Ultrafast Thermal Modification of Strong Coupling in an Organic Microcavity

TL;DR

This study demonstrates that ultrafast thermal effects in organic microcavities can transiently modify strong coupling conditions, revealing potential for cavity polaritons as sensors for non-equilibrium phenomena.

Contribution

It introduces a method to use cavity polaritons as sensitive probes for ultrafast thermal and electronic dynamics in organic microcavities.

Findings

Transient visible spectral response induced by infrared excitation.

Ultrafast heating modifies the effective refractive index and strong coupling.

No real polariton population exists during the transient response.

Abstract

There is growing interest in using strongly coupled organic microcavities to tune molecular dynamics, including the electronic and vibrational properties of molecules. However, very little attention has been paid to the utility of cavity polaritons as sensors for out-of-equilibrium phenomena, including thermal excitations. Here, we demonstrate that non-resonant infrared excitation of an organic microcavity system induces a transient response in the visible spectral range near the cavity polariton resonances. We show how these optical response can be understood in terms of ultrafast heating of electrons in the metal cavity mirror, which modifies the effective refractive index and subsequently the strong coupling conditions. The temporal dynamics of the microcavity are strictly determined by carriers in the metal, including the cooling of electrons via electron-phonon coupling and excitation of propagating coherent acoustic modes in the lattice. We rule out multiphoton excitation processes and verify that no real polariton population exists despite their strong transient features. These results suggest the promise of cavity polaritons as sensitive probes of non-equilibrium phenomena.