Ultrafast Nonlinear Optical Excitation Behaviors of Mono- and Few-Layer Two Dimensional MoS 2

The layered MoS 2 has recently attracted significant attention for its excellent nonlinear optical properties. Here, the ultrafast nonlinear optical (NLO) absorption and excited carrier dynamics of layered MoS 2 (monolayer, 3–4 layers, and 6–8 layers) are investigated via Z-scan and transient absorption spectra. Our experimental results reveal that NLO absorption coefficients of these MoS 2 increase from–27 × 10 3 cm/GW to–11 × 10 3 cm/GW with more layers at 400-nm laser excitation, while the values decrease from 2.0 × 10 3 cm/GW to 0.8 × 10 3 cm/GW at 800 nm. In addition, at high pump fluence, when the NLO response occurs, the results show that not only the reformation of the excitonic bands, but also the recovery time of NLO response decreases from 150 ps to 100 ps with an increasing number of layers, while the reductive energy of A excitonic band decreases from 191.7 meV to 51.1 meV. The intriguing NLO response of MoS 2 provides excellent potentials for the next-generation optoelectronic and photonic devices.