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Visualizing and controlling vibrational wave packets of single molecules


Brinks, Daan ; Stefani, Fernando D. ; Kulzer, Florian ; Hildner, Richard ; Taminiau, Tim H. ; Avlasevich, Yuri ; Müllen, Klaus ; van Hulst, Niek F.:
Visualizing and controlling vibrational wave packets of single molecules.
In: Nature. Bd. 465 (2010) Heft 7300 . - 905 - 908.
ISSN 1476-4687
DOI: https://doi.org/10.1038/nature09110


The active steering of the pathways taken by chemical reactions and the optimization of energy conversion processes provide striking examples of the coherent control of quantum interference through the use of shaped laser pulses. Experimentally, coherence is usually established by synchronizing a subset ofmolecules in an ensemble with ultra-short laser pulses. But in complex systems where even chemically identical molecules exist with different conformations and in diverse environments, the synchronized subset will have an intrinsic inhomogeneity that limits the degree of coherent control that can be achieved. A natural - and, indeed, the ultimate - solution to overcoming intrinsic inhomogeneities is the investigation of the behaviour of onemolecule at a time. The single-molecule approach has provided useful insights into phenomena as diverse as biomolecular interactions, cellular processes and the dynamics of supercooled liquids and conjugated polymers. Coherent state preparation of single molecules has so far been restricted to cryogenic conditions, whereas at room temperature only incoherent vibrational relaxation pathways have been probed. Here we report the observation and manipulation of vibrational wave-packet interference in individual molecules at ambient conditions. We show that adapting the time and phase distribution of the optical excitation field to the dynamics of each molecule results in a high degree of control, and expect that the approach can be extended to achieve single-molecule coherent control in other complex inhomogeneous systems.

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Publikationsform: Artikel in einer Zeitschrift
Begutachteter Beitrag: Ja
Keywords: fluorescence spectroscopy; low molecular weight system; single molecule; terrylene; time resolved spectroscopy; wave packet
Institutionen der Universität: Fakultäten > Fakultät für Mathematik, Physik und Informatik > Physikalisches Institut > Lehrstuhl Experimentalphysik IX - Spektroskopie weicher Materie
Profilfelder > Advanced Fields > Polymer- und Kolloidforschung
Fakultäten > Fakultät für Mathematik, Physik und Informatik
Fakultäten > Fakultät für Mathematik, Physik und Informatik > Physikalisches Institut
Profilfelder > Advanced Fields
Titel an der UBT entstanden: Nein
Themengebiete aus DDC: 500 Naturwissenschaften und Mathematik > 530 Physik
Eingestellt am: 20 Apr 2015 06:52
Letzte Änderung: 16 Apr 2018 11:30
URI: https://eref.uni-bayreuth.de/id/eprint/10531