Ultrafast motion in a third generation photomolecular motor

Roy, Palas, Browne, Wesley R., Feringa, Ben L. and Meech, Stephen R. ORCID: https://orcid.org/0000-0001-5561-2782 (2023) Ultrafast motion in a third generation photomolecular motor. Nature Communications, 14. ISSN 2041-1723

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Abstract

Controlling molecular translation at the nanoscale is a key objective for development of synthetic molecular machines. Recently developed third generation photochemically driven molecular motors (3GMs), comprising pairs of overcrowded alkenes capable of cooperative unidirectional rotation offer the possibility of converting light energy into translational motion. Further development of 3GMs demands detailed understanding of their excited state dynamics. Here we use time-resolved absorption and emission to track population and coherence dynamics in a 3GM. Femtosecond stimulated Raman reveals real-time structural dynamics as the excited state evolves from a Franck-Condon bright-state through weakly-emissive dark-state to the metastable product, yielding new insight into the reaction coordinate. Solvent polarity modifies the photoconversion efficiency suggesting charge transfer character in the dark-state. The enhanced quantum yield correlates with suppression of a low-frequency flapping motion in the excited state. This detailed characterization facilitates development of 3GMs, suggesting exploitation of medium and substituent effects to modulate motor efficiency.

Item Type:	Article
Additional Information:	Acknowledgements: Financial support provided by The Netherlands Ministry of Education, Culture and Science (Gravity Program 024.001.035 to WRB, BLF) and the EPSRC (grants EP/R042357/1, EP/J009148/1 to SRM) is acknowledged.
Uncontrolled Keywords:	general,physics and astronomy(all),chemistry(all),biochemistry, genetics and molecular biology(all),3*,good journal and high quality data though limited novelty ,/dk/atira/pure/subjectarea/asjc/1000
Faculty \ School:	Faculty of Science > School of Chemistry
UEA Research Groups:	Faculty of Science > Research Groups > Centre for Photonics and Quantum Science Faculty of Science > Research Groups > Chemistry of Light and Energy
Related URLs:	http://www.scopus.com/inward/record.url?...
Depositing User:	LivePure Connector
Date Deposited:	16 Feb 2023 09:30
Last Modified:	09 Mar 2024 09:31
URI:	https://ueaeprints.uea.ac.uk/id/eprint/91148
DOI:	10.1038/s41467-023-36777-6

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