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Title: Efficient Calculation of the Negative Thermal Expansion in ZrW2O8

Journal Article · · Frontiers in Chemistry
 [1];  [1];  [1]
  1. Univ. of Washington, Seattle, WA (United States). Dept. of Physics

We present a study of the origin of the negative thermal expansion (NTE) on ZrW2O8 by combining an efficient approach for computing the dynamical matrix with the Lanczos algorithm for generating the phonon density of states in the quasi-harmonic approximation. The simulations show that the NTE arises primarily from the motion of the O-sublattice, and in particular, from the transverse motion of the O atoms in the W–O and W–O–Zr bonds. In the low frequency range these combine to keep the WO4 tetrahedra rigid and induce internal distortions in the ZrO6 octahedra. The force constants associated with these distortions become stronger with expansion, resulting in negative Grüneisen parameters and NTE from the low frequency modes that dominate the positive contributions from the high frequency modes. This leads us to propose an anharmonic, two-frequency Einstein model that quantitatively captures the NTE behavior.

Research Organization:
Univ. of Illinois, Urbana-Champaign, IL (United States) Stanford Univ., CA (United States)
Sponsoring Organization:
USDOE Office of Science (SC); USDOE
Grant/Contract Number:
FG02-03ER15476; AC02-05CH11231; CSGBD Grant No. DE-FG02-03ER15476
OSTI ID:
1462120
Alternate ID(s):
OSTI ID: 1510436
Journal Information:
Frontiers in Chemistry, Vol. 6; ISSN 2296-2646
Publisher:
Frontiers Research FoundationCopyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 9 works
Citation information provided by
Web of Science

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Figures / Tables (11)