Crystallographic origin of pressure-induced bond order in the frustrated spinel CuIr₂S₄
Abstract
CuIr ₂ S ₄ is a frustrated pyrochlore spinel in which pressure reshapes competing charge- and bond-ordered states. Here we determine the crystallographic nature of its pressure-induced ordered phases up to about 25 GPa by high-pressure synchrotron powder X-ray diffraction combined with first-principles-guided structural analysis. Pressure first stabilizes the ambient-pressure low-temperature ordered state to room temperature and then induces a distinct high-pressure phase. Using single-phase datasets collected at 19.8 and 25.7 GPa, we perform full-atom refinements that consistently establish the Phase-IV symmetry and Ir–Ir short-bond topology. The resulting Phase IV pattern differs from Phase II and is not captured by a simple orbitally induced Peierls picture. Instead, it is consistent with an Anderson-type local tetrahedron rule on the pyrochlore lattice. Total-energy calculations reproduce a pressure-induced reversal in the relative stability of the Phase-II- and Phase-IV-type structural models.
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BibTeX
@article{emi2026crystallographic,
title = {{Crystallographic origin of pressure-induced bond order in the frustrated spinel CuIr₂S₄}},
author = {Masatoshi Emi and Tsubasa Ohashi and Keita Kojima and Koudai Sugimoto and Kazuyuki Matsubayashi and Kenta Oka and Hirokazu Kadobayashi and Saori Kawaguchi-Imada and Daigo Ito and Taisei Kubo and Kenta Hashimoto and Hitoshi Kawaji and Hiroyuki S. Suzuki and Shoichi Nagata and Naoyuki Katayama},
journal = {Communications Chemistry},
year = {2026},
month = oct,
doi = {10.1038/s42004-026-02240-y},
url = {https://www.nature.com/articles/s42004-026-02240-y},
note = {CC BY 4.0},
}
RIS
TY - JOUR
TI - Crystallographic origin of pressure-induced bond order in the frustrated spinel CuIr₂S₄
AU - Masatoshi Emi
AU - Tsubasa Ohashi
AU - Keita Kojima
AU - Koudai Sugimoto
AU - Kazuyuki Matsubayashi
AU - Kenta Oka
AU - Hirokazu Kadobayashi
AU - Saori Kawaguchi-Imada
AU - Daigo Ito
AU - Taisei Kubo
AU - Kenta Hashimoto
AU - Hitoshi Kawaji
AU - Hiroyuki S. Suzuki
AU - Shoichi Nagata
AU - Naoyuki Katayama
PY - 2026
DA - 2026/10/26
JO - Communications Chemistry
DO - 10.1038/s42004-026-02240-y
UR - https://www.nature.com/articles/s42004-026-02240-y
AB - CuIr ₂ S ₄ is a frustrated pyrochlore spinel in which pressure reshapes competing charge- and bond-ordered states. Here we determine the crystallographic nature of its pressure-induced ordered phases up to about 25 GPa by high-pressure synchrotron powder X-ray diffraction combined with first-principles-guided structural analysis. Pressure first stabilizes the ambient-pressure low-temperature ordered state to room temperature and then induces a distinct high-pressure phase. Using single-phase datasets collected at 19.8 and 25.7 GPa, we perform full-atom refinements that consistently establish the Phase-IV symmetry and Ir–Ir short-bond topology. The resulting Phase IV pattern differs from Phase II and is not captured by a simple orbitally induced Peierls picture. Instead, it is consistent with an Anderson-type local tetrahedron rule on the pyrochlore lattice. Total-energy calculations reproduce a pressure-induced reversal in the relative stability of the Phase-II- and Phase-IV-type structural models.
SN - 2399-3669
ER -