and GaMD/VERLET simulations. For AS-GaMD/BAOAB-RESPA1 we performed 5 iterations of 5x5ns GaMD-dualwat simulations for a total simulation time of 125ns. As in the previous section, the GaMD/VERLET is composed of 3 independent simulation of 60ns (180ns total). In 30% less simulation time and 5 times less computational time, thanks to the natural AS parallelism, the coupled AS-GaMD/multi-timestep integrator scheme greatly enhance the exploration of the free energy surface. We observed that the α L region is already captured at the first iteration, i.e with only 25 ns (SI Figure ). In addition, other states, next to the α L region, are captured within tens of ns and are still not seen after the whole GaMD simulation. This AS-GaMD/multi-timestep coupling can thus represent an important gain for the sampling of biomolecular systems.