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Fluorescence-based multispectral imaging of rapidly moving or dynamic samples requires both fast two-dimensional data acquisition as well as sufficient spectral sensitivity for species separation. As the number of fluorophores in the experiment increases, meeting both these requirements becomes technically challenging. Although several solutions for fast imaging of multiple fluorophores exist, they all have one main restriction; they rely solely on spectrally resolving either the excitation- or the emission characteristics of the fluorophores. This inability directly limits how many fluorophores existing methods can simultaneously distinguish. Here we present a snapshot multispectral imaging approach that not only senses the excitation and emission characteristics of the probed fluorophores but also all cross term combinations of excitation and emission. To the best of the authors’ knowledge, this is the only snapshot multispectral imaging method that has this ability, allowing us to even sense and differentiate between light of equal wavelengths emitted from the same fluorescing species but where the signal components stem from different excitation sources. The current implementation of the technique allows us to simultaneously gather 24 different spectral images on a single detector, from which we demonstrate the ability to visualize and distinguish up to nine fluorophores within the visible wavelength range.

We report on an experimental demonstration of spatially-resolved detection of atomic hydrogen in flames using a single-ended configuration yielding 656-nm lasing in the backward direction upon 2-photon pumping with 205-nm femtosecond laser pulses. Spatial resolution is achieved by temporally-resolved detection of the backward lasing using a streak camera. The method is demonstrated in CH4/O2 flames; both in a setup consisting of two flames, with variable spacing between the flames, and in a single flame. Results from the two-flame experiment show that the backward lasing technique is able to determine changes in the separation between the flames as this distance was altered. By maximizing the temporal resolution of the streak camera, obtaining a highest spatial resolution of 1.65 mm, it is possible to resolve the hydrogen signal present in the two reaction zones in the single flame, where the separation between the reaction zones is ∼2 mm. The lasing signal is strong enough to allow single-shot measurements. Results obtained by backward lasing are compared with 2-photon planar laser-induced fluorescence (LIF) images recorded with detection perpendicular to the laser beam path and the results from the two methods qualitatively agree. Although further studies are needed in order to extract quantitative hydrogen concentrations, the present results indicate great potential for spatially resolved single-ended measurements, which would constitute a very valuable asset for combustion diagnostics in intractable geometries with limited optical access. It appears feasible to extend the technique to detection of any species for which resonant two-photon-excited lasing effect has been observed, such as O, N, C, CO and NH3.

In the present work, the spectral properties of gaseous ozone (O3) have been investigated aiming to perform quantitative concentration imaging of ozone by using a single laser pulse at 248 nm from a KrF excimer laser. The O3 molecule is first photodissociated by the laser pulse into two fragments, O and O2. Then the same laser pulse electronically excites the O2 fragment, which is vibrationally hot, whereupon fluorescence is emitted. The fluorescence intensity is found to be proportional to the concentration of ozone. Both emission and absorption characteristics have been investigated, as well as how the laser fluence affects the fluorescence signal. Quantitative ozone imaging data have been achieved based on calibration measurements in known mixtures of O3. In addition, a simultaneous study of the emission intensity captured by an intensified charge-coupled device (ICCD) camera and a spectrograph has been performed. The results show that any signal contribution not stemming from ozone is negligible compared to the strong fluorescence induced by the O2 fragment, thus proving interference-free ozone imaging. The single-shot detection limit has been estimated to ∼400 ppm. The authors believe that the presented technique offers a valuable tool applicable in various research fields, such as plasma sterilization, water and soil remediation, and plasma-assisted combustion.

