Observation of vibrational dynamics of orientated Rydberg-atom-ion molecules

TL;DR

This paper reports the direct observation and control of vibrational dynamics in ultralong-range Rydberg-atom-ion molecules, revealing slowed-down vibrational motion due to their large bond lengths and demonstrating electric field manipulation.

Contribution

It presents the first direct observation of vibrational dynamics in Rydberg-atom-ion molecules and shows how external electric fields can control their orientation and vibrational behavior.

Findings

Vibrational dynamics occur on a timescale accessible by real-space detection.

Electric fields can control the orientation of Rydberg molecules.

Vibrational motion can be induced and observed in real time.

Abstract

Vibrational dynamics in conventional molecules usually takes place on a timescale of picoseconds or shorter. A striking exception are ultralong-range Rydberg molecules, for which dynamics is dramatically slowed down as a consequence of the huge bond length of up to several micrometers. Here, we report on the direct observation of vibrational dynamics of a recently observed Rydberg-atom-ion molecule. By applying a weak external electric field of a few mV/cm, we are able to control the orientation of the photoassociated ultralong-range Rydberg molecules and induce vibrational dynamics by quenching the electric field. A high resolution ion microscope allows us to detect the molecule's orientation and its temporal vibrational dynamics in real space. Our study opens the door to the control of molecular dynamics in Rydberg molecules.