TY - JOUR
T1 - Tuning the electronic properties of the golden buckyball by endohedral doping
T2 - M@Au16 - (M=Ag,Zn,In)
AU - Wang, Lei Ming
AU - Pal, Rhitankar
AU - Huang, Wei
AU - Zeng, Xiao Cheng
AU - Wang, Lai Sheng
N1 - Funding Information:
The experimental work was supported by the National Science Foundation (Grant No. CHE-0749496) and performed at the W. R. Wiley Environmental Molecular Sciences Laboratory, a national scientific user facility sponsored by DOE’s Office of Biological and Environmental Research and located at Pacific Northwest National Laboratory, operated for DOE by Battelle. The theoretical work was supported in part by grants from the NSF (CHE, CMMI, and DMR/MRSEC), and the Nebraska Research Initiative, and by the Research Computing Facility at University of Nebraska-Lincoln and Holland Supercomputing Center at University of Nebraska-Omaha. X.C.Z. thanks Professor J. M. Dong and Professor W. Fa for helpful discussions.
PY - 2009
Y1 - 2009
N2 - The golden Au 16 - cage is doped systematically with an external atom of different valence electrons: Ag, Zn, and In. The electronic and structural properties of the doped clusters, M Au 16 - (M=Ag,Zn,In), are investigated by photoelectron spectroscopy and theoretical calculations. It is observed that the characteristic spectral features of Au 16 -, reflecting its near tetrahedral (Td) symmetry, are retained in the photoelectron spectra of M Au 16 -, suggesting endohedral structures with little distortion from the parent Au 16 - cage for the doped clusters. Density functional calculations show that the endohedral structures of M@ Au 16 - with Td symmetry are low-lying structures, which give simulated photoelectron spectra in good agreement with the experiment. It is found that the dopant atom does not significantly perturb the electronic and atomic structures of Au 16 -, but simply donate its valence electrons to the parent Au 16 - cage, resulting in a closed-shell 18-electron system for Ag@ Au 16 -, a 19-electron system for Zn@ Au 16 - with a large energy gap, and a 20-electron system for In@ Au 16 -. The current work shows that the electronic properties of the golden buckyball can be systematically tuned through doping.
AB - The golden Au 16 - cage is doped systematically with an external atom of different valence electrons: Ag, Zn, and In. The electronic and structural properties of the doped clusters, M Au 16 - (M=Ag,Zn,In), are investigated by photoelectron spectroscopy and theoretical calculations. It is observed that the characteristic spectral features of Au 16 -, reflecting its near tetrahedral (Td) symmetry, are retained in the photoelectron spectra of M Au 16 -, suggesting endohedral structures with little distortion from the parent Au 16 - cage for the doped clusters. Density functional calculations show that the endohedral structures of M@ Au 16 - with Td symmetry are low-lying structures, which give simulated photoelectron spectra in good agreement with the experiment. It is found that the dopant atom does not significantly perturb the electronic and atomic structures of Au 16 -, but simply donate its valence electrons to the parent Au 16 - cage, resulting in a closed-shell 18-electron system for Ag@ Au 16 -, a 19-electron system for Zn@ Au 16 - with a large energy gap, and a 20-electron system for In@ Au 16 -. The current work shows that the electronic properties of the golden buckyball can be systematically tuned through doping.
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U2 - 10.1063/1.3073884
DO - 10.1063/1.3073884
M3 - Article
C2 - 19206949
AN - SCOPUS:59949084080
SN - 0021-9606
VL - 130
JO - Journal of Chemical Physics
JF - Journal of Chemical Physics
IS - 5
M1 - 051101
ER -