In this Letter, we have investigated 845 nm lasing generation in atomic oxygen, present in a lean methane-air flame, using two-photon pumping with femtosecond 226 nm laser pulses, particularly focusing on the impact of nanosecond repetitively pulsed glow discharges forcing on the backward lasing signal. Characterizations of the backward lasing pulse, in terms of its spectrum, beam profile, pump pulse energy dependence, and divergence, were conducted to establish the presence of lasing. With plasma forcing of the flame, the backward lasing signal was observed to be enhanced significantly, ∼50%. The vertical concentration profile of atomic oxygen was revealed by measuring the backward lasing signal strength as a function of height in the flame. The results are qualitatively consistent with results obtained with two-dimensional femtosecond two-photon-absorption laser-induced fluorescence, suggesting that the backward lasing technique can be a useful tool for studies of plasma-assisted combustion processes, particularly in geometries requiring single-ended standoff detection.

Most emission spectra are characterized by lines of various intensities, a feature making them difficult to probe in their entirety - the limited dynamic range of the detector prohibits the simultaneous observation of both weak and intense spectral features. A further known complication in spectroscopy concerns the generation and detection of stray light, which is an undesired contribution of light, often associated with unavoidable imperfections in the spectrometer. Stray light leads to an offset that often exceeds the intensity of weak lines, especially those that were barely detectable in the absence of stray light. This problem is well-known in, for example, laser-induced Raman spectroscopic measurements. In this paper, we describe a methodology to solve both the stray light problem and that associated with the limited dynamic range of the detector. The method is based on combining the high dynamic range imaging concept commonly employed in digital photography with the periodic shadowing technique, where the former is used to boost the dynamics and the latter to suppress stray light. The capabilities of the approach, which is suitable for investigation of temporally stable sources, are demonstrated and the results are compared with measurements performed with both conventional equipment and the periodic shadowing technique. (Less)

Gaining information of species, temperature, and velocity distributions in turbulent combustion and high-speed reactive flows is challenging, particularly for conducting measurements without influencing the experimental object itself. The use of optical and spectroscopic techniques, and in particular laser-based diagnostics, has shown outstanding abilities for performing non-intrusive in situ diagnostics. The development of instrumentation, such as robust lasers with high pulse energy, ultra-short pulse duration, and high repetition rate along with digitized cameras exhibiting high sensitivity, large dynamic range, and frame rates on the order of MHz, has opened up for temporally and spatially resolved volumetric measurements of extreme dynamics and complexities. The aim of this article is to present selected important laser-based techniques for gas-phase diagnostics focusing on their applications in combustion and aerospace engineering. Applicable laser-based techniques for investigations of turbulent flows and combustion such as planar laser-induced fluorescence, Raman and Rayleigh scattering, coherent anti-Stokes Raman scattering, laser-induced grating scattering, particle image velocimetry, laser Doppler anemometry, and tomographic imaging are reviewed and described with some background physics. In addition, demands on instrumentation are further discussed to give insight in the possibilities that are offered by laser flow diagnostics.

We present an optical solution called DMD-PS to boost the dynamic range of 2D imaging spectroscopic measurements up to 22 bits by incorporating a digital micromirror device (DMD) prior to detection in combination with the periodic shadowing (PS) approach. In contrast to high dynamic range (HDR), where the dynamic range is increased by recording several images at different exposure times, the current approach has the potential of improving the dynamic range from a single exposure and without saturation of the CCD sensor. In the procedure, the spectrum is imaged onto the DMD that selectively reduces the reflection from the intense spectral lines, allowing the signal from the weaker lines to be increased by a factor of 28 via longer exposure times, higher camera gains or increased laser power. This manipulation of the spectrum can either be based on a priori knowledge of the spectrum or by first performing a calibration measurement to sense the intensity distribution. The resulting benefits in detection sensitivity come, however, at the cost of strong generation of interfering stray light. To solve this issue the Periodic Shadowing technique, which is based on spatial light modulation, is also employed. In this proof-of-concept article we describe the full methodology of DMD-PS and demonstrate – using the calibration-based concept – an improvement in dynamic range by a factor of ~100 over conventional imaging spectroscopy. The dynamic range of the presented approach will directly benefit from future technological development of DMDs and camera sensors.

