Exploring the many-body dynamics near a conical intersection with trapped Rydberg ions

TL;DR

This paper proposes using trapped Rydberg ions as a controllable platform to simulate and study conical intersections and their effects on molecular-like dynamics over larger scales than traditional ultrafast spectroscopy allows.

Contribution

It introduces a novel method to engineer and observe conical intersections and their dynamics using trapped Rydberg ions, enabling larger scale and longer duration simulations.

Findings

Conical intersections can be engineered in trapped Rydberg ions.

The presence of a conical intersection inhibits nuclear motion.

Electronic populations can be monitored in real-time.

Abstract

Conical intersections between electronic potential energy surfaces are paradigmatic for the study of non-adiabatic processes in the excited states of large molecules. However, since the corresponding dynamics occurs on a femtosecond timescale, their investigation remains challenging and requires ultrafast spectroscopy techniques. We demonstrate that trapped Rydberg ions are a platform to engineer conical intersections and to simulate their ensuing dynamics on larger length and time scales of the order of nanometers and microseconds, respectively; all this in a highly controllable system. Here, the shape of the potential energy surfaces and the position of the conical intersection can be tuned thanks to the interplay between the high polarizability and the strong dipolar exchange interactions of Rydberg ions. We study how the presence of a conical intersection affects both the nuclear and electronic dynamics demonstrating, in particular, how it results in the inhibition of the nuclear motion. These effects can be monitored in real-time via a direct spectroscopic measurement of the electronic populations in a state-of-the-art experimental setup.