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Excited-State Dynamics of Carotenoids in Light-Harvesting Complexes. 2. Dissecting Pulse Structures from Optimal Control Experiments

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Faculty of Sciences, Vrije Universiteit Amsterdam, De Boelelaan 1081, 1081 HV Amsterdam, The Netherlands, Faculty of Physics, Vilnius University, Sauletekio Avenue 9, Block 3, 10222 Vilnius, Lithuania, Institute of Physics, Savanoriu Avenue 231, 02300 Vilnius, Lithuania, Institute of Biomedical & Life Sciences, University of Glasgow, Glasgow, United Kingdom, and Department of Chemistry University of California, Davis, One Shields Avenue, Davis, California 95616
Cite this: J. Phys. Chem. B 2006, 110, 11, 5737–5746
Publication Date (Web):February 28, 2006
https://doi.org/10.1021/jp054634+
Copyright © 2006 American Chemical Society

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    Abstract

    Dispersed multipump−probe (PPP) spectroscopy was used to explore the role of saturation, annihilation, and structured pulses in recent coherent control experiments on the light-harvesting 2 complex from Rhodopseudomonas acidophila (Herek et al. Nature2002, 417, 533). We discuss the complimentary aspects between the PPP technique and coherent control studies, in particular the ability to dissect complicated pulse structures and the utility in exploring incoherent mechanisms. With the aid of a simple multistate model involving only population dynamics, we illustrate how the optimized structured pulses may be explained in terms of an interplay between excited-state populations, saturation, and annihilation. Furthermore, we discuss the experimental conditions that are required for incoherent effects to contribute to control experimental signals, with particular emphasis on pulse intensities, and show that the optimization of a ratio of conservative signals (i.e., not modulated by external dynamics) is required to exclude saturation effects from coherent control studies.

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     Vrije Universiteit Amsterdam.

     Vilnius University.

    §

     Institute of Physics.

     University of Glasgow.

    *

     Author to whom correspondence should be addressed. E-mail:  [email protected].

     University of California, Davis.

    Supporting Information Available

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    Multipump signals from the LH2 complex isolated from Rb. sphaeroides, annihilation parameters, turnovers in action simulated traces, and potential mechanisms. This material is available free of charge via the Internet at http://pubs.acs.org.

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