Structural and Trap‐State Density Enhancement in Flash Infrared Annealed Perovskite Layers

Perovskite solar cells are well-known for their high energy conversion efficiency, low-temperature processing, and cost-effective production. Flash infrared annealing (FIRA) of slot-die cast perovskite precursors offers an attractive manufacturing route using high-throughput roll-to-roll technology. Despite the recent progress in FIRA perovskite annealing, the optimal composition of the perovskite precursor is yet to be developed. Here, the effect of methylammonium chloride (MACl) on the perovskite structure and trap-state density as a function of the FIRA annealing time is investigated. In situ real-time grazing-incidence wide-angle X-ray scattering (GIWAXS) is employed to monitor the perovskite layer formation during FIRA annealing with millisecond temporal resolution. In addition, the density of states in the bandgap is estimated using ex situ energy-resolved electrochemical impedance spectroscopy. Evidence is found that adding 10% MACl into the perovskite precursor solution significantly improves the crystallographic orientation of the perovskite layers while reducing the trap-state density by one order of magnitude. In addition, using time-resolved GIWAXS, the most favorable time window for the FIRA processing of perovskite films with the lowest mosaicity and trap-state density is identified. The results are of general importance for elucidating the appropriate temporal windows in complex and fast-evolving crystallization processes

Effect of the doping of PC61BM electron transport layer with carbon nanodots on the performance of inverted planar MAPbI3 perovskite solar cells

The doping effect of carbon nanodots (CNDs) in the PC61BM electron-transport layer on the performance of inverted planar MAPbI3 perovskite solar cells (PSCs) having two different kinds of the hole-transport layer, namely organic PEDOT:PSS and inorganic NiOx, was investigated. The CH3NH3PbI3 perovskite layer was deposited in air at 35% humidity. An average 11% and 12% enhancement of the power conversion efficiency (PCE) was achieved for 1 wt% CNDs doping in the PSCs with PEDOT:PSS and NiOx, respectively. This improvement is attributed to high electron density of CNDs resulting in a triple increase of the electrical conductivity of the PC61BM layer and passivation of the perovskite/PC61BM interface that is reflected by an increase of the open-circuit voltage. In line with this, parallel resistance and fill factor of the PSCs are also improved. Moreover, the energy-resolved electrochemical impedance spectroscopy revealed additional free-charge carriers in the PC61BM layer generated under illumination that were detected via the polaron states formation in the band gap with positive effect on the short-circuit current. All these factors contribute to the PCE improvement. Stability tests of the PSC with PEDOT:PSS under a continuous 24 hour 1.5 AM illumination showed a five times smaller final PCE decrease for the 1 wt% CNDs doping of the PC61BM layer comparing to the undoped counterpart. The passivation effect of CNDs, namely electron filling the traps formed by the photo-dimerization and photo-oxidation of PC61BM molecules, is responsible for this remarkable improvement of the short-term stability. © 2019 International Solar Energy Societ

Crystallization of 2D Hybrid Organic–Inorganic Perovskites Templated by Conductive Substrates

2D hybrid organic–inorganic perovskites are valued in optoelectronic applications for their tunable bandgap and excellent moisture and irradiation stability. These properties stem from both the chemical composition and crystallinity of the layer formed. Defects in the lattice, impurities, and crystal grain boundaries generally introduce trap states and surface energy pinning, limiting the ultimate performance of the perovskite; hence, an in-depth understanding of the crystallization process is indispensable. Here, a kinetic and thermodynamic study of 2D perovskite layer crystallization on transparent conductive substrates are provided—fluorine-doped tin oxide and graphene. Due to markedly different surface structure and chemistry, the two substrates interact differently with the perovskite layer. A time-resolved grazing-incidence wide-angle X-ray scattering (GIWAXS) is used to monitor the crystallization on the two substrates. Molecular dynamics simulations are employed to explain the experimental data and to rationalize the perovskite layer formation. The findings assist substrate selection based on the required film morphology, revealing the structural dynamics during the crystallization process, thus helping to tackle the technological challenges of structure formation of 2D perovskites for optoelectronic devices