Two-dimensional (2D) nonlinear optical mediums with high and tunable light modulation capability can significantly stimulate the development of ultrathin, compact, and integrated optoelectronics devices and photonic elements. 2D carbides and nitrides of transition metals (MXenes) are a new class of 2D materials with excellent intrinsic and strong light-matter interaction characteristics. However, the current understanding of their photo-physical properties and strategies for improving optical performance is insufficient. To address this issue, we rationally designed and in situ synthesized a 2D Nb₂C/MoS₂ heterostructure that outperforms pristine Nb₂C in both linear and nonlinear optical performance. Excellent agreement between experimental and theoretical results demonstrated that the Nb₂C/MoS₂ inherited the preponderance of Nb₂C and MoS₂ in absorption at different wavelengths, resulting in the broadband enhanced optical absorption characteristics. In addition to linear optical modulation, we also achieved stronger near infrared nonlinear optical modulation, with a nonlinear absorption coefficient of Nb₂C/MoS₂ being more than two times that of the pristine Nb₂C. These results were supported by the band alinement model which was determined by the X-ray photoelectron spectroscopy (XPS) experiment and first-principal theory calculation. The presented facile synthesis approach and robust light modulation strategy pave the way for broadband optoelectronic devices and optical modulators.

The reorientation of 2D materials caused by nonlocal electron coherence is the formation mechanism of 2D material spatial self-phase modulation under laser irradiation, which is widely known as the “wind-chime” model. Here, we present a method that provides strong evidence for the reorientation of 2D-material-induced spatial self-phase modulation. The traditional “wind-chime” model was modified by taking into account the attenuation, i.e., damping of the incident light beam in the direction of the optical path. Accordingly, we can extract the nonlinear refractive index of a single MoS2 nanosheet, instead of simply obtaining the index from an equivalent MoS2 film that was constructed by all nanosheets. Our approach introduces a universal and accurate method to extract intrinsic nonlinear optical parameters from 2D material systems.