Mid-Infrared Generated Laser-Induced Grating Signals in Methane-Containing Gas Mixtures as Indicators of Composition, Pressure, and Temperature.

The present work is aimed at studying how spatially periodic modulations of the refractive index of the medium, i.e., laser-induced gratings (LIGs), generated in a gas mixture containing methane (CH4) by nanosecond pulses of resonant mid-infrared laser radiation, can be used to measure various gas parameters. It is investigated to what extent the temporal profiles of the LIG signals, recorded as the power of the diffracted by LIGs continuous wave probe radiation, are specific to the composition, pressure, and temperature of a selected buffer gas. This specificity is illustrated by the LIG signal profiles recorded in the experiments in different gas mixtures under various conditions. Experimental data show that large LIG signals can be obtained even in mixtures with CH4 concentrations as low as ∼100 parts per million due to the strong absorption of the excitation light and subsequent rapid, highly exothermic, and partner-dependent collisional energy exchange of the laser-excited molecules with the environment. These two factors ensure high LIG generation efficiency by a small number of CH4 molecules and high sensitivity of signal strength and profile to variations of gas parameters.

Laser-induced thermal grating spectroscopy based on femtosecond laser multi-photon absorption.

Laser-induced grating spectroscopy (LIGS) is for the first time explored in a configuration based on the crossing of two focused femtosecond (fs) laser pulses (800-nm wavelength) and a focused continuous-wave (cw) laser beam (532-nm wavelength). A thermal grating was formed by multi-photon absorption of the fs-laser pulses by [Formula: see text] with a pulse energy around 700 [Formula: see text]J ([Formula: see text] 45 TW/[Formula: see text]). The feasibility of this LIGS configuration was investigated for thermometry in heated nitrogen gas flows. The temperature was varied from room temperature up to 750 K, producing strong single-shot LIGS signals. A model based on the solution of the linearized hydrodynamic equations was used to extract temperature information from single-shot experimental data, and the results show excellent agreement with the thermocouple measurements. Furthermore, the fluorescence produced by the fs-laser pulses was investigated. This study indicates an 8-photon absorption pathway for [Formula: see text] in order to reach the [Formula: see text] state from the ground state, and 8 + 5 photon excitation to reach the [Formula: see text] state of the [Formula: see text] ion. At pulse energies higher than 1 mJ, the LIGS signal was disturbed due to the generation of plasma. Additionally, measurements in argon gas and air were performed, where the LIGS signal for argon shows lower intensity compared to air and [Formula: see text].

Saturation Dependence of Flame Thermometry Using Mid-IR Degenerate Four Wave Mixing.

It has previously been demonstrated that the ratio of the degenerate four wave mixing signal from two hot water line groups near 3231 cm-1 can be used for seedless flame temperature measurements. This paper presents an investigation of the impact of saturation effects on the measured signal intensity from each line group, as well as an estimation of the accuracy of the method. The saturation effects observed here would result in a large systematic error if they are not taken into account when using the degenerate four-wave mixing intensity of these water line groups to calculate the flame temperature.

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.

Comparison of an InSb Detector and Upconversion Detector for Infrared Polarization Spectroscopy.

This paper compares the signal-to-noise ratio obtained using an InSb photodiode for infrared (IR) polarization spectroscopy to that obtained using an upconversion detector, and shows a factor 64 improvement by the change. Upconversion detection is based on using sum frequency generation to move the IR optical signal to near-visible wavelengths to improve the sensitivity.

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.

Misalignment Effects in Laser-Induced Grating Experiments.

Laser-induced grating spectroscopy (LIGS) is an experimental method in which two pulsed laser beams and a continuous-wave laser beam have to be superimposed under well-defined angles to generate a coherent signal beam. In this Note, the possible effects of different forms of misalignment are examined. This includes the overlap of the pump lasers as well as the influence of the probe laser alignment on the temporal profile of the signal.