Quasiparticle electronic structure and optical absorption of diamond nanoparticles from ab initio many-body perturbation theory

Journal Article · Sat Jun 07 00:00:00 EDT 2014 · Journal of Chemical Physics

DOI:https://doi.org/10.1063/1.4880695· OSTI ID:22304235

Yin, Huabing; Ma, Yuchen; Mu, Jinglin; Liu, Chengbu ^[1]; Hao, Xiaotao ^[2]; Yi, Zhijun ^[3]

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1. School of Chemistry and Chemical Engineering, Shandong University, Jinan 250100 (China)
2. School of Physics, State Key Laboratory of Crystal Materials, Shandong University, Jinan 250100 (China)
3. Department of Physics, China University of Mining and Technology, Xuzhou 221116 (China)

The excited states of small-diameter diamond nanoparticles in the gas phase are studied using the GW method and Bethe-Salpeter equation (BSE) within the ab initio many-body perturbation theory. The calculated ionization potentials and optical gaps are in agreement with experimental results, with the average error about 0.2 eV. The electron affinity is negative and the lowest unoccupied molecular orbital is rather delocalized. Precise determination of the electron affinity requires one to take the off-diagonal matrix elements of the self-energy operator into account in the GW calculation. BSE calculations predict a large exciton binding energy which is an order of magnitude larger than that in the bulk diamond.

• OSTI ID: 22304235
• Journal Information: Journal of Chemical Physics, Vol. 140, Issue 21; Other Information: (c) 2014 AIP Publishing LLC; Country of input: International Atomic Energy Agency (IAEA); ISSN 0021-9606
• Country of Publication: United States
• Language: English

Related Subjects

74 ATOMIC AND MOLECULAR PHYSICS
37 INORGANIC
ORGANIC
PHYSICAL AND ANALYTICAL CHEMISTRY
ABSORPTION
AFFINITY
BETHE-SALPETER EQUATION
BINDING ENERGY
DIAMONDS
ELECTRONIC STRUCTURE
EXCITED STATES
IONIZATION POTENTIAL
MANY-BODY PROBLEM
MATRIX ELEMENTS
MOLECULAR ORBITAL METHOD
NANOPARTICLES
PERTURBATION THEORY