Electric-field-induced wave-packet dynamics and geometrical rearrangement of trilobite Rydberg molecules

We investigate the quantum dynamics of ultra-long-range trilobite molecules exposed to homogeneous electric fields. A trilobite molecule consists of a Rydberg atom and a ground-state atom, which is trapped at large internuclear distances in an oscillatory potential due to scattering of the Rydberg electron off the ground-state atom. Within the Born-Oppenheimer approximation, we derive an analytic expression for the two-dimensional adiabatic electronic potential energy surface in weak electric fields valid up to 500 V/m. This is used to unravel the molecular quantum dynamics employing the multiconfigurational time-dependent Hartree method. Quenches of the electric field are performed to trigger the wave-packet dynamics including the case of field inversion. Depending on the initial wave packet, we observe radial intrawell and interwell oscillations as well as angular oscillations and rotations of the respective one-body probability densities. Opportunities to control the molecular configuration are identified, a specific example being the possibility to superimpose different molecular bond lengths by a series of periodic quenches of the electric field.