Fluorescence lifetime imaging through scattering media.

Fluorescence lifetime determination has proven to be useful, e.g. identification of molecules, quantitative estimation of species concentration and determination of temperatures. Lifetime determination of exponentially decaying signals is challenging if signals of different decay rates are being mixed, resulting in erroneous results. Such issues occur when the contrast of the measurement object is low, which can be limiting in applied measurements due to spurious light scattering. A solution is presented here where structured illumination is used to enhance image contrast in fluorescence lifetime wide-field imaging. Lifetime imaging determination was carried out using Dual Imaging Modeling Evaluation (DIME), and spatial lock-in analysis was used for removing spurious scattered signal to enable fluorescence lifetime imaging through scattering media.

Quantitative Hydrogen Chloride Detection in Combustion Environments Using Tunable Diode Laser Absorption Spectroscopy with Comprehensive Investigation of Hot Water Interference.

Hydrogen chloride (HCl) monitoring during combustion/gasification of biomass fuels and municipal solid waste, such as polyvinyl chloride (PVC) and food residues, is demanded to avoid the adverse effect of HCl to furnace operation and to improve the quality of the gas products. Infrared tunable diode laser absorption spectroscopy (IR-TDLAS) is a feasible nonintrusive in-situ method for HCl measurements in harsh environments. In the present work, the measurement was performed using the R(3) line of the ν2 vibrational band of HCl at 5739.25 cm-1 (1742.4 nm). Water vapor is ubiquitous in combustion/gasification environments, and its spectral interference is one of the most common challenges for IR-TDLAS. Spectral analysis based on the current well-known databases was found to be insufficient to achieve an accurate measurement. The lack of accurate temperature-dependent water spectra can introduce thousands parts per million (ppm) HCl overestimation. For the first time, accurate spectroscopic data of temperature-dependent water spectra near 5739.3 cm-1 were obtained based on a systematic experimental investigation of the hot water lines in a well-controlled, hot flue gas with a temperature varying from 1100 to 1950 K. With the accurate knowledge of hot water interference, the HCl TDLAS system can achieve a detection limit of about 100 ppm⋅m at around 1500 K, and simultaneously the gas temperature can be derived. The technique was applied to measure the temporally resolved HCl release and local temperature over burning PVC particles in hot flue gas at 1790 K.

Transition from saliva droplets to solid aerosols in the context of COVID-19 spreading.

To control the evolution of a pandemic such as COVID-19, knowing the conditions under which the pathogen is being transmitted represents a critical issue, especially when implementing protection strategies such as social distancing and wearing face masks. For viruses and bacteria that spread via airborne and/or droplet pathways, this requires understanding how saliva droplets evolve over time after their expulsion by speaking or coughing. Within this context, the transition from saliva droplets to solid residues, due to water evaporation, is studied here both experimentally, considering the saliva from 5 men and 5 women, and via numerical modeling to accurately predict the dynamics of this process. The model assumes saliva to be a binary water/salt mixture and is validated against experimental results using saliva droplets that are suspended in an ultrasound levitator. We demonstrate that droplets with an initial diameter smaller than 21 µm will produce a solid residue that would be considered an aerosol of <5 µm diameter in less than 2 s (for any relative humidity less than 80% and/or any temperature greater than 20°C). Finally, the model developed here accounts for the influence of the saliva composition, relative humidity and ambient temperature on droplet drying. Thus, the travel distance prior to becoming a solid residue can be deduced. We found that saliva droplets of initial size below 80 µm, which corresponds to the vast majority of speech and cough droplets, will become solid residues prior to touching the ground when expelled from a height of 160 cm.

Stereoscopic high-speed imaging of iron microexplosions and nanoparticle-release.

In this work, the combustion behavior of seeded iron particles (d50 = 70 µm) in a laminar diffusion flame was studied in a modified Mckenna flat-flame burner. Two high speed cameras in stereo configuration allowed 3D position and 3D velocity measurements of burning iron particles as well as 3D evaluation of particle microexplosions. Microexplosive processes are important since it can affect both combustion stability and formation of product components. The observed microexplosions happened before particle extinction resulting in change of trajectories, velocities, radiation intensities and fragmentation into smaller particles. It was observed for the first time that fragments of these microexplosions tend to produce planar structures. A frequent release phenomenon was observed during the iron particle combustion using magnified thermal radiation imaging and high-speed shadowgraphy. This release phenomenon was indirectly confirmed with scanning electron microscopy of combust products, revealing multiple cracked particle shells and hollow structures. Black body radiation characteristics was observed indicating the release being in condensed phase and emission spectroscopy identified FeO as intermediate species during combustion. The observed release is believed to mainly consist of iron-oxide nanoparticles formed in the homogenous reaction between vapor iron and oxidizers.

