Femtosecond Two-photon Laser-induced Fluorescence Research Articles

Simultaneous single-shot imaging of H and O atoms in premixed turbulent flames using femtosecond two-photon laser-induced fluorescence.

A method based on femtosecond two-photon excitation has been developed for simultaneous visualization of interference-free fluorescence of H and O atoms in turbulent flames. This work shows pioneering results on single-shot simultaneous imaging of these radicals under non-stationary flame conditions. The fluorescence signal, showing the distribution of H and O radicals in premixed CH4/O2 flames was investigated for equivalence ratios ranging from ϕ = 0.8 to ϕ = 1.3. The images have been quantified through calibration measurements and indicate single-shot detection limits on the order of a few percent. Experimental profiles have also been compared with profiles from flame simulations, showing similar trends.

Temperature measurements in heated gases and flames using carbon monoxide femtosecond two-photon laser-induced fluorescence

Temperature measurements in heated gases and flames using carbon monoxide femtosecond two-photon laser-induced fluorescence

Temperature Measurements in Heated Gases and Flames Using Carbon Monoxide Femtosecond Two-Photon Laser-Induced Fluorescence

Temperature Measurements in Heated Gases and Flames Using Carbon Monoxide Femtosecond Two-Photon Laser-Induced Fluorescence

Femtosecond two-photon laser-induced fluorescence imaging of atomic hydrogen in a laminar methane–air flame assisted by nanosecond repetitively pulsed discharges

Sustainable and low-emission combustion is in need of novel schemes to enhance combustion efficiency and control to meet up with new emission standards and comply with varying quality of renewable fuels. Plasma actuation is a promising candidate to achieve this goal but few detailed experiments have been carried out that target how specific combustion and plasma related species are affected by the coupling of plasma and combustion chemistry. Atomic hydrogen is such a species that here is imaged by using the two-photon absorption laser induced fluorescence (TALIF) technique as an atmospheric pressure methane–air flame is actuated by nanosecond repetitively pulsed (NRP) discharges. Atomic hydrogen is observed both in the flame and in the discharge channel and plasma actuation results in a wide modification of the flame shape. A local 50% increase of fluorescence occurs at the flame front where it is crossed by the discharge. Atomic hydrogen in the discharge channel in the fresh-gases is found to decay with a time constant of about 2.4 μs. These results provide new insights on the plasma flame interaction at atmospheric pressure that can be further used for cross-validation of numerical calculations.

Pressure-scaling characteristics of femtosecond two-photon laser-induced fluorescence of carbon monoxide.

Broadband femtosecond (fs) two-photon laser-induced fluorescence (TP-LIF) of the B1Σ+←X1Σ+, Hopfield-Birge system of carbon monoxide (CO) is believed to have two major advantages compared to narrowband nanosecond excitation. It should (i) minimize the effects of pressure-dependent absorption line broadening and shifting, and (ii) produce pressure-independent TP-LIF signals as the effect of increased quenching due to molecular collisions is offset by the increase in number density. However, there is an observed nonlinear drop in the CO TP-LIF signal with increasing pressure. In this work, we systematically investigate the relative impact of potential deexcitation mechanisms, including collisional quenching, forward lasing, attenuation of the source laser by the test cell windows or by the gas media, and a 2+1 photoionization process. As expected, line broadening and collisional quenching play minor roles in the pressure-scaling behavior, but the CO fs TP-LIF signals deviate from theory primarily because of two major reasons. First, attenuation of the excitation laser at high pressures significantly reduces the laser irradiance available at the probe volume. Second, a 2+1 photoionization process becomes significant as the number density increases with pressure and acts as a major deexcitation pathway. This work summarizes the phenomena and strategies that need to be considered for performing CO fs TP-LIF at high pressures.

