Broadband nonlinear optical response of monolayer MoSe2under ultrafast excitation

Due to their strong light-matter interaction, monolayer transition metal dichalcogenides (TMDs) have proven to be promising candidates for nonlinear optics and optoelectronics. Here, we characterize the nonlinear absorption of chemical vapour deposition (CVD)-grown monolayer MoSe2 in the 720–810 nm wavelength range. Surprisingly, despite the presence of strong exciton resonances, monolayer MoSe2 exhibits a uniform modulation depth of ∼80 ± 3% and a saturation intensity of ∼2.5 ± 0.4 MW/cm2. In addition, pump-probe spectroscopy is performed to confirm the saturable absorption and reveal the photocarrier relaxation dynamics over hundreds of picoseconds. Our results unravel the unique broadband nonlinear absorptive behavior of monolayer MoSe2 under ultrafast excitation and highlight the potential of using monolayer TMDs as broadband ultrafast optical switches with customizable saturable absorption characteristics.