Correction procedure for a tomographic optical setup employing imaging fiber bundles and intensified cameras.

For reliable tomographic measurements the underlying 2D images from different viewing angles must be matched in terms of signal detection characteristics. Non-linearity effects introduced by intensified cameras and spatial intensity variations induced from inhomogeneous transmission of the optical setup can lead, if not corrected, to a biased tomographic reconstruction result. This paper presents a complete correction procedure consisting of a combination of a non-linearity and flatfield correction for a tomographic optical setup employing imaging fiber bundles and four intensified cameras. Influencing parameters on the camera non-linearity are investigated and discussed. The correction procedure is applied to 3D temperature measurements by two-color pyrometry and compared to results without correction. The present paper may serve as a guideline for an appropriate correction procedure for any type of measurement involving optical tomography and intensified cameras.

Light curves and colours of the ejecta from Dimorphos after the DART impact.

On 26 September 2022, the Double Asteroid Redirection Test (DART) spacecraft struck Dimorphos, a satellite of the asteroid 65803 Didymos1. Because it is a binary system, it is possible to determine how much the orbit of the satellite changed, as part of a test of what is necessary to deflect an asteroid that might threaten Earth with an impact. In nominal cases, pre-impact predictions of the orbital period reduction ranged from roughly 8.8 to 17 min (refs. 2,3). Here we report optical observations of Dimorphos before, during and after the impact, from a network of citizen scientists' telescopes across the world. We find a maximum brightening of 2.29 ± 0.14 mag on impact. Didymos fades back to its pre-impact brightness over the course of 23.7 ± 0.7 days. We estimate lower limits on the mass contained in the ejecta, which was 0.3-0.5% Dimorphos's mass depending on the dust size. We also observe a reddening of the ejecta on impact.

Single-pulse real-time billion-frames-per-second planar imaging of ultrafast nanoparticle-laser dynamics and temperature in flames.

Unburnt hydrocarbon flames produce soot, which is the second biggest contributor to global warming and harmful to human health. The state-of-the-art high-speed imaging techniques, developed to study non-repeatable turbulent flames, are limited to million-frames-per-second imaging rates, falling short in capturing the dynamics of critical species. Unfortunately, these techniques do not provide a complete picture of flame-laser interactions, important for understanding soot formation. Furthermore, thermal effects induced by multiple consecutive pulses modify the optical properties of soot nanoparticles, thus making single-pulse imaging essential. Here, we report single-shot laser-sheet compressed ultrafast photography (LS-CUP) for billion-frames-per-second planar imaging of flame-laser dynamics. We observed laser-induced incandescence, elastic light scattering, and fluorescence of soot precursors - polycyclic aromatic hydrocarbons (PAHs) in real-time using a single nanosecond laser pulse. The spatiotemporal maps of the PAHs emission, soot temperature, primary nanoparticle size, soot aggregate size, and the number of monomers, present strong experimental evidence in support of the theory and modeling of soot inception and growth mechanism in flames. LS-CUP represents a generic and indispensable tool that combines a portfolio of ultrafast combustion diagnostic techniques, covering the entire lifecycle of soot nanoparticles, for probing extremely short-lived (picoseconds to nanoseconds) species in the spatiotemporal domain in non-repeatable turbulent environments. Finally, LS-CUP's unparalleled capability of ultrafast wide-field temperature imaging in real-time is envisioned to unravel mysteries in modern physics such as hot plasma, sonoluminescence, and nuclear fusion.

Measurement of Secondary Structure Changes in Poly-L-lysine and Lysozyme during Acoustically Levitated Single Droplet Drying Experiments by In Situ Raman Spectroscopy.

Drying processes such as spray drying, as commonly used in the pharmaceutical industry to convert protein-based drugs into their particulate form, can lead to an irreversible loss of protein activity caused by protein secondary structure changes. Due to the nature of these processes (high droplet number, short drying time), an in situ investigation of the structural changes occurring during a real drying process is hardly possible. Therefore, an approach for the in situ investigation of the expected secondary structural changes during single droplet protein drying in an acoustic levitator by time-resolved Raman spectroscopy was developed and is demonstrated in this paper. For that purpose, a self-developed NIR-Raman sensor generates and detects the Raman signal from the levitated solution droplet. A mathematical spectral reconstruction by multiple Voigt functions is used to quantify the relative secondary structure changes occurring during the drying process. With the developed setup, it was possible to detect and quantify the relative secondary structure changes occurring during single droplet drying experiments for the two chosen model substances: poly-L-lysine, a homopolypeptide widely used as a protein mimic, and lysozyme. Throughout drying, an increase in the ß-sheet structure and a decrease in the other two structural elements, α-helix, and random coil, could be identified. In addition, it was observed that the degree of structural changes increased with increasing temperature.

