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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Vydané v:Proceedings of the National Academy of Sciences - PNAS Ročník 105; číslo 46; s. 17642
Hlavní autori: 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
Médium: Journal Article
Jazyk:English
Vydavateľské údaje: United States 18.11.2008
Predmet:
Isomerism
Molecular Mimicry
Photochemistry
Retinal Pigments - chemistry
Spectrophotometry, Ultraviolet
Spectroscopy, Fourier Transform Infrared
Time Factors
ISSN:1091-6490, 1091-6490
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Abstract 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.
AbstractList 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.
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.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.
Author Chergui, Majed
Fusi, Stefania
Olivucci, Massimo
Santoro, Fabrizio
Basosi, Riccardo
Haacke, Stefan
Zanirato, Vinicio
Helbing, Jan
Sinicropi, Adalgisa
Martin, Elena
Ryazantsev, Mikhail
Briand, Julien
Léonard, Jérémie
Cannizzo, Andrea
Ferré, Nicolas
Sharma, Divya
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Snippet 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...
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SubjectTerms Isomerism
Molecular Mimicry
Photochemistry
Retinal Pigments - chemistry
Spectrophotometry, Ultraviolet
Spectroscopy, Fourier Transform Infrared
Time Factors
Title An artificial molecular switch that mimics the visual pigment and completes its photocycle in picoseconds
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