Triplet Correlations Dominate the Transition from Simple to Tetrahedral Liquids

Murari Singh, Debdas Dhabal, Andrew Huy Nguyen, Valeria Molinero, and Charusita Chakravarty

Phys. Rev. Lett. 112, 147801 – Published 10 April 2014

Abstract

The total, triplet, and pair contributions to the entropy with increasing tetrahedrality are mapped out for the Stillinger-Weber liquids to demonstrate the qualitative and quantitative differences between triplet-dominated, tetrahedral liquids and pair-dominated, simple liquids with regard to supercooling and crystallization. The heat capacity anomaly of tetrahedral liquids originates in local ordering due to both pair and triplet correlations. The results suggest that structural correlations can be directly related to thermodynamic anomalies, phase changes, and self-assembly in other atomic and colloidal fluids.

Received 10 August 2013

DOI:https://doi.org/10.1103/PhysRevLett.112.147801

Authors & Affiliations

Murari Singh¹, Debdas Dhabal², Andrew Huy Nguyen³, Valeria Molinero³, and Charusita Chakravarty^2,*

¹School of Physical Sciences, Jawaharlal Nehru University, New Delhi 110067, India
²Department of Chemistry, Indian Institute of Technology-Delhi, New Delhi 110016, India
³Department of Chemistry, The University of Utah, Salt Lake City, Utah 84112-0850, USA

^*Corresponding author. charus@chemistry.iitd.ac.in

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Issue

Vol. 112, Iss. 14 — 11 April 2014

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