An artificial molecular switch that mimics the visual pigment and completes its photocycle in picoseconds

Single molecules that act as light-energy transducers (e.g., converting the energy of a photon into atomic-level mechanical motion) are examples of minimal molecular devices. Here, we focus on a molecular switch designed by merging a conformationally locked diarylidene skeleton with a retinal-like S...

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Veröffentlicht in:Proceedings of the National Academy of Sciences - PNAS Jg. 105; H. 46; S. 17642
Hauptverfasser: Sinicropi, Adalgisa, Martin, Elena, Ryazantsev, Mikhail, Helbing, Jan, Briand, Julien, Sharma, Divya, Léonard, Jérémie, Haacke, Stefan, Cannizzo, Andrea, Chergui, Majed, Zanirato, Vinicio, Fusi, Stefania, Santoro, Fabrizio, Basosi, Riccardo, Ferré, Nicolas, Olivucci, Massimo
Format: Journal Article
Sprache:Englisch
Veröffentlicht: United States 18.11.2008
Schlagworte:
Isomerism
Molecular Mimicry
Photochemistry
Retinal Pigments - chemistry
Spectrophotometry, Ultraviolet
Spectroscopy, Fourier Transform Infrared
Time Factors
ISSN:1091-6490, 1091-6490
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Zusammenfassung:Single molecules that act as light-energy transducers (e.g., converting the energy of a photon into atomic-level mechanical motion) are examples of minimal molecular devices. Here, we focus on a molecular switch designed by merging a conformationally locked diarylidene skeleton with a retinal-like Schiff base and capable of mimicking, in solution, different aspects of the transduction of the visual pigment Rhodopsin. Complementary ab initio multiconfigurational quantum chemistry-based computations and time-resolved spectroscopy are used to follow the light-induced isomerization of the switch in methanol. The results show that, similar to rhodopsin, the isomerization occurs on a 0.3-ps time scale and is followed by <10-ps cooling and solvation. The entire (2-photon-powered) switch cycle was traced by following the evolution of its infrared spectrum. These measurements indicate that a full cycle can be completed within 20 ps.
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ISSN:1091-6490
1091-6490
DOI:10.1073/pnas.0802376105