Airborne Gold Nanoparticle Detection Using Photoluminescence Excited with a Continuous Wave Laser.

We report the observation of photoluminescence emission from airborne gold, silver, and copper nanoparticles. A continuous wave 532 nm laser was employed for excitation. Photoluminescence from gold nanoparticles carried in a nitrogen gas flow was both spectrally resolved and directly imaged in situ using an intensified charge-coupled device camera. The simultaneously detected Raman signal from the nitrogen molecules enables quantitative estimation of the photoluminescence quantum yield of the gold nanoparticles. Photoluminescence from metal nanoparticles carried in a gas flow provides a potential tool for operando imaging of plasmonic metal nanoparticles in aerosol reactions.

Structure and Laminar Flame Speed of an Ammonia/Methane/Air Premixed Flame under Varying Pressure and Equivalence Ratio.

This paper presents a joint experimental and numerical study on premixed laminar ammonia/methane/air flames, aiming to characterize the flame structures and NO formation and determine the laminar flame speed under different pressure, equivalence ratio, and ammonia fraction in the fuel. The experiments were carried out in a lab-scale pressurized vessel with a Bunsen burner installed with a concentric co-flow of air. Measurements of NH and NO distributions in the flames were made using planar laser-induced fluorescence. A novel method was presented for determination of the laminar flame speed from Bunsen-burner flame measurements, which takes into account the non-uniform flow in the unburned mixture and local flame stretch. NH profiles were chosen as flame front markers. Direct numerical simulation of the flames and one-dimensional chemical kinetic modeling were performed to enhance the understanding of flame structures and evaluate three chemical kinetic mechanisms recently reported in the literature. The stoichiometric and fuel-rich flames exhibit a dual-flame structure, with an inner premixed flame and an outer diffusion flame. The two flames interact, which affects the NO emissions. The impact of the diffusion flame on the laminar flame speed of the inner premixed flame is however minor. At elevated pressures or higher ammonia/methane ratios, the emission of NO is suppressed as a result of the reduced radical mass fraction and promoted NO reduction reactions. It is found that the laminar flame speed measured in the present experiments can be captured by the investigated mechanisms, but quantitative predictions of the NO distribution require further model development.

Fiber-based stray light suppression in spectroscopy using periodic shadowing.

Stray light is a known strong interference in spectroscopic measurements. Photons from high-intensity signals that are scattered inside the spectrometer, or photons that enter the detector through unintended ways, will be added to the spectrum as an interference signal. A general experimental solution to this problem is presented here by introducing a customized fiber for signal collection. The fiber-mount to the spectrometer consists of a periodically arranged fiber array that, combined with lock-in analysis of the data, is capable of suppressing stray light for improved spectroscopy. The method, which is referred to as fiber-based periodic shadowing, was applied to Raman spectroscopy in combustion. The fiber-based stray-light suppression method is implemented in an experimental setup with a high-power high-repetition-rate laser system used for Raman measurements in different room-temperature gas mixtures and a premixed flame. It is shown that the stray-light level is reduced by up to a factor of 80. Weak spectral lines can be distinguished, and therefore better molecular species identification, as well as concentration and temperature evaluation, were performed. The results show that the method is feasible and efficient in practical use and that it can be employed as a general tool for improving spectroscopic accuracy.

Suppression of unpolarized background interferences for Raman spectroscopy under continuous operation.

A time-resolving filtering technique developed to improve background suppression in Raman spectroscopy is presented and characterized. The technique enables separation of signal contributions via their polarization dependency by the addition of a waveplate to a normal measurement system and data post-processing. As a result, background interferences of broadband laser-induced fluorescence and incandescence, as well as flame luminosity and blackbody radiation, were effectively suppressed from Raman spectra. Experimental setting parameters of the method were investigated under well-controlled conditions to assess their impact on the background-filtering ability, and the overall trend was understood. The fluorescence background was effectively suppressed for all investigated settings of modulation period, number of accumulations, and recording duration, with the spectrum quality preserved after the filtering. For practical application, the method was tested for measurements in a sooting flame accompanied by a strong luminosity and interfering laser-induced background signals. The technique resulted in a 200-fold decrease of the background and allowed for quantitative analyses of concentrations and temperatures from the filtered data. Thus, the method shows strong potential to extend the applicability of Raman spectroscopy, in particular for in situ diagnostics under challenging experimental conditions.

