TY - JOUR
T1 - Probing the structural evolution of medium-sized gold clusters
T2 - Au n- (n = 27-35)
AU - Shao, Nan
AU - Huang, Wei
AU - Gao, Yi
AU - Wang, Lei-Ming
AU - Li, Xi
AU - Wang, Lai-Sheng
AU - Zeng, Xiao Cheng
N1 - Publication details (e.g. title, author(s), publication statuses and dates) are captured on an “AS IS” and “AS AVAILABLE” basis at the time of record harvesting from the data source. Suggestions for further amendments or supplementary information can be sent to [email protected].
PY - 2010/5/12
Y1 - 2010/5/12
N2 - The structural evolution of negatively charged gold clusters (Au n-) in the medium size range for n = 27-35 has been investigated using photoelectron spectroscopy (PES) and theoretical calculations. New PES data are obtained using Ar-seeded He supersonic beams to achieve better cluster cooling, resulting in well-resolved spectra and revealing the presence of low-lying isomers in a number of systems. Density-functional theory calculations are used for global minimum searches. For each cluster anion, more than 200 low-lying isomers are generated using the basin-hopping global minimum search algorithm. The most viable structures and low-lying isomers are obtained using both the relative energies and comparisons between the simulated spectra and experimental PES data. The global minimum structures of Aun- (n = 27, 28, 30, and 32-35) are found to exhibit low-symmetry core-shell structures with the number of core atoms increasing with cluster size: Au27-, Au28-, and Au30- possess a one-atom core; Au32- features a three-atom triangular core; and Au33- to Au35- all contain a four-atom tetrahedral core. The global searches reveal that the tetrahedral core is a popular motif for low-lying structures of Au33- to Au35-. The structural information forms the basis for future chemisorption studies to unravel the catalytic effects of gold nanoparticles. © 2010 American Chemical Society.
AB - The structural evolution of negatively charged gold clusters (Au n-) in the medium size range for n = 27-35 has been investigated using photoelectron spectroscopy (PES) and theoretical calculations. New PES data are obtained using Ar-seeded He supersonic beams to achieve better cluster cooling, resulting in well-resolved spectra and revealing the presence of low-lying isomers in a number of systems. Density-functional theory calculations are used for global minimum searches. For each cluster anion, more than 200 low-lying isomers are generated using the basin-hopping global minimum search algorithm. The most viable structures and low-lying isomers are obtained using both the relative energies and comparisons between the simulated spectra and experimental PES data. The global minimum structures of Aun- (n = 27, 28, 30, and 32-35) are found to exhibit low-symmetry core-shell structures with the number of core atoms increasing with cluster size: Au27-, Au28-, and Au30- possess a one-atom core; Au32- features a three-atom triangular core; and Au33- to Au35- all contain a four-atom tetrahedral core. The global searches reveal that the tetrahedral core is a popular motif for low-lying structures of Au33- to Au35-. The structural information forms the basis for future chemisorption studies to unravel the catalytic effects of gold nanoparticles. © 2010 American Chemical Society.
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U2 - 10.1021/ja102145g
DO - 10.1021/ja102145g
M3 - RGC 21 - Publication in refereed journal
C2 - 20405837
SN - 0002-7863
VL - 132
SP - 6596
EP - 6605
JO - Journal of the American Chemical Society
JF - Journal of the American Chemical Society
IS - 18
ER -