Abstract
PHASE separation of liquid mixtures into two liquids with different compositions is a well-known phenomenon. It has been proposed1–9 that another type of liquid–liquid phase separation, driven by fluctuations in density rather than in composition, may occur in some elemental systems. Transitions between low- and high-density amorphous phases have been described for the one-component oxides H2O, SiO2and GeO2 (refs 10–17), and it has been suggested18–21 that a liquid–liquid phase transition might occur in supercooled water. If density-driven phase separation truly does occur in liquid mixtures, it should be possible to observe the coexistence of two liquids with the same composition but different density. Here we report the direct observation of such a situation. We observe two coexisting liquid phases in the supercooled melt of AI2O3–Y2O3 just above the glass transition at ambient pressure, both of which have the same composition. We propose that these two phases must differ solely in density, and that the transition is entropically driven. The occurrence of the phase transition in this system may explain why the crystallization of yttrium aluminium garnet, the host material for Nd3 +ions in YAG lasers, is sluggish22–25.
This is a preview of subscription content, access via your institution
Access options
Subscribe to this journal
Receive 51 print issues and online access
$199.00 per year
only $3.90 per issue
Buy this article
- Purchase on Springer Link
- Instant access to full article PDF
Prices may be subject to local taxes which are calculated during checkout
Similar content being viewed by others
References
Ferraz, A. & March, N. H. Phys. Chem. Liq. 8, 289–298 (1979).
Brazhkin, V. V., Voloshin, R. N. & Popova, S. V. Zh. eksp. teor. Fiz. 50, 392–395 (1989).
Brazhkin, V. V., Popova, S. V., Voloshin, R. N. & Umnov, A. G. High. Press. Res. 6, 363–369 (1991).
Brazhkin, V. V., Voloshin, R. N., Popova, S. V. & Umnov, A. G. Phys. Lett. A154, 413–415 (1991).
van Thiel, M. & Ree, F. H. Phys. Rev. B48, 3591–3599 (1993).
Rapoport, E. J. chem. Phys. 46, 2891–2895 (1967).
Rapoport, E. J. chem. Phys. 48, 1433–1437 (1968).
Endo, H., Tamura, K. & Yao, M. Can. J. Phys. 65, 266–285 (1987).
Tsuji, K. J. non-cryst. Solids 117/118, 27–34 (1990).
Mishima, O., Calvert, L. D. & Whalley, E. Nature 314, 76–78 (1985)
Gibbons, R. V. & Ahrens, T. J. J. geophys. Res. 76, 5489–5498 (1971).
Sugiura, H., Kondo, K.-l. & Sawaoka, A. in High-Pressure Research in Geophysics (eds Akimoto, S. & Manghnani, M. H.) 551–561 (Reidel, Dordrecht, 1982).
Grimsditch, M. Phys. Rev. Lett. 52, 2379–2381 (1984).
Hemley, R. J., Mao, H. K., Bell, P. M. & Mysen, B. O. Phys. Rev. Lett. 57, 747–750 (1986).
Williams, Q. & Jeanloz, R. Science 239, 902–905 (1988).
Itie, J. P. et al. Phys. Rev. Lett. 63, 398–401 (1989).
Smith, K. H., Chizmeshya, A. V. G. & Wolf, G. H. EOS 74, 630 (1993).
Poole, P. H., Scortino, F., Essmann, U. & Stanley, H. E. Nature 360, 324–328 (1992).
Poole, P. H., Essmann, U., Scortino, F. & Stanley, H. E. Phys. Rev. E48, 4605–4610 (1993).
Poole, P. H., Scortino, F., Essmann, U. & Stanley, H. E. Phys. Rev. E48, 3799–3817 (1993).
Angell, C. A. J. phys. Chem. 97, 6339–6341 (1993).
Cockayne, B. & Lent, B. J. cryst. Growth 46, 371–378 (1979).
Caslavsky, J. L. & Viechnicki, D. J. J. mater. Sci. 15, 1709–1718 (1980).
Gervais, M., Le Floch, S., Rifflet, J. C., Coutures, J. & Coutures, J. P. J. Am. Ceram. Soc. 75, 3166–3168 (1992).
Nicolas, J., Coutures, J., Coutures, J. P. & Boudot, B. J. Solid St. Chem. 52, 101–113 (1984).
Brückner, R. J. non-cryst. Solids 5, 123–175 (1970).
Angell, C. A. & Kanno, H. Science 193, 1121–1122 (1976).
Burton, E. F. & Oliver, W. F. Nature 135, 505–506 (1935).
Bellissent-Funel, J. & Feixeira, J. J. chem. Phys. 87, 2231–2235 (1987).
Fratello, V. J. & Brandle, C. D. J. cryst. Growth 128, 1006–1010 (1993).
Voron'ko, Y. K. et al. Soviet Phys. Dokl. 32, 61–64 (1988).
Merezio, M., Remeika, J. P. & Jayaraman, A. J. chem. Phys. 45, 1821–1824 (1966).
Wells, A. F. Structural Inorganic Chemistry (Clarendon, Oxford, 1984).
Douy, A. & Odier, P. Mater. Res. Bull. 24, 1119–1126 (1989).
Richet, P. et al. J. appl. Phys. 74, 5451–5456 (1993).
McMillan, P. F., Poe, B. T., Gillet, P. & Reynard, B. Geochim. cosmochim. Acta (in the press).
Poe, B. T., McMillan, P. F., Coté, B., Massiot, D. & Coutures, J. P. J. Am. Ceram. Soc. (in the press).
Zarzycki, J. Les Verres et I'Etat Vitreux (Masson, Paris, 1982).
Coutures, J. P., Berjoan, R., Benezech, G., & Granier, B. Revue. int. Hautes Temp. Réfractaires 15, 103–114 (1978).
Badets, M. C., Coté, B., Simon, P. & Coutures, J. P. Ann. Chim. Fr. 15, 455–461 (1990).
Nordine, P. & Atkins, R. M. Rev. Sci. Instrumen. 53, 1456–1464 (1982).
Hurrell, J. P., Porto, S. P. S., Chang, I. F., Mitra, S. S. & Bauman, R. P. Phys. Rev. 173, 851–856 (1968).
Hofmeister, A. M. & Campbell, K. R. J. appl. Phys. 72, 638–645 (1992).
Author information
Authors and Affiliations
Rights and permissions
About this article
Cite this article
Aasland, S., McMillan, P. Density-driven liquid–liquid phase separation in the system AI2O3–Y2O3. Nature 369, 633–636 (1994). https://doi.org/10.1038/369633a0
Received:
Accepted:
Issue Date:
DOI: https://doi.org/10.1038/369633a0
This article is cited by
-
Pressure-induced liquid-liquid transition in a family of ionic materials
Nature Communications (2022)
-
In situ scattering study of multiscale structural evolution during liquid–liquid phase transition in Mg-based metallic glasses
Rare Metals (2021)
-
Y2O3–Al2O3 microsphere crystallization analyzed by electron backscatter diffraction (EBSD)
Scientific Reports (2020)
-
Liquid–liquid transition and critical point in sulfur
Nature (2020)
-
Pressureless glass crystallization of transparent yttrium aluminum garnet-based nanoceramics
Nature Communications (2018)
Comments
By submitting a comment you agree to abide by our Terms and Community Guidelines. If you find something abusive or that does not comply with our terms or guidelines please flag it as inappropriate.
