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Title: Dynamics and diffusion mechanism of low-density liquid silicon

Abstract

A first-order phase transition from a high-density liquid to a low-density liquid has been proposed to explain the various thermodynamic anomies of water. It also has been proposed that such liquid–liquid phase transition would exist in supercooled silicon. Computer simulation studies show that, across the transition, the diffusivity drops roughly 2 orders of magnitude, and the structures exhibit considerable tetrahedral ordering. The resulting phase is a highly viscous, low-density liquid silicon. Investigations on the atomic diffusion of such a novel form of liquid silicon are of high interest. Here we report such diffusion results from molecular dynamics simulations using the classical Stillinger–Weber (SW) potential of silicon. We show that the atomic diffusion of the low-density liquid is highly correlated with local tetrahedral geometries. We also show that atoms diffuse through hopping processes within short ranges, which gradually accumulate to an overall random motion for long ranges as in normal liquids. There is a close relationship between dynamical heterogeneity and hopping process. We point out that the above diffusion mechanism is closely related to the strong directional bonding nature of the distorted tetrahedral network. Here, our work offers new insights into the complex behavior of the highly viscous low density liquidmore » silicon, suggesting similar diffusion behaviors in other tetrahedral coordinated liquids that exhibit liquid–liquid phase transition such as carbon and germanium.« less

Authors:
 [1];  [2];  [2];  [2];  [2];  [2];  [3];  [4];  [4];  [2]
  1. Fudan Univ., Shanghai (China); Ames Lab., Ames, IA (United States); Iowa State Univ., Ames, IA (United States)
  2. Fudan Univ., Shanghai (China)
  3. Fudan Univ., Shanghai (China); Ames Lab., Ames, IA (United States); Iowa State Univ., Ames, IA (United States); Key Lab. for Information Science of Electromagnetic Waves (MoE), Shanghai (China)
  4. Ames Lab., Ames, IA (United States); Iowa State Univ., Ames, IA (United States)
Publication Date:
Research Org.:
Ames Laboratory (AMES), Ames, IA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1244421
Report Number(s):
IS-J-8887
Journal ID: ISSN 1520-6106
Grant/Contract Number:  
2010CB933703; 2012CB934303; 11374055; 61427815; AC02-07CH11358
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Physical Chemistry. B, Condensed Matter, Materials, Surfaces, Interfaces and Biophysical Chemistry
Additional Journal Information:
Journal Volume: 119; Journal Issue: 47; Journal ID: ISSN 1520-6106
Publisher:
American Chemical Society
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE

Citation Formats

Shen, B., Wang, Z. Y., Dong, F., Guo, Y. R., Zhang, R. J., Zheng, Y. X., Wang, S. Y., Wang, C. Z., Ho, K. M., and Chen, L. Y. Dynamics and diffusion mechanism of low-density liquid silicon. United States: N. p., 2015. Web. doi:10.1021/acs.jpcb.5b09138.
Shen, B., Wang, Z. Y., Dong, F., Guo, Y. R., Zhang, R. J., Zheng, Y. X., Wang, S. Y., Wang, C. Z., Ho, K. M., & Chen, L. Y. Dynamics and diffusion mechanism of low-density liquid silicon. United States. doi:10.1021/acs.jpcb.5b09138.
Shen, B., Wang, Z. Y., Dong, F., Guo, Y. R., Zhang, R. J., Zheng, Y. X., Wang, S. Y., Wang, C. Z., Ho, K. M., and Chen, L. Y. Thu . "Dynamics and diffusion mechanism of low-density liquid silicon". United States. doi:10.1021/acs.jpcb.5b09138. https://www.osti.gov/servlets/purl/1244421.
@article{osti_1244421,
title = {Dynamics and diffusion mechanism of low-density liquid silicon},
author = {Shen, B. and Wang, Z. Y. and Dong, F. and Guo, Y. R. and Zhang, R. J. and Zheng, Y. X. and Wang, S. Y. and Wang, C. Z. and Ho, K. M. and Chen, L. Y.},
abstractNote = {A first-order phase transition from a high-density liquid to a low-density liquid has been proposed to explain the various thermodynamic anomies of water. It also has been proposed that such liquid–liquid phase transition would exist in supercooled silicon. Computer simulation studies show that, across the transition, the diffusivity drops roughly 2 orders of magnitude, and the structures exhibit considerable tetrahedral ordering. The resulting phase is a highly viscous, low-density liquid silicon. Investigations on the atomic diffusion of such a novel form of liquid silicon are of high interest. Here we report such diffusion results from molecular dynamics simulations using the classical Stillinger–Weber (SW) potential of silicon. We show that the atomic diffusion of the low-density liquid is highly correlated with local tetrahedral geometries. We also show that atoms diffuse through hopping processes within short ranges, which gradually accumulate to an overall random motion for long ranges as in normal liquids. There is a close relationship between dynamical heterogeneity and hopping process. We point out that the above diffusion mechanism is closely related to the strong directional bonding nature of the distorted tetrahedral network. Here, our work offers new insights into the complex behavior of the highly viscous low density liquid silicon, suggesting similar diffusion behaviors in other tetrahedral coordinated liquids that exhibit liquid–liquid phase transition such as carbon and germanium.},
doi = {10.1021/acs.jpcb.5b09138},
journal = {Journal of Physical Chemistry. B, Condensed Matter, Materials, Surfaces, Interfaces and Biophysical Chemistry},
number = 47,
volume = 119,
place = {United States},
year = {2015},
month = {11}
}

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