Quasi-two-dimensional Ruddlesden-Popper perovskites driving carrier self-separation have rapidly advanced the development of high-performance optoelectronic devices. However, insightful understanding of carrier dynamics in the perovskites is still inadequate. The distribution of multiple perovskite phases, crucial for carrier separation, is controversial. Here we report a systematic study on carrier dynamics of spin-coated (CHCHCHNH)(CHNH)PbI (n = 3 and 5) perovskite thin films. Efficient electrons transfer from small-n to large-n perovskite phases, and holes transfer reversely with time scales from ∼0.3 to 30.0 ps. The multiple perovskite phases are arranged perpendicularly to substrate from small to large n and also coexist randomly in the same horizontal planes. Further, the carrier separation dynamics is tailored by engineering the crystalline structure of the perovskite film, which leads to controllable emission properties. These results have important significance for the design of optoelectronic devices from solar cells, light-emitting diodes, lasers, and so forth.

Traps in the photoactive layer or interface can critically influence photovoltaic device characteristics and stabilities. Here, traps passivation and retardation on device degradation for methylammonium lead trihalide (MAPbI ) perovskite solar cells enabled by a biopolymer heparin sodium (HS) interfacial layer is investigated. The incorporated HS boosts the power conversion efficiency from 17.2 to 20.1% with suppressed hysteresis and Shockley-Read-Hall recombination, which originates primarily from the passivation of traps near the interface between the perovskites and the TiO cathode. The incorporation of an HS interfacial layer also leads to a considerable retardation of device degradation, by which 85% of the initial performance is maintained after 70 d storage in ambient environment. Aided by density functional theory calculations, it is found that the passivation of MAPbI and TiO surfaces by HS occurs through the interactions of the functional groups (COO , SO , or Na ) in HS with undersaturated Pb and I ions in MAPbI and Ti in TiO . This work demonstrates a highly viable and facile interface strategy using biomaterials to afford high-performance and stable perovskite solar cells.

Ion transport is an essential process for various applications including energy storage, sensing, display, memory and so on, however direct visualization of oxygen ion motion has been a challenging task, which lies in the fact that the normally used electron microscopy imaging mainly focuses on the mass attribute of ions. The lack of appropriate understandings and analytic approaches on oxygen ion motion has caused significant difficulties in disclosing the mechanism of oxides-based memristors. Here we show evidence of oxygen ion migration and accumulation in HfO2 by in situ measurements of electrostatic force gradient between the probe and the sample, as systematically verified by the charge duration, oxygen gas eruption and controlled studies utilizing different electrolytes, field directions and environments. At higher voltages, oxygen-deficient nano-filaments are formed, as directly identified employing a CS-corrected transmission electron microscope. This study could provide a generalized approach for probing ion motions at the nanoscale.

Graphene field effect transistor sensitized by a layer of semiconductor (sensitizer/GFET) is a device structure that is investigated extensively for ultrasensitive photodetection. Among others, organometallic perovskite semiconductor sensitizer has the advantages of long carrier lifetime and solution processable. A further step to improve the responsivity is to design a structure that can promote electron-hole separation and selective carrier trapping in the sensitizer. Here, the use of a hybrid perovskite-organic bulk heterojunction (BHJ) as the light sensitizer to achieve this goal is demonstrated. Our spectroscopy and device measurements show that the CH 3 NH 3 PbI 3 -PCBM BHJ/GFET device has improved charge separation yield and carrier lifetime as compared to a reference device with a CH 3 NH 3 PbI 3 sensitizer only. The key to these enhancement is the presence of [6,6]-phenyl-C 61 -butyric acid methyl ester (PCBM), which acts as charge separation and electron trapping sites, resulting in a 30-fold increase in the photoresponsivity. This work shows that the use of a small amount of electron or hole acceptors in the sensitizer layer can be an effective strategy for improving and tuning the photoresponsivity of sensitizer/GFET photodetectors.