Efficient and clean production of electrical energy and mechanical (shaft) energy for use in industrial and domestic applications, surface- and ground transportation and aero-propulsion is currently of significant general concern. Fossil fuels are mainly used for transportation and aero-propulsion, but also for power generation. Combustion of fossil fuels typically give rise to undesired emissions such as unburned hydrocarbons, carbon dioxide, carbon monoxide, soot and nitrogen oxides. The most widespread approach to minimize these is to apply various lean-burn technologies, and sometimes also dilute the fuel with hydrogen. Although efficient in reducing emissions, lean-burn often results in combustion instabilities and igniteon issues, and thus become challenging itself. Another desired aspect of today’s engines is to increase the fuel flexibility. One possible technique that may be useful for circumventing these issues is plasma-assisted combustion, i.e. to supply a small amount of electric energy to the flame to stimulate the chemical kinetics. Although not new, this approach has not yet been fully explored, partly because of it’s complexity, and partly because of apparent sufficiency. Recently, however, several research studies of this area have emerged. This paper attempts to provide a brief summary of microwave-assisted combustion, in which microwaves are utilized to supply the electrical energy to the flame, and to demonstrate that this method is useful to enhance flame stabilization, delay lean blow-off, and to increase combustion efficiency. The main effect of microwaves (or electrical energy) is to enhance the chemical kinetics, resulting in increased reactivity and laminar and turbulent flame speeds. Here we will demonstrate that this will improve the performance of gas turbine combustors. (Less)

Many important scientific questions in physics, chemistry and biology require effective methodologies to spectroscopically probe ultrafast intra- and inter-atomic/molecular dynamics. However, current methods that extend into the femtosecond regime are capable of only point measurements or single-snapshot visualizations and thus lack the capability to perform ultrafast spectroscopic videography of dynamic single events. Here we present a laser-probe-based method that enables two-dimensional videography at ultrafast timescales (femtosecond and shorter) of single, non-repetitive events. The method is based on superimposing a structural code onto the illumination to encrypt a single event, which is then deciphered in a post-processing step. This coding strategy enables laser probing with arbitrary wavelengths/bandwidths to collect signals with indiscriminate spectral information, thus allowing for ultrafast videography with full spectroscopic capability. To demonstrate the high temporal resolution of our method, we present videography of light propagation with record high 200 femtosecond temporal resolution. The method is widely applicable for studying a multitude of dynamical processes in physics, chemistry and biology over a wide range of time scales. Because the minimum frame separation (temporal resolution) is dictated by only the laser pulse duration, attosecond-laser technology may further increase video rates by several orders of magnitude.

A method for simultaneous measurements of fluorescence lifetimes of two species along a line is described. The experimental setup is based on picosecond laser pulses from two tunable optical parametric generator/optical parametric amplifier systems together with a streak camera. With an appropriate optical time delay between the two laser pulses, whose wavelengths are tuned to excite two different species, laser-induced fluorescence can be both detected temporally and spatially resolved by the streak camera. Hence, our method enables one-dimensional imaging of fluorescence lifetimes of two species in the same streak camera recording. The concept is demonstrated for fluorescence lifetime measurements of CO and OH in a laminar methane/air flame on a Bunsen-type burner. Measurements were taken in flames with four different equivalence ratios, namely ϕ = 0.9, 1.0, 1.15, and 1.25. The measured one-dimensional lifetime profiles generally agree well with lifetimes calculated from quenching cross sections found in the literature and quencher concentrations predicted by the GRI 3.0 mechanism. For OH, there is a systematic deviation of approximately 30 % between calculated and measured lifetimes. It is found that this is mainly due to the adiabatic assumption regarding the flame and uncertainty in H2O quenching cross section. This emphasizes the strength of measuring the quenching rates rather than relying on models. The measurement concept might be useful for single-shot measurements of fluorescence lifetimes of several species pairs of vital importance in combustion processes, hence allowing fluorescence signals to be corrected for quenching and ultimately yield quantitative concentration profiles.

