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Title: The ground state and electronic structure of Gd@C{sub 82}: A systematic theoretical investigation of first principle density functionals

As a representative lanthanide endohedral metallofullerene, Gd@C{sub 82} has attracted a widespread attention among theorists and experimentalists ever since its first synthesis. Through comprehensive comparisons and discussions, as well as references to the latest high precision experiments, we evaluated the performance of different computational methods. Our results showed that the appropriate choice of the exchange-correlation functionals is the decisive factor to accurately predict both geometric and electronic structures for Gd@C{sub 82}. The electronic structure of the ground state and energy gap between the septet ground state and the nonet low-lying state obtained from pure density functional methods, such as PBE and PW91, are in good agreement with current experiment. Unlike pure functionals, the popularly used hybrid functionals in previous studies, such as B3LYP, could infer the qualitative correct ground state only when small basis set for C atoms is employed. Furthermore, we also highlighted that other geometric structures of Gd@C{sub 82} with the Gd staying at different positions are either not stable or with higher energies. This work should provide some useful references for various theoretical methodologies in further density functional studies on Gd@C{sub 82} and its derivatives in the future.
Authors:
;  [1] ;  [1] ;  [2] ;  [1] ;  [2] ;  [1] ;  [3] ;  [3]
  1. Institute of Atomic and Molecular Physics, Jilin University, Changchun 130012 (China)
  2. (China)
  3. (United States)
Publication Date:
OSTI Identifier:
22415420
Resource Type:
Journal Article
Resource Relation:
Journal Name: Journal of Chemical Physics; Journal Volume: 141; Journal Issue: 24; Other Information: (c) 2014 AIP Publishing LLC; Country of input: International Atomic Energy Agency (IAEA)
Country of Publication:
United States
Language:
English
Subject:
75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITY; ATOMS; B CODES; COMPARATIVE EVALUATIONS; COMPUTERIZED SIMULATION; DENSITY FUNCTIONAL METHOD; ELECTRONIC STRUCTURE; ENERGY GAP; EV RANGE; FULLERENES; GADOLINIUM COMPOUNDS; GROUND STATES; P CODES; SYNTHESIS