Monday, June 30, 2008
Emerald Grand Ballroom (Sheraton Burlington Hotel and Conference Center)
236

Luminescence of Heterogeneous Nanoclusters Containing d8 and d10 Ions with Energy Transfer to Tb3+Lanthanide Acceptor Ions In Aqueous Solution

Zhonghua Guo, David Welch, Shaun Christian, Nathan Cookson, and Howard H. Patterson. University of Maine at Orono, Orono, ME

Luminescent studies of aqueous solutions containing d10 Cu(CN)2- and d8 Pt(CN)42- ions show evidence of hetero exciplex clusters involving CuI-PtII metal-metal bonding.

The broad, structureless band, large Stokes' shift, and large red shift from the monomer absorption bands are typical features of exciplex bands, because they indicate a very large displacement of the excited state relative to the ground state. Also, exciplexes are usually characterized by a charge transfer nature. We assign this new, broad, structureless band around 432 nm as due to a heterogeneous cluster containing Pt(CN)42- and Cu(CN)2- ions and having a charge transfer nature. The sharp decrease and disappearance of the strong characteristic bands of Cu(CN)2- aqueous solutions at 379nm and the characteristic bands of Pt(CN)42- aqueous solutions at about 406 and 482 nm after mixing indicates evidence of the breakdown of the original homogeneous clusters of [CuI]2 and [PtII]2; further, the appearance of a new peak around 426~438 nm after mixing indicates the formation of d8 and d10 heterogeneous CuI-PtII metal-metal nanoclusters at room temperature. The luminescence intensity is linearly dependent on oligomer concentration. Plots of [CuI]n[PtII]m vs. stoichiometric ratio for different possible values of m and n should give the empirical formula of the mixed metal oligomer when compared to the experimental plot of oligomer concentration vs. stoichiometric ratio. The values n = 2 and m = 3 provide the best match, in terms of both curvature and overall change in luminescence intensity from ratio = 0.3 to ratio = 0.8, to the experimental curve.

The CuI-PtII exciplex exhibits greater efficiency of energy transfer with Tb3+ acceptor ions in comparison to Cu(CN)2--Tb3+ or Pt(CN)42--Tb3+ aqueous solutions at room temperature.