Controlling the Manifold of Polariton States Through Molecular Disorder
arXiv:2309.13178 · doi:10.1002/adom.202302387
Abstract
Exciton polaritons, arising from the interaction of electronic transitions with confined electromagnetic fields, have emerged as a powerful tool to manipulate the properties of organic materials. However, standard experimental and theoretical approaches overlook the significant energetic disorder present in most materials now studied. Using the conjugated polymer P3HT as a model platform, we systematically tune the degree of energetic disorder and observe a corresponding redistribution of photonic character within the polariton manifold. Based on these subtle spectral features, we develop a more generalized approach to describe strong light-matter coupling in disordered systems that captures the key spectroscopic observables and provides a description of the rich manifold of states intermediate between bright and dark. Applied to a wide range of organic systems, our method challenges prevailing notions about ultrastrong coupling and whether it can be achieved with broad, disordered absorbers.
References in corpus (8)
- The role of intermolecular coupling in the photophysics of disordered organic semiconductors: Aggregate emission in regioregular polythiophene
- Dressed Collective Qubit States and the Tavis-Cummings Model in Circuit QED
- Tuning the coherent propagation of organic exciton-polaritons through dark state delocalization
- Unusual Dynamical Properties of Disordered Polaritons in Micocavities
- Disorder enhanced vibrational entanglement and dynamics in polaritonic chemistry
- Effects of disorder on polaritonic and dark states in a cavity using the disordered Tavis-Cummings model
- Organic charged polaritons in the ultrastrong coupling regime
- Spin-orbit coupling in organic microcavities: Lower polariton splitting, triplet polaritons, and disorder-induced dark-states relaxation