Stacking-Polarity-Controlled Interlayer Photocarrier Dynamics in MoSe2/MoS2 Heterostructures

Abstract Control of interlayer photocarrier dynamics is central to optoelectronic applications of van der Waals heterostructures, yet deterministic and spatially uniform tuning strategies remain limited. Here we show that stacking polarity provides a global control parameter for photocarrier dynamics in MoSe2/MoS2 heterostructures. By comparing hexagonal (2H) and rhombohedral (3R) MoS2 bilayers and engineering opposite interface terminations in 3R stacking, we resolve stacking-dependent interlayer charge-transfer dynamics using ultrafast pump–probe spectroscopy. While charge transfer in the 2H heterostructure occurs faster than the experimental resolution, the 3R heterostructures show time-resolvable charge transfer that slows from 0.25 to 0.37 ps depending on stacking polarity. Furthermore, the interlayer exciton lifetime is tuned from ∼40 to ∼160 ps. These effects arise from stacking-induced layer polarization in 3R MoS2, which modulates the interfacial wave function overlap.