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Visualizing and controlling vibrational wave packets of single molecules

Title data

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. Vol. 465 (2010) Issue 7300 . - 905 - 908.
ISSN 1476-4687
DOI: https://doi.org/10.1038/nature09110

Abstract in another language

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.

Further data

Item Type: Article in a journal
Refereed: Yes
Keywords: fluorescence spectroscopy; low molecular weight system; single molecule; terrylene; time resolved spectroscopy; wave packet
Institutions of the University: Faculties > Faculty of Mathematics, Physics und Computer Science > Department of Physics > Lehrstuhl Experimentalphysik IX - Spektroskopie weicher Materie
Profile Fields > Advanced Fields > Polymer and Colloid Science
Faculties
Faculties > Faculty of Mathematics, Physics und Computer Science
Faculties > Faculty of Mathematics, Physics und Computer Science > Department of Physics
Profile Fields
Profile Fields > Advanced Fields
Result of work at the UBT: No
DDC Subjects: 500 Science > 530 Physics
Date Deposited: 20 Apr 2015 06:52
Last Modified: 16 Apr 2018 11:30
URI: https://eref.uni-bayreuth.de/id/eprint/10531