Experimental realization of a single-layer multiferroic

ORAL

Abstract

Multiferroic materials have garnered wide interest for their exceptional static and dynamical magnetoelectric properties. In particular, type-II multiferroics exhibit an inversion-symmetry-breaking magnetic order which directly induces a ferroelectric polarization through various mechanisms, such as the inverse Dzyaloshinskii-Moriya effects. This intrinsic coupling between the magnetic and dipolar order parameters results in record-strength magnetoelectric effects. Two-dimensional materials possessing such intrinsic multiferroic properties have been long sought for harnessing magnetoelectriccoupling in nanoelectronic devices. Here, we report the discovery of type-II multiferroic order in a single atomic layer of the transition metal-based van der Waals material NiI2. We use circular dichroic Raman measurements to directly probe the magneto-chiral ground state and its long-lived electromagnon modes which reflect the presence of dynamic magnetoelectric coupling. From birefringence and second-harmonic generation measurements, we detect a highly anisotropic electronic state simultaneously breaking three-fold rotationaland inversion symmetry, and supporting polar order. The evolution of the optical signatures as a function of temperature and layer number surprisingly reveals an ordered magnetic, polar state that persists down to the ultrathin limit of monolayer NiI2. These observations establish NiI2 and transition metal dihalides as a new platform for studying emergent multiferroic phenomena, chiral magnetic textures and ferroelectricity in the two-dimensional limit.

*This work was supported by the STC Center for Integrated Quantum Materials, NSF Grant No. DMR-1231319, the US Department of Energy, BES DMSE and Gordon and Betty Moore Foundation's EPiQS Initiative grant GBMF9459.

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Publication: arxiv.org/abs/2106.07661

Presenters

  • Qian Song

    • Massachusetts Institute of Technology
    • Massachusetts Institute of Technology MI

Authors

  • Qian Song

    • Massachusetts Institute of Technology
    • Massachusetts Institute of Technology MI

  • Connor A Occhialini

    • Massachusetts Institute of Technology
    • Massachusetts Institute of Technology MIT
    • Massachusetts Institute of Technology MI

  • Emre Ergecen

    • Massachusetts Institute of Technology MIT

  • Batyr Ilyas

    • Massachusetts Institute of Technology MIT

  • Danila Amoroso

    • CNR-SPIN
    • Consiglio Nazionale delle Ricerche CNR-SPIN (Italy) ; Université de Liège, Nanomat/Q-mat/CESAM (Belgium)
    • Consiglio Nazionale delle Ricerche, CNR-SPIN

  • Paolo Barone

    • CNR-SPIN
    • SPIN-CNR, c/o Università G. D'Annunzio, Chieti, Italy
    • Consiglio Nazionale delle Ricerche CNR-SPIN (Italy)
    • Consiglio Nazionale delle Ricerche, CNR-SPIN
    • SPIN-CNR

  • Jesse Kapeghian

    • Arizona State University

  • Kenji Watanabe

    • National Institute for Materials Science, Tsukuba, Japan
    • National Institute for Materials Science
    • NIMS
    • Research Center for Functional Materials, National Institute for Materials Science, Tsukuba, Ibaraki 305-0044, Japan
    • Research Center for Functional Materials, National Institute for Materials Science, 1-1 Namiki, Tsukuba 305-0044, Japan.
    • Research Center for Functional Materials, National Institute for Materials Science
    • Advanced, Materials Laboratory, NIMS
    • 3 National Institute for Materials Science, Tsukuba, Japan
    • National Institute for Materials Science; 1-1 Namiki, Tsukuba, Ibaraki 305-0044, Japan
    • National Institute of Materials Science, Tsukuba, Japan
    • National Institute of Materials Science
    • Advanced Materials Laboratory, National Institute for Materials Science, 1-1 Namiki, Tsukuba, 305-0044, Japan
    • National Institute for Materials Science (Japan)
    • National Institute for Materials Science, Japan
    • Research Center for Functional Materials, National Institute for Materials Science, 1-1 Namiki, Tsukuba 305-0044, Japan
    • Research Center for Functional Materials
    • Research Center for Functional Materials, National Institute for Materials Science, Tsukuba, Japan
    • Research Center for Functional Materials, National Institute for Materials Science, Japan
    • Research Center for Functional Materials, National Institute for Materials Science, 1-1Namiki, Tsukuba 305-0044, Japan
    • National Institute for Material Science, Japan
    • National Institute for Material Science
    • National Institute of Material Sciences, Japan
    • NIMS, Tsukuba
    • 2National Institute for Materials Science, Namiki 1-1, Ibaraki 305-0044, Japan.
    • National Institute of Materials Science, Tsukuba, Ibaraki 305-0044, Japan
    • National Institute for Materials Science Japan
    • NIMS, Japan
    • nims
    • National Institute for Materials Science, Research Center for Functional Materials, Japan
    • National Institute for Materials Science Tsukuba
    • National Institute for Materials Science, 1-1 Namiki
    • National Institute for Materials Science of Japan
    • National Institute for Materials Science, 1-1 Namiki, Tsukuba 305-0044, Japan
    • NIMS - National Institute for Material Science, Japan
    • Research Center for Functional Materials, National Institute for Material Science, Tsukuba, Ibaraki, 305-0044, Japan.
    • National Institute for Material Science, Tsukuba
    • National Institute for Materials Science, Tsukuba, Ibaraki 305-0044, Japan
    • National Institute for Materials Science (NIMS)
    • National Institute for Materials Science, Research Center for Functional Materials
    • Research Center for Functional Materials, National Institute for Materials Science, 1-1 Namiki, Tsukuba, Ibaraki 305-0044, Japan
    • National Institute of Material Science
    • Kyoto Univ
    • National Institute for Materials Science,1-1 Namiki, Tsukuba, 305-0044, Japan

