Abstract
The Na-flux method has great potential for growing high-quality GaN single crystals. In this study, we used a simple pre-stirring process to grow GaN crystals by the Na-flux method. The yield of GaN crystals was 95.6% and the average growth thickness was about 412 μm on a hydride vapor-phase epitaxy (HVPE)-grown GaN seed with pre-stirring. The photoluminescence (PL) spectra showed that the relative intensity of blue and yellow band luminescence peaks of liquid-phase epitaxy (LPE) of GaN crystals was reduced when pre-stirring was employed. The x-ray rocking curve (XRC) showed that the full width at half maximum (FWHM) of the (002) peak for the LPE-GaN crystal with pre-stirring was 125 arcsec, which is smaller than that without pre-stirring. Therefore, we conclude that pre-stirring may be useful for fabricating high-quality bulk GaN crystals.
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References
H. Amano, M. Kito, K. Hiramatsu, and I. Akasaki, P-type conduction in Mg-doped GaN treated with low-energy electron Beam irradiation (LEEBI). Jpn. J. Appl. Phys. 28, L2112 (1989).
W. Saito, Y. Takada, M. Kuraguchi, K. Tsuda, I. Omura, T. Ogura, and H. Ohashi, High breakdown voltage AlGaN-GaN power-HEMT design and high current density switching behavior. IEEE Trans. Electron Devices 50, 2528 (2003).
S.W. Lee, D.C. Oh, H. Goto, J.S. Ha, H.J. Lee, T. Hanada, M.W. Cho, T. Yao, S.K. Hong, and H.Y. Lee, Origin of forward leakage current in GaN-based light-emitting devices. Appl. Phys. Lett. 89, 132117 (2006).
H. Yamane, M. Shimada, S.J. Clarke, and F.J. DiSalvo, Preparation of GaN single crystals using a Na flux. Chem. Mater. 9, 413 (1997).
F. Kawamura, H. Umeda, M. Morishita, M. Kawahara, M. Yoshimura, Y. Mori, T. Sasaki, and Y. Kitaoka, Growth of a two-inch GaN single crystal substrate using the Na flux method. Jpn. J. Appl. Phys. 45, L1136 (2006).
M. Imade, K. Murakami, D. Matsuo, H. Imabayashi, H. Takazawa, Y. Todoroki, A. Kitamoto, M. Maruyama, M. Yoshimura, and Y. Mori, Centimeter-sized bulk GaN single crystals grown by the Na-flux method with a necking technique. Cryst. Growth. Des. 12, 3799 (2012).
Y. Mori, M. Imanishi, K. Murakami, and M. Yoshimura, Recent progress of Na-flux method for GaN crystal growth. Jpn. J. Appl. Phys. 58, SC0803 (2019).
F. Kawamura, T. Iwahashi, M. Morishita, K. Omae, M. Yoshimura, Y. Mori, and T. Sasaki, Growth of transparent, large size GaN single crystal with low dislocations Using Ca-Na flux system. Jpn. J. Appl. Phys. 42, L729 (2003).
M. Morishita, F. Kawamura, T. Iwahashi, M. Yoshimura, Y. Mori, and T. Sasaki, Growth of bulk GaN single crystals using Li-Na mixed flux system. Jpn. J. Appl. Phys. 42, L565 (2003).
F. Kawamura, M. Morishita, M. Tanpo, M. Imade, M. Yoshimura, Y. Kitaoka, Y. Mori, and T. Sasaki, Effect of carbon additive on increases in the growth rate of 2 in GaN single crystals in the Na flux method. J. Cryst. Growth 310, 3946 (2008).
K. Murakami, S. Ogawa, M. Imanishi, M. Imade, M. Maruyama, M. Yoshimura, and Y. Mori, Increase in the growth rate of GaN crystals by using gaseous methane in the Na flux method. Jpn. J. Appl. Phys. 56, 055502 (2017).
K. Murakami, D. Matsuo, H. Imabayashi, H. Takazawa, Y. Todoroki, A. Kitamoto, M. Maruyama, M. Imade, M. Yoshimura, and Y. Mori, Effects of solution stirring on the growth of Bulk GaN single crystals by Na flux method. Jpn. J. Appl. Phys. 52, 08JA03 (2013).
T. Sasaki, Y. Mori, F. Kawamura, M. Yoshimura, and Y. Kitaoka, New developments in crystal growth from solutions: oxides, proteins, and nitrides. J. Cryst. Growth 310, 1288 (2008).
M. Morishita, F. Kawamura, M. Kawahara, M. Yoshimura, Y. Mori, and T. Sasaki, Promoted nitrogen dissolution due to the addition of Li or Ca to Ga-Na melt; some effects of additives on the growth of GaN single crystals using the sodium flux method. J. Cryst. Growth 284, 91 (2005).
F. Kawamura, M. Morishita, K. Omae, M. Yoshimura, Y. Mori, and T. Sasaki, The effects of Na and some additives on nitrogen dissolution in the Ga-Na system: a growth mechanism of GaN in the Na flux method. J. Mater. Sci Mater Electron. 16, 29 (2005).
