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Building symmetric two-dimensional two-photon materials.

Ajit Bhaskar1, Ramakrishna Guda, Michael M Haley

  • 1Department of Chemistry and Department of Macromolecular Science and Engineering, University of Michigan, Ann Arbor, MI 48109, USA.

Journal of the American Chemical Society
|October 26, 2006
PubMed
Summary
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Two-dimensional carbon networks show enhanced two-photon absorption (TPA) with more building blocks and higher symmetry. Excited-state properties, not ground-state ones, explain this TPA enhancement in annulenes.

Area of Science:

  • Materials Science
  • Organic Chemistry
  • Optoelectronics
  • Nonlinear Optics

Background:

  • Two-dimensional multi-annulenic carbon networks are promising for optoelectronic and nonlinear optical applications.
  • Understanding their photophysical properties, particularly two-photon absorption (TPA), is crucial for device development.

Purpose of the Study:

  • To investigate the factors influencing two-photon absorption (TPA) cross sections in multi-annulenic carbon systems.
  • To correlate molecular structure, symmetry, and excited-state properties with TPA enhancement.

Main Methods:

  • Employed a building block approach to synthesize a series of annulenes with varying numbers of units and symmetries.
  • Measured two-photon absorption (TPA) cross sections.

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  • Utilized femtosecond transient absorption spectroscopy to estimate excited-state transition dipole moments.

    • Main Results:

    • TPA cross sections increased with the number of building blocks and the order of molecular symmetry.
    • Ground-state properties (transition dipole moment, chromophore density) were insufficient to explain the observed TPA enhancement.
    • Excited-state transition dipole moments, determined via transient absorption, successfully predicted the trend in TPA cross sections.

    Conclusions:

    • Molecular symmetry significantly enhances the two-photon absorption (TPA) cross section in these carbon networks.
    • The enhancement is primarily driven by an increase in the excited-state transition dipole moment, not ground-state characteristics.
    • This study provides critical insights for designing novel materials with tailored nonlinear optical properties.