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Si clusters are more metallic than bulk Si

Journal Article · · Journal of Chemical Physics
DOI:https://doi.org/10.1063/1.4972813· OSTI ID:1418170
 [1];  [2]
  1. Central Michigan Univ., Mount Pleasant, MI (United States)
  2. Argonne National Lab. (ANL), Argonne, IL (United States). Chemical Sciences and Engineering Division
+ Show Author Affiliations
Dipole polarizabilities were computed using density functional theory for silicon clusters over a broad range of sizes up to N = 147 atoms. The calculated total effective polarizabilities, which include contributions from permanent dipole moments of the clusters, are in very good agreement with recently measured values. We show that the permanent dipole contributions are most important for clusters in the intermediate size range and that the measured polarizabilities can be used to distinguish between energetically nearly degenerate cluster isomers at these sizes. We decompose the computed total polarizabilities into the so-called dipole and charge transfer contributions, $α^p$ and $α^q$, using a sitespecific analysis. When the per-atom values of these quantities are plotted against $$N^{-1/3}$$, clear linear trends emerge that can be extrapolated to the large size limit ($$N^{-1/3}$$ → 0), resulting in a value for $$\frac{α}{N}$$ of 30.5 bohrs3/atom that is significantly larger than the per-atom polarizability of semiconducting bulk Si, 25.04 bohrs3/atom. This indicates that Si clusters possess a higher degree of metallicity than bulk Si, a conclusion that is consistent with the strong electrostatic screening of the cluster interiors made evident by the analysis of the calculated atomic polarizabilities.
Research Organization:
Argonne National Laboratory (ANL), Argonne, IL (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Chemical Sciences, Geosciences & Biosciences Division
Grant/Contract Number:
AC02-06CH11357; SC0001330
OSTI ID:
1418170
Alternate ID(s):
OSTI ID: 1364074
Journal Information:
Journal of Chemical Physics, Journal Name: Journal of Chemical Physics Journal Issue: 24 Vol. 145; ISSN 0021-9606
Publisher:
American Institute of Physics (AIP)Copyright Statement
Country of Publication:
United States
Language:
English

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Related Subjects

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
Chemical bonding
Density functional theory
Dielectric properties
Electrodynamics
Electrostatic screening
Fullerenes
HOMO-LUMO gap
Isomerism
Polarizability
Thermal fluctuations