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Theoretical, analytical, and experimental investigations of electrospray operation in vacuum facilities show that secondary species emission (SSE) plays a significant role in the behavior of electrospray thrusters during ground testing. A review of SSE mechanisms, along with an analysis of onset thresholds for electrospray thruster conditions, indicates that secondary species (e.g., electrons, anions, cations, etc.) must be carefully considered for accurate measurements and determination of performance and life. Presented models and experiments show that SSE-induced thruster-to-facility coupling can lead to considerable measurement uncertainty but can be effectively mitigated with an appropriate beam target design. The Electrospray SSE Control-volume Analysis for Resolving Ground Operation of Thrusters model is applied to experimental data to analyze SSE behavior. A heat and mass flux analysis of the Air Force Electrospray Thruster Series 2 (AFET-2) shows that SSE-induced Ohmic dissipation can cause performance limitations in ionic liquid ion source thrusters. The presented analytical models show that backstreaming current density contributing to less than 0.1% of measured emitter current density can cause substantial variation in propellant properties. Additionally, backstreaming current density contributing to less than 3% of emitted current can cause the 0.86 μg s−1 neutral loss rate estimated during AFET-2 testing. Arguments are presented to support the notion that glow discharges observed in electrospray thrusters during vacuum operation are a consequence of secondary species backstreaming to the emission site, rather than a process intrinsically caused by ion evaporation. Recommendations for general best practices to minimize the effects of SSE on electrospray thruster operation are provided.