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Title: Influence of spin-orbit effects on structures and dielectric properties of neutral lead clusters

Journal Article · · Journal of Chemical Physics
DOI:https://doi.org/10.1063/1.4872369· OSTI ID:22252983
;  [1];  [2];  [3]
  1. Eduard-Zintl-Institut für Anorganische und Physikalische Chemie, Technische Universität Darmstadt, 64287 Darmstadt (Germany)
  2. School of Chemistry, University of Birmingham, Edgbaston, Birmingham B15 2TT (United Kingdom)
  3. Centre for Theoretical Chemistry and Physics, The New Zealand Institute for Advanced Study, Massey University (Albany), Bob Tindall Bldg., 0745 Auckland (New Zealand)

Combining molecular beam electric deflection experiments and global optimization techniques has proven to be a powerful tool for resolving equilibrium structures of neutral metal and semiconductor clusters. Herein, we present electric molecular beam deflection experiments on Pb{sub N} (N = 7–18) clusters. Promising structures are generated using the unbiased Birmingham Cluster Genetic Algorithm approach based on density functional theory. The structures are further relaxed within the framework of two-component density functional theory taking scalar relativistic and spin orbit effects into account. Quantum chemical results are used to model electric molecular beam deflection profiles based on molecular dynamics calculations. Comparison of measured and simulated beam profiles allows the assignment of equilibrium structures for the most cluster sizes in the examined range for the first time. Neutral lead clusters adopt mainly spherical geometries and resemble the structures of lead cluster cations apart from Pb{sub 10}. Their growth pattern deviates strongly from the one observed for tin and germanium clusters.

OSTI ID:
22252983
Journal Information:
Journal of Chemical Physics, Vol. 140, Issue 16; Other Information: (c) 2014 AIP Publishing LLC; Country of input: International Atomic Energy Agency (IAEA); ISSN 0021-9606
Country of Publication:
United States
Language:
English