Application of a collisional radiative model to atomic hydrogen for diagnostic purposes

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Abstract

Optical emission spectroscopy is one of the standard diagnostic methods to determine plasma parameters. In hydrogen plasmas often the intensity of the Balmer lines is recorded. To analyze such measurements population models for the hydrogen atom are needed. The flexible package Yacora is used to construct a new collisional radiative model for low pressure, low temperature hydrogen plasmas. This model includes six possible excitation channels: effective excitation of H, recombination of H+, dissociative excitation of H2, dissociative recombination of H2+, dissociative recombination of H3+ and mutual neutralization of H- and Hx+. The model is applied to a uniform ECR plasma with high dissociation degree and low ionization degree, i.e. electron collision excitation from H is the dominant excitation channel. The cross sections for this channel taken from literature showed a non-physical discontinuity at electron energies close to the threshold energy. This discontinuity has been removed by using a smoothing procedure. For known plasma parameters the deviation between measured and calculated population densities decreases significantly by using the smoothed data. Furthermore, the agreement of the electron density deduced from the ratio Hβ/Hγ with results of other diagnostic methods is enhanced dramatically.

Introduction

Low pressure, low temperature plasmas are used in a wide range of technical and research applications [1]. Most of these plasmas contain a certain amount of hydrogen atoms produced by dissociation of H2 or other molecules, e.g. hydrocarbons or silanes.

The most important plasma parameters in these plasmas are temperature, density and velocity distribution functions of the particles. Plasma diagnostics which determines the plasma parameters is a key issue to improve the understanding of plasma processes [2], [3].

Plasma diagnostics usually is based on the measurement of externally accessible physical parameters of the plasma. For example a spectrometer can be used to record the intensity of a radiative transition. Models in which the plasma parameters are used as free parameters are applied to predict values of the measured parameter. A comparison of the results of measurement and calculation enables the determination of the plasma parameters.

For low pressure, low temperature plasmas, many different diagnostic methods are available [2], [3]. One of these methods is the optical emission spectroscopy (OES) [4], [5], [6], which is based on a very simple and robust experimental setup. One main advantage of this method is its non-invasive nature, i.e. the plasma is not affected by the measurements.

For the interpretation of spectroscopically measured intensities population models are needed. Such models calculate population densities of excited states in atoms, molecules or ions depending on the plasma parameters. For very high electron densities (ne1024m-3 in hydrogen plasmas) the states thermalize and the local thermodynamic equilibrium (LTE) can be applied. For very low electron densities (ne1017m-3 in hydrogen plasmas) the corona equilibrium which balances electron collision excitation from the ground state with radiative transitions is valid. For intermediate electron densities the excitation and de-excitation processes for all states in the atom, molecule or ion have to be balanced by the population model [7]. Such models are called collisional radiative (CR) models [8], [9], [10]. For high and low electron densities CR models represent the LTE and corona equilibrium, respectively.

The first CR model for H was developed by Johnson and Hinnov [11]. Since then other CR models for the hydrogen atom have been presented [12], [13], the most prominent one is the ADAS package [13]. The typical application ranges of these models are recombining (Te<1eV) or ionizing plasmas (Te>10eV) which means that the population densities of exited states are determined mainly by recombination from H+ and electron collision excitation from H, respectively.

In typical process plasmas [14] and sources for positive [15] or negative hydrogen ions [16] the electron temperature is between these values. In this intermediate parameter range population processes from additional neutral particles (H2) or ions (H2+, H-) can have an influence on the population of excited states. Additionally, the average energy of the plasma particles is either below or close to the threshold energy of some of the excitation processes. Thus, the corresponding cross sections and the energy distribution functions of the involved particles have to be known very accurately for low energies.

The flexible package Yacora was developed and used to construct a new CR model for hydrogen plasmas. This paper describes in more detail the application of the model to an uniform ECR plasma with electron temperatures in the parameter range between recombining and ionizing plasmas (1eV<Te<10eV), high dissociation degree and low ionization degree, i.e. electron collision excitation from H is the dominant excitation channel. This regime is outside the parameter ranges in which the previously existing CR models for H have been tested. Comparison of measured and calculated population densities enables the revision of the cross sections available in literature for collision excitation from the ground state of H at electron energies close to the threshold.

Section snippets

Physics of CR models

When an excited state p in an atom, molecule or ion is de-excited by a radiative transition to an energetically lower-lying state q, the intensity of the emitted radiation can be expressed by the line emission coefficient ɛpq:ɛpq=npApqhν4π,where np is the population density of p, Apq the transition probability and ν the frequency of the transition. If the transition probability and frequency are known, the population density can be deduced from a measured value of the line emission coefficient:n

Fundamental characteristics of the CR model for H

Hydrogen represents the simplest atom. It consists of a number of electronically excited states which are degenerate due to different possible orientations of angular momentum and spin of the valence electron. In case of non-existing strong external fields, the energetic splitting of the degenerate states can be neglected. Due to strong coupling processes with non-metastable states of the same main quantum number, the metastable sub-state 2s is not needed to be considered explicitly [20]. Thus,

The experiment

Spectroscopic measurements on a low pressure, low temperature plasma with known plasma parameters were performed. Since measurements by OES average the emitted intensity over a specific line-of-sight, the measurements were performed on an uniform and stationary ECR plasma.

The ECR reactor used to generate the plasma is shown schematically in Fig. 4. The experiment consists of a cylindrical vacuum vessel (d=15cm, h=31cm). The top and bottom of this cylinder are closed by a quartz plate and an

Results

For investigating the influence of the smoothing procedure described in Section 3.2, the CR model was applied to the experiment described in Section 4. Plasmas containing 10% hydrogen, 5% argon and 85% helium were generated at 0.5, 4, 10 and 15 Pa pressure.

Using Langmuir probe and double probe measurements it was shown that the spatial profile of the electron density inside the experiment is almost flat [38]. The EEDF follows a Maxwellian shape and thus the electron energy distribution can be

Conclusion

The flexible package Yacora was used to construct a CR model for the hydrogen atom based on the most recent cross sections available in literature. The model incorporates six different excitation channels which can be of relevance in low pressure, low temperature plasmas: effective excitation of H, recombination of H+, dissociative excitation of H2, dissociative recombination of H2+, dissociative recombination of H3+ and mutual neutralization of H- and Hx+.

The model was used to interpret Balmer

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