DOI: 10.1126/science.1068521. Ordering in a Fluid Inert Gas Confined by Flat Surfaces

Ordering in a Fluid Inert Gas Confined by Flat Surfaces

10.1126/science.1068521

Crossref journal-article

American Association for the Advancement of Science (AAAS)

Science (221)

Abstract

High-resolution transmission electron microscopy images of room-temperature fluid xenon in small faceted cavities in aluminum reveal the presence of three well-defined layers within the fluid at each facet. Such interfacial layering of simple liquids has been theoretically predicted, but observational evidence has been ambiguous. Molecular dynamics simulations indicate that the density variation induced by the layering will cause xenon, confined to an approximately cubic cavity of volume ≈ 8 cubic nanometers, to condense into the body-centered cubic phase, differing from the face-centered cubic phase of both bulk solid xenon and solid xenon confined in somewhat larger (≥20 cubic nanometer) tetradecahedral cavities in face-centered cubic metals. Layering at the liquid-solid interface plays an important role in determining physical properties as diverse as the rheological behavior of two-dimensionally confined liquids and the dynamics of crystal growth.

Bibliography

Donnelly, S. E., Birtcher, R. C., Allen, C. W., Morrison, I., Furuya, K., Song, M., Mitsuishi, K., & Dahmen, U. (2002). Ordering in a Fluid Inert Gas Confined by Flat Surfaces. Science, 296(5567), 507â510.

Authors 8

Stephen E. Donnelly (first)
Robert C. Birtcher (additional)
Charles W. Allen (additional)
Ian Morrison (additional)
Kazuo Furuya (additional)
Minghui Song (additional)
Kazutaka Mitsuishi (additional)
Ulrich Dahmen (additional)

References 28 Referenced 117

10.1080/14786437708235972
10.1103/PhysRevB.31.4300
10.1021/cr00016a007
10.1016/S0081-1947(08)60638-4
10.1063/1.450311
J. N. Israelachvili Intermolecular Forces and Surface Forces (Academic Press San Diego CA 1992) pp. 261–275.
10.1038/37069
10.1103/PhysRevLett.82.2326
10.1080/01418619608243540
10.1080/00337578508222514
10.1016/0025-5416(85)90373-8
10.1103/PhysRevLett.53.922
10.1126/science.230.4731.1272
10.1046/j.1365-2818.1999.00451.x
MacTempas; Total Resolution Berkeley CA.
Experimental and simulated through-focus sequences are available on Science Online at www.sciencemag.org/cgi/content/full/1068521/DC1.
S. E. Donnelly K. Furuya M. Song R. C. Birtcher C. W. Allen Proceedings of the International Centennial Symposium on the Electron A. Kirkland P. D. Brown Eds. (Institute of Materials London 1999) pp. 306–312.
10.1103/PhysRevLett.83.1617
S. E. Donnelly et al. unpublished data.
The starting point for the fluid Xe simulations was a tetragonal slab of solid fcc Xe with a lattice parameter 1.5 times that of Al confined between two walls 8.06 nm apart each consisting in the first instance of three {111} Al planes. The dimensions of the cell were 8.06 nm 6.86 nm and 7.43 nm in the [1 1 1] [1 −1 0] and [1 1 −2] directions respectively and the crystallographic axes of the Xe were aligned with those of the Al. Periodic boundary conditions were used in the two latter directions. A total of 6720 Xe atoms were used in the simulations. To achieve fluid Xe the volume of the cell was expanded by 30% and the temperature was increased to 2000 K for 1 ps resulting in complete disordering of the Xe layer. The system was then cooled back to 300 K and the simulation continued for a further 10 ps. Two separate simulations were performed: in the first which was performed with the MOLDY code (24) a Lennard-Jones interaction potential was used for all interactions including the Xe-Al interaction. With this approach however equipotential surfaces near the interface were corrugated due to the individual atoms in the interface. This gave rise to a keying effect that resulted in ordering in the first Xe layer that was visible in the simulated images; however such ordering was not observed in the experimental images. The second approach was to replace the three Al layers by a planar repulsive potential of the form V ( R ) = c / R 12 where R is the distance from the facet and c was chosen to give equivalence to the repulsive term in the Lennard-Jones potential. This simulation was performed with the DLPOLY code (25) with an adaptation of the external field routine to represent the planar confining potential. This gave rise to equipotential surfaces that were flat. A realistic Xe-Al potential which is not currently available would result in equipotential surfaces between these two extremes. The planar potential was also used for all six facets in the simulation of the small cubic cavity. Although both simulations are physically unrealistic as far as the Xe-Al interaction is concerned in addition to inducing ordering in the first Xe layer the effect of changing the Al-Xe potential is to change the separation between the Xe and Al interface layers. Hence in this work the separation between the first Xe layer and the Al layers has no quantitative importance.
10.1103/PhysRevE.55.7228
10.1103/PhysRevLett.83.5298
Although metastable Cu precipitates with a bcc structure have been identified in irradiated Fe alloys it is likely that factors other than the confining geometry may play a role in this system (26).
10.1016/S0010-4655(99)00496-8
10.1016/S0263-7855(96)00043-4
10.1080/09500839008202362
Density is determined from the number of atoms contained in a tetragonal box whose faces are located half way between the surface layers and the second layer in each direction. This avoids problems associated with defining the volume associated with the surface atoms.
S.E.D. R.C.B. C.W.A. and U.D. acknowledge funding from the National Institute for Materials Science for collaborative visits to Japan; S.E.D. acknowledges funding from the Materials Science Division at Argonne National Laboratory for extended visits to the laboratory.

Dates

Type	When
Created	23 years, 1 month ago (July 27, 2002, 5:54 a.m.)
Deposited	1 year, 7 months ago (Jan. 9, 2024, 10:38 p.m.)
Indexed	1 year ago (Aug. 7, 2024, 7:56 a.m.)
Issued	23 years, 4 months ago (April 19, 2002)
Published	23 years, 4 months ago (April 19, 2002)
Published Print	23 years, 4 months ago (April 19, 2002)

Funders 0

None

BibTeX

@article{Donnelly_2002, title={Ordering in a Fluid Inert Gas Confined by Flat Surfaces}, volume={296}, ISSN={1095-9203}, url={http://dx.doi.org/10.1126/science.1068521}, DOI={10.1126/science.1068521}, number={5567}, journal={Science}, publisher={American Association for the Advancement of Science (AAAS)}, author={Donnelly, Stephen E. and Birtcher, Robert C. and Allen, Charles W. and Morrison, Ian and Furuya, Kazuo and Song, Minghui and Mitsuishi, Kazutaka and Dahmen, Ulrich}, year={2002}, month=apr, pages={507–510} }

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