Probing the interlayer correlations of spin helical propagations in van der Waals multiferroic NiI<sub>2</sub>

Photon Scattering Group at Massachusetts Institute of Technology, REIXS beamline team at Canadian Light Source, CSX beamline team at NSLS-II, Brookhaven National Laboratory, MODEM Group at CNR-SPIN

Type-II multiferroics attract broad interest with potential electrical control of spontaneous ferroelectricity enabled by a non-collinear magnetic order. Such phenomena were recently expanded to two-dimensional systems, opening up opportunities for multiferroic nano-electronics. Here we investigate the helical magnetic order in triangular-lattice van der Waals multiferroic NiI₂ by Ni L₃-edge resonant X-ray scattering. We report an intense anomalous diffraction that exhibits an order-parameter-like ordering melting and circular-dichroism reversal upon translation reflection, both of which support a long-range spin helical structure as predicted. Combining lateral truncation with thin-film growth, we observe another spin ordering of same vector length yet planarly rotated by 30° down to ~15 nm thickness. We connect this observation to a spin-shear mechanism. This illustrates a competition between distinctive spin ordering orientations that can be energetically-favored by anisotropic spin-exchange and lattice interactions, which suffice to subtle changes from the structural confinement in thin-films. These findings highlight a pivotal realization to directly control finite-momentum spin spirals in nano-scale multiferroics, providing paramount insight to general magnetism studies.

*This work was supported by the U.S. Department of Energy, Office of Science, National Quantum Information Science Research Center's Co-design Center for Quantum Advantage (C2QA) under contract number DE-SC0012704. This work was supported by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, under Award Number DE-SC0019126. This work was supported by the Air Force Office of Scientific Research Young Investigator Program under Grant No.FA9550-19-1-0063. This work was supported the National Science Foundation under Grant No. 1751739. This work was supported by the U.S. Department of Energy (DOE) Office of Science, Early Career Research Program.

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Bulletin of the American Physical Society

2024 APS March Meeting

Monday–Friday, March 4–8, 2024; Minneapolis & Virtual

Session S64: Characterizations of 2D Materials by Photoemission and Scanning Probe

Abstract: S64.00014 : Probing the interlayer correlations of spin helical propagations in van der Waals multiferroic NiI2*

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Abstract: S64.00014 : Probing the interlayer correlations of spin helical propagations in van der Waals multiferroic NiI₂*