Ultraviolet Absorption Cross-Sections of Ammonia at Elevated Temperatures for Nonintrusive Quantitative Detection in Combustion Environments.

Ammonia (NH3) is regarded as an important nitrogen oxides (NOx) precursor and also as an effective reductant for NOx removal in energy utilization through combustion, and it has recently become an attractive non-carbon alternative fuel. To have a better understanding of thermochemical properties of NH3, accurate in situ detection of NH3 in high temperature environments is desirable. Ultraviolet (UV) absorption spectroscopy is a feasible technique. To achieve quantitative measurements, spectrally resolved UV absorption cross-sections of NH3 in hot gas environments at different temperatures from 295 K to 590 K were experimentally measured for the first time. Based on the experimental results, vibrational constants of NH3 were determined and used for the calculation of the absorption cross-section of NH3 at high temperatures above 590 K using the PGOPHER software. The investigated UV spectra covered the range of wavelengths from 190 nm to 230 nm, where spectral structures of the A∼ 1A″2X∼ 1A'1 transition of NH3 in the umbrella bending mode, v2, were recognized. The absorption cross-section was found to decrease at higher temperatures. For example, the absorption cross-section peak of the (6, 0) vibrational band of NH3 decreases from ∼2 × 10-17 to ∼0.5 × 10-17 cm2/molecule with the increase of temperature from 295 K to 1570 K. Using the obtained absorption cross-section, in situ nonintrusive quantification of NH3 in different hot gas environments was achieved with a detection limit varying from below 10 parts per million (ppm) to around 200 ppm as temperature increased from 295 K to 1570 K. The quantitative measurement was applied to an experimental investigation of NH3 combustion process. The concentrations of NH3 and nitric oxide (NO) in the post flame zone of NH3-methane (CH4)-air premixed flames at different equivalence ratios were measured.

Investigating photomultiplier tube nonlinearities in high-speed phosphor thermometry using light emitting diode simulated decay curves.

Photomultiplier tube (PMT) nonlinearities relevant for single shot high-speed lifetime phosphor thermometry were investigated by simulating decay curves with a light emitting diode (LED) at repetition rates between 1 Hz and 10 kHz. The PMT gain, LED decay time, and background radiant flux were also varied to investigate their impact on the measured decay time error. Errors in the measured decay time due to nonlinear PMT performance lead to temperature measurement errors; therefore, having the measured decay time sensitive to only phosphor temperature is highly valuable for more reliable temperature measurements. Photocathode bleaching had a significant impact on the signal level linearity for PMTs with excitation frequency in the kHz regime but had a smaller impact on the decay time error. Space charge effects were most noticeable at high radiant flux levels and high repetition rates. Strong background radiant flux may lead to decay time errors, and a gateable photocathode could be an effective method to reduce decay time errors. The best decay time measurement configuration to maximize precision without sacrificing accuracy is to use PMT gain in the recommended range and the highest radiant flux where the PMT response is still linear. The degree of nonlinearity in the PMT response is partly detector dependent; therefore, the results in this work may differ among detectors; however, the analysis presented in this work provides guidelines for improving the temperature accuracy of kHz lifetime phosphor thermometry measurements.

Dual-laser-induced Breakdown Thermometry via Sound Speed Measurement：A New Procedure for Improved Spatiotemporal Resolution.

Measurement of acoustic waves from laser-induced breakdown has been developed as gas thermometry in combustion atmospheres. In the measurement, two laser-induced breakdown spots are generated and the local gas temperature between these two spots is determined through the measurement of the sound speed between them. In the previous study, it was found that the local gas breakdown can introduce notable system uncertainty, about 5% to the measured temperature. To eliminate the interference, in present work, a new measurement procedure was proposed, where two individual laser pulses with optimized firing order and delay time were employed. With the new measurement procedure, the system uncertainty caused by local gas breakdown can be largely avoided and the temporal and spatial resolutions can reach up to 0.5 ms and 10 mm, respectively. The improved thermometry, dual-laser-induced breakdown thermometry (DLIBT), was applied to measure temperatures of hot flue gases provided by a multijet burner. The measured temperatures covering the range between 1000 K and 2000 K were compared with the ones accurately obtained through the two-line atomic fluorescence (TLAF) thermometry with a measurement uncertainty of ~3%, and a very good agreement was obtained.

A versatile, low-cost, snapshot multidimensional imaging approach based on structured light.

