The Texas A&M University Hypervelocity Impact Laboratory: A modern aeroballistic range facility.

Novel engineering materials and structures are increasingly designed for use in severe environments involving extreme transient variations in temperature and loading rates, chemically reactive flows, and other conditions. The Texas A&M University Hypervelocity Impact Laboratory (HVIL) enables unique ultrahigh-rate materials characterization, testing, and modeling capabilities by tightly integrating expertise in high-rate materials behavior, computational and polymer chemistry, and multi-physics multiscale numerical algorithm development, validation, and implementation. The HVIL provides a high-throughput test bed for development and tailoring of novel materials and structures to mitigate hypervelocity impacts (HVIs). A conventional, 12.7 mm, smooth bore, two-stage light gas gun (2SLGG) is being used as the aeroballistic range launcher to accelerate single and simultaneously launched projectiles to velocities in the range 1.5-7.0 km/s. The aeroballistic range is combined with conventional and innovative experimental, diagnostic, and modeling capabilities to create a unique HVI and hypersonic test bed. Ultrahigh-speed imaging (10M fps), ultrahigh-speed schlieren imaging, multi-angle imaging, digital particle tracking, flash x-ray radiography, nondestructive/destructive inspection, optical and scanning electron microscopy, and other techniques are being used to characterize HVIs and study interactions between hypersonic projectiles and suspended aerosolized particles. Additionally, an overview of 65 2SLGG facilities operational worldwide since 1990 is provided, which is the most comprehensive survey published to date. The HVIL aims to (i) couple recent theoretical developments in shock physics with advances in numerical methods to perform HVI risk assessments of materials and structures, (ii) characterize environmental effects (water, ice, dust, etc.) on hypersonic vehicles, and (iii) address key high-rate materials and hypersonics research problems.

Hydroxyl radical planar laser-induced fluorescence imaging in flames using frequency-tripled femtosecond laser pulses.

Ultra-short optical pulses in the ultraviolet (UV) region are of significant interest for combustion and reacting flow diagnostics, as most important chemical species have electronic resonance transitions in the UV region. Optical parametric amplifiers are typically used for frequency conversion of femtosecond (fs) pulses from near-IR to UV; however, their implementation for practical imaging applications is limited because of the low conversion efficiency and extreme sensitivity to ambient conditions. In this work, we report the implementation of direct-frequency-tripled, fs laser pulses from a tunable amplified laser system for high-resolution imaging of hydroxyl (OH) radical in flames. The fundamental laser output near 850 nm is frequency tripled to obtain approximately 283.3-nm UV radiation. OH planar laser-induced fluorescence (PLIF) imaging at 1 kHz is demonstrated in turbulent flames with image sheet heights in excess of 45 mm and a signal-to-noise ratio better than 25. These results represent over 3× increase in the imaging dimensionality compared to traditional OPA-based systems. Additionally, the third-harmonic generation apparatus is compact, robust, and easy to operate while providing near-Gaussian beam profiles. Simple power scaling suggests another factor of 3 or more increase in sheet height can be achieved for kilohertz-rate practical combustion diagnostics applications.

Spectroscopic investigation of high-pressure femtosecond two-photon laser-induced fluorescence of carbon monoxide up to 20 bar.

Extension of laser diagnostic methods to high pressure is critically important because most practical combustion systems operate at elevated pressures. However, increased collisional quenching, fluorescence trapping, and other spectroscopic complications make high-pressure laser diagnostics extremely challenging. As the pressure increases, collisional effects broaden and shift excitation spectral lines, reducing the excitation quantum efficiency of the laser-induced fluorescence (LIF) technique, in particular when using conventional narrowband, nanosecond (ns)-duration laser pulses. In this work, spectroscopic investigation of broadband, femtosecond two-photon LIF (fs-TPLIF) of carbon monoxide (CO) was performed in a high-pressure static gas cell, up to total pressures of 20 bar. The fluorescence emission spectrum broadened marginally at the highest pressure investigated and hence can be neglected in most cases. The subquadratic dependence of the CO fs-TPLIF signal on the laser fluence increased as the pressure is increased. Moreover, the CO fs-TPLIF signal decays more slowly with increasing pressure compared to the previously reported ns-TPLIF data. The signal drop when the total pressure is increased from 1 to 13 bar is approximately 30% in the fs excitation, as compared to approximately a 60% drop in the ns excitation in CO/N2/O2 mixtures. The pressure effects on the fluorescence signal were observed to be similar in the Ångström and third positive bands, suggesting that the third positive band could also be used for CO measurements with broadband fs laser pulses. Furthermore, experimentally investigated are the effect of pressure on the CO fluorescence signal in different quenching gases using fixed CO mole fractions, as well as number densities. Overall, the fs-TPLIF scheme is shown to be a promising diagnostics tool for CO detection in practical combustion systems at elevated pressures.

