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Title: An atomistic mechanism study of GaN step-flow growth in vicinal m-plane orientations

Abstract

We present elucidation of homoepitaxial growth mechanisms on vicinal non-polar surfaces of GaN that is highly important for gaining an understanding of and control thin film surface morphology and properties. Using first-principles calculations, we study the step-flow growth in m-plane GaN based on atomic row nucleation and kink propagation kinetics. Ga–N dimer adsorption onto the m-plane is energetically more favorable than that of Ga and N isolated adatoms. Therefore, we have treated the dimers as the dominant growth species attached to the step edges. By calculating the free energies of sequentially attached Ga–N dimers, we have elucidated that the a-step edge kink growth proceeds by parallel attachment rather than by across the step edge approach. We found a series of favorable configurations of kink propagation and calculated the free energy and nucleation barriers for kink evolution on five types of step edges (a, +c, -c, +a + c, and -a - c). By changing the chemical potential μGa and the excess chemical potential Δμ, the growth velocities at the five types of edges are controlled by the corresponding kink pair nucleation barrier E* in their free energy profiles. To explore the kink-flow growth instability observed at different Ga/N flux ratios,more » calculations of kink pairs on the incompact -c and +c-step edges are further performed to study their formation energies. Variations of these step edge morphologies with a tuned chemical environment are consistent with previous experimental observations, including stable diagonal ±a ± c-direction steps. In conclusion, our work provides a first-principles approach to explore step growth and surface morphology of the vicinal m-plane GaN, which is applicable to analyze and control the step-flow growth of other binary thin films.« less

Authors:
 [1];  [1];  [2]
  1. Beijing University of Technology (China). College of Materials Science and Engineering
  2. Argonne National Lab. (ANL), Argonne, IL (United States). Materials Science Division
Publication Date:
Research Org.:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22); National Natural Science Foundation of China (NNSFC); Beijing University of Technology (China)
OSTI Identifier:
1352599
Grant/Contract Number:  
AC02-06CH11357
Resource Type:
Accepted Manuscript
Journal Name:
Physical Chemistry Chemical Physics. PCCP (Print)
Additional Journal Information:
Journal Name: Physical Chemistry Chemical Physics. PCCP (Print); Journal Volume: 18; Journal Issue: 42; Journal ID: ISSN 1463-9076
Publisher:
Royal Society of Chemistry
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; gallium nitride; growth shape; kinks; morphology; step orientation

Citation Formats

Liu, Zhun, Wang, Ru-Zhi, and Zapol, Peter. An atomistic mechanism study of GaN step-flow growth in vicinal m-plane orientations. United States: N. p., 2016. Web. doi:10.1039/c6cp04479d.
Liu, Zhun, Wang, Ru-Zhi, & Zapol, Peter. An atomistic mechanism study of GaN step-flow growth in vicinal m-plane orientations. United States. doi:10.1039/c6cp04479d.
Liu, Zhun, Wang, Ru-Zhi, and Zapol, Peter. Wed . "An atomistic mechanism study of GaN step-flow growth in vicinal m-plane orientations". United States. doi:10.1039/c6cp04479d. https://www.osti.gov/servlets/purl/1352599.
@article{osti_1352599,
title = {An atomistic mechanism study of GaN step-flow growth in vicinal m-plane orientations},
author = {Liu, Zhun and Wang, Ru-Zhi and Zapol, Peter},
abstractNote = {We present elucidation of homoepitaxial growth mechanisms on vicinal non-polar surfaces of GaN that is highly important for gaining an understanding of and control thin film surface morphology and properties. Using first-principles calculations, we study the step-flow growth in m-plane GaN based on atomic row nucleation and kink propagation kinetics. Ga–N dimer adsorption onto the m-plane is energetically more favorable than that of Ga and N isolated adatoms. Therefore, we have treated the dimers as the dominant growth species attached to the step edges. By calculating the free energies of sequentially attached Ga–N dimers, we have elucidated that the a-step edge kink growth proceeds by parallel attachment rather than by across the step edge approach. We found a series of favorable configurations of kink propagation and calculated the free energy and nucleation barriers for kink evolution on five types of step edges (a, +c, -c, +a + c, and -a - c). By changing the chemical potential μGa and the excess chemical potential Δμ, the growth velocities at the five types of edges are controlled by the corresponding kink pair nucleation barrier E* in their free energy profiles. To explore the kink-flow growth instability observed at different Ga/N flux ratios, calculations of kink pairs on the incompact -c and +c-step edges are further performed to study their formation energies. Variations of these step edge morphologies with a tuned chemical environment are consistent with previous experimental observations, including stable diagonal ±a ± c-direction steps. In conclusion, our work provides a first-principles approach to explore step growth and surface morphology of the vicinal m-plane GaN, which is applicable to analyze and control the step-flow growth of other binary thin films.},
doi = {10.1039/c6cp04479d},
journal = {Physical Chemistry Chemical Physics. PCCP (Print)},
number = 42,
volume = 18,
place = {United States},
year = {2016},
month = {10}
}

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