Large and negative Kerr nonlinearity in PdSe2 dichalcogenide 2D films

Abstract: We report a large third order nonlinear optical response of palladium diselenide (PdSe2) films, a two dimensional (2D) noble metal dichalcogenide material. Both open aperture (OA) and closed aperture (CA) Z scan measurements are performed with a femtosecond pulsed laser at 800 nm to investigate the nonlinear absorption and nonlinear refraction, respectively. In the OA experiment, we observe optical limiting behaviour originating from large two photo absorption (TPA) in the PdSe2 film of beta = 3.26 x 10-8 m/W. In the CA experiment, we measure a peak-valley response corresponding to a large and negative Kerr nonlinearity of n2 = -1.33 x 10-15 m2/W, two orders of magnitude larger than bulk silicon. We also characterize the variation of n2 as a function of laser intensity, observing that n2 decreases in magnitude with incident laser intensity, becoming saturated at n2 = -9.96 x 10-16 m2/W at high intensities. These results verify the large third order nonlinear optical response of 2D PdSe2 as well as its strong potential for high performance nonlinear photonic devices.