Ultrashort-pulse laser-induced breakdown spectroscopy for detecting airborne metals during energetic reactions.

Ultrashort-pulse laser-induced breakdown spectroscopy (LIBS), specifically using a femtosecond laser, has certain advantages over longer-pulse, nanosecond-duration lasers, in that they typically have kilohertz repetition rates and reduced background noise along with little-to-no laser-plasma interaction, all of which lead to a better chance of detecting LIBS signals from trace particles. In this work, femtosecond-LIBS is investigated for the detection of metallic particles in the hot flame zone of solid propellant strands burning in the atmosphere. The metallic particles doped into the solid propellants were aluminum (Al), copper, lead, lead stearate, and mercury chloride, which are all either typically found in energetic formulations as additives or impurities. Using an 80-fs-pulse-duration, amplified Ti:Sapphire laser operating at 1000 Hz, single-shot concentration measurement experiments were performed. The femtosecond-LIBS apparatus could detect all metallic additives, whereas a previous nanosecond-LIBS scheme with comparable conditions was able to detect only higher concentrations of Al. The single-shot concentration study, conducted with the Al-doped propellants, indicated that there is a linear relationship between the percentage of laser shots detecting a LIBS signal and the mass percentage of Al initially present in the strands. The present results illustrate the advantages of using a femtosecond laser over a nanosecond laser for LIBS detection during energetics material reactions.

Three-photon-excited laser-induced fluorescence detection of atomic hydrogen in flames.

In many recent studies, ultrashort femtosecond (fs) two-photon (2p) laser-induced fluorescence (LIF) of atomic hydrogen (H) has been demonstrated using a 205 nm excitation. However, 205-nm- deep ultraviolet (UV) pulses can be problematic in practical devices containing thick transmissive optics and can also be susceptible to photolytic production at high laser energies. In this Letter, we investigate the three-photon (3p) excitation scheme of H by using red-shifted 307.7 nm fs laser pulses. Efficient 3p excitation resulting from fs laser pulses enable the 3pLIF detection of H, which was previously unattainable in most flame conditions using ns or ps pulses. Measurements are reported in CH4/O2/N2 Bunsen jet flames and premixed CH4/air flames and compared to similar 2pLIF schemes with fs pulses. Saturation effects, photolytic interferences, and stimulated emissions effects are studied, as well as the benefits of 3pLIF in diagnostic hardware with thick optical windows.

Laser-induced-breakdown-spectroscopy-based detection of metal particles released into the air during combustion of solid propellants.

Numerous metals and metal compounds are often added to propellants and explosives to tailor their properties such as heat release rate and specific impulse. When these materials combust, these metals can be released into the air, causing adverse health effects such as pulmonary and cardiovascular disease, particulate-matter-induced allergies, and cancer. Hence, robust, field-deployable methods are needed to detect and quantify these suspended metallic particles in air, identify their sources, and develop mitigation strategies. Laser-induced breakdown spectroscopy (LIBS) is a technique for elemental detection, commonly used on solids and liquids. In this study, we explored nanosecond-duration LIBS for detecting airborne metals during reactions of solid propellant strands, resulting from additives of aluminum (Al), copper, lead, lead stearate, and mercury chloride. Using the second harmonic of a 10-ns-duration 10-Hz, Nd:YAG laser, plasma was generated in the gas-phase exhaust plume of burning propellant strands containing the target metals. Under the current experimental conditions, the ns-LIBS scheme was capable of detecting Al at concentrations of 5%, 10%, and 16% by weight in the propellant strand. As the weight percentage increased, the LIBS signal was detected by more laser shots, up to a point where the system transition from being nonhomogeneous to a more-uniform distribution of particles. Further measurements and increased understanding of the reacting flow field are necessary to quantify the effects of other metal additives besides Al.

FLEET velocimetry for combustion and flow diagnostics.

