Abstract
The mechanisms of atomic transport in supercooled liquids and the nature of the glass transition are long-standing problems1,2,3,4. Collective atomic motion is thought to play an important role4,5,6 in both phenomena. A metallic supercooled liquid represents an ideal system for studying intrinsic collective motions because of its structural similarity to the “dense random packing of spheres” model7, which is conceptually simple. Unlike polymeric and network glasses, metallic supercooled liquids have only recently become experimentally accessible, following the discovery of bulk metallic glasses8,9,10,11,12. Here we report a 9Be nuclear magnetic resonance study of Zr-based bulk metallic glasses8,9 in which we investigate microscopic transport in supercooled liquids around the glass transition regime. Combining our results with diffusion measurements, we demonstrate that two distinct processes contribute to long-range transport in the supercooled liquid state: single-atom hopping and collective motion, the latter being the dominant process. The effect of the glass transition is clearly visible in the observed diffusion behaviour of the Be atoms.
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
Ediger,M. D., Angell,C. A. & Nagel, S. R. Supercooled liquids and glasses. J. Phys. Chem. 100, 13200–13212 (1996).
Grest,G. S. & Cohen,M. H. Liquids, glasses, and the glass transition: a free-volume approach. Adv. Chem. Phys. 48, 454–525 (1981).
Götze,W. & Sjögren,L. Relaxation processes in supercooled liquids. Rep. Prog. Phys. 55, 241–376 (1992).
Faupel,F. Diffusion in non-crystalline metallic and organic media. Phys. Status. Solidi. A 134, 9–59 (1992).
Stillinger, F. H. Relaxation and flow mechanisms in “fragile” glass-forming liquids. J. Chem. Phys. 89, 6461–6469 (1988).
Kivelson,S. A., Zhao,X., Kivelson,D., Fischer,T. M. & Knobler, C. M. Frustration-limited clusters in liquids. J. Chem. Phys. 101, 2391–2397 (1994).
Bernal,J. D. Geometry of the structure of monatomic liquids. Nature 185, 68–70 (1960).
Peker,A. & Johnson, W. L. A highly processable metallic glass: Zr41.2Ti13.8Cu12.5Ni10Be22.5. Appl. Phys. Lett. 63, 2342–2344 (1993).
Bakke,E., Busch,R. & Johnson, W. L. The viscosity of the Zr46.75Ti8.25Cu7.5Ni10Be27.5 bulk metallic glass forming alloy in the supercooled liquid. Appl. Phys. Lett. 67, 3260–3262 (1995).
Busch,R. & Johnson, W. L. The kinetic glass transition of the Zr46.75Ti8.25Cu7.5Ni10Be27.5 bulk metallic glass former-supercooled liquids on a long time scale. Appl. Phys. Lett. 72, 2695–2697 (1998).
Inoue,A., Zhang, T & Takeuchi,A. Ferrous and nonferrous bulk amorphous alloys. Mater. Sci. Forum 269–272, 855–864 (1998).
Greer,A. L. Metallic glasses. Science 267, 1947–1953 (1995).
Geyer, U. et al. Atomic diffusion in the supercooled liquid and glassy states of the alloy Zr41.2Ti13.8Cu12.5Ni10Be22.5. Phys. Rev. Lett. 75, 2364–2367 (1995).
Geyer,U. et al. Small atom diffusion and breakdown of the Stokes–Einstein relation in the supercooled liquid state of the Zr46. 75Ti8. 25Cu7. 5Ni10Be27. 5 alloy. Appl. Phys. Lett. 69, 2492–2494 (1996).
Knorr,K., Macht, M. -P., Freitag,K. & Mehrer, H. Self-diffusion in the amorphous and supercooled liquid state of the bulk metallic glass Zr46.75Ti8.25Cu7.5Ni10Be27.5. J. Non-Cryst. Solids 250–252, 669–673 (1999).
Fielitz,P., Macht, M. -P., Naundorf,V. & Frohberg,G. Diffusion in ZrTiCuNiBe bulk glasses at temperatures around the glass transition. J. Non-Cryst. Solids 250–252, 674–678 (1999).
Ehmler,H., Heesemann,A., Rätzke,K., Faupel,F. & Geyer,U. Mass dependence of diffusion in a supercooled metallic melt. Phys. Rev. Lett. 80, 4919–4922 (1998).
Tang, X. -P. & Wu,Y. Alignment echo of spin-3/2 9Be nuclei: detection of ultraslow motion. J. Magn. Reson. 133, 155–165 (1998).
Tang, X. -P., Busch,R., Johnson,W. L. & Wu,Y. Slow atomic motion in Zr-Ti-Cu-Ni-Be metallic glasses studied by NMR. Phys. Rev. Lett. 81, 5358–5361 (1998).
Spiess,H. W. Deuteron spin alignment: a probe for studying ultraslow motions in solids and solid polymers. J. Chem. Phys. 72, 6755–6762 (1980).
Fuara,F., Wefing,S. & Kuhs, W. E. Direct observation of tetrahedral hydrogen jumps in ice Ih. J. Chem. Phys. 88, 6801–6809 (1988).
Ehlich,D. & Silescu,H. Tracer diffusion at the glass-transition. Macromolecules 23, 1600–1610 (1990).
Acknowledgements
This work was supported by the US Army Research Office, the US National Science Foundation, and the US Department of Energy.
Author information
Authors and Affiliations
Rights and permissions
About this article
Cite this article
Tang, XP., Geyer, U., Busch, R. et al. Diffusion mechanisms in metallic supercooled liquids and glasses. Nature 402, 160–162 (1999). https://doi.org/10.1038/45996
Received:
Accepted:
Issue Date:
DOI: https://doi.org/10.1038/45996
This article is cited by
-
Resolving aging dynamics of a 3D colloidal glass
Science China Physics, Mechanics & Astronomy (2024)
-
Determining the three-dimensional atomic structure of an amorphous solid
Nature (2021)
-
A medium-range structure motif linking amorphous and crystalline states
Nature Materials (2021)
-
Relaxation Pathways in Metallic Glasses
JOM (2017)
-
Localized crystallization in shear bands of a metallic glass
Scientific Reports (2016)
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.