lack of knowledge of the underlying phenomena. Gas-solid flows are characterized by the particle volume fraction. ϕ p of the flow [1]. For particle volume fractions less than about 0.1%, flow is considered dilute and the effects of particle collisions are negligible [2]. For packed particles, where the .p is greater than about 50%, the flow regime is said to be granular. The dilute and granular regimes have been well studied, but conversely, a substantial knowledge gap exists for dense gas-solid flows, which have intermediate particle volume fractions of about 0.1 to 50%. This regime exists at microsecond time scales during blast-induced dispersal of material when the shocked particles are closely spaced.

We present what we believe to be the first application of the laser-induced incandescence (LII) technique to large-scale fire testing. The construction of an LII instrument for fire measurements is presented in detail. Soot volume fraction imaging from 2 m diameter pool fires burning blended toluene/methanol liquid fuels is demonstrated along with a detailed report of measurement uncertainty in the challenging pool fire environment. Our LII instrument relies upon remotely located laser, optical, and detection systems and the insertion of water-cooled, fiber-bundle-coupled collection optics into the fire plume. Calibration of the instrument was performed using an ethylene/air laminar diffusion flame produced by a Santoro-type burner, which allowed for the extraction of absolute soot volume fractions from the LII images. Single-laser-shot two-dimensional images of the soot layer structure are presented with very high volumetric spatial resolution of the order of 10(-5) cm3. Probability density functions of the soot volume fraction fluctuations are constructed from the large LII image ensembles. The results illustrate a highly intermittent soot fluctuation field with potentially large macroscale soot structures and clipped soot probability densities.

We discuss recent experiments for the characterization of our femtosecond pure rotational CARS facility for observation of Raman transients in N{sub 2} and atmospheric air. The construction of a simplified femtosecond four-wave mixing system with only a single laser source is presented. Pure-rotational Raman transients reveal well-ordered time-domain recurrence peaks associated with the near-uniform spacing of rotational Raman peaks in the spectral domain. Long-time, 100-ps duration observations of the transient Raman polarization are presented, and the observed transients are compared to simulated results. Fourier transformation of the transients reveals two distinct sets of beat frequencies. Simulation results for temperatures from 300-700 K are used to illustrate the temperature sensitivity of the time-domain transients and their Fourier-transform counterparts. And strategies for diagnostics are briefly discussed. These results are being utilized to develop gas-phase measurement strategies for temperature and species concentration.

We discuss two recent diagnostic-development efforts in our laboratory: femtosecond pure-rotational Coherent anti-Stokes Raman scattering (CARS) for thermometry and species detection in nitrogen and air, and nanosecond vibrational CARS measurements of electric fields in air. Transient pure-rotational fs-CARS data show the evolution of the rotational Raman polarization in nitrogen and air over the first 20 ps after impulsive pump/Stokes excitation. The Raman-resonant signal strength at long time delays is large, and we additionally observe large time separation between the fs-CARS signatures of nitrogen and oxygen, so that the pure-rotational approach to fs-CARS has promise for simultaneous species and temperature measurements with suppressed nonresonant background. Nanosecond vibrational CARS of nitrogen for electric-field measurements is also demonstrated. In the presence of an electric field, a dipole is induced in the otherwise nonpolar nitrogen molecule, which can be probed with the introduction of strong collinear pump and Stokes fields, resulting in CARS signal radiation in the infrared. The electric-field diagnostic is demonstrated in air, where the strength of the coherent infrared emission and sensitivity our field measurements is quantified, and the scaling of the infrared signal with field strength is verified.

Pump-probe transient thermoreflectance (TTR) techniques are powerful tools for measuring the thermophysical properties of thin films, such as thermal conductivity, Λ, or thermal boundary conductance, G. This paper examines the assumption of one-dimensional heating on, Λ and G, determination in nanostructures using a pump-probe transient thermoreflectance technique. The traditionally used one-dimensional and axially symmetric cylindrical conduction models for thermal transport are reviewed. To test the assumptions of the thermal models, experimental data from Al films on bulk substrates (Si and glass) are taken with the TTR technique. This analysis is extended to thin film multilayer structures. The results show that at 11 MHz modulation frequency, thermal transport is indeed one dimensional. Error among the various models arises due to pulse accumulation and not accounting for residual heating.

