Kajsa Larsson

Single-shot photofragment imaging by structured illumination

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.

Simultaneous Visualization of Water and Hydrogen Peroxide Vapor Using Two-Photon Laser-Induced Fluorescence and Photofragmentation Laser-Induced Fluorescence

A concept based on a combination of photofragmentation laser-induced fluorescence (PF-LIF) and two-photon laser-induced fluorescence (LIF) is for the first time demonstrated for simultaneous detection of hydrogen peroxide (H2O2) and water (H2O) vapor. Water detection is based on two-photon excitation by an injection-locked krypton fluoride (KrF) excimer laser (248.28 nm), which induces broadband fluorescence (400-500 nm) from water. The same laser simultaneously photodissociates H2O2, whereupon the generated OH fragments are probed by LIF after a time delay of typically 50 ns, by a frequency-doubled dye laser (281.91 nm). Experiments in six different H2O2/H2O mixtures of known compositions show that both signals are linearly dependent on respective species concentration. For the H2O2 detection there is a minor interfering signal contribution from OH fragments created by two-photon photodissociation of H2O. Since the PF-LIF signal yield from H2O2 is found to be at least ∼24 000 times higher than the PF-LIF signal yield from H2O at room temperature, this interference is negligible for most H2O/H2O2 mixtures of practical interest. Simultaneous single-shot imaging of both species was demonstrated in a slightly turbulent flow. For single-shot imaging the minimum detectable H2O2 and H2O concentration is 10 ppm and 0.5%, respectively. The proposed measurement concept could be a valuable asset in several areas, for example, in atmospheric and combustion science and research on vapor-phase H2O2 sterilization in the pharmaceutical and aseptic food-packaging industries.

Quantitative Imaging of Ozone Vapor Using Photofragmentation Laser-Induced Fluorescence (LIF)

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.

Simultaneous Visualization of Hydrogen Peroxide and Water Concentrations Using Photofragmentation Laser-Induced Fluorescence

A concept based on photofragmentation laser-induced fluorescence (PFLIF) is for the first time demonstrated for simultaneous detection of hydrogen peroxide (H2O2) and water (H2O) vapor in various mixtures containing the two constituents in a bath of argon gas. A photolysis laser pulse at 248 nm dissociates H2O2 into OH fragments, whereupon a probe pulse, delayed 100 ns and tuned to an absorption line in the A2Σ+ (v = 1) ← X2Π(v = 0) band of OH near 282 nm, induces fluorescence. The total OH fluorescence reflects the H2O2 concentration, while its spectral shape is utilized to determine the H2O concentration via a model predicting the ratio between the fluorescence intensities of the A2Σ+ (v = 1) → X2Π(v = 1) and the A2Σ+ (v = 0) → X2Π(v = 0) bands. The H2O detection scheme requires that the bath gas has a collisional cross-section with OH(A) that is significantly lower than that of H2O, which is the case for argon. Spectrally dispersed OH fluorescence spectra were recorded for five different H2O2/H2O/Ar mixtures; the H2O2 concentration in the range of 30–500 ppm and the H2O concentration in the range of 0–3%. Fluorescence intensity ratios predicted by the model for these mixtures agree very well with corresponding experimental data, which thus validates the model. The concept was also demonstrated for two-dimensional imaging, using two intensified charge-coupled device (CCD) cameras for signal detection. Water content was here sensed through the different temporal characteristics of the two fluorescence bands by triggering the two cameras so that one captures the total OH fluorescence while the other one captures only the early part, which mainly stems from A2Σ+ (v = 1) → X2Π(v = 1) fluorescence. Hence, the H2O2 concentration is reflected by the image of the camera recording the total OH fluorescence, whereas H2O concentration is extracted from the ratio between the two camera images. Quantification of the concentrations was carried out based on calibration measurements performed in known mixtures of H2O2 (30–500 ppm) and H2O (0–3%) in bulk argon. The detection limits for single-shot imaging are estimated to be 20 ppm for H2O2 and 0.05% for H2O. The authors believe that the concept provides a valuable asset in, for example, pharmaceutical or aseptic food packaging applications, where H2O2/H2O vapor is routinely used for sterilization.

Quantitative NO 2 measurements in an industrial sterilization rig using laser induced fluorescence

NO2 concentration measurements have been performed in an industrial test rig using laser-induced fluorescence. The goal is to improve the understanding of the electron-induced chemical species in the plasma, thus improving the neutralization scheme.

Investigation of ps-PFLIF for detection of hydrogen peroxides in laminar flames

Using short (5 ns) pump-probe delay times, photochemical interferences due to CO2 photolysis can be virtually eliminated in flame experiments with photofragmentation laser-induced fluorescence (PFLIF), which enables hydrogen peroxides to be measured with higher accuracy.

Simultaneous Imaging of H2O2 and H2O Concentration Distributions Using Photofragmentation LIF

Simultaneous imaging of H2O2 and H2O vapor, based on photofragmentation laser-induced fluorescence, is demonstrated. The concentrations are determined from the total OH(A-X) fluorescence (H2O2) and the ratio between the 1-1 and 0-0 emission bands (H2O).