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Unravelling the electronic structure and dynamics of an isolated molecular rotary motor in the gas-phase

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Abstract

Light-driven molecular motors derived from chiral overcrowded alkenes are an important class of compounds in which sequential photochemical and thermal rearrangements result in unidirectional rotation of one part of the molecule with respect to another. Here, we employ anion photoelectron spectroscopy to probe the electronic structure and dynamics of a unidirectional molecular rotary motor anion in the gas-phase and quantum chemistry calculations to guide the interpretation of our results. We find that following photoexcitation of the first electronically excited state, the molecule rotates around its axle and some population remains on the excited potential energy surface and some population undergoes internal conversion back to the electronic ground state. These observations are similar to those observed in time-resolved measurements of rotary molecular motors in solution. This work demonstrates the potential of anion photoelectron spectroscopy for studying the electronic structure and dynamics of molecular motors in the gas-phase, provides important benchmarks for theory and improves our fundamental understanding of light-activated molecular rotary motors, which can be used to inform the design of new photoactivated nanoscale devices.

Graphical abstract: Unravelling the electronic structure and dynamics of an isolated molecular rotary motor in the gas-phase

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Publication details

The article was received on 03 May 2017, accepted on 27 Jun 2017 and first published on 27 Jun 2017


Article type: Edge Article
DOI: 10.1039/C7SC01997A
Citation: Chem. Sci., 2017, Advance Article
  • Open access: Creative Commons BY license
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    Unravelling the electronic structure and dynamics of an isolated molecular rotary motor in the gas-phase

    R. Beekmeyer, M. A. Parkes, L. Ridgwell, Jamie W. Riley, J. Chen, B. L. Feringa, A. Kerridge and H. H. Fielding, Chem. Sci., 2017, Advance Article , DOI: 10.1039/C7SC01997A

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