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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

Abstract

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];  [1];  [1]
  1. Institute of Atomic and Molecular Physics, Jilin University, Changchun 130012 (China)
Publication Date:
OSTI Identifier:
22415420
Resource Type:
Journal Article
Journal Name:
Journal of Chemical Physics
Additional Journal Information:
Journal Volume: 141; Journal Issue: 24; Other Information: (c) 2014 AIP Publishing LLC; Country of input: International Atomic Energy Agency (IAEA); Journal ID: ISSN 0021-9606
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

Citation Formats

Dai, Xing, Gao, Yang, Xin, Minsi, School of Science, Changchun University of Science and Technology, Changchun 130022, Wang, Zhigang, State Key Laboratory of Theoretical and Computational Chemistry, Jilin University, Changchun 130023, Zhou, Ruhong, Computational Biology Center, IBM Thomas J. Watson Research Center, Yorktown Heights, New York 10598, and Department of Chemistry, Columbia University, New York, New York 10027. The ground state and electronic structure of Gd@C{sub 82}: A systematic theoretical investigation of first principle density functionals. United States: N. p., 2014. Web. doi:10.1063/1.4904389.
Dai, Xing, Gao, Yang, Xin, Minsi, School of Science, Changchun University of Science and Technology, Changchun 130022, Wang, Zhigang, State Key Laboratory of Theoretical and Computational Chemistry, Jilin University, Changchun 130023, Zhou, Ruhong, Computational Biology Center, IBM Thomas J. Watson Research Center, Yorktown Heights, New York 10598, & Department of Chemistry, Columbia University, New York, New York 10027. The ground state and electronic structure of Gd@C{sub 82}: A systematic theoretical investigation of first principle density functionals. United States. https://doi.org/10.1063/1.4904389
Dai, Xing, Gao, Yang, Xin, Minsi, School of Science, Changchun University of Science and Technology, Changchun 130022, Wang, Zhigang, State Key Laboratory of Theoretical and Computational Chemistry, Jilin University, Changchun 130023, Zhou, Ruhong, Computational Biology Center, IBM Thomas J. Watson Research Center, Yorktown Heights, New York 10598, and Department of Chemistry, Columbia University, New York, New York 10027. 2014. "The ground state and electronic structure of Gd@C{sub 82}: A systematic theoretical investigation of first principle density functionals". United States. https://doi.org/10.1063/1.4904389.
@article{osti_22415420,
title = {The ground state and electronic structure of Gd@C{sub 82}: A systematic theoretical investigation of first principle density functionals},
author = {Dai, Xing and Gao, Yang and Xin, Minsi and School of Science, Changchun University of Science and Technology, Changchun 130022 and Wang, Zhigang and State Key Laboratory of Theoretical and Computational Chemistry, Jilin University, Changchun 130023 and Zhou, Ruhong and Computational Biology Center, IBM Thomas J. Watson Research Center, Yorktown Heights, New York 10598 and Department of Chemistry, Columbia University, New York, New York 10027},
abstractNote = {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.},
doi = {10.1063/1.4904389},
url = {https://www.osti.gov/biblio/22415420}, journal = {Journal of Chemical Physics},
issn = {0021-9606},
number = 24,
volume = 141,
place = {United States},
year = {Sun Dec 28 00:00:00 EST 2014},
month = {Sun Dec 28 00:00:00 EST 2014}
}