It is worth noting that, in our experience, the MPS/TT decomposition along with the tangent-space time propagation scheme for evolving the HEOM in twin space (see Eq. ( )) always allows a significantly larger time step than directly solving Eq. ( ) with a differential equation solver, such as Runge-Kutta integrator. For this work, we employ the time step ∆t = 1fs. The molecular Hamiltonian H mol is described in a discrete variable representation