Micro-Raman thermometry has been demonstrated to be a feasible technique for obtaining surface temperatures with micron-scale spatial resolution for microelectronic and microelectromechanical systems (MEMSs). However, the intensity of the Raman signal emerging from the probed device is very low and imposes a requirement of prolonged data collection times in order to obtain reliable temperature information. This characteristic currently limits Raman thermometry to steady-state conditions and thereby prevents temperature measurements of transient and fast time-scale events. In this paper, we discuss the extension of the micro-Raman thermometry diagnostic technique to obtain transient temperature measurements on microelectromechanical devices with 100 μs temporal resolution. Through the use of a phase-locked technique we are able to obtain temperature measurements on electrically powered MEMS actuators powered with a periodic signal. Furthermore, we demonstrate a way of obtaining reliable temperature measurements on micron-scale devices that undergo mechanical movement during the device operation.

Presented here are broadband, dual-pump CARS measurements which were performed in a 2-meter diameter methanol pool fire. Single-shot temperature and relative mole fractions were obtained simultaneously. The temperatures were compared to traditional thermocouple measurements in the pool fire. It was found that the CARS mean temperatures agree to within 4% of the thermocouple measurements, while the RMS temperatures were an order of magnitude less for the thermocouple. The accuracy and precision of the single-shot temperature measurements were characterized by comparison to a laboratory standard. It was determined that between 500-1400 K the CARS instrument was accurate to better than 4% and the measurements were reproducible to within 6%.

Analysis of the Raman Stokes peak position and its shift has been frequently used to estimate either temperature or stress in microelectronics and microelectromechanical system devices. However, if both fields are evolving simultaneously, the Stokes shift represents a convolution of these effects, making it difficult to measure either quantity accurately. By using the relative independence of the Stokes linewidth to applied stress, it is possible to deconvolve the signal into an estimation of both temperature and stress. Using this property, a method is presented whereby the temperature and stress were simultaneously measured in doped polysilicon microheaters. A data collection and analysis method was developed to reduce the uncertainty in the measured stresses resulting in an accuracy of +/-40 MPa for an average applied stress of -325 MPa and temperature of 520 degrees C. Measurement results were compared to three-dimensional finite-element analysis of the microheaters and were shown to be in excellent agreement. This analysis shows that Raman spectroscopy has the potential to measure both evolving temperature and stress fields in devices using a single optical measurement.

We investigate the utility of dual-pump coherent anti-Stokes Raman scattering (CARS) for investigations of fuel-rich flames with soot volume loadings up to 2.2 ppm. Our initial characterization of a gas-phase propellant simulating burner is presented. The burner investigated consists of alternating fuel and oxidizer tubes with the option for injection of aluminum particles into the flame. We focus on a C2H2-N2-O2 flame, in which no aluminum particles are yet added. For the required flow rates, this burner provides an array of heavily sooting and highly luminous diffusion flames whose temperature is measured by dual-pump CARS. The nature of the observed soot-induced interference in the CARS spectra for several different pump 2 frequencies is documented and CARS temperatures obtained from data in a spectrally “quiet” region, with the CARS signal beam near 483 nm, are presented. Soot volume fractions are imaged by absorption-calibrated laser-induced incandescence (LII) to quantify the soot loadings at which our dual-pump CARS facility provides reliable measurements.

Joint fuel Raman and filtered Rayleigh-scattering (FRS) imaging is demonstrated in a laminar methane-air diffusion flame. These experiments are, to our knowledge, the first reported extension of the FRS technique to nonpremixed combustion. This joint imaging approach allows for correction of the FRS images for the large variations in Rayleigh cross section that occur in diffusion flames and for a secondary measurement of fuel mole fraction. The temperature-dependent filtered Rayleigh cross sections are computed with a six-moment kinetic model for calculation of major-species Rayleigh-Brillouin line shapes and a flamelet-based model for physically judicious estimates of gas-phase chemical composition. Shot-averaged temperatures, fuel mole fractions, and fuel number densities from steady and vortex-strained diffusion flames stabilized on a Wolfhard-Parker slot burner are presented, and a detailed uncertainty analysis reveals that the FRS-measured temperatures are accurate to within +/- 4.5 to 6% of the local absolute temperature.

