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arXiv · 2309.15753

Optical detection of bond-dependent and frustrated spin in the two-dimensional cobalt-based honeycomb antiferromagnet Cu3Co2SbO6

Baekjune Kang·Uksam Choi·Taek Sun Jung·Seunghyeon Noh·Gye-Hyeon Kim·UiHyeon Seo·Miju Park·Jin-Hyun Choi·Minjae Kim·GwangCheol Ji·Sehwan Song·Hyesung Jo·Seokjo Hong·Nguyen Xuan Duong·Tae Heon Kim·Yongsoo Yang·Sungkyun Park·Jong Mok Ok·Jung-Woo Yoo·Jae Hoon Kim·Changhee Sohn
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Abstract

Two-dimensional honeycomb antiferromagnet becomes an important class of materials as it can provide a route to Kitaev quantum spin liquid, characterized by massive quantum entanglement and fractional excitations. The signatures of its proximity to Kitaev quantum spin liquid in the honeycomb antiferromagnet includes anisotropic bond-dependent magnetic responses and persistent fluctuation by frustration in paramagnetic regime. Here, we propose Cu3Co2SbO6 heterostructures as an intriguing honeycomb antiferromagnet for quantum spin liquid, wherein bond-dependent and frustrated spins interact with optical excitons. This system exhibits antiferromagnetism at 16 K with different spin-flip magnetic fields between a bond-parallel and bond-perpendicular directions, aligning more closely with the generalized Heisenberg-Kitaev than the XXZ model. Optical spectroscopy reveals a strong excitonic transition coupled to the antiferromagnetism, enabling optical detection of its spin states. Particularly, such spin-exciton coupling presents anisotropic responses between bond-parallel and bond-perpendicular magnetic field as well as a finite spin-spin correlation function around 40 K, higher than twice its Néel temperature. The characteristic temperature that remains barely changed even under strong magnetic fields highlights the robustness of the spin-fluctuation region. Our results demonstrate Cu3Co2SbO6 as a unique candidate for the quantum spin liquid phase, where the spin Hamiltonian and quasiparticle excitations can be probed and potentially controlled by light.

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Baekjune Kang, Uksam Choi, Taek Sun Jung, Seunghyeon Noh, Gye-Hyeon Kim, UiHyeon Seo, Miju Park, Jin-Hyun Choi, Minjae Kim, GwangCheol Ji, Sehwan Song, Hyesung Jo, Seokjo Hong, Nguyen Xuan Duong, Tae Heon Kim, Yongsoo Yang, Sungkyun Park, Jong Mok Ok, Jung-Woo Yoo, Jae Hoon Kim, Changhee Sohn. 2023-09-27. Optical detection of bond-dependent and frustrated spin in the two-dimensional cobalt-based honeycomb antiferromagnet Cu3Co2SbO6. https://doi.org/10.1038/s41467-025-56652-w

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