First, 10 of the 13 simulations of Motor S and one of the four simulations of Motor N completed THI during their 1 µs duration. The full rotation process, consisting of excited state dynamics, decay to the ground state, ground state dynamics within the metastable form, and THI, is captured by the concatenation of a QM surface-hopping trajectory and its subsequent classical MD trajectory for Motor S in video mndo-amber.mp4 in the ESI.