Calibration-free imaging thermometry via two-line atomic fluorescence in combustion processes.

In this Letter, we demonstrate, for the first time (to the best of our knowledge), calibration-free imaging of full-frame temperature fields for particle-laden flames using two-line atomic fluorescence (TLAF) of indium. Measurements were carried out in laminar premixed flames with indium precursor aerosol added. The technique is based on the excitation of the 52P3/2 → 62S1/2 and 52P1/2 → 62S1/2 transitions of indium atoms and the detection of the subsequent fluorescence signals. To this end, the transitions were excited by scanning two narrowband external cavity diode lasers (ECDL) over the transition bandwidths. To achieve imaging thermometry, the excitation lasers were formed into a light sheet of 1.5 mm width and 24 mm height. Employing this setup on a laminar, premixed flat-flame burner, temperature distributions were measured for various air:fuel ratios of 0.7, 0.8, and 0.9. The presented results demonstrate the capability of the technique and encourage further developments, e.g., for its future use in flame synthesis of nanoparticles containing indium compounds.

In Situ Determination of Droplet and Nanoparticle Size Distributions in Spray Flame Synthesis by Wide-Angle Light Scattering (WALS).

The investigation of droplet and nanoparticle formation in spray flame synthesis requires sophisticated measurement techniques, as often both are present simultaneously. Here, wide-angle light scattering (WALS) was applied to determine droplet and nanoparticle size distributions in spray flames from a standardized liquid-fed burner setup. Solvents of pure ethanol and a mixture of ethanol and titanium isopropoxide, incepting nanoparticle synthesis, were investigated. A novel method for the evaluation of scattering data from droplets between 2 µm and 50 µm was successfully implemented. Applying this, we could reveal the development of a bimodal droplet size distribution for the solvent/precursor system, probably induced by droplet micro-explosions. To determine nanoparticle size distributions, an appropriate filter and the averaging of single-shot data were applied to ensure scattering from a significant amount of nanoparticles homogeneously distributed in the measurement volume. From the multivariate analysis of the scattering data, the presence of spherical particles and fractal aggregates was derived, which was confirmed by analysis of transmission electron microscopy images. Monte Carlo simulations allowed determining the distribution parameters for both morphological fractions in three heights above the burner. The results showed relatively wide size distributions, especially for the spherical fraction, and indicated an ongoing sintering, from fractal to spherical particles.

4D temperature measurements using tomographic two-color pyrometry.

This work presents a new approach for high-speed four-dimensional (3D + t) thermometry using only two high-speed cameras which are equipped with different band pass filters to capture thermal radiation signals at two narrow wavelength bands. With the help of a customized fiber bundle and a beam splitter, a total number of nine projections at each band were recorded, and the temperature distribution was evaluated by tomographic two-color pyrometry. In order to validate the effectiveness of this method, the 3D temperature distribution of a premixed steady flat flame was evaluated. The determined temperatures were compared to those of other studies, as well as to the results from inverse Abel transform and line-of-sight data. Further, the 3D temperature evolution of a weakly turbulent diffusion flame was observed at a repetition rate of 7.5 kHz. Such 4D temperature measurements are expected to be valuable in understanding turbulent combustion mechanisms especially of practical devices.

Application of FRAME for Simultaneous LIF and LII Imaging in Sooting Flames Using a Single Camera.

In this article, the application of the FRAME (Frequency Recognition Algorithm for Multiple Exposures) technique is presented for multi-species measurements in symmetric and asymmetric ethylene/air diffusion flames. Laminar Bunsen-type and swirled diffusion flames are investigated to gain a better understanding of sooting combustion. For this purpose, simultaneous imaging is conducted in terms of Laser-Induced Fluorescence (LIF) of Polycyclic Aromatic Hydrocarbons (PAH) and Laser-Induced Incandescence (LII) of soot particles. Subsequently, the approach is utilized for simultaneous imaging of hydroxyl (OH)-LIF and soot-LII. Here, the modulated LIF- and LII-signals are acquired together as a single sub-image-with a single exposure utilizing the full sensor size of a single camera. By employing the frequency-recognition algorithm on the single image, the LIF- and LII-signals are spectrally isolated-generating two individual LIF- and LII-images. The flame luminosity and out-of-focus light such as reflected surrounding laser light are detected as non-modulated signals in the unprocessed image. These unwanted signals are suppressed using the image post-processing, and, therefore, the image contrast of the two resulting images is improved. It is found that PAHs mainly exist in the inner region near the burner and are surrounded by soot. The majority of the OH is distributed on the outer edges of the flame-representing the reaction zone and soot-oxidation region of the flame.

