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Cited by 158Advanced Condensed Matter PhysicsPhysics of Superconductivity and MagnetismMagnetism in coordination complexes

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Field-induced quantum spin disordered state in spin-1/2 honeycomb magnet Na2Co2TeO6

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Lin, Gaoting, Jeong, Jaehong, Kim, Chaebin, Wang, Yao, Huang, Qing, Masuda, Takatsugu, Asai, Shinichiro, Itoh, Shinichi, Günther, Gerrit, Russina, Margarita, Lu, Zhilun, Sheng, Jieming, Wang, Le, Wang, Jiucai, Wang, Guohua, Ren, Qingyong, Xi, Chuanying, Tong, Wei, Ling, Langsheng, Liu, Zhengxin, Wu, Liusuo, Mei, Jiawei, Qu, Zhe, Zhou, Haidong, Wang, Xiaoqun, Park, Je-Geun, Wan, Yuan, Ma, Jie·2021·Nature Communications
DOI 10.1038/s41467-021-25567-7PMC PMC8455656
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Abstract

Spin-orbit coupled honeycomb magnets with the Kitaev interaction have received a lot of attention due to their potential of hosting exotic quantum states including quantum spin liquids. Thus far, the most studied Kitaev systems are 4 d/5 d-based honeycomb magnets. Recent theoretical studies predicted that 3 d-based honeycomb magnets, including Na 2 Co 2 TeO 6 (NCTO), could also be a potential Kitaev system. Here, we have used a combination of heat capacity, magnetization, electron spin resonance measurements alongside inelastic neutron scattering (INS) to study NCTO’s quantum magnetism, and we have found a field-induced spin disordered state in an applied magnetic field range of 7.5 T < B (⊥ b-axis) < 10.5 T. The INS spectra were also simulated to tentatively extract the exchange interactions. As a 3 d-magnet with a field-induced disordered state on an effective spin-1/2 honeycomb lattice, NCTO expands the Kitaev model to 3 d compounds, promoting further interests on the spin-orbital effect in quantum magnets.

