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Dimensionality crossover to a two-dimensional vestigial nematic state from a three-dimensional antiferromagnet in a honeycomb van der Waals magnet

Nature Physics (2024)Cite this article

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Abstract

The effects of fluctuations and disorder, which are substantially enhanced in reduced dimensionalities, can play a crucial role in producing non-trivial phases of matter such as vestigial orders characterized by a composite order parameter. However, fluctuation-driven magnetic phases in low dimensions have remained relatively unexplored. Here we demonstrate a phase transition from the zigzag antiferromagnetic order in the three-dimensional bulk to a Z3 vestigial Potts nematicity in two-dimensional few-layer samples of van der Waals magnet NiPS3. Our spin relaxometry and optical spectroscopy measurements reveal that the spin fluctuations are enhanced over the gigahertz to terahertz range as the layer number of NiPS3 reduces. Monte Carlo simulations corroborate the experimental finding of threefold rotational symmetry breaking but show that the translational symmetry is restored in thin layers of NiPS3. Therefore, our results show that strong quantum fluctuations can stabilize an unconventional magnetic phase after destroying a more conventional one.

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Fig. 1: Schematic phase diagrams of vestigial order and magnetic states in NiPS3.
Fig. 2: Thickness-dependent spin fluctuations in few-layer NiPS3 measured by NV relaxometry and Raman spectroscopy.
Fig. 3: Thickness dependence of BTS and BRS signatures in Raman spectroscopy.
Fig. 4: Polarization-dependent LD and Raman data for 4L NiPS3.
Fig. 5: Monte Carlo calculations of the magnetic state in 2 L NiPS3.

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Source data are provided with this paper. All other data that support this study are available from the corresponding authors upon reasonable request.

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Acknowledgements

We acknowledge valuable discussions with R. Fernandes and J. Venderbos. L.Z. acknowledges support from the National Science Foundation (NSF; Grant No. DMR-2103731), the Office of Naval Research (ONR; Grant No. N00014-21-1-2770) and the Gordon and Betty Moore Foundation (Award No. GBMF10694). R.H. acknowledges support from the NSF (Grant Nos. DMR-2104036 and DMR-2300640). C.R.D. acknowledges support from the US Department of Energy (DOE), Office of Science, Basic Energy Sciences (Award No. DE-SC0024870). Z.Y.M. acknowledges support from the Research Grants Council (RGC) of the Hong Kong Special Administrative Region (SAR) of China (Project Nos. 17301721, AoE/P-701/20, 17309822, HKU C7037-22GF and 17302223), the ANR/RGC Joint Research Scheme sponsored by the RGC of the Hong Kong SAR of China and the French National Research Agency (Project No. A_HKU703/22). D.M. acknowledges support from the Gordon and Betty Moore Foundation's EPiQS Initiative (Grant GBMF9069). K.S. acknowledges support from the ONR (Grant No. N00014-21-1-2770) and the Gordon and Betty Moore Foundation (Award No. GBMF10694). Q.L. and H.D. acknowledge support from the ONR (Grant No. N00014-21-1-2770) and the Gordon and Betty Moore Foundation (Award No. GBMF10694). L.L acknowledges support from the DOE (Grant No. DE-SC0020184). X.X. and L.Y. acknowledge support from the NSF (Grant No. DMR-2118779). The ab initio simulation used Anvil at Purdue University through allocation DMR100005 from the Advanced Cyberinfrastructure Coordination Ecosystem: Services & Support (ACCESS) programme, which is supported by the NSF (Grant Nos. 2138259, 2138286, 2138307, 2137603 and 2138296).

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Author notes

  1. These authors contributed equally: Zeliang Sun, Gaihua Ye, Chengkang Zhou.

Authors and Affiliations

  1. Department of Physics, University of Michigan, Ann Arbor, MI, USA

    Zeliang Sun, Qiuyang Li, Guoxin Zheng, Lu Li, Hui Deng, Kai Sun & Liuyan Zhao

  2. Department of Electrical and Computer Engineering, Texas Tech University, Lubbock, TX, USA

    Gaihua Ye, Zhipeng Ye, Cynthia Nnokwe & Rui He

  3. Department of Physics and HKU-UCAS Joint Institute of Theoretical and Computational Physics, The University of Hong Kong, Hong Kong SAR, China

    Chengkang Zhou & Zi Yang Meng

  4. School of Physics, Georgia Institute of Technology, Atlanta, GA, USA

    Mengqi Huang & Chunhui Rita Du

  5. Department of Materials Science and Engineering, The University of Tennessee, Knoxville, TN, USA

    Nan Huang & David Mandrus

  6. Department of Physics, Washington University in St Louis, St Louis, MO, USA

    Xilong Xu & Li Yang

  7. Materials Science and Technology Division, Oak Ridge National Laboratory, Oak Ridge, TN, USA

    David Mandrus

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  1. Zeliang Sun
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Contributions

Z.S., R.H. and L.Z. conceived the idea and initiated this project. Z.S. exfoliated the NiPS3 thin flakes with different layer numbers. G.Y., Z.Y., C.N. and Z.S. carried out the Raman experiments under the supervision of L.Z. and R.H. M.H. performed the NV spin relaxometry under the supervision of C.D. C.Z. carried out the Monte Carlo simulations under the supervision of K.S. and Z.Y.M. Q.L. and Z.S. carried out the atomic force microscopy measurements and the PL measurements guided by H.D. and L.Z. N.H. grew the high-quality NiPS3 bulk single crystals under the supervision of D.M. G.Z. performed the susceptibility measurements under the supervision of L.L. X.X. performed the phonon calculations under the supervision of L.Y. Z.S., R.H. and L.Z. analysed the data and wrote the manuscript. All authors participated in discussions about the results.

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Correspondence to Rui He or Liuyan Zhao.

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Sun, Z., Ye, G., Zhou, C. et al. Dimensionality crossover to a two-dimensional vestigial nematic state from a three-dimensional antiferromagnet in a honeycomb van der Waals magnet. Nat. Phys. (2024). https://doi.org/10.1038/s41567-024-02618-6

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