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  Coherent control of the isomerization of retinal in bacteriorhodopsin in the high intensity regime

Prokhorenko, V., Halpin, A., Johnson, P. J. M., Miller, R. J. D., & Brown, L. S. (2011). Coherent control of the isomerization of retinal in bacteriorhodopsin in the high intensity regime. The Journal of Chemical Physics, 134(8): 085105. doi:10.1063/1.3554743.

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 Urheber:
Prokhorenko, Valentyn1, 2, 3, Autor           
Halpin, Alexei1, 2, 3, Autor
Johnson, Philip J. M.1, 2, 3, Autor
Miller, R. J. Dwayne1, 2, 3, Autor           
Brown, Leonid S.4, Autor
Affiliations:
1Atomically Resolved Structural Dynamics Division, Max Planck Research Department for Structural Dynamics, Department of Physics, University of Hamburg, External Organizations, ou_2173636              
2Center for Free Electron Laser Science, Notkestr. 85, 22607 Hamburg, Germany, ou_persistent22              
3Departments of Physics and Chemistry, and the Institute for Optical Sciences, University of Toronto, 80 St. George St., Toronto, Ontario M5S 3H6, Canada, ou_persistent22              
4Department of Physics, University of Guelph, Guelph, Ontario N1G 2W1, Canada, ou_persistent22              

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Schlagwörter: Chirping; Isomerization; Excitation energies; Absorption spectra; Excited states
 Zusammenfassung: Coherent control protocols provide a direct experimental determination of the relative importance of quantum interference or phase relationships of coupled states along a selected pathway. These effects are most readily observed in the high intensity regime where the field amplitude is sufficient to overcome decoherence effects. The coherent response of retinal photoisomerization in bacteriorhodopsin to the phase of the photoexcitation pulses was examined at fluences of 1015 – 2.5 × 1016 photons per square centimeter, comparable to or higher than the saturation excitation level of the S0 − S1 retinal electronic transition. At moderate excitation levels of ∼6 × 1015 photons/cm2 (<100 GW/cm2), chirping the excitation pulses increases the all-trans to 13-cisisomerization yield by up to 16% relative to transform limited pulses. The reported results extend previous weak-field studies [Prokhorenko et al., Science 313, 1257 (2006)] and further illustrate that quantum coherence effects persist along the reaction coordinate in strong fields even for systems as complex as biological molecules. However, for higher excitation levels of ∼200 GW/cm2, there is a dramatic change in photophysics that leads to multiphoton generated photoproducts unrelated to the target isomerizationreaction channel and drastically changes the observed isomerization kinetics that appears, in particular, as a red shift of the transient spectra. These results explain the apparent contradictions of the work by Florean et al. [Proc. Natl. Acad. Sci. U.S.A. 106, 10896 (2009)] in the high intensity regime. We are able to show that the difference in observations and interpretation is due to artifacts associated with additional multiphoton-induced photoproducts. At the proper monitoring wavelengths, coherent control in the high intensity regime is clearly observable. The present work highlights the importance of conducting coherent control experiments in the low intensity regime to access information on quantum interference effects along specific reaction coordinates.

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Sprache(n): eng - English
 Datum: 2010-11-192011-01-202011-02-232011-02-28
 Publikationsstatus: Erschienen
 Seiten: 10
 Ort, Verlag, Ausgabe: -
 Inhaltsverzeichnis: -
 Art der Begutachtung: Expertenbegutachtung
 Identifikatoren: DOI: 10.1063/1.3554743
 Art des Abschluß: -

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Titel: The Journal of Chemical Physics
  Andere : J. Chem. Phys.
Genre der Quelle: Zeitschrift
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Ort, Verlag, Ausgabe: Woodbury, N.Y. : American Institute of Physics
Seiten: - Band / Heft: 134 (8) Artikelnummer: 085105 Start- / Endseite: - Identifikator: ISSN: 0021-9606
CoNE: https://pure.mpg.de/cone/journals/resource/954922836226