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Related Experiment Videos

C 1s -->pi* excitation in variable size benzene clusters.

I L Bradeanu1, R Flesch, N Kosugi

  • 1Institut für Physikalische Chemie, Universität Würzburg, Am Hubland, D-97074, Würzburg, Germany.

Physical Chemistry Chemical Physics : PCCP
|April 25, 2006
PubMed
Summary

Photoion yield spectroscopy reveals redshifted C 1s --> pi* transitions in benzene clusters. This spectral shift increases with cluster size, indicating structural changes from gas to solid benzene.

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Area of Science:

  • Physical Chemistry
  • Molecular Spectroscopy
  • Quantum Chemistry

Background:

  • The C 1s --> pi* transition in benzene is a sensitive probe of electronic and structural changes.
  • Understanding benzene clusters is crucial for bridging the gap between isolated molecules and condensed phases.

Purpose of the Study:

  • To investigate the C 1s --> pi* transition in molecular benzene and its clusters using high-resolution photoion yield spectroscopy.
  • To determine how cluster size influences the spectral properties of this electronic transition.
  • To compare experimental findings with theoretical calculations to understand site-specific spectral shifts.

Main Methods:

  • High-resolution photoion yield spectroscopy was employed to study the C 1s --> pi* transition.
  • Ab initio calculations were performed on model structures of benzene dimers, trimers, and tetramers.

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  • Experimental results were analyzed in conjunction with theoretical predictions.

    • Main Results:

    • The C 1s --> pi* transition band in benzene clusters exhibits the same shape as in molecular benzene but is redshifted.
    • A redshift of 50 meV was observed in small clusters, increasing to 70 meV with larger cluster sizes.
    • Calculations revealed distinct spectral shifts for different carbon sites, with those interacting with the pi-system showing larger redshifts.

    Conclusions:

    • The observed redshift in benzene clusters is attributed to intermolecular interactions and specific site effects.
    • The findings provide insights into the gas-to-solid phase transition of benzene, with an estimated shift of 100-180 meV.
    • This study highlights the utility of high-resolution spectroscopy and theoretical calculations in characterizing molecular clusters.