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

TL;DR

This paper explores how homogeneous electric fields influence the quantum wave-packet dynamics and geometrical structure of trilobite Rydberg molecules, revealing control mechanisms for molecular configurations through electric field manipulation.

Contribution

It provides an analytic expression for the adiabatic potential energy surface of trilobite molecules in weak electric fields and demonstrates how electric field quenches can control molecular configurations.

Findings

Electric fields induce complex wave-packet oscillations and rotations.

Electric field quenches can superimpose different molecular bond lengths.

Control of molecular geometry via electric field manipulation is possible.

Abstract

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 Multi-Configurational 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 intra-well and inter-well 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.