Experimentally measured temperature profiles along the micron-scale beam of a working thermal actuator are reported for the first time. Using a surface Raman scattering technique, temperature measurements are obtained in a noncontact fashion with submicron spatial resolution and to within an uncertainty of better than ±10 K. The experimental data are used to validate computational predictions of the actuator thermal performance with reasonable agreement between the data and predicted temperatures.Copyright © 2005 by ASME

Filtered Rayleigh Scattering (FRS) is demonstrated in a premixed, sooting ethylene-air flame. In sooting flames, traditional laser-based temperature-imaging techniques such linear (unfiltered) Rayleigh scatting (LRS) and planar laser-induced fluorescence (PLIF) are rendered intractable due to intense elastic scattering interferences from in-flame soot. FRS partially overcomes this limitation by utilizing a molecular iodine filter in conjunction with an injection-seeded Nd:YAG laser, where the seeded laser output is tuned to line center of a strong iodine absorption transition. A significant portion of the Doppler-broadened molecular Rayleigh signal is then passed while intense soot scattering at the laser line is strongly absorbed. In this paper, we demonstrate the feasibility of FRS for sooting flame thermometry using a premixed, ethylene-air flat flame. We present filtered and unfiltered laser light-scattering images, FRS temperature data, and laser-induced incandescence (LII) measurements of soot volume fraction for fuel-air equivalence ratios of φ = 2.19 and 2.24. FRS-measured product temperatures for these flames are nominally 1500 K. The FRS temperature and image data are discussed in the context of the soot LII results and a preliminary estimate of the upper sooting limit for our FRS system of order 0.1 ppm volume fraction is obtained.

A Doppler global velocimetry (DGV) system has been designed, assembled, and tested for use in a Mach 3.7 overexpanded jet prior to future implementation in a hypersonic wind tunnel. Measurements were made using an iodine cell pressure-broadened with nitrogen buffer gas to selectively absorb light from a frequency-doubled Nd:YAG laser scattering from condensed ethanol particles in the jet flow. Details of the present implementation of the measurement technique and data reduction are presented herein. Calibrations of a pressure-broadened iodine cell have shown that the induced absorption line shift can create velocity biases unless a second iodine cell is scanned simultaneously to provide an independent frequency reference. Exploratory velocity data in the jet have been acquired that are experimentally repeatable and consistent with physical expectations, which lends confidence towards the performance of the assembled system.

This paper describes the application of a filtered-Rayleigh-scattering (FRS) instrument for nonintrusive temperature imaging in a vortex-driven diffusion flame. The FRS technique provides quantitative, spatially correlated temperature data without the flow intrusion or time lag associated with physical probes. Use of a molecular iodine filter relaxes the requirement for clean, particulate-free flowfields and offers the potential for imaging near walls, test section windows and in sooty flames, all of which are preculded in conventional Rayleigh imaging, where background interference from these sources typically overwhelms the weak molecular scattering signal. For combustion applications, FRS allows for full-field temperature imaging without chemical seeding of the flowfield, which makes FRS an attractive alternative to other laser-based imaging methods such as planar laser-induced fluorescencs (PLIF). In this work, the details of our FRS imaging system are presented and temperature measurements from an acoustically forced diffusion flame are provided. The local Rayleigh crosssection is corrected using Raman imaging measurements of the methane fuel molecule, which are then correlated to other major species using a laminar flamelet approach. To our knowledge, this is the first report of joint Raman/FRS imaging for nonpremixed combustion. Measurements are presented from flames driven at 7.5 Hz, where a single vortex stretches the flame, and at 90 Hz, where two consecutive vortices interact to cause a repeatable strain-induced flame-quenching event.