Plexciton dynamics: exciton-plasmon coupling in a J-aggregate-Au nanoshell complex provides a mechanism for nonlinearity

Nche T Fofang, Nathaniel K Grady, Zhiyuan Fan, Alexander O Govorov, Naomi J Halas
Nano Letters 2011 April 13, 11 (4): 1556-60
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.

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