Nonadiabatic Dynamics near Multiple Light-Induced Conical Intersections under Bichromatic Driving: Quantum...

Light-induced conical intersections (LICIs) create externally tunable pathways for nonadiabatic transitions, enabling the active control of molecular photophysical and photochemical processes. However, both the dynamics near multiple LICIs under bichromatic driving and the applicability of our recently developed two-mode Floquet fewest switches surface hopping (two-mode F-FSSH) method to this regime remain insufficiently understood. Here, we construct a minimal three-channel Floquet Hamiltonian that supports two LICIs for Na2 interacting with a bichromatic field. We characterize its static Floquet properties and investigate the associated nonadiabatic dynamics using numerically exact quantum wave packet dynamics and two-mode F-FSSH. We find that the second-photon energy controls the relative positions of the LICIs, whereas the second-field intensity primarily redistributes and broadens the derivative-coupling landscape around the second LICI. Consequently, electronic population transfer and molecular alignment exhibit distinct and often nonmonotonic responses to the two control parameters. Two-mode F-FSSH reliably captures the principal features of the early time dynamics and provides a semiquantitative description of the post-transient time-averaged observables. These findings advance our understanding of LICI-mediated dynamics at both physical and methodological levels.