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The chemical interactions and physical processes occurring in a high energy spark gap with different combinations of gases, electrodes, and insulators were studied. The electrodes studied were graphite and a tungsten-copper composite; the insulators were Lexan and Blue Nylon; and the gases were N2 and SF6. The gas composition was monitored with a mass spectrometer. Spectroscopic techniques were used to observe the arc channel. The electrode surfaces were studied with several surface analysis techniques, including scanning electron microscopy, electron spectroscopy for chemical analysis, Auger electron spectroscopy, and X-ray fluorescence. The breakdown voltage distribution was examined for different material combinations. The plasma chemistry processes involving the gas, electrode, and insulator materials were found to affect the voltage self-breakdown distribution. The detailed surface analysis gave information about the nature of the chemical processes. The presence of Blue Nylon seemed to have a more adverse effect than Lexan and graphite seemed to have a narrower voltage distribution than the tungsten-copper composite.