Evidence for a single-layer van der Waals multiferroic

Multiferroic materials have attracted wide interest because of their exceptional static1-3 and dynamical4-6 magnetoelectric properties. In particular, type-II multiferroics exhibit an inversion-symmetry-breaking magnetic order that directly induces ferroelectric polarization through various mechanis...

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Main Authors: 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
Other Authors: Massachusetts Institute of Technology. Department of Physics
Format: Article
Language:English
Published: Springer Science and Business Media LLC 2022
Online Access:https://hdl.handle.net/1721.1/142508
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author 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
author2 Massachusetts Institute of Technology. Department of Physics
author_facet Massachusetts Institute of Technology. Department of Physics
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
author_sort Song, Qian
collection MIT
description Multiferroic materials have attracted wide interest because of their exceptional static1-3 and dynamical4-6 magnetoelectric properties. In particular, type-II multiferroics exhibit an inversion-symmetry-breaking magnetic order that directly induces ferroelectric polarization through various mechanisms, such as the spin-current or the inverse Dzyaloshinskii-Moriya effect3,7. This intrinsic coupling between the magnetic and dipolar order parameters results in high-strength magnetoelectric effects3,8. Two-dimensional materials possessing such intrinsic multiferroic properties have been long sought for to enable the harnessing of magnetoelectric coupling in nanoelectronic devices1,9,10. 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. The multiferroic state of NiI2 is characterized by a proper-screw spin helix with given handedness, which couples to the charge degrees of freedom to produce a chirality-controlled electrical polarization. We use circular dichroic Raman measurements to directly probe the magneto-chiral ground state and its electromagnon modes originating from dynamic magnetoelectric coupling. Combining birefringence and second-harmonic-generation measurements with theoretical modelling and simulations, we detect a highly anisotropic electronic state that simultaneously breaks three-fold rotational and inversion symmetry, and supports 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.
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spelling mit-1721.1/1425082023-06-21T18:49:28Z 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 Massachusetts Institute of Technology. Department of Physics Massachusetts Institute of Technology. Department of Materials Science and Engineering Multiferroic materials have attracted wide interest because of their exceptional static1-3 and dynamical4-6 magnetoelectric properties. In particular, type-II multiferroics exhibit an inversion-symmetry-breaking magnetic order that directly induces ferroelectric polarization through various mechanisms, such as the spin-current or the inverse Dzyaloshinskii-Moriya effect3,7. This intrinsic coupling between the magnetic and dipolar order parameters results in high-strength magnetoelectric effects3,8. Two-dimensional materials possessing such intrinsic multiferroic properties have been long sought for to enable the harnessing of magnetoelectric coupling in nanoelectronic devices1,9,10. 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. The multiferroic state of NiI2 is characterized by a proper-screw spin helix with given handedness, which couples to the charge degrees of freedom to produce a chirality-controlled electrical polarization. We use circular dichroic Raman measurements to directly probe the magneto-chiral ground state and its electromagnon modes originating from dynamic magnetoelectric coupling. Combining birefringence and second-harmonic-generation measurements with theoretical modelling and simulations, we detect a highly anisotropic electronic state that simultaneously breaks three-fold rotational and inversion symmetry, and supports 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. 2022-05-12T19:05:23Z 2022-05-12T19:05:23Z 2022-02-24 2022-05-12T18:58:37Z Article http://purl.org/eprint/type/JournalArticle https://hdl.handle.net/1721.1/142508 Song, Qian, Occhialini, Connor A, Ergeçen, Emre, Ilyas, Batyr, Amoroso, Danila et al. 2022. "Evidence for a single-layer van der Waals multiferroic." Nature, 602 (7898). en 10.1038/s41586-021-04337-x Nature Attribution-NonCommercial-ShareAlike 4.0 International https://creativecommons.org/licenses/by-nc-sa/4.0/ application/pdf Springer Science and Business Media LLC Prof. Comin via Barbara Williams
spellingShingle 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
Evidence for a single-layer van der Waals multiferroic
title Evidence for a single-layer van der Waals multiferroic
title_full Evidence for a single-layer van der Waals multiferroic
title_fullStr Evidence for a single-layer van der Waals multiferroic
title_full_unstemmed Evidence for a single-layer van der Waals multiferroic
title_short Evidence for a single-layer van der Waals multiferroic
title_sort evidence for a single layer van der waals multiferroic
url https://hdl.handle.net/1721.1/142508
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