Abstract The High Temperature Test Facility (HTTF) is a quarter-scale integral-effect facility designed to study pressurized and depressurized conduction cooldowns (PCC and DCC, respectively) in high temperature, gas-cooled reactors (HTGR). This study focuses on DCC and aims to characterize the gas exchange between the reactor core and the reactor cavity to assess the risk for air ingress and subsequent potential for natural circulation core cooldowns. High-resolution velocity profile measurements are performed at the coolant pipe break location over a long time-scale using molecular tagging velocimetry. This non-intrusive, laser-based technique is applied for the first time in the field of nuclear thermal hydraulics, providing new insights for understanding the underlying phenomena at play during a DCC event. Such data are also valuable for validation of numerical simulations such as Reactor Excursion and Leak Analysis Program (RELAP). Results are reported here for various gas mixtures of helium (the coolant) and nitrogen (surrogate for air) to study the effect of density ratio. The short transient (30 s) lock-exchange phase is well captured with helium flow velocity between 0.8 and 2 m/s. The flow is shown to persist over much longer time-scales (hours) at a velocity of about 0.2 m/s, a likely consequence of gas mixing in the hot leg and in the lower plenum of the reactor. Flow visualization at the exit of the hot leg shows shear instabilities, which supports the hypothesis of significant mixing.