Exploring vibronic dynamics near a sloped conical intersection with trapped Rydberg ions

Abstract

We study spin-phonon coupled dynamics in the vicinity of a sloped conical intersection created by laser coupling the electronic (spin) and vibrational degrees of freedom of a pair of trapped Rydberg ions. We show that the shape of the potential energy surfaces can be engineered and controlled by exploiting the sideband transitions of the crystal vibration and dipole-dipole interactions between Rydberg ions in the Lamb-Dicke regime. Using the sideband transition, we realize a sloped conical intersection whose cone axis is only tilted along one spatial axis. When the phonon wavepacket is located in the potential minimum of the lower potential surface, the spin and phonon dynamics are largely frozen owing to the geometric phase effect. When starting from the upper potential surface, the electronic and phonon states tunnel to the lower potential surface, leading to a partial revival of the initial state. In contrast, the dynamics drastically change when the initial wavepackets are away from the conical intersection. The initial state is revived, and is almost entirely irrelevant to whether it is from the lower or upper potential surface. Complete Rabi oscillations of the adiabatic states are found when the wavepacket is initialized on the upper potential surface. The dynamics occur on the microsecond and nanometer scales, implying that Rydberg ions provide a platform for simulating nonadiabatic processes in the vicinity of a sloped conical intersection.