Highly Efficient Photo-Induced Charge Separation Enabled by Metal-Chalcogenide Interfaces in Quantum-Dot/Metal-Oxide Hybrid Phototransistors

Quantum dot (QD)-based optoelectronics have received great interest for versatile applications because of their excellent photosensitivity, facile solution processability, and the wide range of band gap tunability. In addition, QD-based hybrid devices, which are combined with various high-mobility semiconductors, have been actively researched to enhance the optoelectronic characteristics and maximize the zero-dimensional structural advantages, such as tunable band gap and high light absorption. However, the difficulty of highly efficient charge transfer between QDs and the semiconductors and the lack of systematic analysis for the interfaces have impeded the fidelity of this platform, resulting in complex device architectures and unsatisfactory device performance. Here, we report ultrahigh detective phototransistors with highly efficient photoinduced charge separation using a Sn2S64--capped CdSe QD/amorphous oxide semiconductor (AOS) hybrid structure. The photo-induced electron transfer characteristics at the interface of the two materials were comprehensively investigated with an array of electrochemical and spectroscopic analyses. In particular, photocurrent imaging microscopy revealed that interface engineering in QD/AOS with chelating chalcometallate ligands causes efficient charge transfer, resulting in photovoltaic-dominated responses over the whole channel area. On the other hand, monodentate ligand-incorporated QD/AOS-based devices typically exhibit limited charge transfer with atomic vibration, showing photo-thermoelectric-dominated responses in the drain electrode area.