Spectral Investigations of Fluorescence Tracers in Automotive and Aviation Fuels under Cryogenic Conditions.

This study investigated spectral laser-induced fluorescence signals of dyes in fuels for automotive and aerospace applications under low temperatures and cryogenic conditions down to 183 K. For this purpose, a fluorescence chamber was developed based on cooling with liquid nitrogen. The design enabled a minimal inner chamber temperature of 153 K. Furthermore, the applicability of two-color LIF for liquid thermometry was evaluated under these conditions. The temperature determination was based on the temperature-sensitive fluorescence intensity ratio of the special dyes doped into the fuels determined in suitable spectral regions, which represented common bandpass filters. For this purpose, the fluorescence signals of the dye doped into the gasoline and jet fuel surrogate isooctane were tested as well as blends of isooctane and the ethanol biofuels E20 (comprising 80 vol.% isooctane and 20 vol.% ethanol), E40, and E100. Additionally, a realistic multi-component fuel Jet A-1 mixed with a suitable fluorescence dye was investigated. E100 was doped with Eosin-Y, and the remaining fuels were doped with Nile red. Temperature-dependent spectral LIF intensities were recorded in the range of 183 K-293 K, which simulate extreme environments for aerospace and automotive applications. Frozen fuel-dye mixtures cause significant extinction effects and prevent sufficient signal detection at low and cryogenic temperatures, defining the detection limit. A temperature decrease led to a spectral shift in the emission peaks of E100 doped with Eosin-Y toward shorter wavelengths, while the spectra of mixtures doped with Nile red were shifted toward longer wavelengths. The suggested bandpass filters produced the temperature-sensitive intensity ratio (the average over the temperature interval) of the dyes with the largest sensitivity for Jet A-1 (5.2%/K), followed by E100 (4.95%/K), E40 (4.07%/K), E20 (3.23%/K), and isooctane (3.07%/K), even at cryogenic temperatures.

Polarization-dependent LIF/Mie ratio for sizing of micrometric ethanol droplets doped with Nile red.

The present study deals with droplet sizing based on laser-induced fluorescence (LIF) and Mie scattering for varied polarization of the utilized laser (parallel or perpendicular). The polarization-dependent LIF/Mie ratio is studied for micrometric droplets (25-60 µm) produced with a droplet generator. The investigations were carried out with the dye Nile red dissolved in ethanol and ethanol/iso-octane mixtures. A spectral absorption and fluorescence characterization at various dye and ethanol concentrations is carried out in a cuvette in order to identify reabsorption effects. The LIF|| droplet images (index ||: parallel polarization) show a more homogeneous intensity distribution in the droplets and slightly stronger morphology-dependent resonances (MDRs) in comparison to LIF⊥ (index ⊥: perpendicular polarization). The spectral LIF emissions reveal a dependence of the MDR on the ethanol admixture. The larger the ethanol content, the lower the MDR peak, which is also shifted further to the red part of the spectrum. The Mie droplet signal images are mainly characterized by two distinct glare points, one at the entrance of the laser light (reflection) and one at the exit (first-order refraction). The Mie⊥ images show a more pronounced entrance glare point, in comparison to Mie||, where the exit glare point is more pronounced. These observations are in accordance with the theory. The calibration curve of the micro droplet signals revealed a volumetric trend of the LIF signals and a slightly higher LIF⊥ signal and sensitivity in comparison to LIF||. The signal Mie⊥ follows roughly a quadratic trend on average, while Mie|| follows a linear trend. Consequently, the calculated LIF⊥/Mie⊥ ratio shows a linear trend, whereas the LIF||/Mie|| ratio shows a quadratic trend, which confirms theoretical calculations. A numerical simulation of the Mie signal at various detection angles shows a good agreement with the experimental data at large apertures.

Characterization of Fluorescence Tracers for Thermometry and Film Thickness Measurements in Liquid Coolants Relevant for Thermal Management of Electric and Electronic Components.

