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|Title:||An Artificial Molecular Switch that Mimics the Visual Pigment and Completes its Photocycle in Picoseconds||Authors:||Sinicropi, Adalgisa
|Keywords:||CASPT2//CASSCF; mid-IR; photochemical switch; time resolved spectroscopy; UV-vis||Issue Date:||2008||Project:||None||Journal:||PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA||Abstract:||
Single molecules that act as light-energy transducers (e.g., con-verting 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 trans-duction 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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