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Journal of Chemical Physics / Volume 135 / Issue 22 / ARTICLES / Condensed Phase Dynamics, Structure, and Thermodynamics: Spectroscopy, Reactions, and Relaxation

J. Chem. Phys. 135, 224505 (2011); http://dx.doi.org/10.1063/1.3666846 (13 pages)

Selective nonlinear response preparation using femtosecond spectrally resolved four-wave-mixing

Jan Philip Kraack, Marcus Motzkus, and Tiago Buckup

Physikalisch-Chemisches Institut, Ruprecht-Karls Universität Heidelberg, D-69210 Heidelberg, Germany

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(Received 23 September 2011; accepted 16 November 2011; published online 9 December 2011)

A novel method is presented to assist the assignment of vibrational coherence in the homodyne degenerate four-wave-mixing technique. The dependence of vibrational coherence dynamics on the interaction sequence of chirped pump and Stokes excitation pulses is exploited to distinguish quantum beating from polarization interference. Moreover, by combining chirped excitation and variable delays between pump and Stokes pulses, it is possible to achieve a controlled excitation of response pathways from a single electronic state and separation of population dynamics and vibrational coherence dynamics within a single response pathway. Numerical simulations are performed in the response function framework, which clearly show that such an approach applies for oscillatory contributions originated in the electronically excited state as well as in the ground state. The approach is experimentally demonstrated in three different polyatomic molecules in solution.

© 2011 American Institute of Physics

Article Outline

  1. INTRODUCTION
  2. EXPERIMENTAL DETAILS
  3. THEORETICAL FRAMEWORK
  4. SIMULATION RESULTS
    1. Ground-state dynamics
    2. Excited-state dynamics
    3. Calculation of the complete response: Ground and excited state pathways
    4. Design of optimal chirp-values and τ 12 -delays for selective pathway preparation
    5. Discrimination of molecular normal modes from interference contributions
  5. EXPERIMENTAL RESULTS
    1. Experimental demonstration of discrimination between normal modes and interference contributions
  6. CONCLUDING REMARKS

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KEYWORDS and PACS

Keywords

excited states, ground states, molecule-photon collisions, multiwave mixing, numerical analysis, optical pumping, vibrational states

PACS

  • 33.80.Be

    Level crossing and optical pumping

  • 33.15.Mt

    Rotation, vibration, and vibration-rotation constants

  • 31.15.xv

    Molecular dynamics and other numerical methods

ARTICLE DATA

Digital Object Identifier
http://dx.doi.org/10.1063/1.3666846

PUBLICATION DATA

ISSN

0021-9606 (print)  
1089-7690 (online)

Publisher

$abstract.society.value is a Member of CrossRef American Institute of Physics

For access to fully linked references, you need to log in.
    R. W. Schoenlein, D. M. Mittleman, J. J. Shiang, A. P. Alivisatos, and C. V. Shank, Biophys. Rev. Lett. 70, 1014 (1993).

    W. B. Bosma, Y. J. Yan, and S. Mukamel, Phys. Rev. A 42, 6920 (1990).

    J. Erland and I. Balslev, Phys. Rev. A 48, R1765 (1993).

    M. Koch, J. Feldmann, G. Vonplessen, E. O. Gobel, P. Thomas, and K. Kohler, Phys. Rev. Lett. 69, 3631 (1992).

    J. Faeder, I. Pinkas, G. Knopp, Y. Prior, and D. J. Tannor, J. Chem. Phys. 115, 8440 (2001)JCPSA6000115000018008440000001.

    M. Sugisaki, M. Fujiwara, D. Kosumi, R. Fujii, M. Nango, R. J. Cogdell, and H. Hashimoto, Phys. Rev. B 81, 245112 (2010).

    K. Ohta, D. S. Larsen, M. Yang, and G. R. Fleming, J. Chem. Phys. 114, 8020 (2001)JCPSA6000114000018008020000001.

    W. P. deBoeij, M. S. Pshenichnikov, and D. A. Wiersma, J. Chem. Phys. 105, 2953 (1996)JCPSA6000105000008002953000001.

    N. Christensson, Y. Avlasevich, A. Yartsev, K. Müllen, T. Pascher, and T. Pullerits, J. Chem. Phys. 132, 174508 (2010)JCPSA6000132000017174508000001.

    T. Hellerer, A. M. K. Enejder, and A. Zumbusch, Appl. Phys. Lett. 85, 25 (2004)APPLAB000085000001000025000001.

    J. S. Park and T. Joo, J. Chem. Phys. 120, 5269 (2004)JCPSA6000120000011005269000001.

    V. I. Prokhorenko, A. M. Nagy, and R. J. D. Miller, J. Chem. Phys. 122, 184502 (2005)JCPSA6000122000018184502000001.


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