Junction Quality of SnO2-Based Perovskite Solar Cells Investigated by Nanometer-Scale Electrical Potential Profiling.

Electron-selective layers (ESLs) and hole-selective layers (HSLs) are critical in high-efficiency organic-inorganic lead halide perovskite (PS) solar cells for charge-carrier transport, separation, and collection. We developed a procedure to assess the quality of the ESL/PS junction by measuring potential distribution on the cross section of SnO2-based PS solar cells using Kelvin probe force microscopy. Using the potential profiling, we compared three types of cells made of different ESLs but otherwise having an identical device structure: (1) cells with PS deposited directly on bare fluorine-doped SnO2 (FTO)-coated glass; (2) cells with an intrinsic SnO2 thin layer on the top of FTO as an effective ESL; and (3) cells with the SnO2 ESL and adding a self-assembled monolayer (SAM) of fullerene. The results reveal two major potential drops or electric fields at the ESL/PS and PS/HSL interfaces. The electric-field ratio between the ESL/PS and PS/HSL interfaces increased in devices as follows: FTO < SnO2-ESL < SnO2 + SAM; this sequence explains the improvements of the fill factor (FF) and open-circuit voltage (Voc). The improvement of the FF from the FTO to SnO2-ESL cells may result from the reduction in voltage loss at the PS/HSL back interface and the improvement of Voc from the prevention of hole recombination at the ESL/PS front interface. The further improvements with adding an SAM is caused by the defect passivation at the ESL/PS interface, and hence, improvement of the junction quality. These nanoelectrical findings suggest possibilities for improving the device performance by further optimizing the SnO2-based ESL material quality and the ESL/PS interface.

Revealing the Nature of Molecule-Electrode Contact in Tunneling Junctions Using Raw Data Heat Maps.

Mechanistic understanding of charge transport through molecular tunnel junctions requires reproducible and statistically relevant data sets. This challenge has been overcome by development of large area junctions, especially those based on liquid-metal physi-sorbed top-electrodes, such as eutectic gallium-indium. A challenge with these junctions, however, is an inability to diagnose the quality of contact between the top-electrode and the SAMs. Since tunneling currents are dependent on the distance between the two electrodes, we demonstrate that by analyzing all raw unfitted data derived from a measurement using heat-maps, one can deduce the quality of contact and other minor bias-dependent fluctuations in the charge transport behavior. We demonstrate that the use of 3D plots would be challenging to interpret, but adoption of heat maps clearly captures details on junction quality irrespective of the total size of the data set or molecules used. We propose representation of raw data, rather than reliance on statistics, as proof of quality junctions.