Stability Analysis of the Fluorescent Tracer 1-Methylnaphthalene for IC Engine Applications by Supercontinuum Laser Absorption Spectroscopy.

1-methylnaphthalene (1-MN) is a widely used laser-induced fluorescence (LIF) tracer for planar imaging of mixture formation and temperature distributions in internal combustion (IC) engines. As the LIF measurement results can be biased by partial tracer oxidation, the conversion of 1-MN and the base fuel isooctane is analyzed in a calibration cell. First, measurements using supercontinuum laser absorption spectroscopy (SCLAS) are presented in order to quantify the conversion by detection of the produced H2O mole fraction. A single mode fiber (SMF) coupled setup is presented, with the fiber core acting as entrance slit of a Czerny-Turner spectrometer. Dependencies on residence time and global air-fuel ratio are presented at pressures up to 1.5 MPa and temperatures up to 900 K, at which distinct tracer and fuel consumption is observed. Signal loss due to intense beam steering was partially compensated using a self-stabilizing double-pass setup with a retroreflector.

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.

High-speed, inline measurement of protein activity and inactivation processes by supercontinuum attenuation spectroscopy.

Some proteins such as catalase and glutamate dehydrogenase (GDH) are very sensitive to external factors such as irradiation or heat, which may cause inactivation. Since proteins are used in a wide field of applications, the entire activity has to be ensured during the whole process. By default, activity is measured by invasive and offline activity assays. To avoid the need for a time-consuming offline analysis, we developed an optical high-speed measurement technique, which may form the basis for the non-invasive inline control of enzyme processes e.g. in the textile or food industry. The technique is based on attenuation spectroscopy using a supercontinuum laser source in combination with multivariate data analysis, in particular partial least squares regression (PLSR). For verification of the approach, samples treated by various stresses were analyzed in parallel by activity assays and our new method. Applying this technique, we were able to determine the activity in the turbid catalase samples after heat treatment, addition of guanidine-HCl or irradiation with UV light by applying partial least squares regression. Furthermore, we demonstrate that the combination of broadband attenuation spectroscopy and PLSR enables us to determine also the activity of GDH in clear solutions after heat treatment.

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.

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.

Temperature determination of superheated water vapor by rotational-vibrational Raman spectroscopy.

We present a novel non-invasive laser-based tool for tracer-free spatially resolved temperature measurement in superheated water vapor at atmospheric pressure. The technique exploits the temperature sensitivity of the rotational-vibrational Raman spectrum of the v1 stretching vibration. This Letter demonstrates the Raman sensor, its application to a steam gasification reactor, and four methods to analyze the Raman spectra in order to obtain the temperature: an equal intensity point approach, a pseudo-isosbestic point approach, and two approaches based on the reconstruction of the Raman band by Gaussian/Lorentzian profiles. The evaluated water vapor temperatures inside a reactor for plasma-assisted gasification are compared to data acquired by supercontinuum absorption spectroscopy.

Burst-mode OH/CH2O planar laser-induced fluorescence imaging of the heat release zone in an unsteady flame.

The paper presents simultaneous high-speed (7.5 kHz) planar laser-induced fluorescence (PLIF) of formaldehyde (CH2O) and the hydroxyl-radical (OH) for visualization of the flame structure and heat release zone in a non-premixed unsteady CH4/O2/N2 flame. For this purpose, a dye laser designed for high-speed operation is pumped by the second-harmonic 532 nm output of a Nd:YAG burst-mode laser to produce a tunable, 566 nm beam. After frequency doubling a high-energy kHz-rate narrowband pulse train of approximately 2.2 mJ/pulse at 283 nm is used for excitation of the OH radical. Simultaneously, CH2O is excited by the frequency-tripled output of the same Nd:YAG laser, providing a high-frequency pulse train over 10 ms in duration at high pulse energies (>100 mJ/pulse). The excitation energies enable signal-to-noise ratios (SNRs) of ~10 and ~60 for CH2O and OH PLIF, respectively, using a single high-speed intensified CMOS camera equipped with an image doubler. This allows sufficient SNR for investigation of the temporal evolution of the primary heat release zone and the local flame structure at kHz rates from the spatial overlap of the OH- and CH2O-PLIF signals.

