Plasmon mediated coherent population oscillations in molecular aggregates

Daniel Timmer, Moritz Gittinger, Thomas Quenzel, Sven Stephan, Yu Zhang, Marvin F. Schumacher, Arne Lützen, Martin Silies, Sergei Tretiak, Jin-Hui Zhong, Antonietta De Sio and Christoph Lienau ()
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Daniel Timmer: Carl von Ossietzky Universität
Moritz Gittinger: Carl von Ossietzky Universität
Thomas Quenzel: Carl von Ossietzky Universität
Sven Stephan: Carl von Ossietzky Universität
Yu Zhang: Theoretical Division, Los Alamos National Laboratory
Marvin F. Schumacher: University of Bonn
Arne Lützen: University of Bonn
Martin Silies: Carl von Ossietzky Universität
Sergei Tretiak: Theoretical Division, Los Alamos National Laboratory
Jin-Hui Zhong: Carl von Ossietzky Universität
Antonietta De Sio: Carl von Ossietzky Universität
Christoph Lienau: Carl von Ossietzky Universität

Nature Communications, 2023, vol. 14, issue 1, 1-10

Abstract: 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.

Date: 2023
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DOI: 10.1038/s41467-023-43578-4

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