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Photoelectron spectroscopic and computational studies of the Pt@Pb 10 1− and Pt@Pb 12 1−/2− anions
Andrej Grubisic, Haopeng Wang, Xiang Li, Yeon-Jae Ko, F. Sanem Kocak, Mark R. Pederson, Kit H. Bowen and Bryan W. Eichhorn
Proceedings of the National Academy of Sciences of the United States of America
Vol. 108, No. 36 (September 6, 2011), pp. 14757-14762
Published by: National Academy of Sciences
Stable URL: http://www.jstor.org/stable/27979374
Page Count: 6
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A combination of anion photoelectron spectroscopy and density functional theory calculations has elucidated the geometric and electronic structure of gas-phase endohedral Pt/Pb cage cluster anions. The anions, Pt@Pb101− and Pt@Pb121− were prepared from "preassembled" clusters generated from crystalline samples of [K(2,2,2-crypt)]2[Pt@Pb12] that were brought into the gas phase using a unique infrared desorption/photoemission anion source. The use of crystalline [K(2,2,2-crypt)]2[Pt@Pb12] also provided access to K[Pt@Pbn]− anions in the gas phase (i.e., the K+ salts of the Pt@Pbn2− anions). Anion photoelectron spectra of Pt@Pb101−, Pt@Pb121−, and K[Pt@Pb12]1− are presented. Extensive density functional theory calculations on Pt@Pb103−/2−/1−/0 and Pt@Pb122−/1− provided candidate structures and anion photoelectron spectra for Pb@Pb101− and Pt@Pb121−. Together, the calculated and measured photoelectron spectra show that Pt@Pb101− and Pt@Pb122−/1− endohedral complexes maintain their respective D4d and slightly distorted Ih symmetries in the gas phase even for the charge states with open shell character. Aside from the fullerenes, the Pt@Pb122− endohedral complex is the only bare cluster that has been structurally characterized in the solid state, solution, and the gas phase.
Proceedings of the National Academy of Sciences of the United States of America © 2011 National Academy of Sciences