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O: Fachverband Oberflächenphysik
O 58: Plasmonics and Nanooptics II: Light-Matter Interaction and Spectroscopy I
O 58.2: Talk
Wednesday, March 29, 2023, 15:15–15:30, WIL A317
Two-Dimensional Electronic Spectroscopy of Strong Exciton-Surface Plasmon Polariton Coupling — •Daniel Timmer1, Moritz Gittinger1, Thomas Quenzel1, Sven Stephan1, Jennifer Zablocki2, Arne Lützen2, Jin-Hui Zhong1, Martin Silies1, Antonietta De Sio1, and Christoph Lienau1 — 1University of Oldenburg, Germany — 2University of Bonn, Germany
The creation of hybrid light-matter systems due to strong coupling is of major current interest for material science. Of special interest are dipolar interactions between molecular excitons (X) and plasmonic resonators, such as surface plasmon polaritons (SPP). Sufficiently strong coupling to vacuum field fluctuations allows for the coherent flow of energy between X and SPP, i.e. Rabi oscillations, forming new hybridized upper (UP) and lower (LP) polariton states [1]. We explore these strong coupling phenomena and especially their dynamics using two-dimensional electronic spectroscopy (2DES). Here, strong coupling predicts notorious "oscillating cross-peaks" between diagonal UP and LP peaks in a 2DES map. We investigate the polariton dynamics of a prototypical system for X-SPP coupling, a J-aggregate coated periodic gold slit array. In our measurements, the strongly coupled system indeed shows these hallmarks: Rabi oscillations of 2DES cross-peaks. Surprisingly, however, spatial modulations of the plasmon field seem to result in both strongly and weakly coupled excitons, which can then undergo coherent population transfer via the SPP. This conclusion is further supported by FDTD and Frenkel exciton model simulations. [1]: Vasa, Parinda, et al., Nat. Photon 7.2, 128-132 (2013).