Skip to main content

Thank you for visiting nature.com. You are using a browser version with limited support for CSS. To obtain the best experience, we recommend you use a more up to date browser (or turn off compatibility mode in Internet Explorer). In the meantime, to ensure continued support, we are displaying the site without styles and JavaScript.

  • Letter
  • Published:

Congruent melting of gallium nitride at 6 GPa and its application to single-crystal growth

Abstract

The synthesis of large single crystals of GaN (gallium nitride) is a matter of great importance in optoelectronic devices for blue-light-emitting diodes and lasers. Although high-quality bulk single crystals of GaN suitable for substrates are desired, the standard method of cooling its stoichiometric melt has been unsuccessful for GaN because it decomposes into Ga and N2 at high temperatures before its melting point. Here we report that applying high pressure completely prevents the decomposition and allows the stoichiometric melting of GaN. At pressures above 6.0 GPa, congruent melting of GaN occurred at about 2,220 °C, and decreasing the temperature allowed the GaN melt to crystallize to the original structure, which was confirmed by in situ X-ray diffraction. Single crystals of GaN were formed by cooling the melt slowly under high pressures and were recovered at ambient conditions.

This is a preview of subscription content, access via your institution

Access options

Buy this article

Prices may be subject to local taxes which are calculated during checkout

Figure 1: A series of X-ray diffraction profiles of GaN with increasing temperature at 2.0 and 6.0 GPa.
Figure 2: Phase diagram of GaN under high pressure and temperature.
Figure 3
Figure 4: X-ray oscillation photograph of the recovered GaN single crystal.

Similar content being viewed by others

References

  1. Kelly, M.K. et al. Large free-standing GaN substrates by hydride vapor phase epitaxy and laser-induced liftoff. Jpn J. Appl. Phys. 38, L217–L219 (1999).

    Article  CAS  Google Scholar 

  2. Yamane, H., Shimada, M., Sekiguchi, T. & DiSalvo, F.J. Morphology and characterization of GaN single crystals grown in a Na flux. J. Cryst. Growth 186, 8–12 (1998).

    Article  CAS  Google Scholar 

  3. Hasegawa, M. & Yagi, T. Growth of nitride crystals in a supercritical nitrogen fluid under high pressures and high temperatures yield using diamond anvils cells and YAG laser heating. J. Cryst. Growth 217, 349–354 (2000).

    Article  CAS  Google Scholar 

  4. Porowski, S. High pressure growth of GaN – new prospects for blue lasers. J. Cryst. Growth 166, 583–589 (1996).

    Article  CAS  Google Scholar 

  5. Porowski, S. & Grzegory, I. Thermodynamical properties of III–V nitrides and crystals growth of GaN at high N2 pressure. J. Cryst. Growth 178, 174–188 (1997).

    Article  CAS  Google Scholar 

  6. Krukowski, S. Growth of GaN single crystals under high nitrogen pressures and their characterization. Cryst. Res. Technol. 34, 785–795 (1999).

    Article  CAS  Google Scholar 

  7. Utsumi, W. et al. SPring-8 beamlines for the high pressure science with multi-anvil apparatus. Rev. High Press. Sci. Technol. 7, 1484–1486 (1998).

    Article  CAS  Google Scholar 

  8. Utsumi, W. et al. High pressure science with multi-anvil apparatus at the SPring-8. J. Phys. Condens. Matter 14, 10497–10504 (2002).

    Article  CAS  Google Scholar 

  9. Karpinski, J., Jun, J. & Porowski, S. Equilibrium pressure of N2 over GaN and high pressure solution growth of GaN. J. Cryst. Growth 66, 1–10 (1984).

    Article  CAS  Google Scholar 

  10. Van Vechten, J.A. Quantum dielectric theory of electronegativity in covalent systems. III. Pressure–temperature phase diagrams, heats of mixing, and distribution coefficients. Phys. Rev. B 7, 1479–1507 (1973).

    Article  CAS  Google Scholar 

  11. Okada, T., Utsumi, W., Kaneko, H., Yamakata, M. & Shimomura, O. In situ x-ray observations of the decomposition of brucite and graphite-diamond conversion in aqueous fluid under high pressure and high temperature. Phys. Chem. Minerals 29, 439–445 (2002).

    Article  CAS  Google Scholar 

Download references

Acknowledgements

We thank H. Takei and H. Asaoka for encouragement and useful discussion.

Author information

Authors and Affiliations

Authors

Corresponding author

Correspondence to Wataru Utsumi.

Ethics declarations

Competing interests

The authors declare no competing financial interests.

Rights and permissions

Reprints and permissions

About this article

Cite this article

Utsumi, W., Saitoh, H., Kaneko, H. et al. Congruent melting of gallium nitride at 6 GPa and its application to single-crystal growth. Nature Mater 2, 735–738 (2003). https://doi.org/10.1038/nmat1003

Download citation

  • Received:

  • Accepted:

  • Published:

  • Issue Date:

  • DOI: https://doi.org/10.1038/nmat1003

This article is cited by

Search

Quick links

Nature Briefing

Sign up for the Nature Briefing newsletter — what matters in science, free to your inbox daily.

Get the most important science stories of the day, free in your inbox. Sign up for Nature Briefing