Abstract

We report on a theoretical study of a Cs2 molecule illuminated by two lasers and show how this can result in novel quantum dynamics. We reveal that these interactions facilitate the bypass of the non-crossing rule, forming light-induced conical intersections and modifiable avoided crossings. Our findings show how laser field orientation and strength, along with initial phase differences, can control molecular-state transitions, especially on the micromotion scale. We also extensively discuss how the interaction of radiation with matter gives rise to the emergence of potential energy surfaces of hybrids of radiation and molecular states. This research advances a technique for manipulating photoassociation processes in Cs2 molecules, offering potential new avenues in quantum control. © 2024 American Chemical Society