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, Min Jae Kim, GwangCheol Ji, Sehwan Song, Hyesung Jo, Seokjo Hong, Nguyen Xuan Duong, Subhasis Samanta, Heung-Sik Kim, Tae Heon Kim, Yongsoo Yang, Sungkyun Park, Jong Mok Ok, Jung-Woo Yoo (), Jae Hoon Kim () and Changhee Sohn ()
Additional contact information
Baekjune Kang: Ulsan National Institute of Science and Technology
Uksam Choi: Ulsan National Institute of Science and Technology
Taek Sun Jung: Yonsei University
Seunghyeon Noh: Ulsan National Institute of Science and Technology
Gye-Hyeon Kim: Ulsan National Institute of Science and Technology
Uihyeon Seo: Ulsan National Institute of Science and Technology
Miju Park: Ulsan National Institute of Science and Technology
Jin-Hyun Choi: Ulsan National Institute of Science and Technology
Min Jae Kim: Pusan National University
GwangCheol Ji: Pusan National University
Sehwan Song: Pusan National University
Hyesung Jo: Korea Advanced Institute of Science and Technology
Seokjo Hong: Korea Advanced Institute of Science and Technology
Nguyen Xuan Duong: University of Ulsan
Subhasis Samanta: Kangwon National University
Heung-Sik Kim: Kangwon National University
Tae Heon Kim: University of Ulsan
Yongsoo Yang: Korea Advanced Institute of Science and Technology
Sungkyun Park: Pusan National University
Jong Mok Ok: Pusan National University
Jung-Woo Yoo: Ulsan National Institute of Science and Technology
Jae Hoon Kim: Yonsei University
Changhee Sohn: Ulsan National Institute of Science and Technology

Nature Communications, 2025, vol. 16, issue 1, 1-10

Abstract: Abstract Two-dimensional honeycomb antiferromagnets are promising materials class for realizing Kitaev quantum spin liquids. The signature of these materials includes anisotropic bond-dependent magnetic responses and persistent fluctuations in paramagnetic regime. Here, we propose Cu3Co2SbO6 heterostructures as an intriguing candidate, wherein bond-dependent and frustrated spins interact with optical excitons. First-principles spin Hamiltonian calculations and in-plane anisotropic critical fields suggest strong frustration and dominant Kitaev exchange interactions. Optical spectroscopy reveals exciton coupled to frustrated magnetism, enabling optical detection of spin states. Spin-exciton coupling displays anisotropic responses to light polarization along the bond-parallel and the bond-perpendicular directions, highlighting Kitaev interactions and persistent short-range spin correlations above twice the Néel temperatures. The robustness of short-range spin fluctuations under magnetic fields underscores the stability of the spin-fluctuation region. Our results establish Cu3Co2SbO6 as an attractive candidate for exploring quantum spin liquid, where the spin Hamiltonian and quasiparticle excitations can be probed and potentially controlled by light.

Date: 2025
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DOI: 10.1038/s41467-025-56652-w

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