Regulating transient optical responses in twisted bilayer WS2

Abstract The optical response manipulation of two-dimensional materials is crucial for designing and optimizing high-performance optoelectronic devices. Previously, optical modulation in two-dimensional semiconductors primarily relied on adjusting carrier density through optical excitation or charge injection using the energy band-filling effect. Recently, twist angle has been found to tune the optical and optoelectronic properties of van der Waals structure, but its impact on the transient optical response remains unexplored. Herein, we demonstrate that twist angle can effectively regulate carrier behaviors by tracing the evolution of optical responses in twisted bilayer WS 2 from 0° to 60°. Both Raman and PL spectra consistently show that the optical responses of WS 2 bilayers are highly dependent on the twist angle. Exciton behavior and phonon modes exhibit similarity at twist angles near 0° and 60°, but significantly change as the angle approaches 30°. Moreover, the impact of the twist angle on the transient optical responses was carefully investigated using a femtosecond pump-probe technique. The results reveal a significant decrease in carrier thermalization/relaxation time and exciton formation/recombination time at the WS 2 bilayers with twist angle of ∼31.0°, as compared to twist angles of ∼2.9° and ∼58.9°, which can be attributed to the accumulation of intralayer carriers due to weakened interlayer coupling. These results demonstrate that twist angle can effectively modulate the optical response of twisted 2D materials. Our study elucidates the dynamic carrier behavior in twisted bilayer WS 2 and provides new insights for designing future optoelectronic and photonic devices.