Non-adiabatic molecular dynamics. We used non-adiabatic molecular dynamics (NAMD) to track the photochemical pathways of 1 and 2 along the PESs of the ground and excited states. We sampled the initial conditions (nuclear positions and velocities) from the vibrational modes using the Wigner distribution at the zero-point energy (ZPE). The electronic structure calculations used SA(4)-CASSCF (10,9)/ANO-S-VDZP. The trajectories started from the S 1 (FC)-point, and the simulation time was 1 ps with a 0.5 fs time step. We computed the surface hopping probability at each step using Tully's fewest switches surface hopping method in OpenMolcas. Molecular dynamics simulations. All molecular dynamics (MD) simulations of 1 and 2 in the presence of explicit water molecules were performed in CP2K version 9.1 using Generalized Amber Force Field (GAFF) for the chromophore and SPC/Fw 95 flexible water forcefield. First, a single geometry of the chromophore was solvated by 200 water molecules in a cubic box. Next, energy minimization and equilibration were run using an isobaric-isothermal (NPT) ensemble for 0.5 ns and a canonical (NVT) ensemble for 1 ns. The last snapshot of this pre-equilibration process was taken, and the chromophore was replaced by respective Wigner geometries to initialize 500 parallel MD simulations for each molecule (1 and 2). During these MD simulations, the chromophores were kept frozen at their Wigner positions. The systems were minimized and equilibrated with a 0.1 ns NPT simulation followed by a 2 ns NVT simulation. All MD simulations used the velocity Verlet algorithm to integrate the equations of motion with a time step of 0.5 fs except during the energy minimization steps in which the conjugate gradient algorithm was used. All short-range non-bonded interactions were evaluated with a cutoff of 8 Å. To compute the coulombic interactions, Smooth Partice-Mesh Ewald (SPME) summation was used. To maintain a temperature of 300 K and 1.0 bar pressure during the Md simulations, Nose-Hoover thermostat and barostat were used as needed with time constants of 0.2 ps and 1.0 ps, respectively. The final snapshots of the NVT simulations were used to generate droplets of 20 water molecules surrounding the chromophore for subsequent ground and excited state CASSCF dynamics simulations.