A common problem when applying Raman scattering in applied research is spectral interference from laser-induced fluorescence. Extensive work has been invested in developing spectral and polarization filters as well as modulation schemes to refine spontaneous Raman signals. This current work, however, focuses on utilizing the temporal domain using a picosecond laser system and ICCD cameras with relatively short decay of the camera gate to prevent the fluorescence tail from being captured in Raman experiments. Further, the approach of using an ICCD camera to perform temporal filtering is compared to earlier proposed detection schemes using streak cameras or Kerr gates. The temporal-filtering scheme is evaluated in a spectroscopic investigation where a background subtraction algorithm is presented. The temporal-filtering scheme was also evaluated for Raman imaging of a levitated water droplet surrounded by fluorescing toluene vapor. Furthermore, the temporal-filter detection scheme was simulated in order to provide straight forward evaluation tools to estimate the potential of performing temporal filtering with a laser/camera system considering: laser-pulse duration, time jitter, camera-gate characteristics, gate delay times, fluorescence lifetimes, and relative signal strength between the Raman and fluorescence signal. The fluorescence signal was modeled with a closed two-level system, and the simulated results were compared to results from an investigation of the rising slope of toluene fluorescence. These evaluation tools and experimental investigations may serve as guidelines for planning and performing Raman measurements in situations where traditional filter-rejection schemes are insufficient. Copyright (c) 2013 John Wiley & Sons, Ltd. (Less)

The effect of ozone (O3) in a turbulent, swirl-stabilized natural gas/air flame was experimentally investigated at atmospheric pressure conditions using planar laser-induced fluorescence imaging of formaldehyde (CH2O PLIF) and dynamic pressure monitoring. The experiment was performed using a dry low emission (DLE) gas turbine burner used in both SGT-700 and SGT-800 industrial gas turbines from Siemens. The burner was mounted in an atmospheric combustion test rig at Siemens with optical access in the flame region. CH2O PLIF imaging was carried out for four different seeding gas compositions and seeding injection channel configurations. Two seeding injection-channels were located around the burner tip while the other two were located along the center axis of the burner at different distances upstream the burner outlet. Four different seeding gas compositions were used: nitrogen (N2), oxygen (O2) and two ozone/oxygen (O3/O2) mixtures with different O3 concentration. The results show that the O3 clearly affects the combustion chemistry. The natural gas/air mixture is preheated before combustion which is shown to kick-start the cold combustion chemistry where O3 is highly involved. The CH2O PLIF signal increases with O3 seeded into the flame which indicates that the pre-combustion activity increases and that the cold chemistry starts to develop further upstream. The small increase of the pressure drop over the burner shows that the flame moves upstream when O3 is seeded into the flame, which confirms the increase in pre-combustion activity.

An experimental setup for microwave stimulation of a turbulent flame is presented. A low-swirl flame is being exposed to continuous microwave irradiation inside an aluminum cavity. The cavity is designed with inlets for laser beams and a viewport for optical access. The aluminum cavity is operated as a resonator where the microwave mode pattern is matched to the position of the flame. Two metal meshes are working as endplates in the resonator, one at the bottom and the other at the top. The lower mesh is located right above the burner nozzle so that the low-swirl flame is able to freely propagate inside the cylinder cavity geometry whereas the upper metal mesh can be tuned to achieve good overlap between the microwave mode pattern and the flame volume. The flow is characterized for operating conditions without microwave irradiation using particle imaging velocimetry (PIV). Microwave absorption is simultaneously monitored with experimental investigations of the flame in terms of exhaust gas temperature, flame chemiluminescence (CL) analysis as well as simultaneous planar laser-induced fluorescence (PLIF) measurements of formaldehyde (CH2O) and hydroxyl radicals (OH). Results are presented for experiments conducted in two different regimes of microwave power. In the high-energy regime the microwave field is strong enough to cause a breakdown in the flame. The breakdown spark develops into a swirl-stabilized plasma due to the continuous microwave stimulation. In the low-energy regime, which is below plasma formation, the flame becomes larger and more stable and it moves upstream closer to the burner nozzle when microwaves are absorbed by the flame. As a result of a larger flame the exhaust gas temperature, flame CL and OH PLIF signals are increased as microwave energy is absorbed by the flame.

