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Title: Extent of hydrogen coverage of Si(001) under chemical vapor deposition conditions from ab initio approaches

Abstract

The extent of hydrogen coverage of the Si(001) c(4 × 2) surface in the presence of hydrogen gas has been studied with dispersion corrected density functional theory. Electronic energy contributions are well described using a hybrid functional. The temperature dependence of the coverage in thermodynamic equilibrium was studied computing the phonon spectrum in a supercell approach. As an approximation to these demanding computations, an interpolated phonon approach was found to give comparable accuracy. The simpler ab initio thermodynamic approach is not accurate enough for the system studied, even if corrections by the Einstein model for surface vibrations are considered. The on-set of H{sub 2} desorption from the fully hydrogenated surface is predicted to occur at temperatures around 750 K. Strong changes in hydrogen coverage are found between 1000 and 1200 K in good agreement with previous reflectance anisotropy spectroscopy experiments. These findings allow a rational choice for the surface state in the computational treatment of chemical reactions under typical metal organic vapor phase epitaxy conditions on Si(001).

Authors:
;  [1]
  1. Fachbereich Chemie and Wissenschaftliches Zentrum für Materialwissenschaften, Philipps-Universität Marburg, Hans-Meerwein-Straße, Marburg 35032 (Germany)
Publication Date:
OSTI Identifier:
22657830
Resource Type:
Journal Article
Resource Relation:
Journal Name: Journal of Chemical Physics; Journal Volume: 144; Journal Issue: 20; Other Information: (c) 2016 Author(s); Country of input: International Atomic Energy Agency (IAEA)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL AND ANALYTICAL CHEMISTRY; CHEMICAL VAPOR DEPOSITION; COMPUTER CALCULATIONS; CRYSTALS; DENSITY FUNCTIONAL METHOD; HYDROGENATION; ORGANOMETALLIC COMPOUNDS; SILICON; SURFACES; TEMPERATURE DEPENDENCE; VAPOR PHASE EPITAXY

Citation Formats

Rosenow, Phil, and Tonner, Ralf, E-mail: tonner@chemie.uni-marburg.de. Extent of hydrogen coverage of Si(001) under chemical vapor deposition conditions from ab initio approaches. United States: N. p., 2016. Web. doi:10.1063/1.4952603.
Rosenow, Phil, & Tonner, Ralf, E-mail: tonner@chemie.uni-marburg.de. Extent of hydrogen coverage of Si(001) under chemical vapor deposition conditions from ab initio approaches. United States. doi:10.1063/1.4952603.
Rosenow, Phil, and Tonner, Ralf, E-mail: tonner@chemie.uni-marburg.de. Sat . "Extent of hydrogen coverage of Si(001) under chemical vapor deposition conditions from ab initio approaches". United States. doi:10.1063/1.4952603.
@article{osti_22657830,
title = {Extent of hydrogen coverage of Si(001) under chemical vapor deposition conditions from ab initio approaches},
author = {Rosenow, Phil and Tonner, Ralf, E-mail: tonner@chemie.uni-marburg.de},
abstractNote = {The extent of hydrogen coverage of the Si(001) c(4 × 2) surface in the presence of hydrogen gas has been studied with dispersion corrected density functional theory. Electronic energy contributions are well described using a hybrid functional. The temperature dependence of the coverage in thermodynamic equilibrium was studied computing the phonon spectrum in a supercell approach. As an approximation to these demanding computations, an interpolated phonon approach was found to give comparable accuracy. The simpler ab initio thermodynamic approach is not accurate enough for the system studied, even if corrections by the Einstein model for surface vibrations are considered. The on-set of H{sub 2} desorption from the fully hydrogenated surface is predicted to occur at temperatures around 750 K. Strong changes in hydrogen coverage are found between 1000 and 1200 K in good agreement with previous reflectance anisotropy spectroscopy experiments. These findings allow a rational choice for the surface state in the computational treatment of chemical reactions under typical metal organic vapor phase epitaxy conditions on Si(001).},
doi = {10.1063/1.4952603},
journal = {Journal of Chemical Physics},
number = 20,
volume = 144,
place = {United States},
year = {Sat May 28 00:00:00 EDT 2016},
month = {Sat May 28 00:00:00 EDT 2016}
}