Abstract
The local point symmetry of the short-range order in simple monatomic liquids remains a fundamental open question in condensed-matter science. For more than 40 years it has been conjectured1,2,3,4 that liquids with centrosymmetric interactions may be composed of icosahedral building blocks. But these proposed mobile, randomly orientated structures have remained experimentally inaccessible owing to the unavoidable averaging involved in scattering experiments, which can therefore determine only the isotropic radial distribution function. Here we overcome this limitation by capturing liquid fragments at a solid–liquid interface, and observing the scattering of totally internally reflected (evanescent) X-rays, which are sensitive only to the liquid structure at the interface. Using this method, we observe five-fold local symmetry in liquid lead adjacent to a silicon wall, and obtain an experimental portrait of the icosahedral fragments that are predicted to occur in all close-packed monatomic liquids. By shedding new light on local bond order in disordered structures such as liquids and glasses, these results should lead to a better microscopic understanding of melting, freezing and supercooling.
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
Frank, F. C. Supercooling of liquids. Proc. R. Soc. Lond. A 215, 43–46 (1952).
Bernal, J. D. Geometry of the structure of monatomic liquids. Nature 185, 68–70 (1960).
Scott, G. D. Radial distribution of the random close packing of equal spheres. Nature 194, 956–957 ( 1962).
Bernal, J. D. The structure of liquids. Proc. R. Soc. Lond. A 280 , 299–322 (1964).
Turnbull, D. Kinetics of solidification of supercooled liquid mercury droplets. J. Chem. Phys. 20, 411–424 (1952).
Finney, J. L. Random packings and the structure of simple liquids. Proc. R. Soc. Lond. A 319, 497–493; 495–507 (1970).
Steinhardt, P. J., Nelson, D. R. & Ronchetti, M. Bond-orientational order in liquids and glasses. Phys. Rev. B 28, 784–805 (1983).
Nelson, D. R. & Spaepen, F. Polytetrahedral order in condensed matter. Solid State Phys. 42, 1– 90 (1989).
Ocko, B. (ed.) Focus on Liquid Interfaces (Vol. 12, Synchrotron Radiation News, Gordon &&&&& Breach, Newark, 1999).
Tooney, M. F. et al. Voltage-dependent ordering of water molecules at an electrode-electrolyte interface. Nature 368, 444– 446 (1994).
Huisman, W. J. et al. Layering of a liquid metal in contact with a hard wall. Nature 390, 379–381 ( 1997).
Yu, C.-J., Richter, A. G., Datta, A., Durbin, M. K. & Dutta, P. Observation of molecular layering in thin liquid films using x-ray reflectivity. Phys. Rev. Lett. 82, 2326–2329 ( 1999).
Magnussen, O. M. et al. X-ray reflectivity measurements of surface layering in liquid mercury. Phys. Rev. Lett. 74, 4444– 4447 (1995).
Regan, M. J. et al. Surface layering in liquid gallium: an x-ray reflectivity study. Phys. Rev. Lett. 75, 2498– 2501 (1005).
Moss, S. C. et al. X-ray determination of the substrate modulation potential for a two-dimensional Rb liquid in graphite. Phys. Rev. Lett. 57, 3191–3194 (1986).
Broughton, J. Q., Bonissent, A. & Abraham, F. F. The fcc (111) and (100) crystal-melt interface: a comparison by molecular dynamics simulation. J. Chem. Phys. 74, 4029–4037 (1981).
Rhykerd, C. L., Schoen, M., Diestler, D. J. & Cushman, J. H. Epitaxy in simple classical fluids in micropores and near-solid surfaces. Nature 330, 461–463 (1987).
Curtin, W. A. Density-functional theory of the solid-liquid interface. Phys. Rev. Lett. 59, 1228–1231 (1987).
Bouchard, B. et al. A triple-crystal diffractometer for high-energy synchrotron radiation at the HASYLAB high-field wiggler beamline BW5. J. Synch. Radiat. 5, 90–101 ( 1998).
Tschentscher, Th. & Suortti, P. Experiments with very high energy synchrotron radiation. J. Synch. Radiat. 5, 286–292 (1998).
North, D. M., Enderby, J. E. & Egelstaff, P. A. The structure factor for liquid metals. Proc. Phys. Soc. Ser. 2 1, 784– 794; 1075–1087 (1968).
Barton, S. W. et al. Distribution of atoms at the surface of liquid mercury. Nature 321, 685–687 ( 1986).
Grey, F., Feidenhans’l, R., Pedersen, J. S., Nielsen, M. & Johnson, R. L. Pb/Ge(111) 1x1: An anisotropic two-dimensional liquid. Phys. Rev. B 41, 9519–9522 (1990).
Dosch, H. Critical Phenomena at Surfaces and Interfaces (Vol. 126, Tracts in Modern Physics, Springer, Berlin, 1992).
Acknowledgements
We dedicate this Letter to the memory of O. Klein, who died on 23 May 2000. We thank H.R. Trebin and S.C. Moss for discussions, and H. Trenkler for assistance at the ESRF. This work was funded by the Deutsche Forschungsgemeinschaft.
Author information
Authors and Affiliations
Corresponding author
Rights and permissions
About this article
Cite this article
Reichert, H., Klein, O., Dosch, H. et al. Observation of five-fold local symmetry in liquid lead. Nature 408, 839–841 (2000). https://doi.org/10.1038/35048537
Received:
Accepted:
Issue Date:
DOI: https://doi.org/10.1038/35048537
This article is cited by
-
Hierarchical amorphous ordering in colloidal gelation
Nature Physics (2023)
-
Three-dimensional atomic packing in amorphous solids with liquid-like structure
Nature Materials (2022)
-
Predicting the splash of a droplet impinging on solid substrates
Scientific Reports (2022)
-
Quantitative Relationship Between the Nucleation Undercooling of Liquid Iron and Its Liquid Structure: Investigated by In Situ Synchrotron Radiation
Metallurgical and Materials Transactions A (2020)
-
Revealing key structural features hidden in liquids and glasses
Nature Reviews Physics (2019)
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.
