English
 
User Manual Privacy Policy Disclaimer Contact us
  Advanced SearchBrowse

Item

ITEM ACTIONSEXPORT
  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.

Item is

Basic

show hide
Item Permalink: http://hdl.handle.net/11858/00-001M-0000-0028-1F98-1 Version Permalink: http://hdl.handle.net/11858/00-001M-0000-0028-1FA3-9
Genre: Journal Article

Files

show Files
hide Files
:
1.3554743.pdf (Publisher version), 898KB
Name:
1.3554743.pdf
Description:
-
Visibility:
Public
MIME-Type / Checksum:
application/pdf / [MD5]
Technical Metadata:
Copyright Date:
2011
Copyright Info:
© American Institute of Physics. This article may be downloaded for personal use only. Any other use requires prior permission of the author and the American Institute of Physics.
License:
-

Locators

show
hide
Locator:
http://dx.doi.org/10.1063/1.3554743 (Publisher version)
Description:
-

Creators

show
hide
 Creators:
Prokhorenko, Valentyn1, 2, 3, Author              
Halpin, Alexei1, 2, 3, Author
Johnson, Philip J. M.1, 2, 3, Author
Miller, R. J. Dwayne1, 2, 3, Author              
Brown, Leonid S.4, Author
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              

Content

show
hide
Free keywords: Chirping; Isomerization; Excitation energies; Absorption spectra; Excited states
 Abstract: 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.

Details

show
hide
Language(s): eng - English
 Dates: 2010-11-192011-01-202011-02-232011-02-28
 Publication Status: Published in print
 Pages: 10
 Publishing info: -
 Table of Contents: -
 Rev. Method: Peer
 Identifiers: DOI: 10.1063/1.3554743
 Degree: -

Event

show

Legal Case

show

Project information

show

Source 1

show
hide
Title: The Journal of Chemical Physics
  Other : J. Chem. Phys.
Source Genre: Journal
 Creator(s):
Affiliations:
Publ. Info: Woodbury, N.Y. : American Institute of Physics
Pages: - Volume / Issue: 134 (8) Sequence Number: 085105 Start / End Page: - Identifier: ISSN: 0021-9606
CoNE: /journals/resource/954922836226