Two-photon absorption and nonlinear optical properties of octupolar molecules

W. H. Lee, H. Lee, J. A. Kim, J. H. Choi, M. Cho, S. J. Jeon, B. R. Cho

Research output: Contribution to journalArticlepeer-review

211 Citations (Scopus)


Two-photon absorption (TPA) cross sections of four representative series of octupolar molecules are theoretically investigated. The general structure - TPA-property relationship is described by using the effective four-state valence-bond three-charge-transfer model. As the charge-transfer character of the ground electronic state increases due to the strong donors or acceptors, (i) the transition dipole matrix elements between the ground and 2-fold degenerate excited states increase, (ii) the energy gap decreases, and consequently (iii) the TPA transition amplitude monotonically increases. Thus, the design strategy to maximize the TPA cross section of the octupolar molecule is established. On the basis of the four-state model, the first hyperpolarizability of the octupolar molecule is found to be linearly proportional to the TPA cross section. This theoretical relationship is confirmed by using the ab initio calculation results. The Hammett correlation analysis of the TPA cross section and first hyperpolarizability is also presented.

Original languageEnglish
Pages (from-to)10658-10667
Number of pages10
JournalJournal of the American Chemical Society
Issue number43
Publication statusPublished - 2001 Oct 31

ASJC Scopus subject areas

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


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