Generation of high-energy, kilohertz-rate narrowband tunable ultraviolet pulses using a burst-mode dye laser system.

Typical commercial pulsed dye laser systems used in the generation of narrowband, tunable ultraviolet radiation for planar laser-induced fluorescence (PLIF) imaging are optimized for either high (∼5-10 kHz) repetition rates at comparatively low ultraviolet pulse energies (hundreds of microjoules) or high-output pulse energies (>10 mJ) at comparatively low repetition rates (∼10 Hz). In this work we use a frequency-doubled Nd:YAG burst-mode laser to pump a custom dye laser system for high pulse energies and repetition rates of 7.5, 10, and 20 kHz at 566 nm. The frequency-doubled output of over 2.2 mJ/pulse at 283 nm, which can be used for PLIF imaging of combustion radicals, is an order of magnitude higher per pulse energy as compared with continuously pulsed dye laser systems and is ∼3× higher in overall efficiency than a burst-mode optical parametric oscillator at similar wavelengths. The influence of repetition rate, pump energy, and dye concentration on the output conversion efficiency and pulse-to-pulse stability of the current system is discussed.

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.

High-speed combustion diagnostics in a rapid compression machine by broadband supercontinuum absorption spectroscopy.

The first results under fired internal combustion engine conditions based on a supercontinuum absorption spectrometer are presented and discussed. Temperature, pressure, and water mole fraction are inferred simultaneously from broadband H2O absorbance spectra ranging from 1340 nm to 1440 nm. The auto-ignition combustion process is monitored for two premixed n-heptane/air mixtures with 10 kHz in a rapid compression machine. Pressure and temperature levels during combustion exceed 65 bar and 1900 K, respectively. To allow for combustion measurements, the robustness of the spectrometer against beam steering has been improved compared to its previous version. Additionally, the detectable wavelength range has been extended further into the infrared region to allow for the acquisition of distinct high-temperature water transitions located in the P-branch above 1410 nm. Based on a theoretical study, line-of-sight (LOS) effects introduced by temperature stratification on the broadband fitting algorithm in the complete range from 1340 nm to 1440 nm are discussed. In this context, the recorded spectra during combustion were evaluated only within a narrower spectral region exhibiting almost no interference from low-temperature molecules (here, P-branch from 1410 nm to 1440 nm). It is shown that this strategy mitigates almost all of the LOS effects introduced by cold molecules and the evaluation of the spectrum in the entirely recorded wavelength range at engine combustion conditions.

Influence of Sodium Chloride on the Formation and Dissociation Behavior of CO2 Gas Hydrates.

We present an experimental study on the formation and dissociation characteristics of carbon dioxide (CO2) gas hydrates using Raman spectroscopy. The CO2 hydrates were formed from sodium chloride/water solutions with salinities of 0-10 wt %, which were pressurized with liquid CO2 in a stirred vessel at 6 MPa and a subcooling of 9.5 K. The formation of the CO2 hydrate resulted in a hydrate gel where the solid hydrate can be considered as the continuous phase that includes small amounts of a dispersed liquid water-rich phase that has not been converted to hydrate. During the hydrate formation process we quantified the fraction of solid hydrate, xH, and the fraction of the dispersed liquid water-rich phase, xL, from the signature of the hydroxyl (OH)-stretching vibration of the hydrate gel. We found that the fraction of hydrate xH contained in the hydrate gel linearly depends on the salinity of the initial liquid water-rich phase. In addition, the ratio of CO2 and water was analyzed in the liquid water-rich phase before hydrate formation, in the hydrate gel during growth and dissociation, and after its complete dissociation again in the liquid water-rich phase. We observed a supersaturation of CO2 in the water-rich phase after complete dissociation of the hydrate gel and were able to show that the excess CO2 exists as dispersed micro- or nanoscale liquid droplets in the liquid water-rich phase. These residual nano- and microdroplets could be a possible explanation for the so-called memory effect.

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.