Ultrafast carrier dynamics and third-order nonlinear optical properties of AgInS2/ZnS nanocrystals

Broad photoluminescence (PL) emission, a large Stokes shift and extremely long-lived radiative lifetimes are the characteristics of ternary I-II-VI semiconductor nanocrystals (NCs), such as CuInS2 and AgInS2 . However, the lack of understanding regarding the intriguing PL mechanisms and photo-carrier dynamics limits their further applications. Here, AgInS2 and AgInS2/ZnS NCs were chemically synthesized and their carrier dynamics were studied by time-resolved PL spectroscopy. The results demonstrated that the surface defect state, which contributed dominantly to the non-radiative decay processes, was effectively passivated through ZnS alloying. Femtosecond transient absorption spectroscopy was also used to investigate the carrier dynamics, revealing the electron storage at the surface state and donor state. Furthermore, the two photon absorption properties of AgInS2 and AgInS2/ZnS NCs were measured using an open-aperture Z-scan technique. The improved third-order nonlinear susceptibility chi((3)) of AgInS2 through ZnS alloying demonstrates potential application in two photon PL biological imaging.