Document Type

Article

Language

eng

Publication Date

2002

Publisher

Royal Society of Chemistry

Source Publication

Journal of the Chemical Society, Perkin Transactions 2

Source ISSN

1472-779X

Abstract

The unusual charge-transfer complexes of various arene donors (ArH) with the nitrosonium cation (NO+) resulting from bimolecular [1 ∶ 1] associations can be extended at suitably high ArH concentrations to termolecular processes leading to the analogous [2 ∶ 1] complexes. Spectral analyses of the intense color changes accompanying the arene interaction with NO+ provide optimum conditions for the isolation of pure crystalline ternary complexes. Single crystal X-ray crystallographic determinations establish the unique sandwich structure consisting of the NO moiety interposed (parallel) between a pair of cofacial arene donors—reminiscent of the well-known transition metal sandwich complexes with aromatic ligands. The electronic structure associated with the arene binding to NO in the ternary complex is analyzed by the application of the semi-empirical LCAO molecular-orbital methodology and the Mulliken (charge-transfer) formulation of the electronic (UV–VIS–NIR) transitions. The resultant evaluation of the electronic coupling (matrix) elements HAB indicates strong donor/acceptor interactions of the frontier orbitals of the arene donor (HOMO) and nitrosonium acceptor (LUMO) that are only slightly less than those extant in the corresponding binary [1 ∶ 1] complexes.

Comments

Accepted version. Journal of the Chemical Society, Perkin Transactions 2, No. 8 (2002): 1468-1474. DOI. © 2002 The Royal Society of Chemistry. Used with permission.

Sergey V. Lindeman was affiliated with the University of Houston at the time of publication.

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