Tunable Ultrafast Nonlinear Optical Properties of Graphene/MoS₂ van der Waals Heterostructures and Their Application in Solid-State Bulk Lasers

TLDR

In van der Waals heterostructures, interlayer coupling strongly modulates optical and electrical properties through charge transfer and band recombination, and theoretical studies indicate that graphene/MoS₂ heterostructures combine complementary properties to serve as key building blocks for optoelectronic devices. The study employed density‑functional theory to compute work functions and relaxation dynamics of G/MoS₂ with varying MoS₂ thickness, and experimentally probed tunable carrier dynamics and saturable absorption via pump‑probe spectroscopy and open‑aperture Z‑scan, comparing Q‑switched laser performance across different MoS₂ layer counts. The results show that interlayer coupling in G/MoS₂ can be tuned by MoS₂ thickness, enabling ultrafast recovery and strong saturable absorption that produced a 1.0 µm femtosecond solid‑state laser, and suggest that controllable stacking of vdW heterostructures can yield promising ultrafast photonic devices.

Abstract

For van der Waals (vdW) heterostructures, optical and electrical properties ( e.g., saturable absorption and carrier dynamics) are strongly modulated by interlayer coupling, which may be due to effective charge transfer and band structure recombination. General theoretical studies have shown that the complementary properties of graphene and MoS2 enable the graphene/MoS2 (G/MoS2) heterostructure to be used as an important building block for various optoelectronic devices. Here, density functional theory was used to calculate the work function values of G/MoS2 with different thicknesses of MoS2, and its relaxation dynamic mechanism was illustrated. The results reveal that the G/MoS2 heterostructure interlayer coupling can be tuned by changing the thickness of MoS2, furthering the understanding of the fundamental charge-transfer mechanism in few-layer G/MoS2 heterostructures. The tunable carrier dynamics and saturable absorption were investigated by pump-probe spectroscopy and open-aperture Z-scan technique, respectively. In the experiments, we compared the performances of Q-switched lasers based on G/MoS2 heterostructures with different MoS2 layers. Taking advantage of ultrafast recovery time and good saturable absorption properties, a femtosecond solid-state laser at 1.0 μm with G/MoS2 heterostructure saturable absorber was successfully achieved. This study on interlayer coupling in G/MoS2 may allow various vdW heterostructures with controllable stacking to be fabricated and shows the promising applications of vdW heterostructures for ultrafast photonic devices.