Legion: A Platformfor Gaussian Wavepacket NonadiabaticDynamics

Nonadiabatic molecular dynamics is crucial in investigating the time evolution of excited states in molecular systems. Among the various methods for performing such dynamics, those employing frozen Gaussian wavepacket propagation, particularly the multiple spawning approach, offer a favorable balance between computational cost and reliability. It propagates on-the-fly trajectories used to build and propagate the nuclear wavepacket. Despite its potential, efficient, flexible, and easily accessible software for Gaussian wavepacket propagation is less common compared to other methods, such as surface hopping. To address this, we present Legion, a software that facilitates the development and application of classical-trajectory-guided quantum wavepacket methods. The version presented here already contains a highly flexible and fully functional ab initio multiple spawning implementation, with different strategies to improve efficiency. Legion is written in Python for data management and NumPy/Fortran for numerical operations. It is created under the umbrella of the Newton-X platform and inherits all of its electronic structure interfaces beyond other direct interfaces. It also contains new approximations that allow it to circumvent the computation of the nonadiabatic coupling, extending the electronic structure methods that can be used for multiple spawning dynamics. We test, validate, and demonstrate Legion’s functionalities through multiple spawning dynamics of fulvene (CASSCF and CASPT2) and DMABN (TDDFT).