Dresden 2020 – scientific programme
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O: Fachverband Oberflächenphysik
O 18: Plasmonics and Nanooptics II: Ultrafast and Nonlinear Phenomena (joint session O/CPP)
O 18.2: Talk
Monday, March 16, 2020, 15:30–15:45, WIL A317
Time-resolved and spatially-resolved mode dynamics within a plasmonic nanoslit cavity investigated by coherent two-dimensional nanoscopy — Sebastian Pres1, Daniel Friedrich2, Daniel Fersch1, Enno Krauss2, Bernhard Huber1, Victor Lisinetskii1, •Matthias Hensen1, Bert Hecht2, and Tobias Brixner1 — 1Institut für Physikalische und Theoretische Chemie, Universität Würzburg, Am Hubland, 97074 Würzburg, Germany — 2NanoOptics & Biophotonics Group, Experimental Physics 5, University of Würzburg, Am Hubland, 97074 Würzburg, Germany
Recently, we revealed the impact of off-resonant eigenmodes on the local field dynamics of plasmonic hot-spots within a single nanoslit cavity with a spatial and temporal resolution of 10 nm and 20 fs, respectively, by combining photoemission electron microscopy and interferometric two-pulse sequences [1]. Here, we extend the excitation scheme of the nanoslit cavity to a three-pulse sequence using an LCD-based pulse shaper to perform two-dimensional spectroscopy with unprecedented spatial resolution [2]. Due to the nonlinearity of the photoelectron emission process higher-order signals are easily disclosed. These results are supported by quantum dynamical simulations in which the plasmonic nanoslit is modelled as a quantized harmonic oscillator instead of classical fields. Detecting such signal contributions will be helpful in future experiments to reveal the impact of many-body interactions in molecular or solid-state systems with nanometer resolution.
[1] M. Hensen et al., Nano Lett. 19, 4651 (2019)
[2] B. Huber et al., Rev. Sci. Intrum. 90, 113103 (2019)