Observation of Square-Planar Distortion in Lanthanide-Doped Skutterudite Crystals

Bethany M. Hudak; Weiwei Sun; Jon MacKey; Ahamed Ullah; Alp Sehirlioglu; Frederick Dynys; Sokrates T. Pantelides; Beth S. Guiton

doi:10.1021/acs.jpcc.9b02110

Observation of Square-Planar Distortion in Lanthanide-Doped Skutterudite Crystals

Bethany M. Hudak, Weiwei Sun, Jon MacKey, Ahamed Ullah, Alp Sehirlioglu, Frederick Dynys, Sokrates T. Pantelides, Beth S. Guiton

Chemistry

Research output: Contribution to journal › Article › peer-review

1 Scopus citations

Abstract

Skutterudite crystals are of interest for their thermoelectric properties and in particular for the flexibility the structure offers for tuning such properties. One strategy to enhance the thermoelectric capabilities of these structures is to dope the "cage" site to disrupt phonon modes. Observation of such changes in these structures on the atomic scale is challenging, however, and understanding atomic-scale changes is crucial to understanding its macroscopic properties. Here, a series of polycrystalline Co₂Ni₂Sb₈Sn₄ skutterudites doped with Ce, Dy, and Yb were synthesized. Using scanning transmission electron microscopy, we observe small tilts in the square-planar Sb-Sn rings. Using density functional theory to calculate a relaxed structure, we attribute these distortions to under-bonding of the rings with the lanthanide dopants.

Original language	English
Pages (from-to)	14632-14638
Number of pages	7
Journal	Journal of Physical Chemistry C
Volume	123
Issue number	23
DOIs	https://doi.org/10.1021/acs.jpcc.9b02110
State	Published - Jun 13 2019

Bibliographical note

Funding Information:
This research was supported in part by the U.S. Department of Energy, Office of Science, Basic Energy Sciences, Materials Sciences and Engineering Division. Funding for this work was provided by funding source NASA/USRA 04555-004, the NASA Radioisotope Power System Program, by NASA Kentucky under NASA Award No: NNX10AL96H (BMH), by the National Science Foundation under award number DMR 1455154 (BSG), and by the Research Corporation for Scientific Advancement via Scialog Award number 26329 (AU). Theoretical work by WS and STP was supported by DOE grant DE-FG02-09ER46554.

Publisher Copyright:
© 2019 American Chemical Society.

ASJC Scopus subject areas

Electronic, Optical and Magnetic Materials
Energy (all)
Physical and Theoretical Chemistry
Surfaces, Coatings and Films

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AU - Hudak, Bethany M.

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AU - Sehirlioglu, Alp

AU - Dynys, Frederick

AU - Pantelides, Sokrates T.

AU - Guiton, Beth S.

N1 - Funding Information: This research was supported in part by the U.S. Department of Energy, Office of Science, Basic Energy Sciences, Materials Sciences and Engineering Division. Funding for this work was provided by funding source NASA/USRA 04555-004, the NASA Radioisotope Power System Program, by NASA Kentucky under NASA Award No: NNX10AL96H (BMH), by the National Science Foundation under award number DMR 1455154 (BSG), and by the Research Corporation for Scientific Advancement via Scialog Award number 26329 (AU). Theoretical work by WS and STP was supported by DOE grant DE-FG02-09ER46554. Publisher Copyright: © 2019 American Chemical Society.

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Observation of Square-Planar Distortion in Lanthanide-Doped Skutterudite Crystals

Abstract

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