Single molecule pump-probe detection resolves ultrafast pathways in individual and coupled quantum systems

E.M.H.P. van Dijk, J. Hernando Campos, J.J. Garcia lopez, Mercedes Crego Calama, David Reinhoudt, L. Kuipers, M.F. Garcia Parajo, N.F. van Hulst

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Abstract

We report the first experimental study of individual molecules with femtosecond time resolution using a novel ultrafast single-molecule pump-probe method. A wide range of relaxation times from below 100 up to 400 fs is found, revealing energy redistribution over different vibrational modes and phonon coupling to the nanoenvironment. Addressing quantum-coupled molecules we find longer decay times, pointing towards inhibited intramolecular decay due to delocalized excitation. Interestingly, each individual system shows discrete jumps in femtosecond response, reflecting sudden breakup of the coupled superradiant state.
Original languageUndefined
Pages (from-to)078302-
JournalPhysical review letters
Volume94
Issue number7
DOIs
Publication statusPublished - 2005

Keywords

  • IR-50958
  • METIS-229071

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