Each AIMD trajectory, both constrained and unconstrained, was equilibrated for approximately 5-10 ps and **data** was collected for analysis from at least 10 ps of well-equilibrated trajectory. The sum total of the overall compiled AIMD trajectories accounts for approximately 2.0 ns of total simulation time (system-specific simulation times are recorded in Supplementary Table 1). This **data** set represents over 10 6 DFT configurations for systems of total size of ~500 atoms.