Towards the engineering of a photon-only two-stroke rotary molecular motor

Michael Filatov(Gulak) (), Marco Paolino (), Robin Pierron, Andrea Cappelli, Gianluca Giorgi, Jérémie Léonard (), Miquel Huix-Rotllant, Nicolas Ferré, Xuchun Yang, Danil Kaliakin, Alejandro Blanco-González and Massimo Olivucci ()
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Michael Filatov(Gulak): Kyungpook National University
Marco Paolino: Università di Siena
Robin Pierron: Université de Strasbourg, CNRS UMR 7504
Andrea Cappelli: Università di Siena
Gianluca Giorgi: Università di Siena
Jérémie Léonard: Université de Strasbourg, CNRS UMR 7504
Miquel Huix-Rotllant: Aix-Marseille Université, CNRS
Nicolas Ferré: Aix-Marseille Université, CNRS
Xuchun Yang: Bowling Green State University
Danil Kaliakin: Bowling Green State University
Alejandro Blanco-González: Bowling Green State University
Massimo Olivucci: Università di Siena

Nature Communications, 2022, vol. 13, issue 1, 1-10

Abstract: Abstract The rational engineering of photoresponsive materials, e.g., light-driven molecular motors, is a challenging task. Here, we use structure-related design rules to prepare a prototype molecular rotary motor capable of completing an entire revolution using, exclusively, the sequential absorption of two photons; i.e., a photon-only two-stroke motor. The mechanism of rotation is then characterised using a combination of non-adiabatic dynamics simulations and transient absorption spectroscopy measurements. The results show that the rotor moiety rotates axially relative to the stator and produces, within a few picoseconds at ambient T, an intermediate with the same helicity as the starting structure. We discuss how such properties, that include a 0.25 quantum efficiency, can help overcome the operational limitations of the classical overcrowded alkene designs.

Date: 2022
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DOI: 10.1038/s41467-022-33695-x

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