Instantaneous one-dimensional ammonia measurements with femtosecond two-photon laser-induced fluorescence (fs-TPLIF)

Ammonia (NH3) has been identified as a potential hydrogen-carrier fuel with no carbon emissions. Non-intrusive in-situ NH3 diagnostic technique is of great interest. In this work, femtosecond two-photon laser-induced fluorescence (fs-TPLIF) was demonstrated in NH3/N2 mixtures to achieve NH3 measurements. A femtosecond laser at 305 nm was used for two-photon excitation of NH3 to its excited state (X–C′), and the subsequent fluorescence at ~565 nm from transition C′-A was detected. In addition, a detection limit of 730 ppm was achieved in NH3/N2 mixtures. Furthermore, one-dimensional single-shot images of NH3 were obtained in both laminar and turbulent flow fields. This work is the first attempt of fs-TPLIF for polyatomic molecular gases measurements, and the obtained results indicate that fs-TPLIF could be a promising tool for NH3 measurements.

Ammonia Measurements with Femtosecond Two-Photon Laser-Induced Fluorescence in Premixed NH3/Air Flames

Ammonia (NH3), which can be a hydrogen carrier, is a promising alternative to fossil fuels in the future carbon-free economy. In situ techniques feasible for the remote and non-intrusive detection of NH3 will provide strong support for developing clean NH3 combustion. Here, we demonstrated a femtosecond two-photon laser-induced fluorescence (fs-TPLIF) technique for interference-free in situ NH3 measurements in laminar premixed NH3/air flames. The two-head band of NH3 at ∼565 nm was observed, which verifies the feasibility of fs-TPLIF for NH3 measurements in a combustion environment. The single-shot NH3 fs-TPLIF images with efficient signal-to-noise ratios were obtained. The variation of the thickness of the reaction zone with the equivalence ratio of NH3 flames was also obtained. As a result of the broad line width of the femtosecond laser, the OH fluorescence was also observed together with the NH3 fluorescence. The potential of fs-TPLIF for simultaneous measurements of NH3 and OH with only one laser was analyzed. The laser power dependence of NH3 and NH emissions was investigated. The radial distributions of NH3, NH, and OH in the flame were also discussed. This work is the first attempt of fs-TPLIF for NH3 measurements in a combustion environment, and the results indicate that fs-TPLIF is a feasible tool for NH3 measurements in combustion diagnostics. (Less)

Quantitative femtosecond, two-photon laser-induced fluorescence of atomic oxygen in high-pressure flames.

Quantitative femtosecond two-photon laser-induced fluorescence of atomic oxygen was demonstrated in an H2/air flame at pressures up to 10atm. Femtosecond excitation at 226.1nm was used to pump the 3pP3J'=0,1,2←←2pP3J''=0,1,2 electronic transition of atomic oxygen. Contributions from multiphoton de-excitation, production of atomic oxygen, and photolytic interferences were investigated and minimized by limiting the laser irradiance to ∼1011 W/cm2. Quantitative agreement was achieved with the theoretical equilibrium mole fraction of atomic oxygen over a wide range of fuel-air ratios and pressures in an H2/air laminar calibration burner.

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.

Detection of carbon monoxide (CO) in sooting hydrocarbon flames using femtosecond two-photon laser-induced fluorescence (fs-TPLIF)

Ultrashort-pulse, femtosecond (fs)-duration, two-photon laser-induced fluorescence (fs-TPLIF) measurements of carbon monoxide (CO) are reported in rich, sooting hydrocarbon flames. CO-TPLIF detection using conventional nanosecond or picosecond lasers are often plagued by photochemical interferences, specifically under fuel-rich flames conditions. In the current study, we investigate the commonly used CO two-photon excitation scheme of the B1Σ+ ← X1Σ+ electronic transition, using approximately 100-fs-duration excitation pulses. Fluorescence emission was observed in the Angstrom band originating from directly populated B1Σ+ upper state, as well as, in the third positive band from collisionally populated b3Σ+ upper state. The current work was focused on the Angstrom band emission. Interference from nascent C2 emissions originating from hot soot particles in the flame could be reduced to a negligible level using a narrower detection gate width. In contrast, avoiding interferences from laser-generated C2 Swan-band emissions required specific narrowband spectral filtering in sooting flame conditions. The observed less than quadratic laser pulse energy dependence of the TPLIF signal suggests the presence of strong three-photon ionization and stimulated emission processes. In a range of CH4/air and C2H4/air premixed flames investigated, the measured CO fluorescence signals agree well with the calculated equilibrium CO number densities. Reduced-interference CO-TPLIF imaging in premixed C2H4/O2/N2 jet flames is also reported.

