Spin-orbit coupling in organic microcavities: Lower polariton splitting, triplet polaritons, and disorder-induced dark-states relaxation

TL;DR

This paper investigates how spin-orbit coupling affects polariton states in organic microcavities, revealing splitting, triplet polaritons, and disorder-induced dark-state relaxation through an extended theoretical model.

Contribution

It introduces an extended Tavis-Cummings model to analyze spin-orbit effects, including dark state relaxation and the creation of triplet polaritons in organic microcavities.

Findings

Spin-orbit coupling splits the lower polariton into two branches.

A triplet polariton state can form when in resonance with triplet excitons.

Disorder enables weak coupling between bright and dark excitons, affecting relaxation pathways.

Abstract

Using an extended Tavis-Cummings model, we study the effect of the spin-orbit coupling between the singlet and the triplet molecular excitons in organic microcavities in the strong coupling regime. The model is solved in the single excitation space for polaritons, which contains the bright (permutation symmetric) singlet and triplet excitons, as well as the dark bands consisting of the nonsymmetric excitons of either type. We find that the spin-orbit coupling splits the lower polariton into two branches, and also creates a triplet polariton when the cavity mode is in resonance with the triplet excitons. The optical absorption spectrum of the system that can reveal this splitting in experiments is presented and the effect of disorder in exciton energies and couplings is explored. An important consequence of the disorder in the spin-orbit coupling -- a weak coupling between the otherwise decoupled bright and dark sectors -- is explored and detailed calculations of the squared transition matrix elements between the dark bands and polaritons are presented along with derivation of some approximate yet quite accurate analytical expressions. This relaxation channel for the dark states contains an interference between two transition paths that, for a given polariton state, suppresses the relaxation of one dark band and enhances it for the other.