Limitations of essential-state models for the description of two-photon absorption processes: The example of bis(dioxaborine)-substituted chromophores

Egbert Zojer*, Wim Wenseleers, Peter Pacher, Stephen Barlow, Marcus Halik, Cara Grasso, Joseph W. Perry, Seth R. Marder, Jean Luc Brédas

*Corresponding author for this work

Research output: Contribution to journalArticlepeer-review

32 Scopus citations


We report spectroscopic and quantum-chemical investigations comparing the two-photon absorption (TPA) properties of a bis(dioxaborine)-substituted derivative of biphenyl with those of a bis(dioxaborine) carbazole derivative. The former molecule is close to linear and centrosymmetric, while the dioxaborine groups of the latter are in a V-shaped arrangement, due to their linkage to the 3 and 6 positions of the bridging group. For both systems, we find sizable TPA cross sections (on the order of 360-530 × 10 -50 cm 4 s/photon). Interestingly, while the TPA response in the biphenyl-based system can be well described on the basis of the traditional three-state model, a significantly larger number of excited states needs to be considered for the carbazole derivative. We present a detailed comparison of the convergence of the theoretical approaches and an analysis of the various channels that contribute to the TPA response in molecules with low effective symmetries.

Original languageEnglish (US)
Pages (from-to)8641-8646
Number of pages6
JournalJournal of Physical Chemistry B
Issue number25
StatePublished - Jun 24 2004
Externally publishedYes

ASJC Scopus subject areas

  • Surfaces, Coatings and Films
  • Physical and Theoretical Chemistry
  • Materials Chemistry

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