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

Murilo L. Tiago; P. R.C. Kent; Randolph Q. Hood; Fernando A. Reboredo

doi:10.1063/1.2973627

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

Murilo L. Tiago, P. R.C. Kent, Randolph Q. Hood, Fernando A. Reboredo

Research output: Contribution to journal › Article › peer-review

83 Scopus citations

Abstract

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.

Original language	English
Article number	084311
Journal	Journal of Chemical Physics
Volume	129
Issue number	8
DOIs	https://doi.org/10.1063/1.2973627
State	Published - 2008

Funding

Research performed at the Materials Science and Technology Division, sponsored by the Division of Materials Sciences Engineering BES, U.S. DOE, and at the Center for Nanophase Materials Sciences, sponsored by the Division of Scientific User Facilities, U.S. Department of Energy under contract with UT-Battelle, LLC. Work at the Lawrence Livermore National Laboratory was performed under the auspices of the U.S. Department of Energy under Contract No. DE-AC52-07NA27344. Computational support was provided by the Texas Advanced Computing Center (TACC) and the National Energy Research Scientific Computing Center (NERSC) and Lawrence Livermore National Laboratory.

Funders	Funder number
Center for Nanophase Materials Sciences
Texas Advanced Computing Center
U.S. Department of Energy	DE-AC52-07NA27344
Basic Energy Sciences
Lawrence Livermore National Laboratory
Division of Materials Sciences and Engineering
National Energy Research Scientific Computing Center

Access to Document

10.1063/1.2973627

Cite this

@article{1c34a612f94241a592086e1de30fab46,

title = "Neutral and charged excitations in carbon fullerenes from first-principles many-body theories",

abstract = "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.",

author = "Tiago, {Murilo L.} and Kent, {P. R.C.} and Hood, {Randolph Q.} and Reboredo, {Fernando A.}",

year = "2008",

doi = "10.1063/1.2973627",

language = "English",

volume = "129",

journal = "Journal of Chemical Physics",

issn = "0021-9606",

publisher = "American Institute of Physics",

number = "8",

}

TY - JOUR

T1 - Neutral and charged excitations in carbon fullerenes from first-principles many-body theories

AU - Tiago, Murilo L.

AU - Kent, P. R.C.

AU - Hood, Randolph Q.

AU - Reboredo, Fernando A.

PY - 2008

Y1 - 2008

N2 - 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.

AB - 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.

UR - http://www.scopus.com/inward/record.url?scp=50849113774&partnerID=8YFLogxK

U2 - 10.1063/1.2973627

DO - 10.1063/1.2973627

M3 - Article

AN - SCOPUS:50849113774

SN - 0021-9606

VL - 129

JO - Journal of Chemical Physics

JF - Journal of Chemical Physics

IS - 8

M1 - 084311

ER -

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

Abstract

Funding

Access to Document

Other files and links

Fingerprint

Cite this