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A density functional theory study of shake-up satellites in photoemission of carbon fullerenes and nanotubes
KTH, School of Biotechnology (BIO), Theoretical Chemistry.
Chinese Acad Sci, Inst High Energy Phys, Beijing.
KTH, School of Biotechnology (BIO), Theoretical Chemistry.ORCID iD: 0000-0003-0007-0394
2008 (English)In: Journal of Chemical Physics, ISSN 0021-9606, E-ISSN 1089-7690, Vol. 128, no 23, 234704-1-234704-7 p.Article in journal (Refereed) Published
Abstract [en]

Carbon 1s shake-up spectra of fullerenes C-60, C-70, and C-82 and single-walled carbon nanotubes (SWCNTs) of (5,5), (6,5), and (7,6) have been investigated by using equivalent core hole Kohn-Sham density functional theory approach, in which only one-electron transition between molecular orbitals within core-hole potential is considered. The calculated spectra are generally in good agreement with results of equivalent core-hole time-dependent density functional theory calculations and available experiments, and reliable assignments for the complicated shake-up spectra of such large systems are provided. Calculations have also been performed for endohedral metallofullerene Gd@C-82 to demonstrate the possible use of shake-up processes to identify the charge transfer between the metal ion and the carbon cage. It is found that the exciton binding energy of all systems under investigation is around 0.5 eV.

Place, publisher, year, edition, pages
2008. Vol. 128, no 23, 234704-1-234704-7 p.
Keyword [en]
Binding energy; Carbon; Carbon nanotubes; Charge transfer; Chemical bonds; Emission spectroscopy; Fullerenes; Gadolinium; Ion exchange; Metal ions; Metals; Molecular orbitals; Nanopores; Nanostructures; Nanotubes; Probability density function; Quantum chemistry; Single-walled carbon nanotubes (SWCN)
National Category
Natural Sciences
Identifiers
URN: urn:nbn:se:kth:diva-8344DOI: 10.1063/1.2943676ISI: 000256936700031Scopus ID: 2-s2.0-47249130886OAI: oai:DiVA.org:kth-8344DiVA: diva2:13638
Note
QC 20100726. Uppdaterad från submitted till published (20100726). Tidigare titel: Shake-up satellites in photoemission of carbon fullerenes and nanotubes: a DFT studyAvailable from: 2008-05-06 Created: 2008-05-06 Last updated: 2010-07-26Bibliographically approved
In thesis
1. First Principles Studies of Carbon Based Molecular Materials
Open this publication in new window or tab >>First Principles Studies of Carbon Based Molecular Materials
2008 (English)Doctoral thesis, comprehensive summary (Other academic)
Abstract [en]

The aim of this thesis was to investigate carbon based molecular materials at first principles levels. Special attention has been paid to simulations of X-ray spectroscopies, including near edge X-ray absorption fine structure (NEXAFS), X-ray photoelectron, and X-ray emission spectroscopy, which can provide detailed information about core, occupied and unoccupied molecular orbitals of the systems under investigation. Theoretical calculations have helped to assign fine spectral structures in high resolution NEXAFS spectra of five azabenzenes (pyridine, pyrazine, pyrimidine, pyridazine and s-triazine), and to identify different local chemical environments among them. With the help of NEXAFS, the characters of important chemical bonds that might be responsible for the unique magnetic properties of the tetracyanoethylene compound has been revealed. Calculations have demonstrated that X-ray spectroscopies are powerful tools for isomer identification and structure determination of fullerenes and endohedral metallofullerenes. A joint experimental and theoretical study on metallofullerene Gd@C82 has firmly determined its equilibrium structure, in which the gadolinium atom lies above the hexagon on the C2 axis. It is found that the gadolinium atom could oscillate around its equilibrium position and that its oscillation amplitude increases with increasing temperature.

In this thesis, several new computational schemes for large-scale systems have been proposed. Parallel implementation of a central insertion scheme (CIS) has been realized, which allows to effectively calculate electronic structures of very large systems, up to 150,000 electrons, at hybrid density functional theory levels. In comparison with traditional computational methods, CIS provides results with the same high accuracy but requires only a fraction of computational time. One of its applications is to calculate electronic structures of nanodiamond clusters varying from 0.76 nm (29 carbons) to 7.3 nm (20,959 carbons) in diameter, which enabled to resolve the long-standing debate about the validity of the quantum confinement model for nanodiamonds. Electronic structures and X-ray spectroscopies of a series of single-walled carbon nanotubes (SWCNTs) with different diameters and lengths have been calculated, which have made it possible to interpret the existing experimental results.

Place, publisher, year, edition, pages
Stockholm: KTH, 2008. x, 63 p.
Series
Trita-BIO-Report, ISSN 1654-2312 ; 2008:10
Keyword
first principles simulations, carbon based molecular materials, X-ray spectroscopies
National Category
Theoretical Chemistry
Identifiers
urn:nbn:se:kth:diva-4724 (URN)978-91-7178-963-1 (ISBN)
Public defence
2008-05-23, FB42, AlbaNova, Roslagstullsbaken 21, Stockholm, 10:00
Opponent
Supervisors
Note
QC 20100727Available from: 2008-05-06 Created: 2008-05-06 Last updated: 2010-07-27Bibliographically approved

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