Coherence and interaction in confined room-temperature polariton condensates with Frenkel excitons

Abstract

The strong light-matter coupling of a microcavity mode to tightly bound Frenkel excitons in organic materials emerged as a versatile, room-temperature compatible platform to study nonlinear many-particle physics and bosonic condensation. However, various aspects of the optical response of Frenkel excitons in this regime remained largely unexplored. Here, we utilize a hemispheric optical cavity filled with the fluorescent protein mCherry to address two important questions in the field of room-temperature polariton condensates. First, combining the high quality factor of the microcavity with a well-defined mode structure allows us to provide a definite answer whether temporal coherence in such systems can become competitive with their low-temperature counterparts. We observe highly monochromatic and coherent light beams emitted from the condensate, characterized by a coherence time greater than 150 ps, which exceeds the polariton lifetime by two orders of magnitude. Second, the high quality of our device allows to sensibly trace the emission energy of the condensate, and thus to establish a fundamental picture which quantitatively explains the core nonlinear processes yielding the characteristic density-dependent blueshift. We find that the energy shift of Frenkel excitonpolaritons is largely dominated by the reduction of the Rabi-splitting due to phase space filling effects, which is influenced by the redistribution of polaritons in the system. While our finding of highly coherent condensation at ambient conditions addresses the suitability of organic polaritonics regarding their utilization as highly coherent room temperature polariton lasers, shedding light on the non-linearity is of great benefit towards implementing non-linear devices, optical switches, and lattices based on exciton-polaritons at room temperature.