Theoretical modeling of single-laser-shot, chirped-probe-pulse femtosecond coherent anti-Stokes Raman scattering thermometry

Chirped-probe-pulse (CPP) femtosecond (fs) coherent anti-Stokes Raman scattering (CARS) spectroscopy for single-laser-shot temperature measurements in flames is discussed. In CPP fs CARS, a giant Raman coherence is created in the medium by impulsive pump-Stokes excitation, and the temperature-dependent temporal decay of this initial coherence is mapped into the frequency of the CARS signal using a CPP. The theory of the CPP fs CARS technique is presented. A computer code has been developed to calculate theoretical CPP fs CARS spectra. The input parameters for the calculation of the theoretical spectra include the temperature, probe time delay, ratio of the resonant and nonresonant susceptibilities, and parameters for characterizing the pump, Stokes and probe pulses. The parameters for characterizing the pump, Stokes and probe pulses are determined from the best fit of theoretical spectra to experimental spectra acquired from calibration flames at a known temperature. For spectra acquired in subsequent measurements, these laser parameters are fixed and temperature is determined as one of the fit parameters from the best fit of theoretical spectra to experimental spectra. For single-laser-shot CPP fs CARS temperature measurements performed in steady, near-adiabatic flames, the best-fit temperature distribution width is typically less than 1.5% of the mean temperature. The mean temperature is accurate to within approximately 3% with respect to the adiabatic flame temperature. The most significant limitation on temperature measurement accuracy is associated with the evaluation of the theoretical laser parameters. Significant improvements in the temperature measurement accuracy are expected once monitoring equipment capable of characterizing the spectrum and phase of each laser pulse is incorporated in the experiments.     

Femtosecond two-photon LIF imaging of atomic species using a frequency-quadrupled Ti:sapphire laser

Femtosecond (fs)-duration laser pulses are well suited for two-photon laser-induced-fluorescence (TPLIF) imaging of key atomic species such as H, N, and O in gas-phase reacting flows. Ultrashort pulses enable efficient nonlinear excitation, while reducing interfering photochemical processes. Furthermore, amplified fs lasers enable high-repetition-rate imaging (typically 1–10 kHz) for capturing the dynamics of turbulent flow fields. However, two-dimensional (2D), single-laser-shot fs-TPLIF imaging of the above species is challenging in most practical flow fields because of the limited ultraviolet pulse energy available in commercial optical parametric amplifier (OPA)-based tunable laser sources. In this work, we report the development of an efficient, fs frequency-quadrupling unit [i.e., fourth-harmonic generator (FHG)] with overall conversion efficiency more than six times greater than that of commercial OPA-based systems. The development, characterization, and application of the fs-FHG system for 2D imaging of H atoms in flames are described in detail. The potential application of the same laser system for 2D imaging of N and O atoms is also discussed.     

Simultaneous high-speed measurement of temperature and lifetime-corrected OH laser-induced fluorescence in unsteady flames

A means of performing simultaneous, high-speed measurements of temperature and OH lifetime-corrected laser-induced fluorescence (LIF) for tracking unsteady flames has been developed and demonstrated. The system uses the frequency-doubled and frequency-tripled output beams of an 80 MHz mode-locked Ti:sapphire laser to achieve ultrashort laser pulses (order 2 ps) for Rayleigh-scattering thermometry at 460 nm and lifetime-corrected OH LIF at 306.5 nm, respectively. Simultaneous, high-speed measurements of temperature and OH number density enable studies of flame chemistry, heat release, and flame extinction in unsteady, strained flames where the local fluorescence-quenching environment is unknown.     

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.     

Compact, 1.5 mJ, 450 MHz, CdSiP2 picosecond optical parametric oscillator near 6.3 μm

We report a compact, efficient, high-energy, and high-repetition-rate mid-IR picosecond optical parametric oscillator (OPO) based on the new nonlinear material CdSiP(2) (CSP). The OPO is synchronously pumped by a master oscillator power amplifier system at 1064.1 nm, providing 1 μs long macropulses constituting 8.6 ps micropulses at 450 MHz, and it can be tuned over 486 nm across 6091-6577 nm, covering the technologically important wavelength range for surgical applications. Using a compact (～30 cm) cavity and improved, high-quality nonlinear crystal, idler macropulse energy as high as 1.5 mJ has been obtained at 6275 nm at a photon conversion efficiency of 29.5%, with >1.2 mJ over more than 68% of the tuning range, for an input macropulse energy of 30 mJ. Both the signal and idler beams are recorded to have good beam quality with a Gaussian spatial profile, and the extracted signal pulses are measured to have durations of 10.6 ps. Further, from the experimentally measured transmission data at 1064 nm, we have estimated the two-photon absorption coefficient of CSP to be β=2.4 cm/GW, with a corresponding energy bandgap, E(g)=2.08 eV.     

