Intermolecular coupling enhancement of the molecular hyperpolarizability in multichromophoric dipolar dendrons

Shiyoshi Yokoyama, Tatsuo Nakahama, Akira Otomo, Shinro Mashiko

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Abstract

Nonlinear optical dendritic macromolecules, called azobenzene dendrons, were synthesized, and their conformational properties and molecular nonlinear optical properties were clarified by second-order nonlinear optical measurement. The synthesized molecules were modified by introducing 1-15 numbers of azobenzene branching units as the nonlinear optical chromophore and by placing aliphatic chains at the end the dendritic chains. In these topologically complex molecules, each chromophore contributed coherently to the macroscopic nonlinear optical activity. The first-order molecular hyperpolarizability of the azobenzene dendron having 15 chromophoric units was measured to be 3010 x 10-30 esu using the hyper-Rayleigh scattering method. This level of molecular hyperpolarizability was much higher than that for an azobenzene monomer (150 x 10-30 esu). The polarized nonlinear optical measurement provided structural information on the dendrons and indicated that each chromophore was oriented noncentrosymmetrically along the molecular axis to become a cone shape rather than a spreading or spherical shape. This structure gave rise to a large electronically dipolar macromolecule system, in which each chromophoric unit coherently contributed to the second harmonic generation.

Original languageEnglish
Pages (from-to)3174-3181
Number of pages8
JournalJournal of the American Chemical Society
Volume122
Issue number13
DOIs
Publication statusPublished - Apr 5 2000
Externally publishedYes

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All Science Journal Classification (ASJC) codes

  • Catalysis
  • Chemistry(all)
  • Biochemistry
  • Colloid and Surface Chemistry

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