Nonlinear Optical Signatures of the Transition from Semiconductor to Semimetal in PtSe2

Abstract The demand for an ultrabroad optical material with a bandgap tunable from zero to at least 1–2 eV has been one of the driving forces for exploring new 2D materials since the emergence of graphene, transition metal dichalcogenides, and black phosphorus. As an ultra‐broadband 2D material with energy bandgap ranging from 0 to 1.2 eV, PtSe 2 shows much better air stability than its analogue, black phosphorous. In this work, the superior nonlinear optical performance and ultrafast dynamics of layered PtSe 2 , and signatures of the transition from semiconductor to semimetal are systematically studied. Combining with rate equations, first‐principles calculation, and electrical measurements, a comprehensive understanding about the evolution of nonlinear absorption and carrier dynamics with increasing layer thickness is provided, indicating its promising potential in nanophotonic devices such as infrared detectors, optical switches, and saturable absorbers.