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

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

Publisher Copyright:
© 2019 American Chemical Society.

Funding

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.

Funders	Funder number
Kentucky NASA EPSCoR RIA	NNX10AL96H
NASA Radioisotope Power System Program
U.S. Department of Energy Chinese Academy of Sciences Guangzhou Municipal Science and Technology Project Oak Ridge National Laboratory Extreme Science and Engineering Discovery Environment National Science Foundation National Energy Research Scientific Computing Center National Natural Science Foundation of China	DMR 1455154
U.S. Department of Energy Chinese Academy of Sciences Guangzhou Municipal Science and Technology Project Oak Ridge National Laboratory Extreme Science and Engineering Discovery Environment National Science Foundation National Energy Research Scientific Computing Center National Natural Science Foundation of China
U.S. Department of Energy Oak Ridge National Laboratory U.S. Department of Energy National Science Foundation National Energy Research Scientific Computing Center	DE-FG02-09ER46554
U.S. Department of Energy Oak Ridge National Laboratory U.S. Department of Energy National Science Foundation National Energy Research Scientific Computing Center
National Science Foundation Office of International Science and Engineering
DOE Basic Energy Sciences	NASA/USRA 04555-004
DOE Basic Energy Sciences
Research Corporation for Scientific Advancement	26329
Research Corporation for Scientific Advancement

ASJC Scopus subject areas

Electronic, Optical and Magnetic Materials
General Energy
Physical and Theoretical Chemistry
Surfaces, Coatings and Films

Access to Document

10.1021/acs.jpcc.9b02110

Cite this

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AU - Sehirlioglu, Alp

AU - Dynys, Frederick

AU - Pantelides, Sokrates T.

AU - Guiton, Beth S.

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

Abstract

Bibliographical note

Funding

ASJC Scopus subject areas

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