Chirped-probe-pulse femtosecond CARS thermometry in turbulent spray flames

This paper presents temperature measurements in turbulent dilute and dense spray flames using single-laser-shot chirped-probe-pulse femtosecond coherent anti-Stokes Raman spectroscopy (CPP-fs-CARS). This ultrafast technique, with a repetition rate of 5 kHz, is applied to the piloted Sydney Needle Spray Burner (SYNSBURN^TM). The burner system features air-blast atomization of liquid injected from a needle that can be translated within a co-flowing air stream. The pilot-stabilized spray flames can range between the two extremes of dense and dilute by physically translating the needle tip relative to the burner's exit plane. The CPP-fs-CARS set-up has achieved integration times of 3 picoseconds (ps) as well as spatial resolution of approximately 800 µm along beam propagation and 60 µm in the transverse dimension. Brief details of the technique, calibration, correction of interferences, and spectral fitting processes are presented along with estimates of the associated error. The measurements are compared against well-established, line Raman–Rayleigh data for temperature collected in a turbulent CH₄/air jet diffusion flame, which is largely non-sooting. At peak gaseous flame temperatures of up to 2512 K, the relative accuracy and precision were 2.8% and ±3.4%, respectively. Measurements in turbulent spray flames are shown after applying the relevant corrections based on non-resonant background (NRB) behavior and camera saturation effects on the shape of the CARS signal spectrum. Preliminary mapping of the temperature fields demonstrates the wealth of information available in this dataset which will provide insights into the spatio-temporal structure of spray flames once relevant statistical analysis is applied.     

Development of two-color laser system for high-resolution polarization spectroscopy measurements of atomic hydrogen

We have developed a high-spectral-resolution laser system for two-photon pump, polarization spectroscopy probe (TPP-PSP) measurements of atomic hydrogen in flames. In the TPP-PSP technique, a 243-nm laser beam excites the two-photon 1S-2S transition, and excited n=2 atoms are then detected by polarization spectroscopy of the n=2 to n=3 transition using 656-nm laser radiation. The single-frequency-mode 243 and 656-nm beams are produced using injection-seeded optical parametric generators coupled with pulsed dye amplifiers. The use of single-mode lasers allows accurate measurement of signal line shapes and intensities even with significant pulse-to-pulse fluctuations in pulse energies. Use of single-mode lasers and introduction of a scheme to select nearly constant laser energies enable repeatable extraction of important spectral features in atomic hydrogen transitions.     

Nitric oxide concentration measurements in atmospheric pressure flames using electronic-resonance-enhanced coherent anti-Stokes Raman scattering

We report the application of electronic-resonance-enhanced coherent anti-Stokes Raman scattering (ERE-CARS) for measurements of nitric oxide concentration ([NO]) in three different atmospheric pressure flames. Visible pump (532 nm) and Stokes (591 nm) beams are used to probe the Q-branch of the Raman transition. A significant resonance enhancement is obtained by tuning an ultraviolet probe beam (236 nm) into resonance with specific rotational transitions in the (v’=0, v”=1) vibrational band of the A²Σ⁺–X²Π electronic system of NO. ERE-CARS spectra are recorded at various heights within a hydrogen-air flame producing relatively low concentrations of NO over a Hencken burner. Good agreement is obtained between NO ERE-CARS measurements and the results of flame computations using UNICORN, a two-dimensional flame code. Excellent agreement between measured and calculated NO spectra is also obtained when using a modified version of the Sandia CARSFT code for heavily sooting acetylene-air flames (φ=0.8 to φ=1.6) on the same Hencken burner. Finally, NO concentration profiles are measured using ERE-CARS in a laminar, counter-flow, non-premixed hydrogen-air flame. Spectral scans are recorded by probing the Q₁ (9.5), Q₁ (13.5) and Q₁ (17.5) Raman transitions. The measured shape of the [NO] profile is in good agreement with that predicted using the OPPDIF code, even without correcting for collisional effects. These comparisons between [NO] measurements and predictions establish the utility of ERE-CARS for detection of NO in flames with large temperature and concentration gradients as well as in sooting environments. PACS 07.88.+y; 42.62.Fi; 42.65.Dr     

Effects of O2–CO2 polarization beating on femtosecond coherent anti-Stokes Raman scattering (fs-CARS) spectroscopy of O2

Femtosecond coherent anti-Stokes Raman scattering (fs-CARS) spectroscopy has recently emerged as a promising laser-based temperature-measurement technique in flames. In fs-CARS, the broad spectral bandwidths of the pump and Stokes lasers permit the coupling of each ro-vibrational Raman transition via a large number of pump-Stokes photon pairs, creating a strong Raman coherence. However, the broad-bandwidth fs pulses also excite other molecular transitions that are in resonance. The polarization beating between these closely spaced Raman transitions can affect the coherence dephasing rate of the target molecule, making it difficult to extract accurate medium temperature. In a previous study our group investigated N₂/CO polarization beating in N₂ fs-CARS; in the present work we study O₂/CO₂ polarization beating in O₂ fs-CARS. O₂ fs-CARS can be particularly important for thermometry in non-air-breathing combustion in the absence of N₂. The effects of O₂/CO₂ polarization beating are investigated in the temperature range 300–900 K at atmospheric pressure and also at 300 K for pressures up to 10 bar. Unlike in the N₂/CO system, it was observed in the O₂/CO₂ system that the presence of CO₂ can significantly alter the time evolution of the Raman coherence and, hence, affect the measured temperature.     

