Unprecedentedly Large Photocurrents in Colloidal PbS Quantum-Dot Solar Cells Enabled by Atomic Layer Deposition of Zinc Oxide Electron Buffer Layer

Due to the excitonic nature, colloidal PbS quantum-dot solar cells have suffered from lower photocurrent densities than expected from the absorber band gap. The heterojunction between solution-processed ZnO and PbS quantum-dots has been predominantly explored for photovoltaic applications. However, the deeper conduction band minimum of typical PbS quantum-dots than that of solution-processed ZnO imposes a high electron barrier, limiting the short-circuit current densities of the resulting solar cells mostly below 30 mA/cm2. Here, we report that atomic layer deposition (ALD) of ZnO buffer at a low temperature can favor the interfacial band alignment and boost the photocurrent density over 35 mA/cm2 at PbS quantum-dot band gap of 1.18 eV. From our band structure analysis, the electron barrier with ALD-ZnO can be 0.55 eV lower compared to that with sol-gel ZnO. Furthermore, photoactivation of shallow gap states formed by hydroxyl species in ALD-ZnO induces band bending and efficient electron tunneling from PbS to ZnO. Due to the improved band alignment, the device with ALD-ZnO exhibits a significantly enhanced lifetime compared to that with sol-gel ZnO upon constant illumination at 1-sun.