In this work, a unique pentagonal TMD material, palladium disulfide (PdS2) nanosheets were fabricated by the liquid-phase exfoliation (LPE) process, and the physical characteristics were also investigated. The nonlinear transmittance is measured by the power scanning method and the modulation depth is fitted to be 15.3%. Based on the transmittance curve, the saturable absorption parameters of PdS2 are calculated, including 5.85 × 10−19 cm2 ground-state absorption cross-section, 1.63 × 10−19 cm2 excited-state absorption cross-section, and 683.5 μs excited-state lifetime. By employing both PdS2 as a saturable absorber (SA) and an acousto-optic modulator (AOM), a doubly Q-switched and mode-locked (QML) laser-pumped intracavity KTiOPO4 (KTP) optical parametric oscillator (OPO) was realized. The pulse energy and the pulse width of the Q-switched envelope for signal wave have been measured. At higher pump power, the high-peak-power low-repetition-rate sub-nanosecond mode-locking pulse of signal wave is generated, in which there is only one mode-locked pulse underneath a Q-switched envelope. The measured shortest signal pulse duration is 530 ps, corresponding to a peak power of 337 kW, at an incident pump power of 9.81 W and an acousto-optic modulator (AOM) repetition rate of 1 kHz. In addition, by considering the Gauss distribution of intracavity photon density, a set of coupled rate equations for a doubly QML laser-pumped intracavity OPO was given and the numerical simulations agreed with the experimental results. These results indicate that PdS2 is a promising nonlinear optical material for optical applications in the near-infrared (NIR) region.
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