Lattice Dynamics and Thermomechanical Properties of Zirconium(IV) Chloride: Evidence for Low-temperature Negative Thermal Expansion

Document Type

Article

Publication Date

11-1-2017

Publication Title

Chemical Physics Letters

Volume

691

First page number:

98

Last page number:

102

Abstract

The crystal structure, lattice dynamics and themomechanical properties of bulk monoclinic zirconium tetrachloride (ZrCl4) have been investigated using zero-damping dispersion-corrected density functional theory [DFT-D3(zero)]. Phonon analysis reveals that ZrCl4(cr) undergoes negative thermal expansion (NTE) near T≈10 K, with a coefficient of thermal expansion of α=-1.2 ppm K−1 and a Grüneisen parameter of γ=-1.1. The bulk modulus is predicted to vary from K0=8.7 to 7.0 GPa in the temperature range 0–550 K. The isobaric molar heat capacity derived from phonon calculations within the quasi-harmonic approximation is in fair agreement with existing calorimetric data.

Disciplines

Biological and Chemical Physics

Language

English

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