The computational and theoretical framework used here is modular, so future studies could use refined forms of each component method. For example, photoisomerization could be modeled with higher level QM techniques, such as Ab Initio Multiple Spawning methods , and the classical simulations could use improved functional forms of the force field, such as a more realistic van der Waals potential or a more detailed description of torsional energy profiles. The present framework can also be extended to other classes of fast light-driven molecular motors, especially those that share the same overcrowded alkene core Figure : Dependence of the motor rotation rate in steady state on the total photoisomerization rate, assuming 10000 times smaller k 13 than its value obtained from MSM and used in Figure . The three curves correspond to three different distributions of metastable substates generated by photoisomerization: the distribution that leads to the fastest rotation (MS1:MS2:MS3:MS4=1:0:0:0), the distribution that leads to the slowest rotation (MS1:MS2:MS3:MS4=0:1:0:0), and the distribution inferred from our surface-hopping MD trajectories (MS1:MS2:MS3:MS4=7:2:4:0).