Please use this identifier to cite or link to this item: http://hdl.handle.net/20.500.12779/5486
Title: An Artificial Molecular Switch that Mimics the Visual Pigment and Completes its Photocycle in Picoseconds
Authors: Sinicropi, Adalgisa 
Martin, E.
Ryasantsev, M.
Helbing, J.
Briand, J.
Sharma, D.
Leonard, J.
Haacke, S.
Canizzo, A.
Chergui, M.
Zanirato, V.
Fusi, Stefania 
Santoro, F.
Basosi, Riccardo 
Ferré, N.
Olivucci, Massimo 
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.
Description: 
37054
URI: http://hdl.handle.net/20.500.12779/5486
ISSN: 0027-8424
DOI: 10.1073/pnas.0802376105
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