Plasmon mediated coherent population oscillations in molecular aggregates

Abstract

The strong coherent coupling of quantum emitters to vacuum fluctuations of the light field offers opportunities for manipulating the optical and transport properties of nanomaterials, with potential applications ranging from ultrasensitive all-optical switching to creating polariton condensates. Often, ubiquitous decoherence processes at ambient conditions limit these couplings to such short time scales that the quantum dynamics of the interacting system remains elusive. Prominent examples are strongly coupled exciton-plasmon systems, which, so far, have mostly been investigated by linear optical spectroscopy. Here, we use ultrafast two-dimensional electronic spectroscopy to probe the quantum dynamics of J-aggregate excitons collectively coupled to the spatially structured plasmonic fields of a gold nanoslit array. We observe rich coherent Rabi oscillation dynamics reflecting a plasmon-driven coherent exciton population transfer over mesoscopic distances at room temperature. This opens up new opportunities to manipulate the coherent transport of matter excitations by coupling to vacuum fields.

References in corpus (5)

• Strong coupling between surface plasmon polaritons and emitters
• Extraordinary exciton conductance induced by strong coupling
• Watching the coherent birth of polaron pairs in conjugated polymers
• The Excitation Ladder of Cavity Polaritons
• Coherent Population Oscillation-Based Light Storage

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• Phase-cycling and double-quantum two-dimensional electronic spectroscopy using a common-path birefringent interferometer
• Engineering strong coupling in ultra-compact photonic crystal/2D material platforms