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

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

Microwave discharges (MD) are widely used as a source of non-equilibrium low pressure plasma for different applications. This paper reviews the methods of microwave plasma generation at pressures from 10−2 approximately to 30 kPa with centimeter–millimeter wavelength microwaves on the basis of scientific publications since 1950 up to the present. The review consists of 16 sections. A general look at MDs and their application is given in the introduction, together with a description of a typical block-schema of the microwave plasma generator, classification of MD, and attractive features of MD. Sections 2–12 describe the different methods of microwave plasma generators on the basis of cavity and waveguide discharges, surface and slow wave discharges, discharges with distributed energy input, initiated and surface discharges, discharges in wave beams, discharges with stochastically jumping phases of microwaves, discharges in an external magnetic field and discharges with a combination of microwave field and dc and RF fields. These methods provide the possibility of producing nonequilibriun high density plasma in small and large chambers for many applications. Plasma chemical activity of nonequilibrium microwave plasma is analyzed in section 13. A short consideration of the history and status of the problem is given. The main areas of microwave plasma application are briefly described in section 14. Non-uniformity is the inherent property of the majority of electrical discharges and MDs are no exception. Peculiarities of physical–chemical processes in strongly non-uniform MDs are demonstrated placing high emphasis on the influence of small noble gas additions to the main plasma gas (section 15). The review is illustrated by 80 figures. The list of references contains 350 scientific publications.

https://iopscience.iop.org/article/10.1088/0963-0252/24/5/053001/pdf

Microwave discharges at low pressures and peculiarities of the processes in strongly non-uniform plasma

We investigated the efficiency and formation mechanism of ammonia generation in recombining plasmas generated from mixtures of N2 and H2 under various plasma conditions. In contrast to the Haber-Bosch process, in which the molecules are dissociated on a catalytic surface, under these plasma conditions the precursor molecules, N2 and H2, are already dissociated in the gas phase. Surfaces are thus exposed to large fluxes of atomic N and H radicals. The ammonia production turns out to be strongly dependent on the fluxes of atomic N and H radicals to the surface. By optimizing the atomic N and H fluxes to the surface using an atomic nitrogen and hydrogen source ammonia can be formed efficiently, i.e., more than 10% of the total background pressure is measured to be ammonia. The results obtained show a strong similarity with results reported in literature, which were explained by the production of ammonia at the surface by stepwise addition reactions between adsorbed nitrogen and hydrogen containing radicals at the surface and incoming N and H containing radicals. Furthermore, our results indicate that the ammonia production is independent of wall material. The high fluxes of N and H radicals in our experiments result in a passivated surface, and the actual chemistry, leading to the formation of ammonia, takes place in an additional layer on top of this passivated surface.

/pdf/detailed-study-of-the-plasma-activated-catalytic-generation-3o8f9b6e51.pdf

Detailed study of the plasma-activated catalytic generation of ammonia in N2-H2 plasmas

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

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IRMA: A tunable infrared multicomponent acquisition system for plasma diagnostics