The starting system is a droplet with an initial solvent radius of 37 Å around the chromophore. For initial thermalization and equilibration before the AIMD trajectory, the generalized amber force field version 2 (GAFF2) was parameterized for the ground and excited state potential energy surfaces using the RESP procedure for dyes; see Supplementary Material, section S1, for additional details. Restrained classical force field MD was performed without periodic boundary conditions, followed by the use of the TeraChem-AMBER interface for AIMD QM/MM simulations, wherein only the chromophore is treated with QM, while the solvent is treated with parameterized GAFF2, with the MM point charges coupled to the QM region with an electrostatic embedding approach. . During the AIMD simulations, the temperature of the system was maintained at 300 K using the Berendsen 99 thermostat with a time constant of 1 ps for the heat bath coupling. For ground state AIMD, the CAM-B3LYP range-separated density functional 100 and the 6-31G(d) basis set was used for the chromophore and for the excited state AIMD, we use the Tamm-Dancoff approximation (TDA) 101 to TDDFT 102 with the same level of theory. For both the ground and excited state trajectories, the initial 10 ps of the AIMD QM/MM trajectories were discarded to let the system equilibrate with the new Hamiltonian. After the system was equilibrated, a few snapshots were chosen randomly to act as the starting points for separate independent AIMD simulations. These simulations are used for the production run. From the independent trajectories, a total of 100 uncorrelated snapshots were obtained, separated by at least 200 fs.