Full-wave nonlinear microscopy reveals guided channel for ultrafast polariton transport

Abstract

We show how finite-difference time-domain (FDTD) simulations can be extended to model ultrafast nonlinear microscopy, enabling the prediction of spatially-resolved pump--probe signals in arbitrary electromagnetic environments. Focusing on polariton transport in strongly coupled light--matter systems, we develop a perturbative framework to study the ultrafast propagation of hybrid light--matter excitations in nanophotonic structures. We first apply the framework to a standard distributed Bragg reflector (DBR) cavity, reproducing established results for polariton transport from a multimode Tavis--Cummings model. We then consider the full modal landscape of the same cavity, including guided modes below the light line that are typically neglected in single-mode-family descriptions. Exploiting these modes, we design compact mode converters that transfer radiative cavity polaritons into photon-like guided polaritons and back, utilizing the guided modes for low-loss propagation. Despite molecular dephasing, this enables transport of molecular excitation over a millimeter, an order of magnitude beyond current transport experiments. We further compute the pump--probe differential transmission signal, providing an experimental signature of the mechanism. Our results show that the modal landscape of a photonic cavity can be engineered to bypass limitations commonly assumed to be intrinsic to the transport of molecular polaritons.