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Electronic transitions of molecules: vibrating Lewis structures.

Yu Liu1, Philip Kilby2, Terry J Frankcombe3

  • 1ARC Centre of Excellence in Exciton Science , School of Chemistry , UNSW Sydney , NSW 2052 , Australia . Email: timothy.schmidt@unsw.edu.au ; Tel: +61 439 386 109.

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|August 9, 2019
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Summary

This study introduces a new way to visualize molecular excited states using localized electron vibrations, akin to Lewis structures. This method simplifies understanding electronic resonances and transitions without molecular orbitals.

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Area of Science:

  • Quantum Chemistry
  • Theoretical Chemistry
  • Spectroscopy

Background:

  • Lewis structures effectively depict ground-state molecular electronic configurations.
  • Excited-state descriptions typically rely on complex molecular orbital theory.
  • A simplified, intuitive model for excited states is needed.

Purpose of the Study:

  • To develop a localized, vibration-based model for electronic resonances and excited states.
  • To demonstrate the connection between this model and traditional Lewis structures.
  • To provide an alternative to molecular orbital theory for excited-state analysis.

Main Methods:

  • Partitioning the many-electron wavefunction space into symmetry-related hyper-regions.
  • Analyzing the admixture of electronic wavefunctions to represent electronic transitions.
  • Mapping electronic transitions to localized electron vibrations.

Main Results:

  • A model where chemical structures with single/double bonds and lone pairs emerge naturally from wavefunction partitioning.
  • π-π* transitions visualized as oscillating double-bonding electrons.
  • n-π* transitions visualized as vibrating lone pairs.
  • Correspondence between electronic transitions and molecular normal mode vibrations observed in butadiene and hexatriene.

Conclusions:

  • Electronic excitations can be intuitively understood as localized electron vibrations building upon ground-state Lewis structures.
  • This approach offers a simplified, visualizable alternative to molecular orbital theory for excited states.
  • The model provides a new perspective on the dynamics of electronic transitions in molecules.