This study investigated a novel two-color LIF (laser-induced fluorescence) technique for thermometry in coolants relevant for electric components. In principle, this diagnostic enables thermometry in liquid flows but also a simultaneous determination of film thickness and film temperature, which is relevant, e.g., for jet impingement cooled electric components. Temperature measurements are based on a temperature-sensitive intensity ratio of special tracers realized by suitable band pass filters within the respective emission spectra. For this purpose, the heat transfer fluids Fragoltherm F12, Marlotherm LH, and a water-glycol mixture WG20 (80 vol.% water, 20 vol.% glycol) and its individual components were doped with suitable tracers. The tracer Eosin-Y was utilized for polar coolants (water, WG20, and glycol) and Nile red was utilized for non-polar solvents (Fragoltherm F12 and Marlotherm LH). The spectral LIF intensities were recorded for a wide range of temperatures (253-393 K), which are relevant for cooling of electric motors, batteries, and power electronics. Furthermore, absorption spectra were analyzed as well. The temperature-dependent fluorescence measurements revealed different behavior for the polar and non-polar solvents. A temperature increase in the polar solvents (water, WG20, glycol) led to a spectral shift of the emission peaks of Eosin-Y towards longer wavelengths (red-shifted), while the peaks of Nile red in the non-polar solvents (Fragoltherm F12 and Marlotherm LH) showed an opposite behavior and were blue-shifted. The highest average temperature sensitivity was achieved for Marlotherm LH (4.22%/K), followed by glycol (1.99%/K), WG20 (1.80%/K), water (1.62%/K), and Fragoltherm F12 (1.12%/K). These sensitivities are similar to or even much higher than the literature data of other LIF tracers, which were, however, not determined in those coolants. Consequently, the two novel proposed dyes for the studied heat transfer liquids enable a reliable temperature determination.

Morphology-dependent resonances in laser-induced fluorescence images of micrometric gasoline/ethanol droplets utilizing the dye nile red.

The present study deals with the solvent-dependent morphology-dependent resonances (MDR) in the laser-induced fluorescence (LIF) signal of monodisperse gasoline droplets (30 µm-60 µm) generated with a droplet generator. To investigate the influence of an ethanol addition to gasoline and the respective LIF signal of the dye nile red dissolved in these fuel blends, a reference gasoline fuel is blended with various ethanol concentrations from E0 (gasoline) to E100 (pure ethanol). A spectral fluorescence characterization of the investigated fuel mixtures at various concentrations is carried out in a micro cell in order to identify the dye and ethanol concentration influence of the respective fuel mixtures. The absorption and emission spectra of the fuel mixtures show a Stokes shift with increasing ethanol concentration towards larger wavelengths. The coefficient of variation (COV) of the fluorescence signals of spherical droplets was utilized to characterize the MDR effects within the droplet LIF images. The investigations revealed an increase of MDR contribution in terms of the COV of LIF signals with larger droplet diameters. For small droplets, no monotonic trend was found for contribution of MDR in the LIF signal as a function of the ethanol concentration. For larger droplets (e.g., 50 µm-60 µm), a lower contribution of MDR in LIF signals was observed with increasing ethanol content. For E80 and most of the studied ethanol blends, the normalized integrated COV values exhibited maxima at certain droplet sizes (40 µm, 47.5 µm, and 55 µm), which indicate the presence of distinct MDR effects.

Characterization of fuel/water mixtures and emulsions with ethanol using laser-induced fluorescence.

In charged spark-ignition engines, additional water injection allows for the reduction of temperature under stoichiometric mixture conditions. However, a higher complexity of the injection and combustion processes is introduced when a mixture of fuel and water ("emulsion") is injected directly into the combustion chamber using the same injector. For this purpose, the mixture must be homogenized before injection so that a reproducible composition can be adjusted. In principle, gasoline and water are not miscible, and may form an unstable macro-emulsion during mixing. However, the addition of ethanol, which is a biofuel component that is admixed to gasoline, can improve the mixing and may lead to a stable micro-emulsion. For the assessment of the distribution of the water and fuel phases in the mixture, a novel imaging concept based on laser-induced fluorescence (LIF) is proposed. In a first spectroscopic study, a fluorescence dye for imaging of the water phase is selected and evaluated. The fluorescence spectra of the dye dissolved in pure water are investigated under varied conditions using a simplified pressure cell equipped with a stirrer. The study comprises effects of temperature, dye concentration, and photo-dissociation on fluorescence signals. In a second step, fuel is mixed with water (5 vol. % to 10 vol. %) containing the dye, and the water dispersion in the fuel is investigated in an imaging study. Additionally, the miscibility of fuel and water is studied for varying ethanol content, and the homogeneity of the mixture is determined. These first investigations are also essential for the assessment of the potential of the LIF technique for studying the distribution of the water phase in internal combustion engine injection systems and sprays.

