Wavelength modulation absorption spectrometry — an extensive scrutiny of the generation of signals

Over the past few years mid-infrared absorption spectroscopy based on quantum cascade lasers operating over the region from 3 to 12 µm and called quantum cascade laser absorption spectroscopy or QCLAS has progressed considerably as a powerful diagnostic technique for in situ studies of the fundamental physics and chemistry of molecular plasmas. The increasing interest in processing plasmas containing hydrocarbons, fluorocarbons, nitrogen oxides and organo-silicon compounds has led to further applications of QCLAS because most of these compounds and their decomposition products are infrared active. QCLAS provides a means of determining the absolute concentrations of the ground states of stable and transient molecular species at time resolutions below a microsecond, which is of particular importance for the investigation of reaction kinetics and dynamics. Information about gas temperature and population densities can also be derived from QCLAS measurements. Since plasmas with molecular feed gases are used in many applications such as thin film deposition, semiconductor processing, surface activation and cleaning, and materials and waste treatment, this has stimulated the adaptation of QCLAS techniques to industrial requirements including the development of new diagnostic equipment. The recent availability of external cavity (EC) QCLs offers a further new option for multi-component detection. The aim of this paper is fourfold: (i) to briefly review spectroscopic issues arising from applying pulsed QCLs, (ii) to report on recent achievements in our understanding of molecular phenomena in plasmas and at surfaces, (iii) to describe the current status of industrial process monitoring in the mid-infrared and (iv) to discuss the potential of advanced instrumentation based on EC-QCLs for plasma diagnostics.

Applications of quantum cascade lasers in plasma diagnostics: a review

A one-dimensional fluid model for a dielectric barrier discharge in methane, used as a chemical reactor for gas conversion, is developed. The model describes the gas phase chemistry governing the conversion process of methane to higher hydrocarbons. The spatially averaged densities of the various plasma species as a function of time are discussed. Besides, the conversion of methane and the yields of the reaction products as a function of the residence time in the reactor are shown and compared with experimental data. Higher hydrocarbons (C2Hy and C3Hy) and hydrogen gas are typically found to be important reaction products. Furthermore, the main underlying reaction pathways are determined.

Fluid Modeling of the Conversion of Methane into Higher Hydrocarbons in an Atmospheric Pressure Dielectric Barrier Discharge

Signal processing and calibration procedures for in situ diode-laser absorption spectroscopy.

Within the last decade mid-infrared absorption spectroscopy over a region from 3 to 17?m and based on tuneable lead salt diode lasers, often called tuneable diode laser absorption spectroscopy or TDLAS, has progressed considerably as a powerful diagnostic technique for in situ studies of the fundamental physics and chemistry in molecular plasmas. The increasing interest in processing plasmas containing hydrocarbons, fluorocarbons, organo-silicon and boron compounds has led to further applications of TDLAS because most of these compounds and their decomposition products are infrared active. TDLAS provides a means of determining the absolute concentrations of the ground states of stable and transient molecular species, which is of particular importance for the investigation of reaction kinetic phenomena. Information about gas temperature and population densities can also be derived from TDLAS measurements. A variety of free radicals and molecular ions have been detected by TDLAS. Since plasmas with molecular feed gases are used in many applications such as thin film deposition, semiconductor processing, surface activation and cleaning, and materials and waste treatment, this has stimulated the adaptation of infrared spectroscopic techniques to industrial requirements. The recent development of quantum cascade lasers (QCLs) offers an attractive new option for the monitoring and control of industrial plasma processes. The aim of the present paper is threefold: (i) to review recent achievements in our understanding of molecular phenomena in plasmas, (ii) to report on selected studies of the spectroscopic properties and kinetic behaviour of radicals and (iii) to describe the current status of advanced instrumentation for TDLAS in the mid-infrared.

/pdf/application-of-mid-infrared-tuneable-diode-laser-absorption-2k14spqes6.pdf

Application of mid-infrared tuneable diode laser absorption spectroscopy to plasma diagnostics: a review

A compact and transportable infrared multicomponent acquisition (IRMA) system based on infrared absorption spectroscopy has been developed for plasma diagnostics and control. The IRMA system contains four independent tunable diode lasers which can be temporally multiplexed and directed into plasma reactors or into a multipass cell for exhaust gas detection. Rapid scan software with real-time line shape analysis provides simultaneous measurements of the absolute concentrations of several molecular species.

IRMA: A tunable infrared multicomponent acquisition system for plasma diagnostics

Infrared diode laser spectroscopy has been used as a diagnostic probe to measure the concentrations of the methyl radical and stable products in an ac methane/hydrogen/oxygen (CH4−H2−O2) plasma. Among the products detected were all of the stable C-2 hydrocarbons and oxygen-containing species including methanol, formaldehyde, formic acid, carbon monoxide, and carbon dioxide. A simple one-dimensional chemical modeling program has been written to calculate and compare the model concentrations of all the detected species with their observed concentrations. Good agreement between these values has been obtained which enables some insights to be gained into the gas-phase mechanism in mixed methane plasmas.

A diode laser and modeling study of mixed (ch4-h2-o2) ac plasmas

Tunable infrared diode laser absorption spectroscopy has been used to detect the methyl radical and ten stable molecules in H2-Ar-O2microwave plasmas containing up to 7.2% of methane or methanol, under both flowing and static conditions. The degree of dissociation of the hydrocarbons varied between 30 and 90% and the methyl radical concentration was found to be in the range 1010–1012molecules cm−3. The methyl radical concentration and the concentrations of the stable C-2 hydrocarbons C2H2, C2H4, and C2H6, produced in the plasma decayed exponentially when increasing amounts of O2were added at fixed methane or methanol partial pressures. In addition to detecting the hydrocarbon species, the major products CO, CO2, and H2O were also monitored. For the first time, formaldehyde, formic acid, and methane were detected in methanol microwave plasmas, formaldehyde was detected in methane microwave plasmas. Chemical modeling with 57 reactions was used to successfully predict the concentrations in methane plasmas in the absence of oxygen and the trends for the major chemical product species as oxygen was added.

Tunable Diode Laser Diagnostic Studies of H2-Ar-O2 Microwave Plasmas Containing Methane or Methanol

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IRMA: A tunable infrared multicomponent acquisition system for plasma diagnostics

A diode laser and modeling study of mixed (ch4-h2-o2) ac plasmas

Tunable Diode Laser Diagnostic Studies of H2-Ar-O2 Microwave Plasmas Containing Methane or Methanol