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| Auteurs principaux: | , , , , |
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| Format: | Preprint |
| Publié: |
2025
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| Sujets: | |
| Accès en ligne: | https://arxiv.org/abs/2503.21238 |
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| _version_ | 1866912302128693248 |
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| author | Guan, Zhizi Peng, Zhiwei Srolovitz, David J. Khurgin, Jacob Lei, Dangyuan |
| author_facet | Guan, Zhizi Peng, Zhiwei Srolovitz, David J. Khurgin, Jacob Lei, Dangyuan |
| contents | Symmetry governs the selection rules of light-matter interactions in crystalline materials, making symmetry manipulation a powerful tool for tuning their optical properties. Here, we demonstrate that the hot-electron injection from a plasmonic resonator breaks the centrosymmtry of an adjacent transition metal dichalcogenide bilayer, probed via second-harmonic generation (SHG) in a Au-nanoparticle@bilayer-MoS$_2$@Au-film hybrid system. Power-dependent SHG measurements exhibit saturation behavior, consistent with a capacitor model where interfacial charge accumulation creates a dynamic barrier limiting further electron injection. Polarization-resolved SHG measurements reveal anisotropic second-order susceptibility response under hot-electron injection, where the contrast between different susceptibility components provides a quantitative measure of symmetry-breaking anisotropy. First-principles calculations elucidate the nonlinear optical responses evolution in bilayer MoS$_2$ and comfirm the anisotropic modification of susceptibility components under hot-electron injection, modeled by a perpendicular electric field. Our work establishes SHG as an effective probe of hot-electron-induced symmetry breaking in 2D materials, demonstrating a promising approach for ultrafast manipulation of material properties through controlled charge injection at the nanoscale. |
| format | Preprint |
| id |
arxiv_https___arxiv_org_abs_2503_21238 |
| institution | arXiv |
| publishDate | 2025 |
| record_format | arxiv |
| spellingShingle | Hot-electron-injection-induced symmetry breaking in bilayer MoS$_2$ probed by second-harmonic generation Guan, Zhizi Peng, Zhiwei Srolovitz, David J. Khurgin, Jacob Lei, Dangyuan Optics Symmetry governs the selection rules of light-matter interactions in crystalline materials, making symmetry manipulation a powerful tool for tuning their optical properties. Here, we demonstrate that the hot-electron injection from a plasmonic resonator breaks the centrosymmtry of an adjacent transition metal dichalcogenide bilayer, probed via second-harmonic generation (SHG) in a Au-nanoparticle@bilayer-MoS$_2$@Au-film hybrid system. Power-dependent SHG measurements exhibit saturation behavior, consistent with a capacitor model where interfacial charge accumulation creates a dynamic barrier limiting further electron injection. Polarization-resolved SHG measurements reveal anisotropic second-order susceptibility response under hot-electron injection, where the contrast between different susceptibility components provides a quantitative measure of symmetry-breaking anisotropy. First-principles calculations elucidate the nonlinear optical responses evolution in bilayer MoS$_2$ and comfirm the anisotropic modification of susceptibility components under hot-electron injection, modeled by a perpendicular electric field. Our work establishes SHG as an effective probe of hot-electron-induced symmetry breaking in 2D materials, demonstrating a promising approach for ultrafast manipulation of material properties through controlled charge injection at the nanoscale. |
| title | Hot-electron-injection-induced symmetry breaking in bilayer MoS$_2$ probed by second-harmonic generation |
| topic | Optics |
| url | https://arxiv.org/abs/2503.21238 |