A novel method for two-dimensional fluorescence lifetime imaging is presented. The technique is demonstrated on averaged planar laser-induced fluorescence (PLIF) signals recorded in a flame. Although demonstrated on averaged images, the concept applies equally well to single-shot images. Formaldehyde was probed through pico-second excitation at 355 nm in a rich methane/oxygen flame (Phi = 2.6). Images were recorded with a dual ICCD camera detection setup with different gate characteristics of the two cameras. The recorded images were analyzed using simulated values of LIF signal detection to generate two-dimensional images of effective lifetimes. Measured lifetimes range from roughly 1 to 4.5 ns. The lifetime image data were used for quenching correction of the LIF images, which, after correction, showed better qualitative agreement compared to a formaldehyde concentration profile simulated with the GRI 3.0 mechanism. (C) 2010 The Combustion Institute. Published by Elsevier Inc. All rights reserved. (Less)

A laser method to suppress background interferences in pump-probe measurements is presented and demonstrated. The method is based on structured illumination, where the intensity profile of the pump beam is spatially modulated to make its induced photofragment signal distinguishable from that created solely by the probe beam. A spatial lock-in algorithm is then applied on the acquired data, extracting only those image components that are characterized by the encoded structure. The concept is demonstrated for imaging of OH photofragments in a laminar methane/air flame, where the signal from the OH photofragments produced by the pump beam is spatially overlapping with that from the naturally present OH radicals. The purpose was to perform for the first time, to the best of our knowledge, single-shot imaging of HO(2) in a flame. These results show an increase in signal-to-interference ratio of about 20 for single-shot data.

A laser diagnostic concept for measurement of potassium chloride (KCl) and potentially other alkali compounds in large-scale boilers and furnaces of limited optical access is presented. Single-ended, range-resolved, quantitative detection of KCl is achieved by differential absorption light detection and ranging (DIAL) based on picosecond laser pulses. Picosecond DIAL results have been compared experimentally with line-of-sight measurements using a commercial instrument, the in situ alkali chloride monitor (IACM), utilizing differential optical absorption spectroscopy. For centimeter-scale range resolution and a collection distance of 2.5 m, picosecond DIAL allowed for measurement of KCl concentrations around 130 ppm at 1200 K, in good agreement with values obtained by IACM. The DIAL data indicate a KCl detection limit of around 30 ppm for the present experimental conditions. In addition, a double-pulse DIAL setup has been developed and demonstrated for measurements under dynamic conditions with strong Mie scattering. The picosecond DIAL results are discussed and related to possible implementations of the method for measurements in industrial environments.

Laser-induced Rayleigh scattering is commonly employed for two-dimensional temperature measurements and offers benefits such as high accuracy, easily interpreted data and low experimental complexity. Yet the approach suffers from an interference often referred to as stray light, an umbrella term used for all spurious light being detected. As Rayleigh scattering is an elastic scattering phenomenon, distinguishing between stray light and the signal of interest is not straightforward. In high-temperature environments, Rayleigh signals are weak due to low molecular densities, which make stray light interferences particularly cumbersome, impairing both the reliability and accuracy of Rayleigh thermometry, especially when applied in harsh combustion environments. In this paper we present an experimental solution to greatly mitigate this issue. The method, Structured Laser Illumination Planar Imaging (SLIPI), employs an intensity modulated laser light sheet to add a recognizable signature to the signal photons. This unique signature allows utilization of a post-processing algorithm that isolates and extracts the desired Rayleigh signal, thereby minimizing measurement uncertainties caused by stray light. The fidelity of the proposed method is first verified by comparing with conventional Rayleigh thermometry under ideal, i.e., stray light-free, measurement conditions. The technique is then employed under more realistic measurement conditions, where the results conclusively illustrate that the current operating range for Rayleigh thermometry can be increased significantly by means of SLIPI. (C) 2014 The Combustion Institute. Published by Elsevier Inc. All rights reserved. (Less)

