Single-Molecule Pump-Probe Detection Resolves Ultrafast Pathways in Individual and Coupled Quantum Systems

Dijk van, Erik M.H.P. and Hernando, Jordi and Garcia-Lopez, Juan José and Crego-Calama, Mercedes and Reinhoudt, David N. and Kuipers, Laurens and Garcia-Parajo, Maria F. and Hulst van, Niek F. (2005) Single-Molecule Pump-Probe Detection Resolves Ultrafast Pathways in Individual and Coupled Quantum Systems. Physical Review Letters, 94 (7). 078302. ISSN 0031-9007

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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.
Item Type:	Article
Copyright:	© 2005 The American Physical Society
Research Group:	Supramolecular Chemistry and Technology (SMCT) Optical Sciences (OS)
Link to this item:	http://purl.utwente.nl/publications/50958
Official URL:	http://dx.doi.org/10.1103/PhysRevLett.94.078302
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