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

doi:10.1021/acs.jpcc.8b05682

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

Division of Renewable Energy Dynamics

Research output: Contribution to journal › Article › peer-review

6 Citations (Scopus)

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 NH_x 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 language	English
Pages (from-to)	24665-24671
Number of pages	7
Journal	Journal of Physical Chemistry C
Volume	122
Issue number	43
DOIs	https://doi.org/10.1021/acs.jpcc.8b05682
Publication status	Published - Nov 1 2018

All Science Journal Classification (ASJC) codes

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

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10.1021/acs.jpcc.8b05682

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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 journal › Article › peer-review

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

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.",

author = "Bui, {Kieu My} and Iwata, {Jun Ichi} and Yoshihiro Kangawa and Kenji Shiraishi and Yasuteru Shigeta and Atsushi Oshiyama",

note = "Funding Information: This work was supported by the Ministry of Education, Culture, Sports, Science and Technology (MEXT) Japan under the research projects “Social and Scientific Priority Issue (Creation of New Functional Devices and High-Performance Materials to Support Next-Generation Industries) to be Tackled by Using Post-K Computer” and “Program for Research and Development of Next-Generation Semiconductors to Realize an Energy-Saving Society”. Computations were performed by K computer and other supercomputers at the Institute for Solid State Physics of The University of Tokyo, The Research Center for Computational Science of National Institutes of Natural Sciences, and the Center for Computational Science of University of Tsukuba. Publisher Copyright: Copyright {\textcopyright} 2018 American Chemical Society.",

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AU - Bui, Kieu My

AU - Iwata, Jun Ichi

AU - Kangawa, Yoshihiro

AU - Shiraishi, Kenji

AU - Shigeta, Yasuteru

AU - Oshiyama, Atsushi

N1 - Funding Information: This work was supported by the Ministry of Education, Culture, Sports, Science and Technology (MEXT) Japan under the research projects “Social and Scientific Priority Issue (Creation of New Functional Devices and High-Performance Materials to Support Next-Generation Industries) to be Tackled by Using Post-K Computer” and “Program for Research and Development of Next-Generation Semiconductors to Realize an Energy-Saving Society”. Computations were performed by K computer and other supercomputers at the Institute for Solid State Physics of The University of Tokyo, The Research Center for Computational Science of National Institutes of Natural Sciences, and the Center for Computational Science of University of Tsukuba. Publisher Copyright: Copyright © 2018 American Chemical Society.

PY - 2018/11/1

Y1 - 2018/11/1

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

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