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Journal of Chemical Physics / Volume 129 / Issue 8 / ARTICLES / Gas Phase Dynamics and Structure: Spectroscopy, Molecular Interactions, Scattering, and Photochemistry

J. Chem. Phys. 129, 084311 (2008); http://dx.doi.org/10.1063/1.2973627 (7 pages)

Neutral and charged excitations in carbon fullerenes from first-principles many-body theories

Murilo L. Tiago1, P. R. C. Kent1, Randolph Q. Hood2, and Fernando A. Reboredo1

1Oak Ridge National Laboratory, Oak Ridge, Tennessee 37831, USA
2Lawrence Livermore National Laboratory, Livermore, California 94550, USA

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(Received 30 June 2008; accepted 29 July 2008; published online 28 August 2008)

We investigate the accuracy of first-principles many-body theories at the nanoscale by comparing the low-energy excitations of the carbon fullerenes C20, C24, C50, C60, C70, and C80 with experiment. Properties are calculated via the GW–Bethe–Salpeter equation and diffusion quantum Monte Carlo methods. We critically compare these theories and assess their accuracy against available photoabsorption and photoelectron spectroscopy data. The first ionization potentials are consistently well reproduced and are similar for all the fullerenes and methods studied. The electron affinities and first triplet excitation energies show substantial method and geometry dependence. These results establish the validity of many-body theories as viable alternative to density-functional theory in describing electronic properties of confined carbon nanostructures. We find a correlation between energy gap and stability of fullerenes. We also find that the electron affinity of fullerenes is very high and size independent, which explains their tendency to form compounds with electron-donor cations.

© 2008 American Institute of Physics

Article Outline

  1. INTRODUCTION
  2. METHOD
  3. RESULTS
  4. CONCLUSION

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KEYWORDS and PACS

Keywords

ab initio calculations, Bethe-Salpeter equation, density functional theory, electron affinity, energy gap, fullerenes, many-body problems, Monte Carlo methods, photoelectron spectra

PACS

  • 71.15.Mb

    Density functional theory, local density approximation, gradient and other corrections

  • 71.20.Tx

    Fullerenes and related materials; intercalation compounds

  • 61.48.-c

    Structure of fullerenes and related hollow and planar molecular structures

  • 79.60.Bm

    Clean metal, semiconductor, and insulator surfaces

ARTICLE DATA

Digital Object Identifier
http://dx.doi.org/10.1063/1.2973627

PUBLICATION DATA

ISSN

0021-9606 (print)  
1089-7690 (online)

Publisher

$abstract.society.value is a Member of CrossRef American Institute of Physics

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    J. G. Xue, S. Uchida, B. P. Rand, and S. R. Forrest, Appl. Phys. Lett. 84, 3013 (2004)APPLAB000084000016003013000001.

    F. Yang, M. Shtein, and S. R. Forrest, J. Appl. Phys. 98, 014906 (2005)JAPIAU000098000001014906000001.

    J. B. Neaton, M. S. Hybertsen, and S. G. Louie, Phys. Rev. Lett. 97, 216405 (2006).

    C. D. Spataru, S. Ismail-Beigi, L. X. Benedict, and S. G. Louie, Phys. Rev. Lett. 92, 077402 (2004).

    G. Onida, L. Reining, and A. Rubio, Rev. Mod. Phys. 74, 601 (2002).

    W. M. C. Foulkes, L. Mitas, R. J. Needs, and G. Rajagopal, Rev. Mod. Phys. 73, 33 (2001).

    M. L. Tiago and J. R. Chelikowsky, Phys. Rev. B 73, 205334 (2006).

    A. J. Williamson, J. C. Grossman, R. Q. Hood, A. Puzder, and G. Galli, Phys. Rev. Lett. 89, 196803 (2002).

    M. Rohlfing and S. G. Louie, Phys. Rev. B 62, 4927 (2000).

    J. A. Zimmerman, J. R. Eyler, S. B. H. Bach, and S. W. McElvany, J. Chem. Phys. 94, 3556 (1991)JCPSA6000094000005003556000001.

    J. P. Perdew, K. Burke, and M. Ernzerhof, Phys. Rev. Lett. 77, 3865 (1996).

    M. L. D. Puerto, M. L. Tiago, and J. R. Chelikowsky, Phys. Rev. Lett. 97, 096401 (2006).

    M. Casula, Phys. Rev. B 74, 161102 (2006).

    W. M. C. Foulkes, R. Q. Hood, and R. J. Needs, Phys. Rev. B 60, 4558 (1999).

    N. D. Drummond, A. J. Williamson, R. J. Needs, and G. Galli, Phys. Rev. Lett. 95, 096801 (2005).

    F. Furche and R. Ahlrichs, J. Chem. Phys. 114, 10362 (2001)JCPSA6000114000023010362000001.

    L. E. Brus, J. Chem. Phys. 79, 5566 (1983)JCPSA6000079000011005566000001.

    X. B. Wang, C. F. Ding, and L. S. Wang, J. Chem. Phys. 110, 8217 (1999)JCPSA6000110000017008217000001.

    X. B. Wang, H. K. Woo, X. Huang, M. M. Kappes, and L. S. Wang, Phys. Rev. Lett. 96, 143002 (2006).

    A. J. Morris, M. Stankovski, K. T. Delaney, P. Rinke, P. García-González, and R. W. Godby, Phys. Rev. B 76, 155106 (2007).

    T. Kotani and M. van Schilfgaarde, Phys. Rev. B 76, 165106 (2007).

    S. Ismail-Beigi and S. G. Louie, Phys. Rev. Lett. 90, 076401 (2003).

    C. J. Umrigar, J. Toulouse, C. Filippi, S. Sorella, and R. G. Hennig, Phys. Rev. Lett. 99, 179902 (2007).


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