Plexciton Dynamics: Exciton−Plasmon Coupling in a J-Aggregate−Au Nanoshell Complex Provides a Mechanism for Nonlinearity

Abstract

Coherently coupled plasmons and excitons give rise to new optical excitations- plexcitons − due to the strong coupling of these two oscillator systems. Time-resolved studies of J-aggregate-Au nanoshell complexes when the nanoshell plasmon and J-aggregate exciton energies are degenerate probe the dynamical behavior of this coupled system. Transient absorption of the interacting plasmon-exciton system is observed, in dramatic contrast to the photoinduced transmission of the pristine J-aggregate. An additional, transient Fano-shaped modulation within the Fano dip is also observable. The behavior of the J-aggregate-Au nanoshell complex is described by a combined one-exciton and two-exciton state model coupled to the nanoshell plasmon.