We report the use of femtosecond laser electronic excitation tagging (FLEET) for velocimetry at a 100-kHz imaging rate. Sequential, single-shot, quantitative velocity profiles of an underexpanded supersonic nitrogen jet were captured at a 100-kHz rate. The signal and lifetime characteristics of the FLEET emission were investigated in a methane flame above a Hencken burner at varying equivalence ratios, and room temperature gas mixtures involving air, methane, and nitrogen. In the post-flame region of the Hencken burner, the emission lifetime was measured as two orders of magnitude lower than lab air conditions. Increasing the equivalence ratio above 1.1 leads to a change in behavior, with a doubled lifetime. By measuring the emission in a cold methane flow, a short-lived signal was measured that decayed after the first microsecond. As a proof of concept for velocimetry in a reacting environment, the exhaust of a pulsed detonator was measured by FLEET. Quantitative velocity information was obtained that corresponded to a maximum centerline velocity of 1800 m/s for the detonation wave. Extension of FLEET to larger scale, complex flow environments is now a viable option.

Optical ray tracing method for simulating beam-steering effects during laser diagnostics in turbulent media.

In most coherent spectroscopic methods used in gas-phase laser diagnostics, multiple laser beams are focused and crossed at a specific location in space to form the probe region. The desired signal is then generated as a result of nonlinear interactions between the beams in this overlapped region. When such diagnostic schemes are implemented in practical devices having turbulent reacting flow fields with refractive index gradients, the resulting beam steering can give rise to large measurement uncertainties. The objective of this work is to simulate beam-steering effects arising from pressure and temperature gradients in gas-phase media using an optical ray tracing approach. The ZEMAX OpticStudio software package is used to simulate the beam crossing and uncrossing effects in the presence of pressure and temperature gradients, specifically the conditions present in high-pressure, high-temperature combustion devices such as gas turbine engines. Specific cases involving two-beam and three-beam crossing configurations are simulated. The model formulation, the effects of pressure and temperature gradients, and the resulting beam-steering effects are analyzed. The results show that thermal gradients in the range of 300-3000 K have minimal effects, while pressure gradients in the range of 1-50 atm result in pronounced beam steering and the resulting signal fluctuations in the geometries investigated. However, with increasing pressures, the temperature gradients can also have a pronounced effect on the resultant signal levels.

Two-photon-absorption line strengths for nitric oxide: Comparison of theory and sub-Doppler, laser-induced fluorescence measurements.

We discuss the results of high-resolution, sub-Doppler two-photon-absorption laser-induced fluorescence (TPALIF) spectroscopy of nitric oxide at low pressure and room temperature. The measurements were performed using the single-longitudinal mode output of a diode-laser-seeded optical parametric generator (OPG) system with a measured frequency bandwidth of 220 MHz. The measurements were performed using a counter-propagating pump beam geometry, resulting in sub-Doppler TPALIF spectra of NO for various rotational transitions in the (0,0) vibrational band of the A2Σ+ - X2Π electronic transition. The experimental results are compared with the results of a perturbative treatment of the rotational line strengths for the 20 different rotational branches of the X2Π(v″ = 0) → A2Σ+(v' = 0) two-photon absorption band. In the derivation of the expressions for the two-photon transition absorption strength, the closure relation is used for rotational states in the intermediate levels of the two-photon transition in analogy with the Placzek treatment of Raman transitions. The theoretical treatment of the effect of angular momentum coupling on the two-photon rotational line strengths features the use of irreducible spherical tensors and 3j symbols. The final results are expressed in terms of the Hund's case (a) coupling coefficients aJ and bJ for the X2Π(v″ = 0) rotational level wavefunctions, which are intermediate between Hund's case (a) and case (b). Considerable physical insight is provided by this final form of the equations for the rotational line strengths. Corrections to the two-photon absorption rotational line strength for higher order effects such as centrifugal stretching can be included in a straightforward fashion in the analysis by incorporating higher order terms in these coupling coefficients aJ and bJ, although these corrections are essentially negligible for J < 50. The theoretical calculations of relative line intensities are in good agreement both with our experiment and with published experimental results. In addition, the calculated line shapes and relative intensities for closely spaced main branch and satellite transitions are in excellent agreement with our experimental measurements.

Femtosecond two-photon laser-induced fluorescence of krypton for high-speed flow imaging.

Ultrashort-pulse (femtosecond-duration) two-photon laser-induced fluorescence (fs-TPLIF) of an inert gas tracer krypton (Kr) is investigated. A detailed spectroscopic study of fluorescence channels followed by the 5p'←←4p excitation of Kr at 204.1 nm is reported. The experimental line positions in the 750-840 nm emission region agree well with the NIST Atomic Spectra Database. The present work provides an accurate listing of relative line strengths in this spectral region. In the range of laser pulse energies investigated, a quadratic dependence was observed between the Kr-TPLIF signal and the laser pulse energy. The single-laser-shot 2D TPLIF images recorded in an unsteady jet demonstrate the potential of using fs excitation at 204.1 nm for mixing and flow diagnostic studies using Kr as an inert gas tracer.

