Magnetic-Order-Mediated Second Harmonic Generation in a Room-Temperature van der Waals Ferromagnet Fe <sub>3</sub> GaTe <sub>2</sub>

Magnetic order coupled second harmonic generation (SHG) provides a unique nonlinear probe of symmetry breaking in low dimensional magnets. However, its capability to resolve nonuniform magnetic domain structures and identify domain boundaries remains largely unexplored. Here, we demonstrate optical SHG imaging of labyrinthine magnetic domains in room temperature Fe<sub>3</sub>GaTe<sub>2</sub>, showing high sensitivity to magnetic configurations consistent with magnetic force microscopy. Magnetic field dependent SHG measurements reveal coherent interference between structural and magnetization coupled contributions, leading to SHG hysteresis and field tunable polarization rotation. These effects originate from interference between structural and magnetization induced second order susceptibilities, resulting in a magnetically tunable nonlinear optical phase. First-principles calculations support a magnetization coupled χ<sup>(2)</sup> contribution associated with Fe-orbital spin asymmetry and interlayer hybridization. Our results establish SHG as a domain-resolved and fully optical probe of magnetic symmetry in ferromagnets at room temperature.

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Publication Details

Journal
Nano Letters
Published
2026-03-09
DOI
https://doi.org/10.1021/acs.nanolett.5c06338
Primary Topic
2D Materials and Applications
Type
article
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article

Magnetic-Order-Mediated Second Harmonic Generation in a Room-Temperature van der Waals Ferromagnet Fe 3 GaTe 2

Jie Chen, Xi Xie, Shufen Zhang, Yixuan Chen et al.
Nano Letters
2D Materials and Applications
article

Magnetic-Order-Mediated Second Harmonic Generation in a Room-Temperature van der Waals Ferromagnet Fe 3 GaTe 2

Jie Chen, Xi Xie, Shufen Zhang, Yixuan Chen, Jun He, Xian Zhang, Yanping Liu, Shikun Hou, Zongwen Liu, Shaofei Li
article en

Abstract

Magnetic order coupled second harmonic generation (SHG) provides a unique nonlinear probe of symmetry breaking in low dimensional magnets. However, its capability to resolve nonuniform magnetic domain structures and identify domain boundaries remains largely unexplored. Here, we demonstrate optical SHG imaging of labyrinthine magnetic domains in room temperature Fe<sub>3</sub>GaTe<sub>2</sub>, showing high sensitivity to magnetic configurations consistent with magnetic force microscopy. Magnetic field dependent SHG measurements reveal coherent interference between structural and magnetization coupled contributions, leading to SHG hysteresis and field tunable polarization rotation. These effects originate from interference between structural and magnetization induced second order susceptibilities, resulting in a magnetically tunable nonlinear optical phase. First-principles calculations support a magnetization coupled χ<sup>(2)</sup> contribution associated with Fe-orbital spin asymmetry and interlayer hybridization. Our results establish SHG as a domain-resolved and fully optical probe of magnetic symmetry in ferromagnets at room temperature.

Nano LettersVol. 26(11)
The University of Sydney (AU), Central South University (CN)
Openalex Percentile: Top 30%
2D Materials and Applications
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