A novel technique, designated dual imaging and modeling evaluation (DIME), for evaluating single-laser shot fluorescence lifetimes is presented. The technique is experimentally verified in a generic gas mixing experiment to provide a clear demonstration of the rapidness and sensitivity of the detector scheme. Single-laser shot fluorescence lifetimes of roughly 800 ps with a standard deviation of similar to 120 ps were determined. These results were compared to streak camera measurements. Furthermore, a general fluorescence lifetime determination algorithm is proposed. The evaluation algorithm has an analytic, linear relationship between the fluorescence lifetime and detector signal ratio. In combination with the DIME detector scheme, it is a faster, more accurate and more sensitive approach for rapid fluorescence lifetime imaging than previously proposed techniques. Monte Carlo simulations were conducted to analyze the sensitivity of the detector scheme as well as to compare the proposed evaluation algorithm to previously presented rapid lifetime determination algorithms. (C) 2012 Optical Society of America

Fluoresce lifetime imaging in combination with structured laser illumination planar imaging has been performed in wide field imaging. Measurements were conducted by imaging laminar gaseous flows seeded with toluene through scattering media.

A temporal filtering technique, complementary to spectral filtering, has been developed for laser-induced fluorescence measurements. The filter is applicable in cases where the laser-induced interfering signals and the signal of interest have different temporal characteristics. For the interfering-signal discrimination a picosecond laser system along with a fast time-gated intensified CCD camera were used. In order to demonstrate and evaluate the temporal filtering concept two measurement situations were investigated; one where toluene fluorescence was discriminated from interfering luminescence of an aluminum surface, and in the other one Mie scattering signals from a water aerosol were filtered out from acetone fluorescence images. A mathematical model was developed to simulate and evaluate the temporal filter for a general measurement situation based on pulsed-laser excitation together with time-gated detection. Using system parameters measured with a streak camera, the model was validated for LIF imaging of acetone vapor inside a water aerosol. The results show that the temporal filter is capable of efficient suppression of interfering signal contributions. The photophysical properties of several species commonly studied by LIF in combustion research have been listed and discussed to provide guidelines for optimum use of the technique.

It is well known that spectroscopic measurements suffer from an interference known as stray light, causing spectral distortion that reduces measurement accuracy. In severe situations, stray light may even obscure the existence of spectral lines. Here a novel general method is presented, named Periodic Shadowing, that enables effective stray light elimination in spectroscopy and experimental results are provided to demonstrate its capabilities and versatility. Besides its efficiency, implementing it in a spectroscopic arrangement comes at virtually no added experimental complexity. (C) 2014 Optical Society of America

In the present work, a picosecond lidar system aiming at single-ended combustion diagnostics in full-scale combustion devices with limited optical access, such as power plants, is described. The highest overall range resolution of the system was found to be

Laser-based Raman spectroscopy is a powerful technique for non-intrusive measurements of chemical composition in gas, liquid, and solids. However, weak signals make it challenging to employ the technique for diagnostics under harsh conditions with various background interferences. To overcome such limitations, we have devised a method, polarization lock-in filtering (PLF) based on temporal modulation of the excitation laser polarization, to filter out polarization-independent signals from acquired data. The PLF method applied for continuous Raman spectroscopy measurements of a biomass pyrolysis process showed promising filtering abilities for unwanted background fluorescence signals. A broadband fluorescence background interference was suppressed by up to a factor of 50. Therefore, released species during the biomass pyrolysis process were readily identified with their Raman spectrum signatures and their amounts quantified. In addition, the PLF method provided Raman spectra of low background, from which a gradual change in hydrocarbons released at different stages during the pyrolysis could be observed. Altogether, the efficient background suppression method increases the general applicability of Raman spectroscopy under conditions where interfering signals present a challenge and a limiting factor.