Temperature measurements in reacting flows by time-resolved femtosecond coherent anti-Stokes Raman scattering (fs-CARS) spectroscopy

Time-resolved femtosecond coherent anti-Stokes Raman scattering (fs-CARS) spectroscopy of the nitrogen molecule is used for the measurement of temperature in atmospheric-pressure, near-adiabatic, hydrogen-air diffusion flames. The initial frequency-spread dephasing rate of the Raman coherence induced by the ultrafast (∼85 fs) Stokes and pump beams is used as a measure of gas-phase temperature. This initial frequency-spread dephasing rate of the Raman coherence is completely independent of collisions and depends only on the frequency spread of the Raman transitions at different temperatures. A simple theoretical model based on the assumption of impulsive excitation of Raman coherence is used to extract temperatures from time-resolved fs-CARS experimental signals. The extracted temperatures from fs-CARS signals are in excellent agreement with the theoretical temperatures calculated from an adiabatic equilibrium calculation. The estimated absolute accuracy and the precision of the measurement technique are found to be ±40 K and ±50 K, respectively, over the temperature range 1500-2500 K.     

Wavelength modulation absorption spectroscopy with 2 f detection using multiplexed diode lasers for rapid temperature measurements in gaseous flows

Multiplexed fiber-coupled diode lasers are used to probe second-harmonic line shapes of two near-infrared water absorption features, at 1343 nm and 1392 nm, in order to infer temperatures in gases containing water vapor, such as combustion flows. Wavelength modulation is performed at 170 kHz, and is superimposed on 1-kHz wavelength scans in order to recover full second-harmonic line shapes. Digital waveform generation and lock-in detection are performed using a data-acquisition card installed in a PC. An optimal selection of the modulation indices is shown to greatly simplify data interpretation over extended temperature ranges and to minimize the need for calibration when performing 2 f ratio thermometry. A theoretical discussion of this optimized strategy for 2 f ratio thermometry, as well as results from experimental validations in a heated cell, at pressures up to atmospheric, are presented in order to illustrate the utility of this technique for rapid temperature measurements in gaseous flow fields. PACS 42.62.Fi; 42.55.Px; 42.60.Fc; 39.30.+w     

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.     

Laser imaging system for determination of three-dimensional scalar gradients in turbulent flames

An imaging system for the measurement of three-dimensional (3D) scalar gradients in turbulent hydrocarbon flames is described. Combined line imaging of Raman scattering, Rayleigh scattering, and CO laser-induced fluorescence (LIF) allows for simultaneous single-shot line measurements of major species, temperature, mixture fraction, and a one-dimensional surrogate of scalar dissipation rate in hydrocarbon flames, while simultaneous use of two crossed, planar LIF measurements of OH allows for determination of instantaneous flame orientation. In this manner the full 3D scalar dissipation can be estimated in some regions of a turbulent flame on a single-shot basis.     

Development of rotational CARS for combustion diagnostics using a polarization approach

Rotational Coherent anti-Stokes Raman spectroscopy (CARS) has the last decades been developed into a useful tool for thermometry and concentration measurements in combustion. In this paper, we present a novel polarization approach of the technique, which will enhance its potential and widen the range of conditions at which it can be utilized. The theory of the polarization approach is described in detail. It is shown that by specific arrangement of the polarizations of the laser beams, total suppression of the non-resonant background signal can be obtained, and thus by probing only the resonant CARS signal the diagnostic utility of the technique increases. The main benefit of the approach is in situations where the non-resonant background signal is relatively high in comparison with the resonant signal. The high potential of polarization rotational CARS for thermometry is demonstrated in some illustrative examples, for example, nitrogen thermometry on the fuel side of diffusion flames, and carbon monoxide thermometry in the product gas of ethylene/oxygen/argon-flames.     

Saturated-absorption spectroscopy: eliminating crossover resonances by use of copropagating beams

We demonstrate a new technique for saturated-absorption spectroscopy by use of copropagating beams that does not have the problem of crossover resonances. The pump beam is locked to a transition, and its absorption signal is monitored while the probe beam is scanned. As the probe comes into resonance with another transition, the pump absorption is reduced and the signal shows a Doppler-free dip. We use this technique to measure hyperfine intervals in the D2 line of 85Rb with a precision of 70 kHz and to resolve hyperfine levels in the D2 line of 39K that are less than 10 MHz apart.     

