Interfacial Charge Transfer between Excited CsPbBr3 Nanocrystals and TiO2: Charge Injection versus Photodegradation

Record-breaking efficiency achieved with quantum dot solar cells made of perovskite nanocrystals demands understanding of the excited-state interactions between perovskite nanocrystals and metal oxide electron transport layers. The interfacial electron transfer between excited CsPbBr3 perovskite nanocrystals and metal oxides (TiO2, SnO2, and ZnO) was elucidated using transient absorption spectroscopy and found to occur with a rate constant in the range of 2-4 x 10(1) s(-1). In an inert atmosphere, back electron transfer helps to maintain the stability of the perovskite nanocrystals. However, the presence of oxygen introduces instability as it scavenges away transferred electrons from the electron-transporting metal oxide, leaving behind holes to accumulate at CsPbBr3 nanocrystals, which in turn induce anodic corrosion. X-ray photoelectron spectroscopy measurements have enabled us to identify PbO as the major photodegraded product. The importance of the surrounding atmosphere and the supporting metal oxide in governing the stability of perovskite nanocrystals is discussed.