The behaviour and function of dynamic samples can be investigated using optical imaging approaches with high temporal resolution and multidimensional acquisition. Snapshot techniques have been developed in order to meet these demands, however they are often designed to study a specific parameter, such as spectral properties, limiting their applicability. Here we present and demonstrate a frequency recognition algorithm for multiple exposures (FRAME) snapshot imaging approach, which can be reconfigured to capture polarization, temporal, depth-of-focus and spectral information by simply changing the filters used. FRAME is implemented by splitting the emitted light from a sample into four channels, filtering the light and then applying a unique spatial modulation encoding before recombining all the channels. The multiplexed information is collected in a single exposure using a single detector and extracted in post processing of the Fourier transform of the collected image, where each channel image is located in a distinct region of the Fourier domain. The approach allows for individual intensity control in each channel, has easily interchangeable filters and can be used in conjunction with, in principle, all 2D detectors, making it a low cost and versatile snapshot multidimensional imaging technique.

Two-photon-excited fluorescence of CO: experiments and modeling.

A model based on rate-equation analysis has been developed for simulation of two-photon-excited laser-induced fluorescence of carbon monoxide (CO) in the Hopfield-Birge band at 230 nm. The model has been compared with experimental fluorescence profiles measured along focused beams provided by lasers emitting nano-, pico-, and femtosecond pulses. Good quantitative agreement was obtained between simulations and experimental data obtained in premixed CH4/C2H4-air flames. For excitation with femtosecond pulses, experimental and simulated fluorescence signals showed quadratic dependence on laser power under conditions of low laser irradiance, whereas different sublinear dependencies were obtained at higher irradiances due to photoionization. Simulations of CO signal versus femtosecond laser linewidth suggest the strongest signal for a transform-limited pulse, which is sufficiently broad spectrally to cover the CO Q-branch absorption spectrum. Altogether, the developed rate-equation model allows for analysis of two-photon excitation fluorescence to arrange suitable diagnostic configurations and retrieve quantitative data for CO as well as other species in combustion, such as atomic oxygen and hydrogen.

Quantitative SO2 Detection in Combustion Environments Using Broad Band Ultraviolet Absorption and Laser-Induced Fluorescence.

Spectrally resolved ultraviolet (UV) absorption cross sections of SO2 in combustion environments at temperatures from 1120 to 1950 K were measured for the first time in well-controlled conditions through applying broad band UV absorption spectroscopy in specially designed one-dimensional laminar flat flames. The temperature was observed to have a significant effect on the absorption cross-section profiles at wavelength shorter than 260 nm, while at the longer wavelength side, the absorption cross-section profiles have much less dependence on temperature. The absorption cross section at 277.8 nm with a value of 0.68 × 10-18 cm2/molecule was suggested for the evaluation of the SO2 concentration because of the weak dependence on temperature. To make spatially resolved measurements, laser-induced fluorescence (LIF) of SO2 excited by a 266 nm laser was investigated. Spectrally resolved LIF signal was analyzed at different temperatures. The LIF signal showed strong dependence on temperature, which can potentially be used for temperature measurements. At elevated temperatures, spatially resolved LIF SO2 detection up to a few ppm sensitivity was achieved. Combining UV broad band absorption spectroscopy and LIF, highly sensitive and spatially resolved quantitative measurements of SO2 in the combustion environment can be achieved.

Gain mechanism of femtosecond two-photon-excited lasing effect in atomic hydrogen.

By aiming to establish single-ended standoff combustion diagnostics, bidirectional lasing emissions of atomic hydrogen at 656 nm wavelength have been generated via two-photon resonant excitation by focusing 205 nm femtosecond laser pulses into a premixed CH4/O2 flame. The forward lasing strength is approximately one order of magnitude stronger than that of the backward one, due to the geometry of traveling wave excitation over a 2-mm-long pencil-shaped gain volume and the short gain lifetime of 3.5 ps. The gain coefficient of hydrogen lasing was determined to approximate 52/cm. As for the underlying physics of hydrogen lasing, amplified spontaneous emission (ASE) occurs simultaneously with four-wave mixing (FWM), and ASE dominates in the forward direction, whereas the backward lasing is virtually only ASE.

Ultraviolet Absorption Cross Sections of KOH and KCl for Nonintrusive Species-Specific Quantitative Detection in Hot Flue Gases.

