Two stable phosphorus-containing four-membered ring radical cations with inverse spin density distributions

RIS ID

108695

Publication Details

Su, Y., Zheng, X., Wang, X., Zhang, X., Sui, Y. & Wang, X. (2014). Two stable phosphorus-containing four-membered ring radical cations with inverse spin density distributions. Journal of the American Chemical Society, 136 (17), 6251-6254.

Abstract

Two phosphorus-containing four-membered ring radical cations 1 •+ and 2•+ have been isolated and characterized by UV-vis absorption spectroscopy, electron paramagnetic resonance (EPR), and single-crystal X-ray diffraction. Compared with neutral molecules 1 and 2, radical 1•+ has elongated P-P bonds and more pyramidalized phosphorus atoms, while shortened P-Nring distances and larger angles around phosphorus centers are observed for 2•+. EPR studies indicate that for 1•+ spin density mainly resides on the exocyclic nitrogen atoms with very minor contribution from endocyclic phosphorus atoms, while the situation is opposite for 2•+. Such an inverse spin density distribution is controlled by the exocyclic substituents, which is supported by DFT calculations.

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Link to publisher version (DOI)

http://dx.doi.org/10.1021/ja502675d