Cage disorder and gas encapsulation as routes to tailor properties of inorganic clathrates

Khabibullin, A. R.; Huan, T. D.; Nolas, G. S.; Woods, L. M.

doi:10.1016/j.actamat.2017.03.059

Cage disorder and gas encapsulation as routes to tailor properties of inorganic clathrates

Journal Article · Thu Mar 30 00:00:00 EDT 2017 · Acta Materialia

DOI:https://doi.org/10.1016/j.actamat.2017.03.059· OSTI ID:1533472

Khabibullin, A. R. ^[1]; ^[2]; Nolas, G. S. ^[3]; Woods, L. M. ^[3]

Univ. of South Florida, Tampa, FL (United States). Dept. of Physics; DOE/OSTI
Univ. of Connecticut, Storrs, CT (United States). Dept. of Materials Science & Engineering. Inst. of Materials Science
Univ. of South Florida, Tampa, FL (United States). Dept. of Physics

Inorganic clathrates with the type II crystal structure are of interest as potential materials for high temperature thermoelectric applications. In this study we present ab initio calculations for the electronic and phonon properties of several Sn type II clathrate compositions with partial Ga substitution on the framework, empty cage Sn₁₃₆, and compounds of Sn₁₃₆ filled with inert Xe atoms. It is found that cage disorder due to atomic substitution and guest encapsulation affect the fundamental characteristics of these materials in profound ways. We determine that the stability of these materials is enhanced by the presence of guests and lack of direct Ga-Ga bonds in disordered clathrates. Inert Xe atoms provide a unique opportunity to preserve the overall electronic structure of Sn₁₃₆ and take advantage of the loosely bound guest rattling for enhanced phonon scattering. The calculated energy bands and density of states, as well as phonon band structure and mode Gruneisen parameter, enable further analysis of type II Sn clathrates and reveal interesting structure-property relations.

View Accepted Manuscript (DOE)

Research Organization:: Univ. of South Florida, Tampa, FL (United States)

Sponsoring Organization:: USDOE; USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: FG02-04ER46145

OSTI ID:: 1533472

Alternate ID(s):: OSTI ID: 22647146
OSTI ID: 1398630

Journal Information:: Acta Materialia, Journal Name: Acta Materialia Vol. 131; ISSN 1359-6454

Publisher:: ElsevierCopyright Statement

Country of Publication:: United States

Language:: English

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