An understanding of potassium chemistry in energy conversion processes supports the development of complex biomass utilization with high efficiency and low pollutant emissions. Potassium exists mainly as potassium hydroxide (KOH), potassium chloride (KCl), and atomic potassium (K) in combustion and related thermochemical processes. We report, for the first time, the measurement of the ultraviolet (UV) absorption cross sections of KOH and KCl at temperatures between 1300 K and 1800 K, using a newly developed method. Using the spectrally resolved UV absorption cross sections, the concentrations of KOH and KCl were measured simultaneously. In addition, we measured the concentrations of atomic K using tunable diode laser absorption spectroscopy, both at 404.4 and 769.9 nm. The 404.4 nm line was utilized to expand the measurement dynamic range to higher concentrations. A constant amount of KCl was seeded into premixed CH4/air flames with equivalence ratios varied from 0.67 to 1.32, and the concentrations of KOH, KCl, and atomic K in the hot flue gas were measured nonintrusively. The results indicate that these techniques can provide comprehensive data for quantitative understanding of the potassium chemistry in biomass combustion/gasification.

Mid-Infrared Polarization Spectroscopy Measurements of Species Concentrations and Temperature in a Low-Pressure Flame.

We demonstrate quantitative measurements of methane (CH4) mole fractions in a low-pressure fuel-rich premixed dimethyl ether/oxygen/argon flat flame (Φ = 1.87, 37 mbar) using mid-infrared (IR) polarization spectroscopy (IRPS). Non-intrusive in situ detection of CH4, acetylene (C2H2), and ethane (C2H6) in the flame was realized by probing the fundamental asymmetric C-H stretching vibration bands in the respective molecules in the spectral range 2970-3340 cm-1. The flame was stabilized on a McKenna-type porous plug burner hosted in a low-pressure chamber. The temperature at different heights above the burner (HAB) was measured from the line ratio of temperature-sensitive H2O spectral lines recorded using IRPS. Quantitative measurements of CH4 mole fractions at different HAB in the flame were realized by a calibration measurement in a low-pressure gas flow of N2 with a small admixture of known amount of CH4. A comprehensive study of the collision effects on the IRPS signal was performed in order to quantify the flame measurement. The concentration and temperature measurements were found to agree reasonably well with simulations using Chemkin. These measurements prove the potential of IRPS as a sensitive, non-intrusive, in situ technique in low pressure flames.

Scheimpflug Lidar for combustion diagnostics.

A portable Lidar system developed for large-scale (~1-20 m) combustion diagnostics is described and demonstrated. The system is able to perform remote backscattering measurements with range and temporal resolution. The range resolution is obtained by sharply imaging a part of the laser beam onto a CMOS-array or ICCD detector. The large focal depth required to do this is attained by placing the laser beam, the collection optics and the detector in a so-called Scheimpflug configuration. Results from simulations of the range capabilities and range resolution of the system are presented and its temporal resolution is also discussed. Various applications, important for combustion diagnostics, are also demonstrated, including Rayleigh scattering thermometry, aerosol detection and laser-induced fluorescence measurements. These measurements have been carried out using various continuous-wave GaN diode lasers, emitting in the violet-blue (405 - 450 nm) wavelength regime. It is anticipated that Scheimpflug Lidar will provide a useful and versatile diagnostic tool for combustion research, not only for fundamental studies, but in particular for applications at industrial sites.

Gas Temperature Measurement Using Differential Optical Absorption Spectroscopy (DOAS).

A nonintrusive method for flow gas temperature measurement using differential optical absorption spectroscopy (DOAS) was demonstrated. A temperature-dependent spectra (TDS) originated from the DOAS spectra of sulfur dioxide (SO2) in the wavelength range of 276-310 nm was introduced, and the relationship between the TDS and the temperature was built through experimental calibration process. This relationship is found to be independent of SO2 concentration and can be used for temperature measurements. The experimental results indicated that the precision of the TDS method is < ± 0.3% for SO2 concentrations higher than 150 ppm with the optical path length of 170 mm. For lower concentrations, the precision is estimated to be ± 0.4% at 1 ppm. The relative deviation between the temperature measured by the TDS method and that measured by a thermocouple is within 3% in the temperature range of 298-750 K, and the TDS method has a quicker response to the fast-changing temperature than the thermocouple.

Femtosecond two-photon-excited backward lasing of atomic hydrogen in a flame.

We report on an observation of bi-directional 656 nm lasing action of atomic hydrogen in a premixed CH4/air flame induced by resonant femtosecond 205 nm two-photon excitation. In particular, the backward-propagating lasing pulse is characterized in the spatial and temporal domains for the sake of a single-ended diagnostic. Its picosecond-scale duration and smooth temporal profile enable spatially resolved detection of hydrogen atoms in the millimeter range, which is successfully demonstrated using two narrow welding flames.