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Figures

Fig. 1 Heat capacity of Na2Co2TeO6. a Temperature dependence of the magnetic specific heat of NCTO for different magnetic fields up to 14 T. The inset shows the differential magnetic specific heat dCmag/dT, and three transitions are observed as TN, TF, and T*, respectively. b The magnetic entropy Smag(T) at 0, 9, and 12 T. The olive dashed line refers to Smag(T → ∞) calculated with effective spin Jeff = 1/2 for Co2+. In order to better observe the residual magnetic entropy, the Smag(T) curves are shifted vertically so that their maxima coincide with the Smag(T → ∞). The black, red, and blue dashed line refer to the possible residual magnetic entropy below 2 K under different magnetic field. Compared with the total magnetic entropy Smag(T → ∞), the percentage of residual magnetic entropy in different magnetic fields is shown in the figure. c A zoom-in of magnetic entropy below TN at various magnetic fields. Note the data are not shifted vertically as opposed to (b). The inset shows the field dependence of the Smag at 17 K.
Fig. 1 Heat capacity of Na2Co2TeO6. a Temperature dependence of the magnetic specific heat of NCTO for different magnetic fields up to 14 T. The inset shows the differential magnetic specific heat dCmag/dT, and three transitions are observed as TN, TF, and T*, respectively. b The magnetic entropy Smag(T) at 0, 9, and 12 T. The olive dashed line refers to Smag(T → ∞) calculated with effective spin Jeff = 1/2 for Co2+. In order to better observe the residual magnetic entropy, the Smag(T) curves are shifted vertically so that their maxima coincide with the Smag(T → ∞). The black, red, and blue dashed line refer to the possible residual magnetic entropy below 2 K under different magnetic field. Compared with the total magnetic entropy Smag(T → ∞), the percentage of residual magnetic entropy in different magnetic fields is shown in the figure. c A zoom-in of magnetic entropy below TN at various magnetic fields. Note the data are not shifted vertically as opposed to (b). The inset shows the field dependence of the Smag at 17 K.CC BY · PubMed Central
Fig. 2 Magnetic susceptibility of Na2Co2TeO6 for B ⊥ b-axis. a, b Temperature dependence of susceptibility χ(T) in NCTO measured at various magnetic fields. The inset of Fig. 2b shows the honeycomb lattices of Co viewed along the c-axis. The cartoon shows the moments to be in the basal plane and parallel to the b-axis40, 41, and the TeO6 octahedra sit at the center of each honeycomb unit. The first NN ferromagnetic (FM) interaction J originated from a collaboration between Co–O–Co (red bond) superexchange interactions and Co–Co (blue bond) direct exchange interactions. The second NN J2 has multiple superexchange interaction pathways, which may lead to a wide range of variations, mainly determined by J and J3. The third NN AFM interaction J3 arises from the existence of the Te atom in the center of the honeycomb lattice, which leads to the unique superexchange interaction pathway Co–O–Te–O–Co (golden bond). The olive arrow refers to the direction of applied magnetic field B in the magnetization. c The isothermal magnetization M(B) with the applied magnetic field B ⊥ b, B // b, and B // c-axis at 0.5 K, respectively. The dashed line indicates the Van-Vleck paramagnetic background. d The differential isothermal magnetization as functions of fields dM/dB vs. B at different temperatures with B ⊥ b.
Fig. 2 Magnetic susceptibility of Na2Co2TeO6 for B ⊥ b-axis. a, b Temperature dependence of susceptibility χ(T) in NCTO measured at various magnetic fields. The inset of Fig. 2b shows the honeycomb lattices of Co viewed along the c-axis. The cartoon shows the moments to be in the basal plane and parallel to the b-axis40, 41, and the TeO6 octahedra sit at the center of each honeycomb unit. The first NN ferromagnetic (FM) interaction J originated from a collaboration between Co–O–Co (red bond) superexchange interactions and Co–Co (blue bond) direct exchange interactions. The second NN J2 has multiple superexchange interaction pathways, which may lead to a wide range of variations, mainly determined by J and J3. The third NN AFM interaction J3 arises from the existence of the Te atom in the center of the honeycomb lattice, which leads to the unique superexchange interaction pathway Co–O–Te–O–Co (golden bond). The olive arrow refers to the direction of applied magnetic field B in the magnetization. c The isothermal magnetization M(B) with the applied magnetic field B ⊥ b, B // b, and B // c-axis at 0.5 K, respectively. The dashed line indicates the Van-Vleck paramagnetic background. d The differential isothermal magnetization as functions of fields dM/dB vs. B at different temperatures with B ⊥ b.CC BY · PubMed Central
Fig. 3 High-field ESR of Na2Co2TeO6. a–j Frequency-dependence of ESR at 2 K; k ESR frequency-field diagram of NCTO at 2 K. The unit conversion with meV (1 meV ≈241.8 GHz) is shown on the right axis. The inset shows the EPR spectra measured at 50 K with 214 GHz. The red lines are the fitting line by Supplementary S(2). The olive squares and magenta stars are obtained from the EPR data at 50 K.
Fig. 3 High-field ESR of Na2Co2TeO6. a–j Frequency-dependence of ESR at 2 K; k ESR frequency-field diagram of NCTO at 2 K. The unit conversion with meV (1 meV ≈241.8 GHz) is shown on the right axis. The inset shows the EPR spectra measured at 50 K with 214 GHz. The red lines are the fitting line by Supplementary S(2). The olive squares and magenta stars are obtained from the EPR data at 50 K.CC BY · PubMed Central
Fig. 4 Phase diagram of Na2Co2TeO6. Temperature–magnetic field phase diagram for NCTO. The stars symbol the first-ordered phase boundary. The color background is used only as a simple guide.
Fig. 4 Phase diagram of Na2Co2TeO6. Temperature–magnetic field phase diagram for NCTO. The stars symbol the first-ordered phase boundary. The color background is used only as a simple guide.CC BY · PubMed Central
Fig. 5 Powder INS of Na2Co2TeO6. a Powder INS using 11.4 meV incident neutron for NCTO at 3 K on spectrometer HRC. The high-temperature data (95 K) was subtracted as background and the thermal effect was simulated by the Bose factor. b The calculated powder-averaged scattering including the magnetic form factor with K = Γ =0.125 meV, J = −2.325 meV, and J3 = 2.5 meV. The black and white dashed lines label M and K points at the first Brillouin zone with Q = 0.72 and 0.83 Å −1, respectively. c Constant-E cuts over the energy ranges centered at the locations labeled dashed lines in Fig. 5d. The solid blue line is constant-E cuts over the energy ranges centered at 0.66 meV from our LSWT. The absence of structured scattering below 0.4 meV confirms the gap in the magnetic excitation spectrum. d Powder inelastic neutron scattering using 5 Å (~3.27 meV) incident neutrons for NCTO at T = 3 K on spectrometer NEAT II, HZB, Deutschland.
Fig. 5 Powder INS of Na2Co2TeO6. a Powder INS using 11.4 meV incident neutron for NCTO at 3 K on spectrometer HRC. The high-temperature data (95 K) was subtracted as background and the thermal effect was simulated by the Bose factor. b The calculated powder-averaged scattering including the magnetic form factor with K = Γ =0.125 meV, J = −2.325 meV, and J3 = 2.5 meV. The black and white dashed lines label M and K points at the first Brillouin zone with Q = 0.72 and 0.83 Å −1, respectively. c Constant-E cuts over the energy ranges centered at the locations labeled dashed lines in Fig. 5d. The solid blue line is constant-E cuts over the energy ranges centered at 0.66 meV from our LSWT. The absence of structured scattering below 0.4 meV confirms the gap in the magnetic excitation spectrum. d Powder inelastic neutron scattering using 5 Å (~3.27 meV) incident neutrons for NCTO at T = 3 K on spectrometer NEAT II, HZB, Deutschland.CC BY · PubMed Central

