Tailoring the ultrafast and nonlinear photonics of MXenes through elemental replacement.

Due to the outstanding electronic properties, unique chemical surface termination units and rich elemental compositions, MXenes have become promising candidates for the development of new generation optoelectronic devices. However, there is still a gap between advanced photonics applications and fundamental understanding of ultrafast carrier photo-physics dynamics and a nonlinear optical response in layered MXenes. Here, we present insight into the excited state relaxation processes and nonlinear optical response of few-layer Ti3CN and Ti3C2 nanosheets (NSs) via transient absorption spectroscopy and Z-scan measurements. Owing to similar structural compositions, the transient absorption and nonlinear absorption characteristics behave totally opposite. In addition, photo-induced bandgap renormalization and Pauli blocking phenomena exist in Ti3C2 and Ti3CN NSs, respectively. The element replacement may be a new strategy for tunable carrier kinetics and nonlinear optical response of MXenes. These research studies may provide insight into ultrafast carrier photo-physics dynamics as well as promote MXene-based advanced photonics and their applications in optoelectronic devices.