Changes in the densities of fluorocarbon radicals and fluorine atoms in a size-scalable large-area compact permanent magnet electron cyclotron resonance etching plasma source employing C4F8 gas with CH4 addition have been investigated. Measurements using infrared laser absorption spectroscopy and actinometric optical emission spectroscopy show that, for a purl C4F8 plasma, the dominant species is CF2 radicals with a density of the order of 10(13) cm(-3), followed by fluorine atoms, CF3 and CF2 radicals which have a density an order of magnitude lower at 10(12) cm(-3), The densities of the different fluorocarbon radical species were found to display different dependencies on increasing CH4 gas addition. Hollow cathode absorption spectroscopy was used to estimate the carbon atom density for the first time, to the best of our knowledge, in an etching plasma. The carbon atom density in the plasma increases linearly with CH4 gas addition between 20 and 80%. Analysis of actual SiO2/Si etching revealed that the etch selectivity and carbon atom to fluorine atom ratio follows a similar trend indicating a direct correlation between the carbon atom density in the plasma and the etch selectivity.