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Issue 15, 2008
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Shaping femtosecond coherent anti-Stokes Raman spectra using optimal control theory

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Abstract

Optimal control theory is used to tailor laser pulses which enhance a femtosecond time-resolved coherent anti-Stokes Raman scattering (fs-CARS) spectrum in a certain frequency range. For this aim the optimal control theory has to be applied to a target state distributed in time. Explicit control mechanisms are given for shaping either the Stokes or the probe pulse in the four-wave mixing process. A simple molecule for which highly accurate potential energy surfaces are available, namely molecular iodine, is used to test the procedure. This approach of controlling vibrational motion and delivering higher intensities to certain frequency ranges might also be important for the improvement of CARS microscopy.

Graphical abstract: Shaping femtosecond coherent anti-Stokes Raman spectra using optimal control theory

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Publication details

The article was received on 18 Sep 2007, accepted on 19 Dec 2007 and first published on 06 Feb 2008


Article type: Paper
DOI: 10.1039/B714268D
Citation: Phys. Chem. Chem. Phys., 2008,10, 2058-2066
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    Shaping femtosecond coherent anti-Stokes Raman spectra using optimal control theory

    S. Pezeshki, M. Schreiber and U. Kleinekathöfer, Phys. Chem. Chem. Phys., 2008, 10, 2058
    DOI: 10.1039/B714268D

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