Gate- and Optically Controlled Nonlinear Optical Response in Graphene via Non-Perturbative Ultrafast Carrier Dynamics
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| Main Authors: | , , , |
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| Format: | Preprint |
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2026
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| _version_ | 1866918465952022528 |
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| author | Lv, Xiaolong Zhang, Yu Wei, Yuxuan Tian, Chuanshan |
| author_facet | Lv, Xiaolong Zhang, Yu Wei, Yuxuan Tian, Chuanshan |
| contents | While the Dirac band structure of graphene has established it as a leading platform for ultrafast optoelectronics, its non-perturbative nonlinear response under intense excitation remains poorly understood. Here, we report ultrafast spectral modulation of nonlinear optical signals in graphene. By utilizing a robust suspended-graphene platform that allows for both wide-range electrostatic gating and high optical damage thresholds, we observe dramatic frequency shifts (up to 8 THz) in third-harmonic generation (THG) and sum-frequency generation (SFG) driven by pump-induced nonequilibrium carrier dynamics. The magnitude and even the direction of this spectral shift can be reversibly controlled by the Fermi level and excitation conditions. A quasiequilibrium theoretical framework based on hot-carrier dynamics quantitatively reproduces the measured spectral evolution, elucidating the critical interplay between carrier heating and the Fermi level. These findings establish a universal mechanism for carrier-mediated spectral control, providing a practical route toward high-speed, gatetunable nonlinear photonic architectures. |
| format | Preprint |
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arxiv_https___arxiv_org_abs_2604_22321 |
| institution | arXiv |
| publishDate | 2026 |
| record_format | arxiv |
| spellingShingle | Gate- and Optically Controlled Nonlinear Optical Response in Graphene via Non-Perturbative Ultrafast Carrier Dynamics Lv, Xiaolong Zhang, Yu Wei, Yuxuan Tian, Chuanshan Optics While the Dirac band structure of graphene has established it as a leading platform for ultrafast optoelectronics, its non-perturbative nonlinear response under intense excitation remains poorly understood. Here, we report ultrafast spectral modulation of nonlinear optical signals in graphene. By utilizing a robust suspended-graphene platform that allows for both wide-range electrostatic gating and high optical damage thresholds, we observe dramatic frequency shifts (up to 8 THz) in third-harmonic generation (THG) and sum-frequency generation (SFG) driven by pump-induced nonequilibrium carrier dynamics. The magnitude and even the direction of this spectral shift can be reversibly controlled by the Fermi level and excitation conditions. A quasiequilibrium theoretical framework based on hot-carrier dynamics quantitatively reproduces the measured spectral evolution, elucidating the critical interplay between carrier heating and the Fermi level. These findings establish a universal mechanism for carrier-mediated spectral control, providing a practical route toward high-speed, gatetunable nonlinear photonic architectures. |
| title | Gate- and Optically Controlled Nonlinear Optical Response in Graphene via Non-Perturbative Ultrafast Carrier Dynamics |
| topic | Optics |
| url | https://arxiv.org/abs/2604.22321 |