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Single-molecule optical switching of terrylene in p-terphenyl

Abstract

The controlled manipulation and switching of single atoms and molecules raise the prospect of ultra-high-density data storage. Switching by motion of a single atom has been reported1, and techniques of single-molecule optical detection and spectroscopy2 in the condensed phase have been refined to a degree that allows the modification of the absorption properties of a single chromophore3. Light-induced jumps in single-molecule excitation frequencies have been reported3,4,5, but in none of these cases could the process be controlled: the jumps varied from molecule to molecule, they were interrupted by spontaneous jumps, and the new excitation frequencies could not be identified unambiguously. Here we report light-induced reversible frequency jumps ofsingle molecules of the aromatic hydrocarbon terrylene embedded in a particular site of a p-terphenyl host crystal6 at temperatures of around 2 K. The changes in absorption frequency for different terrylene molecules were identical (within 0.5%) for all samples studied. Thus we were able to switch single-molecule absorption lines in a controlled way between well-defined frequency positions.

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Figure 1: Light-induced, reversible frequency jumps of the fluorescence excitation lines of two single terrylene molecules in a p-terphenyl crystal at T = 1.4 K.
Figure 2: 24-hour spectral trace of the terrylene molecule marked with an asterisk in Fig. 1 (T = 1.4 K).
Figure 3: a, Low-frequency part of the fluorescence emission spectra of terrylene in p-terphenyl at T = 2.4 K excited at the 0–0′ transition frequencies of the sites X1, XY, XY″ and XY″′.

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Acknowledgements

We thank C. Kryschi for discussions. This work was supported by the Deutsche Forschungsgemeinschaft.

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Kulzer, F., Kummer, S., Matzke, R. et al. Single-molecule optical switching of terrylene in p-terphenyl. Nature 387, 688–691 (1997). https://doi.org/10.1038/42674

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