Hollow cathodes are an integral part of ion, and Hall thrusters are used for electric propulsion in deep space missions and in commercial communications satellites. Hollow cathodes are known to operate in a quiescent “spot mode” and in a noisy “plume mode” in which plasma instabilities generate erosive energetic ions. The onset of the plume mode in hollow cathodes has been defined historically as when the keeper voltage oscillation values exceed 5 Vpp (peak-to-peak). Using a LaB6 hollow cathode in a vacuum chamber setup that simulates operation in ion and Hall thrusters, a set of emissive and Langmuir probes have been used to investigate the plasma properties associated with plume mode onset as a function of discharge current and gas flow rate. We find that the plume mode onset occurs at even less than 2 Vpp of the keeper voltage for the 5–75 A hollow cathode investigated here and starts at higher gas flow rates than expected from the traditional 5 Vpp metric used by those in the field. Mode competition and coupling between three different instabilities observed in the near-cathode plume affect the overall plasma oscillation levels that are correlated to energetic ion production. We find that the plasma oscillation levels measured by in situ plasma diagnostics are more indicative of the presence of oscillations and the generation of energetic ions than indirect keeper voltage measurements.