2-methylterrylene in hexadecane: Do we see single rotational quantum jumps of methyl groups?

A. Sigl, Chr Scharnagl, J. Friedrich, A. Gourdon, M. Orrit

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We performed comparative low temperature (2-30 K) hole-burning and single molecule experiments with 2-methylterrylene with the goal to detect single rotational tunneling jumps of methyl groups. The hole-burned spectrum with its sharply structured side features which are perfectly symmetrically arranged with respect to the central hole supports the assignment to rotational tunneling transitions. However, instead of one, three clearly distinguishable methyl groups show up in the spectrum. Based on molecular mechanics simulations we attribute them to different, nearly degenerate orientations of guest molecules in one specific site of the hexadecane lattice. The frequency distribution of spontaneous jumps of single molecules reflects the features of the hole-burned spectra, although the distribution in the single molecule experiments is significantly broader. The photoinduced frequency transformation of single molecules ("single molecule photobleaching experiments") fits to the features of the hole-burned spectra, except that, surprisingly, no significant number of spectral jumps could be generated in the frequency range where the prominent narrow antiholes are observed in the hole-burned spectra.

Original languageEnglish
Article number044508
JournalJournal of Chemical Physics
Issue number4
StatePublished - 2008


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