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Quadrupole contribution to the third-order optical activity spectroscopy.

Jun-Ho Choi1, Minhaeng Cho

  • 1Department of Chemistry and Center for Multidimensional Spectroscopy, Korea University, Seoul 136-701, Korea.

The Journal of Chemical Physics
|July 21, 2007
PubMed
Summary
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This study generalizes circularly polarized photon echo (CP-PE) spectroscopy to include quadrupole contributions in chiral molecule dynamics. Results show magnetic dipole contributions dominate CP-PE signals in proteins and molecular complexes.

Area of Science:

  • Nonlinear optical spectroscopy
  • Chiral molecular dynamics
  • Biophysics

Background:

  • Time-resolved nonlinear optical spectroscopy studies chiral molecule dynamics.
  • Two-dimensional circularly polarized photon echo (2D CP-PE) spectroscopy has been applied to polypeptides and photosynthetic complexes.
  • Previous studies controlled beam configurations to eliminate quadrupole contributions to the CP-PE signal.

Purpose of the Study:

  • Generalize 2D CP-PE spectroscopy to include transition quadrupole contributions.
  • Investigate the role of quadrupole contributions in peptide amide I and chlorophyll electronic transitions.
  • Determine the significance of quadrupole terms in CP-PE signals for biomolecular systems.

Main Methods:

  • Density functional theory (DFT) calculations to determine quadrupole tensor elements.

Related Experiment Videos

  • Analysis of nonlinear optical transition pathways.
  • Comparison of quadrupole and magnetic dipole contributions.

    • Main Results:

    • Transition quadrupole contributions from peptide amide I and chlorophyll Q(y) electronic transitions were included.
    • Quadrupole transition amplitudes were found comparable to magnetic dipole terms in dipeptides and photosynthetic antenna complexes.
    • Overall quadrupole contribution was an order of magnitude smaller than magnetic dipole contribution due to rotational averaging.

    Conclusions:

    • Conventional 2D photon echo methods can measure 2D CP-PE signals from proteins and molecular complexes.
    • The 2D CP-PE signal is primarily governed by magnetic dipole contributions.
    • This work provides insights into the dynamics of chiral molecules using advanced spectroscopic techniques.