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Title: Diffusivity anomaly in modified Stillinger-Weber liquids

By modifying the tetrahedrality (the strength of the three body interactions) in the well-known Stillinger-Weber model for silicon, we study the diffusivity of a series of model liquids as a function of tetrahedrality and temperature at fixed pressure. Previous work has shown that at constant temperature, the diffusivity exhibits a maximum as a function of tetrahedrality, which we refer to as the diffusivity anomaly, in analogy with the well-known anomaly in water upon variation of pressure at constant temperature. We explore to what extent the structural and thermodynamic changes accompanying changes in the interaction potential can help rationalize the diffusivity anomaly, by employing the Rosenfeld relation between diffusivity and the excess entropy (over the ideal gas reference value), and the pair correlation entropy, which provides an approximation to the excess entropy in terms of the pair correlation function. We find that in the modified Stillinger-Weber liquids, the Rosenfeld relation works well above the melting temperatures but exhibits deviations below, with the deviations becoming smaller for smaller tetrahedrality. Further we find that both the excess entropy and the pair correlation entropy at constant temperature go through maxima as a function of the tetrahedrality, thus demonstrating the close relationship between structural, thermodynamic,more » and dynamical anomalies in the modified Stillinger-Weber liquids.« less
Authors:
 [1] ;  [2] ;  [1] ;  [3]
  1. TIFR Centre for Interdisciplinary Sciences, 21 Brundavan Colony, Narsingi, Hyderabad 500089 (India)
  2. Theoretical Sciences Unit, Jawaharlal Nehru Centre for Advanced Scientific Research, Jakkur Campus, Bangalore 560064 (India)
  3. (India)
Publication Date:
OSTI Identifier:
22255239
Resource Type:
Journal Article
Resource Relation:
Journal Name: Journal of Chemical Physics; Journal Volume: 140; Journal Issue: 4; Other Information: (c) 2014 AIP Publishing LLC; Country of input: International Atomic Energy Agency (IAEA)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL AND ANALYTICAL CHEMISTRY; APPROXIMATIONS; CORRELATION FUNCTIONS; CORRELATIONS; ENTROPY; INTERACTIONS; LIQUIDS; MELTING POINTS; SILICON