Reaction Pathway of Surface-Catalyzed Ammonia Decomposition and Nitrogen Incorporation in Epitaxial Growth of Gallium Nitride

Kieu My Bui, Jun Ichi Iwata, Yoshihiro Kangawa, Kenji Shiraishi, Yasuteru Shigeta, Atsushi Oshiyama

Research output: Contribution to journalArticle

Abstract

We report density functional calculations that clarify atom-scale mechanisms of vapor-phase epitaxial growth of GaN with gas sources of trimethylgallium and ammonia. We identify various stable adsorption structures of a Ga atom and NHx molecules (x = 0-3) on GaN(0001) surfaces and find that NH2 and NH units spontaneously intervene in Ga-Ga surface bonds on Ga-rich GaN(0001) surface. We then explore the reaction in which NH3 on the surface is decomposed and becomes an N-incorporated structure, -Ga-(NH)-Ga-, on the Ga-rich GaN(0001) and find that the reaction occurs with the energy barrier of 0.63 eV. Further exploration reveals that a reaction of H2 desorption occurs with the energy barrier of 2 eV, leaving the N atom incorporated in the Ga-N network. This barrier can be overcome when we consider the chemical potential of an H2 molecule in the gas phase at the growth temperature. This N incorporation on GaN is a new growth mechanism catalyzed by the growing surface.

Original languageEnglish
Pages (from-to)24665-24671
Number of pages7
JournalJournal of Physical Chemistry C
Volume122
Issue number43
DOIs
Publication statusPublished - Nov 1 2018

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Gallium nitride
gallium nitrides
Ammonia
Epitaxial growth
ammonia
Nitrogen
Decomposition
decomposition
nitrogen
Energy barriers
Atoms
Gases
vapor phases
atoms
Molecules
Vapor phase epitaxy
Chemical potential
Growth temperature
Density functional theory
molecules

All Science Journal Classification (ASJC) codes

  • Electronic, Optical and Magnetic Materials
  • Energy(all)
  • Physical and Theoretical Chemistry
  • Surfaces, Coatings and Films

Cite this

Reaction Pathway of Surface-Catalyzed Ammonia Decomposition and Nitrogen Incorporation in Epitaxial Growth of Gallium Nitride. / Bui, Kieu My; Iwata, Jun Ichi; Kangawa, Yoshihiro; Shiraishi, Kenji; Shigeta, Yasuteru; Oshiyama, Atsushi.

In: Journal of Physical Chemistry C, Vol. 122, No. 43, 01.11.2018, p. 24665-24671.

Research output: Contribution to journalArticle

Bui, Kieu My ; Iwata, Jun Ichi ; Kangawa, Yoshihiro ; Shiraishi, Kenji ; Shigeta, Yasuteru ; Oshiyama, Atsushi. / Reaction Pathway of Surface-Catalyzed Ammonia Decomposition and Nitrogen Incorporation in Epitaxial Growth of Gallium Nitride. In: Journal of Physical Chemistry C. 2018 ; Vol. 122, No. 43. pp. 24665-24671.
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AU - Bui, Kieu My

AU - Iwata, Jun Ichi

AU - Kangawa, Yoshihiro

AU - Shiraishi, Kenji

AU - Shigeta, Yasuteru

AU - Oshiyama, Atsushi

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N2 - We report density functional calculations that clarify atom-scale mechanisms of vapor-phase epitaxial growth of GaN with gas sources of trimethylgallium and ammonia. We identify various stable adsorption structures of a Ga atom and NHx molecules (x = 0-3) on GaN(0001) surfaces and find that NH2 and NH units spontaneously intervene in Ga-Ga surface bonds on Ga-rich GaN(0001) surface. We then explore the reaction in which NH3 on the surface is decomposed and becomes an N-incorporated structure, -Ga-(NH)-Ga-, on the Ga-rich GaN(0001) and find that the reaction occurs with the energy barrier of 0.63 eV. Further exploration reveals that a reaction of H2 desorption occurs with the energy barrier of 2 eV, leaving the N atom incorporated in the Ga-N network. This barrier can be overcome when we consider the chemical potential of an H2 molecule in the gas phase at the growth temperature. This N incorporation on GaN is a new growth mechanism catalyzed by the growing surface.

AB - We report density functional calculations that clarify atom-scale mechanisms of vapor-phase epitaxial growth of GaN with gas sources of trimethylgallium and ammonia. We identify various stable adsorption structures of a Ga atom and NHx molecules (x = 0-3) on GaN(0001) surfaces and find that NH2 and NH units spontaneously intervene in Ga-Ga surface bonds on Ga-rich GaN(0001) surface. We then explore the reaction in which NH3 on the surface is decomposed and becomes an N-incorporated structure, -Ga-(NH)-Ga-, on the Ga-rich GaN(0001) and find that the reaction occurs with the energy barrier of 0.63 eV. Further exploration reveals that a reaction of H2 desorption occurs with the energy barrier of 2 eV, leaving the N atom incorporated in the Ga-N network. This barrier can be overcome when we consider the chemical potential of an H2 molecule in the gas phase at the growth temperature. This N incorporation on GaN is a new growth mechanism catalyzed by the growing surface.

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