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Multipole polaron in the devil’s staircase of CeSb

Nature Materials volume 21, pages 410–415 (2022)Cite this article

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Abstract

Rare-earth intermetallic compounds exhibit rich phenomena induced by the interplay between localized f orbitals and conduction electrons. However, since the energy scale of the crystal-electric-field splitting is only a few millielectronvolts, the nature of the mobile electrons accompanied by collective crystal-electric-field excitations has not been unveiled. Here, we examine the low-energy electronic structures of CeSb through the anomalous magnetostructural transitions below the Néel temperature, ~17 K, termed the ‘devil’s staircase’, using laser angle-resolved photoemission, Raman and neutron scattering spectroscopies. We report another type of electron–boson coupling between mobile electrons and quadrupole crystal-electric-field excitations of the 4f orbitals, which renormalizes the Sb 5p band prominently, yielding a kink at a very low energy (~7 meV). This coupling strength is strong and exhibits anomalous step-like enhancement during the devil’s staircase transition, unveiling a new type of quasiparticle, named the ‘multipole polaron’, comprising a mobile electron dressed with a cloud of the quadrupole crystal-electric-field polarization.

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Fig. 1: Magnetostructures established in the devil’s staircase of CeSb.
Fig. 2: Electron–boson coupling of the Sb 5p hole band.
Fig. 3: Raman spectra for CEF excitations and multipole polaron.
Fig. 4: Multipole polaron throughout the devil’s staircase.

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The data that support the findings of this study are available from the corresponding author upon request.

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Acknowledgements

We acknowledge H. Kusunose, M. Kawamura and S. Tsutsui for fruitful discussions, and M. Kohgi, J.-M. Mignot and M. Braden for support of the INS experiments. This work was supported by Japan’s Ministry of Education, Culture, Sports, Science and Technology’s Quantum Leap Flagship Program (MEXT Q-LEAP, grant number JPMXS0118068681), the Ministry of Education, Culture, Sports, Science and Technology’s ‘Program for Promoting Researches on the Supercomputer Fugaku’ (Basic Science for Emergence and Functionality in Quantum Matter Innovative Strongly Correlated Electron Science by Integration of ‘Fugaku’ and Frontier Experiments, project number hp200132), JST ERATO-FS grant number JPMJER2105, the Murata Science Foundation, Grants-in-Aid for Scientific Research (grant numbers JP21H04439, JP20H01848, JP19H00651, JP19H02683, JP19F19030, JP18H01165, JP18H01182A and JP16H06345) and Grants-in-Aids for Scientific Research on Innovative Areas, ‘Quantum Liquid Crystals’ (grant number 19H05825) from the Ministry of Education, Culture, Sports, Science, and Technology of Japan.

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  1. Kenta Kuroda

    Present address: Graduate School of Advanced Science and Engineering, Hiroshima University, Higashihiroshima, Japan

Authors and Affiliations

  1. Institute for Solid State Physics, The University of Tokyo, Kashiwa, Japan

    Y. Arai, Kenta Kuroda, S. Sakuragi, C. Bareille, S. Akebi, K. Kurokawa, Y. Kinoshita, W.-L. Zhang, S. Shin, M. Tokunaga, H. S. Suzuki & Takeshi Kondo

  2. Department of Applied Physics, The University of Tokyo, Tokyo, Japan

    T. Nomoto & R. Arita

  3. Department of Physics, Osaka University, Toyonaka, Japan

    Z. H. Tin, S. Miyasaka & S. Tajima

  4. Department of Engineering and Applied Sciences, Sophia University, Tokyo, Japan

    W.-L. Zhang

  5. Office of University Professor, The University of Tokyo, Kashiwa, Japan

    S. Shin

  6. Trans-scale Quantum Science Institute, The University of Tokyo, Tokyo, Japan

    M. Tokunaga & Takeshi Kondo

  7. National Institute for Materials Science, Tsukuba, Japan

    H. Kitazawa

  8. Advanced Science Research Center, Japan Atomic Energy Agency, Tokai, Japan

    Y. Haga

  9. Frontier Research Center for Applied Atomic Sciences and Institute of Quantum Beam Science, Ibaraki University, Tokai, Japan

    K. Iwasa

  10. RIKEN Center for Emergent Matter Science (CEMS), Wako, Japan

    R. Arita

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Contributions

Y.A. and K. Kuroda performed the laser ARPES experiments and analysed the data. S. Sakuragi, C.B., S.A., K. Kurokawa, S. Shin and T.K. supported the laser ARPES experiments. Y.A., K. Kuroda, S. Sakuragi, W.-L.Z., Z.H.T., S.M. and S.T. conducted the Raman spectroscopy and analysed the data. H.S.S., H.K. and Y.H. made the high-quality CeSb single crystals. Y.A., K. Kuroda., S. Sakuragi, Y.K. and M.T. performed the polarizing microscopy. K.I. performed the neutron scattering spectroscopy. T.N. and R.A. provided theoretical insights. Y.A., K. Kuroda and T.K. wrote the paper. All authors discussed the results and commented on the manuscript.

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Correspondence to Kenta Kuroda.

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Arai, Y., Kuroda, K., Nomoto, T. et al. Multipole polaron in the devil’s staircase of CeSb. Nat. Mater. 21, 410–415 (2022). https://doi.org/10.1038/s41563-021-01188-9

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