Investigation of optical fibers for high-repetition-rate, ultraviolet planar laser-induced fluorescence of OH.

We investigate the fundamental transmission characteristics of nanosecond-duration, 10 kHz repetition rate, ultraviolet (UV) laser pulses through state-of-the-art, UV-grade fused-silica fibers being used for hydroxyl radical (OH) planar laser-induced fluorescence (PLIF) imaging. Studied in particular are laser-induced damage thresholds (LIDTs), nonlinear absorption, and optical transmission stability during long-term UV irradiation. Solarization (photodegradation) effects are significantly enhanced when the fiber is exposed to high-repetition-rate, 283 nm UV irradiation. For 10 kHz laser pulses, two-photon absorption is strong and LIDTs are low, as compared to those of laser pulses propagating at 10 Hz. The fiber characterization results are utilized to perform single-laser-shot, OH-PLIF imaging in pulsating turbulent flames with a laser that operates at 10 kHz. The nearly spatially uniform output beam that exits a long multimode fiber becomes ideal for PLIF measurements. The proof-of-concept measurements show significant promise for extending the application of a fiber-coupled, high-speed OH-PLIF system to harsh environments such as combustor test beds, and potential system improvements are suggested.

Direct measurements of collisionally broadened Raman linewidths of CO2 S-branch transitions.

We report direct measurements of S-branch Raman-coherence lifetimes of CO(2) resulting from CO(2)-CO(2) and CO(2)-N(2) collisions by employing time-resolved picosecond coherent anti-Stokes Raman scattering spectroscopy. The S-branch (ΔJ = +2) transitions of CO(2) with rotational quantum number J = 0-52 were simultaneously excited using a broadband (~5 nm) laser pulse with a full-width-at-half-maximum duration of ~115 ps. The coherence lifetimes of CO(2) for a pressure range of 0.05-1 atm were measured directly by probing the rotational coherence with a nearly transform-limited, 90-ps-long laser pulse. These directly measured Raman-coherence lifetimes, when converted to collisional linewidth broadening coefficients, differ from the previously reported broadening coefficients extracted from frequency-domain rotational Raman and infrared-absorption spectra and from theoretical calculations by 7%-25%.

Photolytic-interference-free, femtosecond two-photon fluorescence imaging of atomic hydrogen.

We discuss photolytic-interference-free, high-repetition-rate imaging of reaction intermediates in flames and plasmas using femtosecond (fs) multiphoton excitation. The high peak power of fs pulses enables efficient nonlinear excitation, while the low energy nearly eliminates interfering single-photon photodissociation processes. We demonstrate proof-of-principle, interference-free, two-photon laser-induced fluorescence line imaging of atomic hydrogen in hydrocarbon flames and discuss the method's implications for certain other atomic and molecular species.

Investigation of optical fibers for gas-phase, ultraviolet laser-induced-fluorescence (UV-LIF) spectroscopy.

We investigate the feasibility of transmitting high-power, ultraviolet (UV) laser pulses through long optical fibers for laser-induced-fluorescence (LIF) spectroscopy of the hydroxyl radical (OH) and nitric oxide (NO) in reacting and non-reacting flows. The fundamental transmission characteristics of nanosecond (ns)-duration laser pulses are studied at wavelengths of 283 nm (OH excitation) and 226 nm (NO excitation) for state-of-the-art, commercial UV-grade fibers. It is verified experimentally that selected fibers are capable of transmitting sufficient UV pulse energy for single-laser-shot LIF measurements. The homogeneous output-beam profile resulting from propagation through a long multimode fiber is ideal for two-dimensional planar-LIF (PLIF) imaging. A fiber-coupled UV-LIF system employing a 6 m long launch fiber is developed for probing OH and NO. Single-laser-shot OH- and NO-PLIF images are obtained in a premixed flame and in a room-temperature NO-seeded N(2) jet, respectively. Effects on LIF excitation lineshapes resulting from delivering intense UV laser pulses through long fibers are also investigated. Proof-of-concept measurements demonstrated in the current work show significant promise for fiber-coupled UV-LIF spectroscopy in harsh diagnostic environments such as gas-turbine test beds.

Laser-induced fluorescence detection of hydroxyl (OH) radical by femtosecond excitation.

