Evidence for a single-layer van der Waals multiferroic

Song, Qian; Occhialini, Connor A.; Ergeçen, Emre; Ilyas, Batyr; Amoroso, Danila; Barone, Paolo; Kapeghian, Jesse; Watanabe, Kenji; Taniguchi, Takashi; Botana, Antia S.; Picozzi, Silvia; Gedik, Nuh; Comin, Riccardo

doi:10.1038/s41586-021-04337-x

Title: Evidence for a single-layer van der Waals multiferroic

Journal Article · 22 February 2022 · Nature (London)

DOI: https://doi.org/10.1038/s41586-021-04337-x · OSTI ID:1846987

Song, Qian ^[1];

^[2]; Ergeçen, Emre ^[2];

^[2]; Amoroso, Danila ^[3];

^[4]; Kapeghian, Jesse ^[5];

^[6];

^[5]; Picozzi, Silvia ^[7];

^[2];

^[2]

Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States); Massachusetts Institute of Technology
Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States)
Consiglio Nazionale delle Ricerche CNR-SPIN, Chieti (Italy); Univ. de Liège (Belgium)
Consiglio Nazionale delle Ricerche CNR-SPIN, Rome (Italy)
Arizona State Univ., Tempe, AZ (United States)
National Inst. for Materials Science, Tsukuba (Japan)
Consiglio Nazionale delle Ricerche CNR-SPIN, Chieti (Italy)

Here we searched for signatures of type-II multiferroic order in ultrathin van der Waals materials, to determine if such a state, comprising coexisting electrical polarization and spin order with strong magnetoelectric effects, could persist down to a single-atomic layer. We reported the first observation of such a state in triangular lattice material NiI₂. This system has a layered structure and built-in magnetic frustration that promotes a complex magnetic ground state with proper-screw spin helices. The spin helix pattern breaks inversion symmetry and induces electrical polarization via magnetoelectric coupling. We use circular dichroic Raman measurements to directly probe the magneto-chiral ground state and its electromagnon modes originating from dynamic magnetoelectric coupling. Using birefringence and second-harmonic generation measurements, we detect a highly anisotropic electronic state simultaneously breaking three-fold rotational and inversion symmetry. The evolution of the optical signatures as a function of temperature and layer number surprisingly revealed a multiferroic 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 2D limit.

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Research Organization:: Massachusetts Inst. of Technology (MIT), Cambridge, MA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: SC0019126

OSTI ID:: 1846987

Journal Information:: Nature (London), Journal Name: Nature (London) Journal Issue: 7898 Vol. 602; ISSN 0028-0836

Publisher:: Nature Publishing GroupCopyright Statement

Country of Publication:: United States

Language:: English

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