Modeling carbon nanostructures with the self-consistent charge density-functional tight-binding method: Vibrational spectra and electronic structure of C 28, C 60, and C 70

Henryk A. Witek; Stephan Irle; Guishan Zheng; Wibe A. De Jong; Keiji Morokuma

doi:10.1063/1.2370877

Modeling carbon nanostructures with the self-consistent charge density-functional tight-binding method: Vibrational spectra and electronic structure of C ₂₈, C ₆₀, and C ₇₀

Henryk A. Witek, Stephan Irle, Guishan Zheng, Wibe A. De Jong, Keiji Morokuma

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Abstract

The self-consistent charge density-functional tight-binding (SCC-DFTB) method is employed for studying various molecular properties of small fullerenes: C28, C60, and C70. The computed bond distances, vibrational infrared and Raman spectra, vibrational densities of states, and electronic densities of states are compared with experiment (where available) and density-functional theory (DFT) calculations using various basis sets. The presented DFT benchmark calculations using the correlation-consistent polarized valence triple zeta basis set are at present the most extensive calculations on harmonic frequencies of these species. Possible limitations of the SCC-DFTB method for the prediction of molecular vibrational and optical properties are discussed. The presented results suggest that SCC-DFTB is a computationally feasible and reliable method for predicting vibrational and electronic properties of such carbon nanostructures comparable in accuracy with small to medium size basis set DFT calculations at the computational cost of standard semiempirical methods.

Original language	English
Article number	214706
Journal	Journal of Chemical Physics
Volume	125
Issue number	21
DOIs	https://doi.org/10.1063/1.2370877
State	Published - 2006
Externally published	Yes

Funding

One of the authors (H.A.W.) would like to acknowledge the National Science Council of Taiwan for financial support (NCC95-2113-M-009-015). This work was partially supported by a grant from the Mitsubishi Chemical Corporation, and computer resources were provided in part by the Air Force Office of Scientific Research DURIP grant (FA9550-04-1-0321) and access to MSRC as well as by the Cherry L. Emerson Center of Emory University. The research was performed in part using the Molecular Science Computing Facility (MSCF) in the William R. Wiley Environmental Molecular Sciences Laboratory, a national scientific user facility sponsored by the U.S. Department of Energy’s Office of Biological and Environmental Research and located at the Pacific Northwest National Laboratory, operated for the Department of Energy by Battettle. In supplemental materials, Table S1 lists Cartesian coordinates in angstroms of , , and isomers at the BLYP/cc-pVTZ, , BLYP/3-21G, and SCC-DFTB levels of theory. Tables S2–S4 list computed BLYP/cc-pVTZ IR intensities and , BLYP/3-21G, and SCC-DFTB IR intensities and Raman activities of , , and .

Funders	Funder number
Cherry L. Emerson Center of Emory University
MSRC
Mitsubishi Chemical Corporation
Molecular Science Computing Facility
William R. Wiley Environmental Molecular Sciences Laboratory
U.S. Department of Energy
Air Force Office of Scientific Research	FA9550-04-1-0321
Biological and Environmental Research
National Science Council	NCC95-2113-M-009-015

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10.1063/1.2370877

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abstract = "The self-consistent charge density-functional tight-binding (SCC-DFTB) method is employed for studying various molecular properties of small fullerenes: C28, C60, and C70. The computed bond distances, vibrational infrared and Raman spectra, vibrational densities of states, and electronic densities of states are compared with experiment (where available) and density-functional theory (DFT) calculations using various basis sets. The presented DFT benchmark calculations using the correlation-consistent polarized valence triple zeta basis set are at present the most extensive calculations on harmonic frequencies of these species. Possible limitations of the SCC-DFTB method for the prediction of molecular vibrational and optical properties are discussed. The presented results suggest that SCC-DFTB is a computationally feasible and reliable method for predicting vibrational and electronic properties of such carbon nanostructures comparable in accuracy with small to medium size basis set DFT calculations at the computational cost of standard semiempirical methods.",

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AB - The self-consistent charge density-functional tight-binding (SCC-DFTB) method is employed for studying various molecular properties of small fullerenes: C28, C60, and C70. The computed bond distances, vibrational infrared and Raman spectra, vibrational densities of states, and electronic densities of states are compared with experiment (where available) and density-functional theory (DFT) calculations using various basis sets. The presented DFT benchmark calculations using the correlation-consistent polarized valence triple zeta basis set are at present the most extensive calculations on harmonic frequencies of these species. Possible limitations of the SCC-DFTB method for the prediction of molecular vibrational and optical properties are discussed. The presented results suggest that SCC-DFTB is a computationally feasible and reliable method for predicting vibrational and electronic properties of such carbon nanostructures comparable in accuracy with small to medium size basis set DFT calculations at the computational cost of standard semiempirical methods.

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Modeling carbon nanostructures with the self-consistent charge density-functional tight-binding method: Vibrational spectra and electronic structure of C ₂₈, C ₆₀, and C ₇₀

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