Layer-dependent photoexcited carrier dynamics of WS2 observed using single pulse pump probe method

Abstract

Understanding the ultrafast carrier dynamics and the mechanism of two-dimensional (2D) transition metal dichalcogenides (TMDs) is key to their applications in the field of optoelectronic devices. In this work, a single pulse pump probe method is introduced to detect the layer-dependent ultrafast carrier dynamics of monolayer and few-layer WS2 excited by a femtosecond pulse. Results show that the ultrafast carrier dynamics of the layered WS2 films can be divided into three stages: the fast photoexcitation phase with the characteristic time of 2–4 ps, the fast decay phase with the characteristic time of 4–20 ps, and the slow decay phase lasting several hundred picoseconds. Moreover, the layer dependency of the characteristic time of each stage has been observed, and the corresponding mechanism of free carrier dynamics has been discussed. It has been observed as well that the monolayer WS2 exhibits a unique rising time of carriers after photoexcitation. The proposed method can be expected to be an effective approach for studying the dynamics of the photoexcited carriers in 2D TMDs. Our results provide a comprehensive understanding of the photoexcited carrier dynamics of layered WS2, which is essential for its application in optoelectronics and photovoltaic devices.