Detection of trace nitric oxide concentrations using 1-D laser-induced fluorescence imaging

Spectrally resolved laser-induced fluorescence (LIF) with one-dimensional spatial imaging was investigated as a technique for detection of trace concentrations of nitric oxide (NO) in high-pressure flames. Experiments were performed in the burnt gases of premixed methane/argon/oxygen flames with seeded NO (15 to 50 ppm), pressures of 10 to 60 bar, and an equivalence ratio of 0.9. LIF signals were dispersed with a spectrometer and recorded on a 2-D intensified CCD array yielding both spectral resolution and 1-D spatial resolution. This method allows isolation of NO-LIF from interference signals due to alternative species (mainly hot O₂ and CO₂) while providing spatial resolution along the line of the excitation laser. A fast data analysis strategy was developed to enable pulse-by-pulse NO concentration measurements from these images. Statistical analyses as a function of laser energy of these single-shot data were used to determine the detection limits for NO concentration as well as the measurement precision. Extrapolating these results to pulse energies of ～?16 mJ/pulse yielded a predicted detection limit of ～?10 ppm for pressures up to 60 bar. Quantitative 1-D LIF measurements were performed in CH₄/air flames to validate capability for detection of nascent NO in flames at 10–60 bar.     

SBN:Cr晶体中孤子诱导的实时平面光波导及其导光特性分析

通过数值模拟和实验对SBN:Cr晶体中的（1+1）维亮屏蔽空间孤子及其诱导的实时平面光波导的导光特性进行了研究.采用分步束传播法和Petviashvili迭代法对（1+1）维亮屏蔽空间孤子的特性进行了模拟.通过求解本征方程,对孤子诱导平面波导中存在的导波模式进行了数值求解.采用633 nm的He-Ne激光作为孤子诱导光束,532 nm的半导体泵浦的固体激光作为探测光,在固液同成分的SBN:Cr晶体中进行了实验研究.实验结果和数值模拟的结果符合的很好.而且结果表明SBN:Cr晶体中红光诱导的波导可以作为实时光波导.     

Measurement of nitric oxide concentrations in flames by using electronic-resonance-enhanced coherent anti-Stokes Raman scattering

We have measured nitric oxide (NO) concentrations in flames by using electronic-resonance-enhanced coherent anti-Stokes Raman spectroscopy (ERE-CARS). Visible pump and Stokes beams were tuned to a Q-branch vibrational Raman resonance of NO. A UV probe beam was tuned into resonance with specific rotational transitions in the (v"=1,v'=0) vibrational band in the A(2)Sigma(+)-X(2)Pi electronic transition, thus providing a substantial electronic-resonance enhancement of the resulting CARS signal. NO concentrations were measured at levels down to 50 parts in 10(6) in H(2)/air flames at atmospheric pressure. NO was also detected in heavily sooting C(2)H(2)/air flames at atmospheric pressure with minimal background interference.     

CO Imaging in piloted liquid-spray flames using femtosecond two-photon LIF

Liquid-spray flames are encountered in many practical combustion devices such as gasoline direct injection and diesel engines, gas turbine combustors as well as industrial furnaces. As opposed to gaseous fuels, additional phase-change steps present in liquid sprays not only complicate the overall combustion process, but also make in-situ, laser-based combustion diagnostics challenging. In particular, the formation of carbon monoxide (CO) due to incomplete fuel-air mixing and partial oxidation becomes a major challenge. In this study, we apply femtosecond, two-photon laser-induced fluorescence (fs-TPLIF) to measure CO concentration in piloted liquid-spray flames, taking into account possible signal interferences in the 230.1-nm, B¹Σ⁺←X¹Σ⁺ excitation scheme. A modified, flat-flame McKenna burner fitted with a direct-injection high-efficiency nebulizer (DIHEN) was used to produce piloted liquid-methanol spray flames. Although single-laser-shot OH-PLIF images show the presence of strong turbulent interactions in the core region, shot-averaged OH-PLIF images indicate that near the nozzle-exit region, the primary reaction takes place in an annular region around the droplet cloud, in general. A detailed spectroscopic study reveals that the signal interference at 460?nm originating from the second-order scattering of the excitation laser, which becomes approximately an order of magnitude stronger than CO fluorescence spectral lines near the nozzle exit region. The specific spectral filtering scheme introduced in our recent work is proved to be capable of suppressing interferences primarily originating from C₂ Swan-band emissions. Two-dimensional CO maps along with OH-PLIF flame structure data provide key insights into the CO formation in piloted liquid-spray flames, while providing critical validation datasets for advanced computational models.