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Title: Lattice dynamics and thermomechanical properties of zirconium(IV) chloride: Evidence for low-temperature negative thermal expansion

For this research, the crystal structure, lattice dynamics and themomechanical properties of bulk monoclinic zirconium tetrachloride (ZrCl 4) have been investigated using zero-damping dispersion-corrected density functional theory [DFT-D3(zero)]. Phonon analysis reveals that ZrCl 4(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 K 0=8.7 to 7.0 GPa in the temperature range 0–550 K. Lastly, the isobaric molar heat capacity derived from phonon calculations within the quasi-harmonic approximation is in fair agreement with existing calorimetric data.
Authors:
 [1] ;  [2] ;  [3] ;  [3]
  1. Univ. of Nevada, Las Vegas, NV (United States). Department of Physics and Astronomy
  2. Sandia National Lab. (SNL-NM), Albuquerque, NM (United States)
  3. Univ. of Nevada, Las Vegas, NV (United States). Department of Chemistry
Publication Date:
Report Number(s):
SAND-2017-9739J
Journal ID: ISSN 0009-2614; PII: S0009261417310084; TRN: US1800250
Grant/Contract Number:
AC04-94AL85000; NA0003525
Type:
Accepted Manuscript
Journal Name:
Chemical Physics Letters
Additional Journal Information:
Journal Volume: 691; Journal Issue: C; Journal ID: ISSN 0009-2614
Publisher:
Elsevier
Research Org:
Sandia National Lab. (SNL-NM), Albuquerque, NM (United States)
Sponsoring Org:
USDOE National Nuclear Security Administration (NNSA); USDOE Office of Nuclear Energy (NE)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
OSTI Identifier:
1411613

Kim, Eunja, Weck, Philippe F., Borjas, Rosendo, and Poineau, Frederic. Lattice dynamics and thermomechanical properties of zirconium(IV) chloride: Evidence for low-temperature negative thermal expansion. United States: N. p., Web. doi:10.1016/j.cplett.2017.10.065.
Kim, Eunja, Weck, Philippe F., Borjas, Rosendo, & Poineau, Frederic. Lattice dynamics and thermomechanical properties of zirconium(IV) chloride: Evidence for low-temperature negative thermal expansion. United States. doi:10.1016/j.cplett.2017.10.065.
Kim, Eunja, Weck, Philippe F., Borjas, Rosendo, and Poineau, Frederic. 2017. "Lattice dynamics and thermomechanical properties of zirconium(IV) chloride: Evidence for low-temperature negative thermal expansion". United States. doi:10.1016/j.cplett.2017.10.065.
@article{osti_1411613,
title = {Lattice dynamics and thermomechanical properties of zirconium(IV) chloride: Evidence for low-temperature negative thermal expansion},
author = {Kim, Eunja and Weck, Philippe F. and Borjas, Rosendo and Poineau, Frederic},
abstractNote = {For this research, 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. Lastly, the isobaric molar heat capacity derived from phonon calculations within the quasi-harmonic approximation is in fair agreement with existing calorimetric data.},
doi = {10.1016/j.cplett.2017.10.065},
journal = {Chemical Physics Letters},
number = C,
volume = 691,
place = {United States},
year = {2017},
month = {11}
}