A Novel Approach for Measurement of Composition and Temperature of N-Decane/Butanol Blends Using Two-Color Laser-Induced Fluorescence of Nile Red.

In this work, the possibility of using a two-color LIF (laser-induced fluorescence) approach for fuel composition and temperature measurements using nile red dissolved in n-decane/butanol blends is investigated. The studies were conducted in a specially designed micro cell enabling the detection of the spectral LIF intensities over a wide range of temperatures (283-423 K) and butanol concentrations (0-100 vol.%) in mixtures with n-decane. Furthermore, absorption spectra were analyzed for these fuel mixtures. At constant temperature, the absorption and LIF signals exhibit a large spectral shift toward higher wavelengths with increasing butanol concentration. Based on this fact, a two-color detection approach is proposed that enables the determination of the butanol concentration. This is reasonable when temperature changes and evaporation effects accompanied with dye enrichment can be neglected. For n-decane, no spectral shift and broadening of the spectrum are observed for various temperatures. However, for butanol admixture, two-color thermometry is possible as long as the dye and butanol concentrations are kept constant. For example, the LIF spectrum shows a distinct broadening for B20 (i.e., 80 vol.% n-decane, 20 vol.% butanol) and a shift of the peak toward lower wavelengths of about 40 nm for temperature variations of 140 K.

Fluorescence Spectroscopy for Studying Evaporating Droplets Using the Dye Eosin-Y.

Laser-induced fluorescence (LIF) spectroscopy using dyes is frequently applied for characterization of liquids and two-phase flows. The technique is utilized e.g., for mixing studies, thermometry, or droplet sizing. One major application of the LIF technique combined with Mie-scattering is the planar measurement of droplet sizes in spray systems. However, its uncertainty is determined, among others, by varying dye concentration and temperature changes occurring during mixing and droplet evaporation. Systematic experimental investigations are necessary to determine the influence of dye enrichment effects on the LIF-signal of single droplets. For these investigations, the fluorescence dye Eosin-Y is dissolved in water and ethanol, which are typical solvents and working fluids in bio-medical applications and power engineering. A photo-physical characterization of the mixtures under various conditions was conducted using a spectrometric LIF setup and a micro cell. For ethanol, a small temperature dependency of the Eosin-Y LIF signal is observed up to 373 K. Photo-dissociation of Eosin-Y is negligible for solution in ethanol while it is distinct in water. The LIF signals of the single droplets are studied with an acoustic levitator. Effects of droplet evaporation, droplet deformation and varying dye concentration on the LIF-signal are studied. The single droplet measurements revealed a complex change of the fluorescence signal with reduced droplet size. This is due to droplet deformations leading to variations in the internal illumination field as well as dye enrichment during evaporation.

3D mapping of droplet Sauter mean diameter in sprays.

In this study, we report on the three-dimensional (3D) characterization of a spray in terms of its droplet Sauter mean diameter (SMD) using the laser-induced fluorescence (LIF)/Mie ratio technique. The spray structure is analyzed for a multi-hole direct-injection spark ignition (DISI) injector. A calibration curve to convert the LIF/Mie ratio to droplet diameter is deduced using LIF/Mie imaging and analysis of single droplets generated by a droplet generator. The DISI spray investigated here is optically sectioned by means of two-phase structured laser illumination planar imaging to suppress the intensity of multiple light scattering from LIF and Mie images prior to their ratio. A series of calibrated LIF/Mie ratio images of spray is then recorded at several depths along the z direction following the light sheet scanning of the spray. The droplet SMD ranges from less than 5 µm up to a maximum of 50 µm in single-shot images. The averaged SMD results (1-30 µm) obtained by using the calibration curve from the droplet generator are compared with measurement results from phase-Doppler anemometry. Finally, a 3D map is reconstructed from the successive 2D layers generated from spray scanning. The resulting 3D representation of the droplet SMD shows a non-symmetric spray structure produced by the studied multi-hole injector, which cannot be resolved by analyzing only one central plane.

