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Understanding the coupling between thermodynamics and propellant sloshing is important for cryogenic upper stages, especially during the lift-off phase and in missions including multiple engine restarts, as the fluid dynamic condition of the propellant is mainly influenced by various flight maneuvers. This paper describes the development and validation of a Volume of Fluid (VOF)-based CFD solver, Loci/STREAM-VOF, to the ullage collapse under violent later slosh conditions. Loci/STREAM-VOF is shown to be able to capture detailed slosh dynamics, including slosh frequency, non-linear slosh damping, and violent surface breakup due to forced acceleration. The comparison of surface shape and small drops formed during large amplitude slosh with experimental imagery shows excellent agreement throughout the sloshing period. Comparison of temperature histories in the ullage, at the gas-liquid interface, and inside liquid with the experiment conducted at JAXA also show very good agreement. The simulation points to a stratified temperature field inside the liquid near the interface, critical to the ullage pressure after the collapse. The predicted pressure collapse matches well with the experimental value due to sloshing. Parametric sensitivity studies suggest that high-fidelity Loci/STREM-VOF simulations can play an essential role in predicting the actual thermodynamics of ullage collapse when following the recommended simulation methodology.