Twisted π-system chromophores for all-optical switching

Guang S. He, Jing Zhu, Alexander Baev, Marek Samoć*, David L. Frattarelli, Naoki Watanabe, Antonio Facchetti, Hans Ågren, Tobin Jay Marks, Paras N. Prasad

*Corresponding author for this work

Research output: Contribution to journalArticle

87 Scopus citations

Abstract

Molecular chromophores with twisted π-electron systems have been shown to possess unprecedented values of the quadratic hyperpolarizability, β, with very large real parts and much smaller imaginary parts. We report here an experimental and theoretical study which shows that these twisted chromophores also possess very large values of the real part of the cubic hyperpolarizability, γ, which is responsible for nonlinear refraction. Thus, for the two-ring twisted chromophore TMC-2 at 775 nm, relatively close to one-photon resonance, n2 extrapolated to neat substance is large and positive (1.87 × 10-13 cm2/W), leading to self-focusing. Furthermore, the third-order response includes a remarkably low two-photon absorption coefficient, which means minimal nonlinear optical losses: the T factor, α2λ/n2, is 0.308. These characteristics are attributed to closely spaced singlet biradical and zwitterionic states and offer promise for applications in all-optical switching.

Original languageEnglish (US)
Pages (from-to)6675-6680
Number of pages6
JournalJournal of the American Chemical Society
Volume133
Issue number17
DOIs
StatePublished - May 4 2011

ASJC Scopus subject areas

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

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    He, G. S., Zhu, J., Baev, A., Samoć, M., Frattarelli, D. L., Watanabe, N., Facchetti, A., Ågren, H., Marks, T. J., & Prasad, P. N. (2011). Twisted π-system chromophores for all-optical switching. Journal of the American Chemical Society, 133(17), 6675-6680. https://doi.org/10.1021/ja1113112