Giant electric field-induced second harmonic generation in polar skyrmions.

Wang, Sixu; Li, Wei; Deng, Chenguang; Hong, Zijian; Gao, Han-Bin; Li, Xiaolong; Gu, Yueliang; Zheng, Qiang et al. · Nat Commun · 2024

basic_science · Level V

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Abstract

Electric field-induced second harmonic generation allows electrically controlling nonlinear light-matter interactions crucial for emerging integrated photonics applications. Despite its wide presence in materials, the figures-of-merit of electric field-induced second harmonic generation are yet to be elevated to enable novel device functionalities. Here, we show that the polar skyrmions, a topological phase spontaneously formed in PbTiO<sub>3</sub>/SrTiO<sub>3</sub> ferroelectric superlattices, exhibit a high comprehensive electric field-induced second harmonic generation performance. The second-order nonlinear susceptibility and modulation depth, measured under non-resonant 800 nm excitation, reach ~54.2 pm V<sup>-1</sup> and ~664% V<sup>-1</sup>, respectively, and high response bandwidth (higher than 10 MHz), wide operating temperature range (up to ~400 K) and good fatigue resistance (>10<sup>10</sup> cycles) are also demonstrated. Through combined in-situ experiments and phase-field simulations, we establish the microscopic links between the exotic polarization configuration and field-induced transition paths of the skyrmions and their electric field-induced second harmonic generation response. Our study not only presents a highly competitive thin-film material ready for constructing on-chip devices, but opens up new avenues of utilizing topological polar structures in the fields of photonics and optoelectronics.