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.

Filatov Gulak, M., Paolino, M., Pierron, R., Cappelli, A., Giorgi, G., Léonard, J., et al. (2022). Towards the engineering of a photon-only two-stroke rotary molecular motor. NATURE COMMUNICATIONS, 13(1), 1-10 [10.1038/s41467-022-33695-x].

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

Paolino, Marco
;
Cappelli, Andrea;Giorgi, Gianluca;Olivucci, Massimo
2022-01-01

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.
2022
Filatov Gulak, M., Paolino, M., Pierron, R., Cappelli, A., Giorgi, G., Léonard, J., et al. (2022). Towards the engineering of a photon-only two-stroke rotary molecular motor. NATURE COMMUNICATIONS, 13(1), 1-10 [10.1038/s41467-022-33695-x].
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Utilizza questo identificativo per citare o creare un link a questo documento: https://hdl.handle.net/11365/1219834