Comprehensive CO detection in flames using femtosecond two-photon laser-induced fluorescence

We demonstrate a femtosecond two-photon laser-induced fluorescence (fs-TPLIF) technique for sensitive CO detection, using a 230 nm pulse of 9 µJ and 45 fs. The advantages of fs-TPLIF in excitation of molecular species were analyzed. Spectra of CO fs-TPLIF were recorded in stable laminar flames spatially resolved across the flame front. A hot band (1, n) together with the conventional band (0, n) of the B→A transitions were observed in the burned zone and attributed to the broadband nature of the fs excitation. The CO fs-TPLIF signal recorded across the focal point of the excitation beam shows a relatively flat intensity distribution despite of the steep laser intensity variation, which is beneficial for CO imaging in contrast to nanosecond and picosecond TPLIF. This phenomenon can be explained by photoionization, which over the short pulse duration dominates the population depletion of the excited B state due to the high peak power, but only contributes in total a negligible X state depletion due to the low pulse energy. Single-shot CO fs-TPLIF images in methane/air flames were recorded by imaging the broadband fluorescence. The results indicate that fs-TPLIF is a promising tool for CO imaging in flames.

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.

Minor-species structure of premixed cellular tubular flames

Quantitative spatially resolved measurements of atomic hydrogen and hydroxyl radicals are reported of cellular phenomena in lean laminar premixed hydrogen–air tubular flames. Femtosecond two-photon laser-induced fluorescence (fs-TPLIF) enables photolytic-interference-free measurement of H atoms. Quenching corrections are calculated from previously measured temperature and major-species concentrations. In the sub-unity Lewis number, highly stretched and curved premixed flame structure, the strong effect of thermal-diffusive imbalance is observed through clear local extinction (dearth of H atoms) and highly curved reaction cells. Peak H-atom number densities of 5*1015cm–3 and peak OH number densities of 9*1015cm−3 are found but remain approximately the same value despite doubling the flame stretch from 200 to 400s–1. Comparisons to non-cellular tubular flame numerical predictions show that the cellular transition increases temperature and local equivalence ratio but lowers peak number densities of H and OH. For cellular instabilities in the tubular flame, the thermal-diffusive imbalance maintains a similar local flame structure (i.e., same curvature and peak values of H, OH, T, and local equivalence ratio) that is insensitive to stretch rate.

Quantitative atomic hydrogen measurements in premixed hydrogen tubular flames

Quantitative measurements of atomic hydrogen are reported in laminar premixed tubular flames using femtosecond two-photon laser-induced fluorescence. The H-atom fluorescence is corrected for collisional quenching by using local values of major-species concentrations and temperature measured by spontaneous Raman scattering. Lean hydrogen flames are sustained with two different diluents (N2, CO2) to investigate low–Lewis number flames under high curvature. When compared to planar stretched flames, the curved tubular flames enhance the H-atom concentration and temperature through increased preferential diffusion. Peak H-atom number densities on the order of 1015 per cm3 are measured, and absolute H-atom profiles show differences up to 40% in peak number density and flame radial position when compared to the pseudo one-dimensional flame model with detailed chemistry and transport. Although the overall agreement in absolute H-atom profiles is “good” considering the relative uncertainties in the model and experiment, the differences suggest the ability for this flame geometry to provide evidence for revision of molecular transport and chemical kinetic modeling in flames with substantial preferential diffusion. Peak absolute H-atom concentrations vary up to 30% depending on the assumed temperature dependency for the collisional quenching factors pointing to the need for high-temperature data for H-atom collisional quenching. Relative H-atom profiles in the flames are minimally affected by the collisional quenching.