Legion: A Platform for Gaussian Wavepacket Nonadiabatic Dynamics

These datasets contain the initial conditions and trajectories generated by the newly developed Legion using Ab Initio Multiple Spawning (AIMS) for both fulvene with different initial condistions and DMABN. We performed the dynamics varying multiple parameters and introduced new approximations that avoid the need to compute the nonadiabatic coupling (NACV).

The initial condition for fulvene were obtained from (doi.org/10.1039/D0CP01353F and doi.org/10.1021/acs.jctc.3c01159) and for DMABN were obtained from (doi.org/10.1039/D0CP01353F). For fulvene the dynamics used CASSCF in the Columbus software (version 7.2) and OpenMolcas (version 24.06). For CASPT2 it used only OpenMolcas.  The DMABN dynamics were performed with TDDFT using ORCA (version 5.0.4) and Gaussian (version 16).