Ultrafast dynamics in the power stroke of a molecular rotary motor

Conyard, Jamie, Addison, Kiri, Heisler, Ismael A., Cnossen, Arjen, Browne, Wesley R., Feringa, Ben L. and Meech, Stephen R. ORCID: https://orcid.org/0000-0001-5561-2782 (2012) Ultrafast dynamics in the power stroke of a molecular rotary motor. Nature Chemistry, 4 (7). pp. 547-551. ISSN 1755-4330

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Abstract

Light-driven molecular motors convert light into mechanical energy through excited-state reactions. Unidirectional rotary molecular motors based on chiral overcrowded alkenes operate through consecutive photochemical and thermal steps. The thermal (helix inverting) step has been optimized successfully through variations in molecular structure, but much less is known about the photochemical step, which provides power to the motor. Ultimately, controlling the efficiency of molecular motors requires a detailed picture of the molecular dynamics on the excited-state potential energy surface. Here, we characterize the primary events that follow photon absorption by a unidirectional molecular motor using ultrafast fluorescence up-conversion measurements with sub 50 fs time resolution. We observe an extraordinarily fast initial relaxation out of the Franck–Condon region that suggests a barrierless reaction coordinate. This fast molecular motion is shown to be accompanied by the excitation of coherent excited-state structural motion. The implications of these observations for manipulating motor efficiency are discussed.

Item Type:	Article
Faculty \ School:	Faculty of Science > School of Chemistry
UEA Research Groups:	Faculty of Science > Research Groups > Chemistry of Light and Energy Faculty of Science > Research Groups > Physical and Analytical Chemistry (former - to 2017) Faculty of Science > Research Groups > Centre for Photonics and Quantum Science
Depositing User:	Users 2731 not found.
Date Deposited:	07 Jan 2013 16:38
Last Modified:	18 Aug 2023 20:30
URI:	https://ueaeprints.uea.ac.uk/id/eprint/40704
DOI:	10.1038/NCHEM.1343

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