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Research works printed but not linked: 1

  1. Candini, A. & Affronte, M. Magnetometry by means of Hall microprobes in the Quantum Design PPMS. Vol. 1084-701 (Application Note, 2008).

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Metadata

Authors
Lin, G., Jeong, J., Kim, C., Wang, Y., Huang, Q., Masuda, T., Asai, S., Itoh, S., Günther, G., Russina, M., Lu, Z., Sheng, J., Wang, L., Wang, J., Wang, G., Ren, Q., Xi, C., Tong, W., Ling, L., Liu, Z., Wu, L., Mei, J., Qu, Z., Zhou, H., Wang, X., Park, J.-G., Wan, Y., & Ma, J.
Affiliations
  • Shanghai Jiao Tong University (CN)
  • Seoul National University (KR)
  • Chinese Academy of Sciences (CN)
  • University of Tennessee at Knoxville (US)
  • High Energy Accelerator Research Organization (JP)
  • The Institute for Solid State Physics, The University of Tokyo (JP)
  • Helmholtz-Zentrum Berlin für Materialien und Energie (DE)
  • Edinburgh Napier University (GB)
  • Southern University of Science and Technology (CN)
  • Renmin University of China (CN)
Corresponding author
  • Wan, Yuan
  • Ma, Jie
ORCID
Venue
Nature Communications
Publisher
Springer Science and Business Media LLC
Published
2021-09-21
Volume
12
Issue
1
Pages
5559-5559
ISSN
2041-1723 (ISSN-L)
DOI
10.1038/s41467-021-25567-7
PMC
PMC8455656
OpenAlex
W3199526042
Cited by
158
References
71
Citations by year
2026: 27 · 2025: 45 · 2024: 32 · 2023: 28 · 2022: 19 · 2021: 7
FWCI
8.99
Type
journal article
Language
en
Open access
Licence
Locations
  • Nature Communications (publishedVersion, cc-by)
  • Europe PMC (PubMed Central) (publishedVersion, other-oa)
  • PubMed Central (publishedVersion, cc-by)
  • PubMed (publishedVersion)
  • White Rose Research Online (University of Leeds, The University of Sheffield, University of York) (acceptedVersion)
  • arXiv (Cornell University) (submittedVersion)
  • White Rose Research Online (University of Leeds, The University of Sheffield, University of York) (submittedVersion)
  • RePEc: Research Papers in Economics (submittedVersion)
  • DOAJ (DOAJ: Directory of Open Access Journals) (submittedVersion, cc-by-sa)
  • HZB Repository (Helmholtz-Zentrum Berlin für Materialien und Energie GmbH (HZB)) (submittedVersion, other-oa)
  • Institutional Repositories DataBase (IRDB) (submittedVersion)
  • Research Output (Edinburgh Napier University) (submittedVersion, cc-by)
  • Edinburgh Napier Research Repository (Edinburgh Napier University) (submittedVersion, cc-by)
  • arXiv (Cornell University) (public-domain)
Funders
  • National Natural Science Foundation of China (12004243)
  • China Postdoctoral Science Foundation (2019M661474)
Topics
  • Physical Sciences › Physics and Astronomy › Condensed Matter Physics › Advanced Condensed Matter Physics
  • Physical Sciences › Physics and Astronomy › Condensed Matter Physics › Physics of Superconductivity and Magnetism
  • Physical Sciences › Materials Science › Electronic, Optical and Magnetic Materials › Magnetism in coordination complexes
Keywords
Na2Co2TeO6, quantum spin liquid, spin-orbit coupling, exchange interaction, inelastic neutron scattering, electron spin resonance, heat capacity, magnetization

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