Mapping the Excited‐State Potential Energy Surface of a Photomolecular Motor

Hall, Christopher R, Browne, Wesley R., Feringa, Ben L. and Meech, Stephen R. (2018) Mapping the Excited‐State Potential Energy Surface of a Photomolecular Motor. Angewandte Chemie International Edition, 57 (21). pp. 6203-6207. ISSN 1433-7851

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      Abstract

      A detailed understanding of the operation and efficiency of unidirectional photomolecular rotary motors is essential for their effective exploitation in molecular nanomachines. Unidirectional motion relies on light‐driven conversion from a stable (1 a) to a metastable (1 b) conformation, which then relaxes through a thermally driven helix inversion in the ground state. The excited‐state surface has thus far only been experimentally characterised for 1 a. Here we probe the metastable, 1 b, excited state, utilising ultrafast transient absorption and femtosecond stimulated Raman spectroscopy. These reveal that the “dark” excited‐state intermediate between 1 a and 1 b has a different lifetime and structure depending on the initial ground‐state conformation excited. This suggests that the reaction coordinate connecting 1 a to 1 b differs to that for the reverse photochemical process. The result is contrasted with earlier calculations.

      Item Type: Article
      Uncontrolled Keywords: energy conversion,excited states,molecular motors,photochemistry,ultrafast dynamics
      Faculty \ School: Faculty of Science > School of Chemistry
      Depositing User: Pure Connector
      Date Deposited: 10 Apr 2018 16:30
      Last Modified: 05 Sep 2018 16:32
      URI: https://ueaeprints.uea.ac.uk/id/eprint/66735
      DOI: 10.1002/anie.201802126

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