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There is a growing interest in the physics of surface flashover between the interface of atmosphere and vacuum in some high-power systems. More specifically, the quantitative role of vacuum ultraviolet (VUV) radiation for the photoionization leading to a streamer development during the initial stages of a breakdown is unknown. This paper describes an experimental setup used to measure the VUV radiation emitted from atmospheric flashover as well as time-resolved imaging of the flashover event. A pulser providing the voltage to the gap was designed with special considerations in mind, including long lifetime, low noise, and high reproducibility. This enabled the study of the flashover in various background gases with an emphasis on spectroscopic measurements. The calculated spectra are compared with the measured spectra, and it is found that atomic oxygen and nitrogen are responsible for most of the VUV production in an air breakdown at atmospheric pressure in the wavelength range of 115-180 nm. Time-resolved spectroscopy reveals that the VUV radiation is emitted during the initial stages while the streamers are developing.