Quantum simulation of molecular interaction and dynamics at surfaces

Feng, Wei Wei, Xü +5 more

Guangming Liu, Siwei Wang, Hsing-Ta Chen

Simulating the dynamics of molecular excitons in complex nanophotonic environments requires integrating rigorous electromagnetic simulations with accurate treatments of open quantum system dynamics. In this work, we develop MQED-QD (Macroscopic Quantum Electrodynamics for Quantum Dynamics), a robust computational package for simulating exciton dynamics in arbitrary dielectric and plasmonic environments. Based on the MQED framework, the package offers a unified workflow for constructing the dyadic Green's functions from classical electromagnetic solvers, parametrizing quantum master equations, and propagating the time evolution to determine the molecular subsystem's dynamical properties. To demonstrate the package's capabilities, we simulate exciton transport within a one-dimensional molecular chain near a silver nanostructure, including benchmarking against planar surfaces and exploring the influence of silver nanorods. Our results reveal that surface plasmon polaritons on nanorods dramatically enhance long-range dipole-dipole interactions, accelerating exciton delocalization and yielding higher participation ratios compared to planar geometries. By elucidating accurate molecular exciton dynamics in conjunction with nanophotonics and plasmonics, MQED-QD provides a powerful, open-source package that facilitates the rational design of nanoscale architectures.

Andrew T. Sornborger, Phillip C. Stancil, Michael R. Geller

Simon Euchner, Mathias B. M. Svendsen, Igor Lesanovsky

Trapped ions excited to high-lying electronic states combine strongly coupled collective vibrational and electronic degrees of freedom with long-ranged interparticle interactions. These ingredients enable the quantum simulation of biochemical processes, associated with the dynamics of excitons in non-perturbative parameter regimes. The key feature of such a quantum simulator are electronic-state-dependent molecular potential surfaces which can be strongly coupled. This allows to shed light on a variety of mechanisms underlying exciton transport. We illustrate this in a system of three trapped ions, which is amenable to an ab initio treatment. Given that ion traps can be routinely prepared with hundreds of ions, these quantum simulators can immediately realise scenarios which are inaccessible by current numerical methods.

Bradley P. Feuston

Momoji Kubo