A.S. Basin and A.N. Solovev, Investigation of the density of liquid lead, cesium, and gallium by the gamma-method. J. Appl. Mech. Tech. Phys. 8, 57 (1967).
G.M. Huang, M.R. Feng, C. Yang, S.M. Li, M. Ma, S. Xia, S.J. Fan, and Z.R. Li, A study on the growth process for liquid phase epitaxy of GaN crystal using Na-Li-Ca flux. Mater. Sci. Semicond. Process. 143, 106565 (2022).
D. Kashiwagi, R. Gejo, Y. Kangawa, L. Liu, F. Kawamura, Y. Mori, T. Sasaki, and K. Kakimoto, Global analysis of GaN growth using a solution technique. J. Cryst. Growth 310, 1790 (2008).
R. Gejo, F. Kawamura, M. Kawahara, M. Yoshimura, Y. Kitaoka, Y. Mori, and T. Sasaki, Effect of thermal convection on liquid phase epitaxy of GaN by Na flux method. Jpn. J. Appl. Phys. 46, 7689 (2007).
V. Avrutin, D.J. Silversmith, Y. Mori, F. Kawamura, Y. Kitaoka, and H. Morkoc, Growth of bulk GaN and AlN: progress and challenges. Proc. IEEE 98, 1302 (2010).
M.B. Zhou, Z.R. Li, S.J. Fan, Z.H. Xiong, and G. Luo, Effects of cooling process on GaN crystal growth by Na flux method. J. Electron. Mater. 49, 1 (2020).
M. Aoki, H. Yamane, M. Shimada, T. Sekiguchi, T. Hanada, T. Yao, S. Sarayama, and F.J. Disalvo, Growth of GaN single crystals from a Na-Ga melt at 750°C and 5MPa of N2. J. Cryst. Growth 218, 7 (2000).
S. Porowski and I. Grzegory, Thermodynamical properties of III–V nitrides and crystal growth of GaN at high N2 pressure. J. Cryst. Growth 178, 174 (1997).
M. Kawahara, F. Kawamura, M. Yoshimura, Y. Mori, T. Sasaki, S. Yanagisawa, and Y. Morikawa, A first-principles study on nitrogen solubility in Na flux toward theoretical search for a novel flux for bulk GaN growth. J. Cryst. Growth 303, 34 (2007).
M. Kawahara, F. Kawamura, M. Yoshimura, Y. Mori, T. Sasaki, S. Yanagisawa, and Y. Morikawa, A first-principles investigation on the mechanism of nitrogen dissolution in the Na flux method. J. Appl. Phys. 101, 066106 (2007).
M. Morishita, F. Kawamura, M. Kawahara, M. Yoshimura, Y. Mori, and T. Sasaki, The influences of supersaturation on LPE growth of GaN single crystals using the Na flux method. J. Cryst. Growth 270, 402 (2004).
F. Kawamura, M. Morishita, N. Miyoshi, M. Imade, M. Yoshimura, Y. Kitaoka, Y. Mori, and T. Sasaki, Study of the metastable region in the growth of GaN using the Na flux method. J. Cryst. Growth 311, 4647 (2009).
H. Adachi, A. Niino, H. Matsumura, K. Takano, T. Inoue, Y. Mori, and T. Sasaki, Pre-stirring promotes nucleation of protein crystals. Jpn. J. Appl. Phys. 43, L243 (2004).
F. Kawamura, T. Iwahashi, K. Omae, M. Morishita, M. Yoshimura, Y. Mori, and T. Sasaki, Growth of a large GaN single crystal using the liquid phase epitaxy (LPE) technique. Jpn. J. Appl. Phys. 42, L4 (2003).
M.A. Reshchikov and H. Morkoc, Luminescence properties of defects in GaN. J. Appl. Phys. 97, 061301 (2005).
G.A. Slack, L.J. Schowalter, D. Morelli, and J.A. Freitas Jr., Some effects of oxygen impurities on AlN and GaN. J. Cryst. Growth 246, 287 (2002).
S.R. Xu, Y. Hao, J.C. Zhang, T. Jiang, L. Yang, X.L. Lu, and Z.Y. Lin, Yellow luminescence of polar and nonpolar GaN nanowires on r-plane sapphire by metal organic chemical vapor deposition. Nano Lett. 13, 3654 (2013).
Acknowledgments
This work was supported by the National Natural Science Foundation of China (Grant Nos. 61764006, 11904324), Jiangxi Provincial Cultivation Program for Academic and Technical Leaders of Major Subjects (Grant No. 20194BCJ22025), Key Program of Jiangxi Provincial Natural Science Foundation (Grant Nos. 20202ACB202006, 20224ACB202005), the Natural Science Foundation of Jiangxi Province of China (Grant No. 20202BABL202022), the Foundation of Jiangxi Educational Committee (Grant No. GJJ211117) and the Scientific Innovation Team of Optoelectronic Information in Nanchang.
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Pan, R., Wu, W., Zhou, M. et al. Promotion of GaN Crystal Growth with Pre-stirring Using the Na-Flux Method. J. Electron. Mater. 52, 5466–5472 (2023). https://doi.org/10.1007/s11664-023-10480-0
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DOI: https://doi.org/10.1007/s11664-023-10480-0