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

Tiago, Murilo L.; Kent, Paul R.; Hood, Randolph Q.; Reboredo, Fernando A.

doi:10.1063/1.2973627

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

Journal Article · Fri Aug 01 04:00:00 EDT 2008 · The Journal of Chemical Physics

DOI:https://doi.org/10.1063/1.2973627· OSTI ID:967095

Tiago, Murilo L. ^[1]; ^[1]; Hood, Randolph Q. ^[2]; ^[1]

ORNL
Lawrence Livermore National Laboratory (LLNL)

We use first-principles many-body theories to investigate the low energy excitations of the carbon fullerenes C_20, C_24, C_50, C_60, C_70, and C_80. Properties are calculated via the GW-Bethe-Salpeter Equation (GW-BSE) and diffusion Quantum Monte Carlo (QMC) methods. At a lower level of theoretical complexity, we also calculate these properties using static and time-dependent density-functional theory. We critically compare these theories and assess their accuracy against available experimental 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. Compared to available experiment, GW-BSE underestimates excitation energies by approximately 0.3 eV while QMC overestimates them by approximately 0.5 eV. We show the GW-BSE errors result primarily from a systematic overestimation of the electron affinities, while the QMC errors likely result from nodal error in both ground and excited state calculations.

Research Organization:: Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)

Sponsoring Organization:: USDOE

DOE Contract Number:: AC05-00OR22725

OSTI ID:: 967095

Journal Information:: The Journal of Chemical Physics, Journal Name: The Journal of Chemical Physics Journal Issue: 8 Vol. 129; ISSN JCPSA6; ISSN 0021-9606

Country of Publication:: United States

Language:: English

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

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