J. Phys. Soc. Jpn. 88, 114601 (2019) [9 Pages]
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Pressure-Induced Collapse of the Guest Eu Off-Centering in Type-I Clathrate Eu8Ga16Ge30

Naoki Ishimatsu1, , Kei Yokoyama1, Takahiro Onimaru2, Toshiro Takabatake2, Koichiro Suekuni3 , Naomi Kawamura4 , Satoshi Tsutsui4 , Masaichiro Mizumaki4, Toshiaki Ina4, Tetsu Watanuki5, Vera Cuartero6, , Olivier Mathon6, Sakura Pascarelli6 , Eiji Nishibori7 , and Tetsuo Irifune8
+ Affiliations
1Department of Physics, Graduate School of Science, Hiroshima University, Higashihiroshima, Hiroshima 739-8526, Japan2Department of Quantum Matter, AdSM, Hiroshima University, Higashihiroshima, Hiroshima 739-8530, Japan3Department of Applied Science for Electronics and Materials, IGSES, Kyusyu University, Kasuga, Fukuoka 816-8580, Japan4Japan Synchrotron Radiation Research Institute (JASRI), SPring-8, Sayo, Hyogo 679-5198, Japan5Synchrotron Radiation Research Center, National Institutes for Quantum and Radiological Science and Technology, Sayo, Hyogo 679-5148, Japan6ESRF-The European Synchrotron 71, Avenue des Martyrs Grenoble, France7Faculty of Pure and Applied Sciences and Tsukuba Research Center for Energy Materials Science (TREMS), University of Tsukuba, Tsukuba, Ibaraki 305-8571, Japan8Geodynamics Research Center (GRC), Ehime University, Matsuyama 790-8577, Japan
Received July 28, 2019; Accepted September 4, 2019; Published October 10, 2019

We have revealed the pressure-induced collapse of the guest Eu off-centering in type-I clathrate Eu8Ga16Ge30 by the measurements of extended X-ray absorption fine structure (EXAFS) at the Ge K-edge in a temperature range of 10–300 K. Our analysis of the EXAFS spectra at ambient pressure confirmed that the guest Eu is located in the off-centered positions at Δoffset = 0.39(1) Å away from the center of the Ga/Ge tetradodecahedron cage (14-cage). However, with applying pressure to 13.1 GPa, Δoffset decreases to zero, and the atomic density of Eu is concentrated near the center of the 14-cage with a broad distribution. The present result demonstrates a close relationship between Δoffset and the size of the cage: Δoffset decreases when the 14-cage shrinks by applying pressure. With further compression, we have observed a drastic change in the EXAFS spectra due to amorphization. In the amorphous phase, the first nearest neighbor Ge–Ga/Ge bond is longer than in the crystal phase, whereas the guest Eu atom is located randomly with respect to the Ge atoms.

©2019 The Physical Society of Japan
https://doi.org/10.7566/JPSJ.88.114601

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