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The mononuclear complex [(EtO 2C-C ^N ^C)Pt(dmpyz)] (1) (dmpyz = 2,5-dimethylpyrazine) has been synthesized by reaction of [(EtO 2C-C ^N ^C)Pt(dmso)] (A) with dmpyz in a 1:1 molar ratio in dichloromethane. Complex 1 is the precursor for preparing the homodinuclear complex [{(EtO 2C-C ^N ^C)Pt} 2(μ-dmpyz)] (2) and the heterotrinuclear clusters [{(EtO 2C-C ^N ^C)Pt(dmpyz)} 2M]X (M = Cu, X = PF 6 (3); M = Ag, X = BF 4 (4)). Compounds 1, 2, and 4 were studied by X-ray diffraction methods. In the crystal packing of 1 and 2, the molecules display short intermolecular π π contacts, which control the solid-state emissive behavior. X-ray study on 4 shows two [Pt 2Ag] sandwich-type clusters in the asymmetric unit, both with the two square-planar >(R-CNC)Pt(dmpyz)> moieties stabilized by two Pt → Ag donor-acceptor bonds as well as by η 1- and η 2-Ag-C interactions. Intramolecular π-π contacts were found between the pyridine rings of the CNC ligands within the same Pt 2Ag cluster. 1H and 195Pt NMR studies confirm that the Pt 2M cluster is also retained in solution at room temperature. 195Pt NMR spectra of 3 and 4 show signals shifted significantly downfield when comparing with that for the monomer (1), which is attributed to the presence of Pt-M dative bonds. At lower temperatures (T = 193 K), the copper derivative definitely falls apart, whereas the silver one still holds up unbroken. In the solid state at 77 K, compounds 1-4 give red emissions arising from 3ππ excited states due to the intra- or intermolecular π-π contacts observed in the crystal structures. As expected, in glassy solutions (77 K), compound 3 displays analogous emissions to those from the starting material (1). Complexes 1 and 2 show structured emission bands that are particularly sensitive to the λ ex (HE and LE). In contrast, 4 displays an unstructured emission at 680 nm with a shoulder at 556 nm; both are not dependent on the λ ex. DFT and TDDFT computational studies have been performed on 1 and 2, which support the conclusions drawn from the photophysical studies. © 2012 American Chemical Society.The authors gratefully acknowledge the European Commission for financial support under the Marie Curie Intra-European Fellowship (PIEF-GA-2009-252883; SFL-PRR) and Prof. Juan Fornies (University of Zaragoza, Project 2008-06669-C02, from the Spanish MICINN) for the use of facilities to do the photophysical studies. The support of the Engineering and Physical Sciences Research Council (U.K.) is also acknowledged and particularly for their award of a Senior Fellowship to P.R.R. and studentships to C.H.W.Peer Reviewe

Heteropolynuclear Pt(II)–M(I) Clusters with a C∧N∧C Biscyclometalated Ligand

Heteropolynuclear Pt(II)–M(I) Clusters with a C^∧N^∧C Biscyclometalated Ligand