Influence of direct dipole-dipole interactions on the optical response of 2D materials in strongly inhomogeneous infrared cavity fields

TL;DR

This paper investigates how direct dipole-dipole interactions within 2D materials influence their optical response when coupled with strongly inhomogeneous infrared cavity fields, emphasizing the importance of including these interactions in certain regimes.

Contribution

It provides a full Hamiltonian diagonalization including dipole-dipole interactions and identifies conditions where these interactions critically affect optical properties.

Findings

Dipole-dipole interactions renormalize the energy of collective excitations.

In extreme confinement, these interactions involve many states and are essential for accurate modeling.

A simple equation is proposed to determine when dipole-dipole interactions significantly alter the optical response.

Abstract

A two-dimensional (2D) material, formed for example by a self-assembled molecular monolayer or by a single layer of a van der Walls material, can couple efficiently with photonic nanocavities, potentially reaching the strong coupling regime. The coupling can be modelled using classical harmonic oscillator models or cavity quantum electrodynamics Hamiltonians that often neglect the direct dipole-dipole interactions within the monolayer. Here, we diagonalize the full Hamiltonian of the system, including these direct dipole-dipole interactions. The main effect on the optical properties of a typical 2D system is simply to renormalize the effective energy of the bright collective excitation of the monolayer that couples with the nanophotonic mode. On the other hand, we show that for situations of extreme field confinement, large transition dipole moments and low losses, fully including the direct dipole-dipole interactions is critical to correctly capture the optical response, with many collective states participating in it. To quantify this result, we propose a simple equation that indicates the condition for which the direct interactions strongly modify the optical response.