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Interlayer carrier transfer at heterointerfaces plays a critical role in light to electricity conversion using organic and nanostructured materials. However, how interlayer carrier extraction at these interfaces is poorly understood, especially in organic-inorganic heterogeneous systems. Here, we provide a direct strategy for manipulating the interlayer carrier diffusion process, transfer rate and extraction efficiency in tetracene/MoS 2  type-II band alignment heterostructure by constructing the 2D–3D organic-inorganic (O-I) system. As a result, the prolonged diffusion length (12.32 nm), enhanced electron transfer rate (9.53 × 10 9  s −1 ) and improved carrier extraction efficiency (60.9%) are obtained in the 2D O-I structure which may be due to the more sufficient charge transfer (CT) state generation. In addition, we have demonstrated that the interlayer carrier transfer behavior complied with the diffusion mechanism based on the one-dimensional diffusion model. The diffusion coefficients have varied from 0.0027 to 0.0036 cm 2  s −1  as the organic layer changes from 3D to 2D structures. Apart from the relationship between the carrier injection and diffusion process, temperature-dependent time-resolved spectra measurement is used to reveal the trap-related recombination that may limit the interlayer carrier extraction. The controllable interlayer carrier transfer behavior enables O-I heterojunction to be optimized for optoelectronic applications.

Manipulating the interlayer carrier diffusion and extraction process in organic-inorganic heterojunctions: from 2D to 3D structures