Berlin 2024 – wissenschaftliches Programm
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O: Fachverband Oberflächenphysik
O 7: Plasmonics and Nanooptics I
O 7.10: Vortrag
Montag, 18. März 2024, 12:45–13:00, MA 043
Plasmon-mediated coherent population oscillations in molecular aggregates — •Daniel Timmer1, Moritz Gittinger1, Thomas Quenzel1, Sven Stephan1, Yu Zhang2, Marvin Schumacher3, Arne Lützen3, Martin Silies1, Sergei Tretiak2, Jin-Hui Zhong1, Antonietta De Sio1, and Christoph Lienau1 — 1University of Oldenburg, Germany — 2Los Alamos National Laboratory, USA — 3University of Bonn, Germany
Strong coupling between plasmonic nanostructures and excitonic quantum emitters is a powerful way to alter material properties on the nanoscale. Dipolar coupling of excitons to vacuum field fluctuations of surface plasmon polaritons (SPPs) leads to a periodic energy transfer (Rabi oscillations) and the creation of hybridized polariton states. Often, experiments are limited to linear spectroscopy and time-domain studies of the energy transfer are lacking. We investigate the coherent dynamics of J-aggregate excitons that strongly couple to structured SPP fields of a periodic nanoslit array using two-dimensional electronic spectroscopy (2DES) [1]. Strong coupling predicts that "oscillating cross-peaks" should appear between diagonal polariton peaks. Our experiment indeed resolves these Rabi oscillations. Their analysis reveals that they reflect a coherent transfer between different, spatially separated excitons. The structured SPP field creates two classes of excitons that either couple strongly or weakly. Our study shows that 2DES allows to directly access the quantum dynamics of the strongly couples system, revealing a new and unexpected plasmon-mediated energy transport. [1]: D. Timmer, et al. arXiv:2307.14708 (2023).
Keywords: strong coupling; plasmons; two-dimensional electronic spectroscopy; Rabi oscillations; excitons