Characterization of Nile Red as a Tracer for Laser-Induced Fluorescence Spectroscopy of Gasoline and Kerosene and Their Mixture with Biofuels.

Suitable fluorescence tracers ("dyes") are needed for the planar measurement of droplet sizes by using a combination of laser-induced fluorescence (LIF) and Mie scattering. Currently, no suitable tracers have been characterized for application in planar droplet sizing in gasoline and kerosene fuels, as well as biofuel blends. One promising tracer is nile red, which belongs to the fluorophore group. For its utilization for droplet size measurements, preliminary characterization of the fluorescence of the respective fuel tracer mixtures are mandatory. For this purpose, the fluorescence and absorption behavior of nile red dissolved in the surrogate fuels Toliso and Jet A-1 as well as in biofuel blends was investigated. The fluorescence signal for nile red that was dissolved in the two base fuels Toliso and Jet A-1 showed a linear behavior as a function of dye concentration. The temperature effect on spectral absorption and emission of nile red was investigated in a specially designed test cell. An ethanol admixture to Toliso led to a spectral shift towards higher wavelengths. The absorption and emission bands were shifted towards lower wavelengths with increasing temperature for all fuels. Both absorption and fluorescence decreased with increasing temperature for all fuels, except for E20, which showed an increased fluorescence signal with increasing temperature. Jet A-1 and its blends with hydroprocessed esters and fatty acids (HEFA) and farnesane did not exhibit explicit variations in spectral absorption or emission, but these blends showed a more distinct temperature dependence compared to the Toliso-ethanol-blends. The effect of photo-dissociation of the LIF signal of the fuel tracer mixtures was studied, and all fuel mixtures besides Toliso showed a more or less distinct decay in the fluorescence signal with time. In summary, all investigated fuel-tracer mixtures are suitable for LIF/Mie ratio droplet sizing in combination with nile red at moderate temperatures and low evaporation cooling rates.

Analysis of LIF and Mie signals from single micrometric droplets for instantaneous droplet sizing in sprays.

Planar droplet sizing (PDS) is a technique relying on the assumption that laser-induced fluorescence (LIF) and Mie scattering optical signals from spherical droplets depend on their volume and surface area, respectively. In this article, we verify the validity of this assumption by experimentally analyzing the light intensity of the LIF and Mie optical signals from micrometric droplets as a function of their diameter. The size of the droplets is controlled using a new flow-focusing monodisperse droplet generator capable of producing droplets of the desired size in the range of 21 µm to 60 µm. Ethanol droplets doped with eosin dye and excited at 532 nm are considered in this study, and the individual droplets were imaged simultaneously at microscopic and macroscopic scale. The effects of laser power, dye concentration, and temperature variation are systematically studied as a function of LIF/Mie ratio in the whole range of droplet sizes. Finally, a calibration curve at tracer concentration of 0.5 vol% is deduced and used to extract the droplet Sauter mean diameter (SMD) from instantaneous images of a transient ethanol spray. This droplet size mapping is done using structured laser illumination planar imaging (SLIPI), in order to suppress the artifacts induced by multiple light scattering.

Two-phase SLIPI for instantaneous LIF and Mie imaging of transient fuel sprays.

We report in this Letter a two-phase structured laser illumination planar imaging [two-pulse SLIPI (2p-SLIPI)] optical setup where the "lines structure" is spatially shifted by exploiting the birefringence property of a calcite crystal. By using this optical component and two cross-polarized laser pulses, the shift of the modulated pattern is not "time-limited" anymore. Consequently, two sub-images with spatially mismatched phases can be recorded within a few hundred of nanoseconds only, freezing the motion of the illuminated transient flow. In comparison with previous setups for instantaneous imaging based on structured illumination, the current optical design presents the advantage of having a single optical path, greatly simplifying its complexity. Due to its virtue of suppressing the effects from multiple light scattering, the 2p-SLIPI technique is applied here in an optically dense multi-jet direct-injection spark-ignition (DISI) ethanol spray. The fast formation of polydispersed droplets and appearance of voids after fuel injection are investigated by simultaneous detection of Mie scattering and liquid laser-induced fluorescence. The results allow for significantly improved analysis of the spray structure.