Photoinduced Interfacial Charge Transfer Tailors Second-Harmonic Generation in NbSe<sub>2</sub>-MoS<sub>2</sub> Heterostructures.

Zhou, Li; Wang, Yiduo; Li, Xin; Kang, Jianlong; Song, Yujian; Chang, Haolin; Zheng, Wanxin; Zhang, Bei et al. · Nano Lett · 2026

basic_science · Level V

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Abstract

Effective modulation of ultrafast nonlinear optical properties in two-dimensional materials is essential for advancing nanophotonic technologies. In this work, we demonstrate precise control over the ultrafast carrier dynamics in NbSe<sub>2</sub> by tailoring the nanosheet thickness and constructing a van der Waals heterostructure with MoS<sub>2</sub>. Transient absorption measurements reveal that carrier lifetimes extend from several to hundreds of picoseconds with increasing layer thickness, due to interlayer coupling. More importantly, interfacial charge transfer from MoS<sub>2</sub> to NbSe<sub>2</sub> in the heterostructure further prolongs carrier relaxation and significantly enhances the second harmonic generation (SHG) response. First-principles calculations attribute this SHG enhancement to a symmetry-breaking electronic imbalance induced by charge redistribution at the interface. These findings establish interfacial charge engineering as a powerful and general strategy for tailoring ultrafast nonlinear optical properties in 2D materials, offering new pathways for designing high-performance optoelectronic devices.