The development of a laser-induced fluorescence detection scheme for probing combustion-relevant species using a high-repetition-rate ultrafast laser is described. A femtosecond laser system with a 1 kHz repetition rate is used to induce fluorescence, following two-photon excitation (TPE), from hydroxyl (OH) radicals that are present in premixed laminar flames. The experimental TPE and one-photon fluorescence spectra resulting from broadband excitation into the (0,0) band of the OH A(2)∑(+)-X(2)Π system are compared to simulated spectra. Additionally, the effects of non-transform-limited femtosecond pulses on TPE efficiency is investigated.

Point and planar ultraviolet excitation/detection of hydroxyl-radical laser-induced fluorescence through long optical fibers.

We demonstrate an all-fiber-coupled, UV, laser-induced-fluorescence (LIF) detection system of the hydroxyl radical (OH) in flames. The nanosecond-pulsed excitation of the (1,0) band of the OH A(2)∑(+)-X(2)Π system at ∼283 nm is followed by fluorescence detection from the (0,0) and (1,1) bands around 310 nm. The excitation-laser beam is delivered through a 400 µm core UV-grade optical fiber of up to 10 m in length, and the fluorescence signal collected is transmitted through a 1.5 mm core 3 m long fiber onto the remote detector. Single-laser-shot planar LIF (PLIF) imaging of OH in flames is also demonstrated using fiber-based excitation. The effects of delivering intense UV beams through long optical fibers are investigated, and the system improvements for an all-fiber-coupled OH-PLIF imaging system are discussed. Development of such fiber-based diagnostics and imaging systems constitutes a major step in transitioning laser diagnostic tools from research laboratories to reacting flow facilities of practical interest.

Gas-phase thermometry using delayed-probe-pulse picosecond coherent anti-Stokes Raman scattering spectra of H2.

We report the development and application of a simple theoretical model for extracting temperatures from picosecond-laser-based coherent anti-Stokes Raman scattering (CARS) spectra of H2 obtained using time-delayed probe pulses. This approach addresses the challenges associated with the effects of rotational-level-dependent decay lifetimes on time-delayed probing for CARS thermometry. A simple procedure is presented for accurate temperature determination based on a Boltzmann distribution using delayed-probe-pulse vibrational CARS spectra of H2; this procedure requires measurement at only a select handful of probe-pulse delays and requires no assumptions about sample environment.

Electronic-resonance-enhanced coherent anti-Stokes Raman scattering of nitric oxide: saturation and Stark effects.

A theoretical analysis of electronic-resonance-enhanced (ERE) coherent anti-Stokes Raman scattering (CARS) of NO is described. The time-dependent density-matrix equations for the nonlinear ERE-CARS process are derived and manipulated into a form suitable for direct numerical integration. In the ERE-CARS configuration considered in this paper, the pump and Stokes beams are far from electronic-resonance. The visible 532 and 591 nm laser beams are used to excite Q-branch Raman resonances in the vibrational bands of the X (2)Pi electronic state of NO. An ultraviolet probe beam at 236 nm is used to excite P-, Q-, or R-branch transitions in the (v'=0, v"=1) band of the A (2)Sigma(+)-X (2)Pi electronic system of NO molecule. Experimental spectra are obtained either by scanning the ultraviolet probe beam while keeping the Stokes frequency fixed (probe scans) or by scanning the Stokes frequency while keeping the probe frequency fixed (Stokes scans). The calculated NO ERE-CARS spectra are compared with experimental spectra, and good agreement is observed between theory and experiment in terms of spectral peak locations and relative intensities. The effects of saturation of the two-photon Raman-resonant Q-branch transitions, the saturation of a one-photon electronic-resonant P-, Q-, or R-branch transitions in the A (2)Sigma(+)-X (2)Pi electronic system, and the coupling of these saturation processes are investigated. The coupling of the saturation processes for the probe and Raman transitions is complex and exhibits behavior similar to that observed in the electromagnetic induced transparency process. The probe scan spectra are significantly affected by Stark broadening due to the interaction of the pump and Stokes radiation with single-photon resonances between the upper vibration-rotation probe level in the A (2)Sigma(+) electronic levels and vibration-rotation levels in higher lying electronic levels. The ERE-CARS signal intensity is found to be much less sensitive to variations in the collisional dephasing rates under saturation conditions.

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.

Comparison of nanosecond and picosecond excitation for interference-free two-photon laser-induced fluorescence detection of atomic hydrogen in flames.

Two-photon laser-induced fluorescence (TP-LIF) line imaging of atomic hydrogen was investigated in a series of premixed CH4/O2/N2, H2/O2, and H2/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< or =Phi< or =1.4, and in H2/O2 flames with 0.3< or =Phi< or =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 (Phi=1.64) CH4/O2/N2 flame and in H2/O2/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.