  • Takashi Taniguchi

    • National Institute for Materials Science, Tsukuba, Japan
    • National Institute for Materials Science
    • NIMS
    • Kyoto Univ
    • International Center for Materials Nanoarchitectonics, National Institute for Materials Science, 1-1 Namiki, Ibaraki 305-0044, Japan.
    • 3 National Institute for Materials Science, Tsukuba, Japan
    • National Institute for Materials Science; 1-1 Namiki, Tsukuba, Ibaraki 305-0044, Japan
    • National Institute of Materials Science, Tsukuba, Japan
    • National Institute of Materials Science
    • Advanced Materials Laboratory, National Institute for Materials Science, 1-1 Namiki, Tsukuba, 305-0044, Japan
    • National Institute for Materials Science (Japan)
    • International Center for Materials Nanoarchitectonics, National Institute for Materials Science
    • International Center for Materials Nanoarchitectonics, National Institute for Materials Science, 1-1 Namiki, Tsukuba 305-0044, Japan
    • Kyoto University
    • International Center for Materials Nanoarchitectonics
    • International Center for Materials Nanoarchitectonics, National Institute for Materials Science, Tsukuba, Japan
    • International Center for Materials Nanoarchitectonics, National Institute for Materials Science, Japan
    • International Center for Materials Nanoarchitectonics, National Institute for MaterialsScience, 1-1 Namiki, Tsukuba 305-0044, Japan
    • National Institute for Material Science, Japan
    • National Institute for Material Science
    • National Institute of Material Sciences, Japan
    • NIMS, Tsukuba
    • 2National Institute for Materials Science, Namiki 1-1, Ibaraki 305-0044, Japan.
    • National Institute of Materials Science, Tsukuba, Ibaraki 305-0044, Japan
    • National Institute for Materials Science, Japan
    • International Center for Materials Nanoarchitectonics (WPI-MANA), National Institute for Materials Science, 1-1 Namiki Tsukuba, Ibaraki 305-0044, Japan.
    • NIMS, Japan
    • National Institute for Materials Science (NIMS)
    • NIMS. Japan
    • International Center for Material Nanoarchitectonics, National Institute for Materials Science, Tsukuba, Japan
    • International Center for Material Nanoarchitectonics, National Institute for Materials Science
    • National Institute for Materials Science Tsukuba
    • National Institute for Materials Science, 1-1 Namiki
    • National Institute for Materials Science of Japan
    • National Institute for Materials Science, 1-1 Namiki, Tsukuba 305-0044, Japan
    • NIMS - National Institute for Material Science, Japan
    • International Center for Materials Nanoarchitectonics, National Institute for Material Science, Tsukuba, Ibaraki 305-0044, Japan.
    • National Institute for Material Science, Tsukuba
    • National Institute for Materials Science, International Center for Materials Nanoarchitectonics
    • International Center for Materials Nanoarchitectonics, National Institute for Materials Science, 1-1 Namiki, Tsukuba, Ibaraki 305-0044, Japan
    • National Institute of Material Science
    • National Institute for Materials Science,1-1 Namiki, Tsukuba, 305-0044, Japan

  • Antia S Botana

    • Arizona State University

  • Silvia Picozzi

    • CNR Institute for Microelectronics and Microsystems
    • Consiglio Nazionale delle Ricerche CNR-SPIN (Italy)
    • Consiglio Nazionale delle Ricerche, CNR-SPIN

  • Nuh Gedik

    • Massachusetts Institute of Technology MI

  • Riccardo Comin

    • Massachusetts Institute of Technology MI
    • Massachusetts Institute of Technology
    • Massachusetts Institute of Technology MIT