uu.seUppsala University Publications
Change search
CiteExportLink to record
Permanent link

Direct link
Cite
Citation style
  • apa
  • ieee
  • modern-language-association
  • vancouver
  • Other style
More styles
Language
  • de-DE
  • en-GB
  • en-US
  • fi-FI
  • nn-NO
  • nn-NB
  • sv-SE
  • Other locale
More languages
Output format
  • html
  • text
  • asciidoc
  • rtf
Theoretical study of the thermodynamic and kinetic aspects of terminated (111) diamond surfaces
Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Materials Chemistry, Inorganic Chemistry.
Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Materials Chemistry, Inorganic Chemistry.
2008 (English)In: The Journal of Physical Chemistry C, ISSN 1932-7447, Vol. 112, no 8, 3018-3026 p.Article in journal (Refereed) Published
Abstract [en]

Diamond surface susceptibility toward the degree and type of termination and reconstruction has been investigated theoretically by using density functional theory methods. The adsorption geometries and energies for H, O, and OH species adsorbed to diamond (111)-1 x 1 and (111)-2 x 1 surfaces under varying surface coverage were studied and compared with corresponding processes on the diamond (100)-2 x 1 surface. Furthermore, the energy barrier for the diamond (111)-1 x 1 to (111)-2 x 1 surface reconstruction for non-, H-, and O-terminated surfaces were also investigated using first-principle synchrotron transit methodologies. The results show that the adsorption energies for H, O, and OH are -4.53, -5.28, and -4.15 eV, respectively, for 100% terminated diamond (111)-1 x 1 surfaces and -3.29, -3.82, and -2.77 eV, respectively, for the diamond (111)-2 x 1 surfaces. Adsorption of 0 was found to be most energetically favorable in the on-top position on the 1 x 1 surface and in the bridge position on the 2 x 1 surface. The OH groups showed less-favorable adsorption energies in comparison to H and O. The calculations also show that the I x I surface configuration is energetically stable against transformation to the 2 x 1 configuration (of type Pandey chain) with a correspondingly small energy barrier; 0.32 eV. For this specific direction of surface reconstruction, significantly higher barriers were found for the H- and O-terminated diamond surfaces (58.4 and 44.0 eV, respectively). Plausible explanations for these observations are that the surface C-H and C-O bonds must be disrupted for the 2 x 1 (Pandey chain) reconstruction to occur.

Place, publisher, year, edition, pages
2008. Vol. 112, no 8, 3018-3026 p.
National Category
Inorganic Chemistry
Identifiers
URN: urn:nbn:se:uu:diva-96585DOI: 10.1021/jp709625aISI: 000253355700031OAI: oai:DiVA.org:uu-96585DiVA: diva2:171211
Available from: 2007-12-18 Created: 2007-12-18 Last updated: 2010-01-12Bibliographically approved
In thesis
1. Surface Stabilization and Electrochemical Properties from a Theoretical Perspective
Open this publication in new window or tab >>Surface Stabilization and Electrochemical Properties from a Theoretical Perspective
2007 (English)Doctoral thesis, comprehensive summary (Other academic)
Abstract [en]

Diamond and cubic boron nitride surfaces have extreme properties that can be exploited in novel tribological, electrochemical and electronic applications. Normally insulating diamond surfaces can exhibit high surface conductivities due to hydrogen termination and the nature of the surrounding atmosphere. Successful growth of cubic boron nitride thin films is hindered when harsh synthesis methods are used.

Three significant surface-related properties are addressed in this thesis using computational methods: (1) the structure, energy stability and reactivity of clean and differently terminated diamond surfaces, (2) the high surface conductivity of diamond, and (3) the adsorption-induced stability, reactivity and reconstruction of the cubic boron nitride (100) surface. Density Functional Theory (DFT) has been used at the GGA level under periodic boundary conditions to simulate the diamond and cubic boron nitride surfaces.

The diamond surface structures are shown to be insensitive to hydrogen desorption. Oxygen atoms bind in different positions and with different bond strengths. Hydroxyl groups experience both attractive hydrogen bonding and steric repulsions within the adsorbed species. The reconstruction of diamond (111)-1x1 is strongly dependent on the species adsorbed onto the surface. Electron transfer was observed from a diamond surface into a water-based adlayer, yielding a p-type doped surface, depending on the nature of the surface and the adlayer. The cubic boron nitride (100)-1x1 surface was shown to reconstruct into a 2x1 configuration on both the boron- and nitrogen-rich side through the formation of B-B bonds, as well as N–N dimer-induced surface relaxation. Hydrogen stabilized the (100)-1x1 surface, but the partial removal of hydrogen yielded non-reactive dimer formation on the surface.

Place, publisher, year, edition, pages
Uppsala: Acta Universitatis Upsaliensis, 2007. 71 p.
Series
Digital Comprehensive Summaries of Uppsala Dissertations from the Faculty of Science and Technology, ISSN 1651-6214 ; 380
Keyword
Inorganic chemistry, DFT, Diamond, High surface conductivity, Surface reactivity, c-BN, Oorganisk kemi
Identifiers
urn:nbn:se:uu:diva-8372 (URN)978-91-554-7059-3 (ISBN)
Public defence
2008-01-18, Häggsalen, Ångström Laboratory, Lägerhyddsvägen 1, 75121, Uppsala, 14:00
Opponent
Supervisors
Available from: 2007-12-18 Created: 2007-12-18Bibliographically approved

Open Access in DiVA

No full text

Other links

Publisher's full text
By organisation
Inorganic Chemistry
In the same journal
The Journal of Physical Chemistry C
Inorganic Chemistry

Search outside of DiVA

GoogleGoogle Scholar

doi
urn-nbn

Altmetric score

doi
urn-nbn
Total: 754 hits
CiteExportLink to record
Permanent link

Direct link
Cite
Citation style
  • apa
  • ieee
  • modern-language-association
  • vancouver
  • Other style
More styles
Language
  • de-DE
  • en-GB
  • en-US
  • fi-FI
  • nn-NO
  • nn-NB
  • sv-SE
  • Other locale
More languages
Output format
  • html
  • text
  • asciidoc
  • rtf