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

  • Filatov, Michael; 
  • Paolino, Marco; 
  • Pierron, Robin; 
  • Cappelli, Andrea; 
  • Giorgi, Gianluca; 
  • 외 7명
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초록

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. Improving the efficiency of light-driven molecular rotary motors is a challenging task. Here, the authors combine theoretical modeling, synthesis and spectroscopy to prepare a prototype molecular motor capable of avoiding inefficient thermally activated motion; thus offering prospects to implement a 2-stroke photon-only molecular motor.

키워드

DENSITY-FUNCTIONAL THEORY; REFERENCED KOHN-SHAM; FRACTIONALLY OCCUPIED STATES; UNIDIRECTIONAL ROTATION; CONICAL INTERSECTIONS; DYNAMICS; PHOTOISOMERIZATION; SPEED; ENSEMBLES; ENERGIES
제목
Towards the engineering of a photon-only two-stroke rotary molecular motor
저자
Filatov, Michael; Paolino, Marco; Pierron, Robin; Cappelli, Andrea; Giorgi, Gianluca; Leonard, Jeremie; Huix-Rotllant, Miquel; Ferre, Nicolas; Yang, Xuchun; Kaliakin, Danil; Blanco-Gonzalez, Alejandro; Olivucci, Massimo
DOI
10.1038/s41467-022-33695-x
발행일
2022-10-28
유형
Article
저널명
Nature Communications
권
13
호
1