Dimer Crystallization Induced by Elemental Substitution in the Honeycomb Lattice of Ru1-xOsxCl3
- Authors
- Kataoka, K.; Wulferding, D.; Yajima, T.; Nishio-Hamane, D.; Hirai, D.; Lee, S.; Choi, K.-Y.; Hiroi, Z.
- Issue Date
- Jan-2022
- Publisher
- Physical Society of Japan
- Citation
- Journal of the Physical Society of Japan, v.91, no.1
- Journal Title
- Journal of the Physical Society of Japan
- Volume
- 91
- Number
- 1
- URI
- https://scholarworks.bwise.kr/cau/handle/2019.sw.cau/61991
- DOI
- 10.7566/JPSJ.91.014801
- ISSN
- 0031-9015
1347-4073
- Abstract
- Substitution effects of Os for Ru in α-RuCl3 are investigated in a wide composition range of 0 ≤ x ≤ 0.67 in Ru1-x-OsxCl3by X-ray and electron diffraction, magnetic susceptibility, heat capacity, and Raman spectroscopy measurements. Apart from the Kitaev physics with antiferromagnetic interactions increasing with x, a rich phase diagram is obtained, which includes an antiferromagnetic long-range order below 12K for x ≤ 0.15, a dome-shaped spin-singlet dimer phase below 130K for 0.15 ≤ x ≤ 0.40, and a magnetic short-range order for x > 0.40. A dimerization as similarly observed in α-RuCl3under high pressure occurs in the spin-singlet phase. It is suggested that Ru-Os pairs in the solid solutions tend to form dimers with short bonds and trigger the first-order transition in the presence of pseudo-threefold rotational symmetry for dimerization around a substituted Os atom only at low substitutions. This is a rare example of molecular orbital crystallization induced by elemental substitution in a highly disordered system. The short-range order at high substitutions may be related to a random-singlet state stabilized by bond disorder in the honeycomb net. © 2022 Physical Society of Japan. All rights reserved.
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