Conformationally tuned large two-photon absorption cross sections in simple molecular chromophores

S. K. Pati, T. J. Marks*, M. A. Ratner

*Corresponding author for this work

Research output: Contribution to journalArticle

94 Scopus citations

Abstract

We investigate here the relationship between molecular architecture and two-photon absorption (TPA) processes in a class of alkyl-substituted 4-quinopyran chromophores. We find that TPA cross sections diverge as the one-photon gap energy nears one-half of the two-photon gap. The molecular strategy proposed here to tune these two-excitation gaps for maximizing TPA cross sections is to twist the molecule about the bond connecting the chromophore donor and acceptor phenylene fragments. Extremely large TPA cross sections, determined by the absorption bandwidth, can then be realized (imaginary part of the third-order polarizability ∼ 2.6 × 105 × 10-36 esu) for fundamental photon energies near 1.0 eV, when the torsional angle approaches 104°. The required torsional angle is achieved by introduction of sterically encumbered 2,2′,2″,2‴ tertiary alkyl substituents.

Original languageEnglish (US)
Pages (from-to)7287-7291
Number of pages5
JournalJournal of the American Chemical Society
Volume123
Issue number30
DOIs
StatePublished - Oct 1 2001

ASJC Scopus subject areas

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

Fingerprint Dive into the research topics of 'Conformationally tuned large two-photon absorption cross sections in simple molecular chromophores'. Together they form a unique fingerprint.

  • Cite this