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Identification and profiling of molecular fragments generated over the lifespan of halide perovskite solar cells are needed to overcome the stability issues associated with these devices. Herein, we report the characterization of buried CH 3 NH 3 PbI 3- x Cl x (HaP)-transport layer (TL) interfaces. By using hard X-ray photoelectron spectroscopy in conjunction with transmission electron microscopy, we reveal that the chemical decomposition of HaP is TL-dependent. With NiO 1-δ , phenyl-C 61 -butyric acid methyl ester (PCBM), or poly(bis(4-phenyl) (2,4,6-trimethylphenyl)amine) (PTAA) as TLs, probing depth analysis shows that the degradation takes place at the interface (HaP/TL) rather than the HaP bulk area. From core-level data analysis, we identified iodine migration toward the PCBM- and PTAA-TLs. Unexpected diffusion of nitrogen inside NiO 1-δ -TL was also found for the HaP/NiO 1-δ sample. With a HaP/PCBM junction, HaP is dissociated to PbI 2 , whereas HaP/PTAA contact favored the formation of CH 3 I. The low stability of HaP solar cells in the PTAA-TL system is attributed to the formation of CH 3 I and iodide ion vacancies. Improved stability observed with NiO 1-δ -TL is related to weak dissociation of stoichiometric HaP. Here, we provide a new insight to further distinguish different mechanisms of degradation to improve the long-term stability and performance of HaP solar cells.

In this work, the effect of carbon dots (C-dots) on the performance of NiO-based dye-sensitized solar cells (DSSCs) was explored. NiO nanoparticles (NPs) with a rectangular shape (average size: 11.4 × 16.5 nm 2 ) were mixed with C-dots, which were synthesized from citric acid (CA) and ethylenediamine (EDA). A photocathode consisting of a composite of C-dots with NiO NPs (NiO@C-dots) was then used to measure the photovoltaic performance of a DSSC. A power conversion efficiency (PCE) of 9.85% (430 nm LED@50 mW/cm 2 ) was achieved by a DSSC fabricated via the adsorption of N719 sensitizer with a C-dot content of 12.5 wt % at a 1.5:1 EDA/CA molar ratio. This PCE value was far larger than the PCE value (2.44 or 0.152%) obtained for a NiO DSSC prepared without the addition of C-dots or N719, respectively, indicating the synergetic effect by the co-adsorption of C-dots and N719. This synergetically higher PCE of the NiO@C-dot-based DSSC was due to the larger amount of sensitizer adsorbed onto the composites with a larger specific surface area and the faster charge transfer in the NiO@C-dot working electrode. In addition, the C-dots bound to the NiO NPs shorten the band gap of the NiO NPs due to energy transfer and give rise to faster charge separation in the electrode. The most important fact is that C-dots are the main sensitizer, while N719 tightly adsorbs on C-dots and NiO behaves as an accelerator of a positive electron transfer and a restrainer of the electron-hole recombination. These results reveal that C-dots are a remarkable enhancer for NiO NPs in DSSCs and that NiO@C-dots are promising photovoltaic electrode materials for DSSCs.

The carrier transport layers (CTLs) have exhibited the influence on performance and stability of halide perovskite solar cells (HaPSCs). The exploration of characteristic impacts on HaPSCs induced by the CTL unveils the key factors underlying the device physics. In this work, we investigate the impacts of the organic or inorganic hole transport layer (HTL) in HaPSCs by analyzing the elemental distribution, the current-voltage characteristics, and the capacitance spectroscopy. The organic HTL device shows the lower activation energy ( E A < E g ) indicating a dominant interface-mediated recombination. The defect analysis reveals that the device with the inorganic HTL induces rather deep antisite defects with slightly higher trap densities. This is attributed to the diffusion of metal cations into the halide perovskite (HaP) during crystallization of HaP layer grown on the inorganic HTLs. Our results suggest that the passivation of deep defect and suppression of trap densities in the HaP either using ideal CTLs or optimizing the fabrication route is crucial to improving the device parameters approaching the theoretical limit.

Wide-band-gap (WB) perovskite devices are promising as the top cell of silicon-perovskite tandem devices to boost the efficiency beyond the Shockley-Queisser limit. Here, we tailor the performance parameters of WB mixed-halide perovskite solar cell with long alkyl chain-substituted fullerene derivatives as an electron transport layer (ETL). The device with C 60 -fused N-methylpyrrolidine- meta-dodecyl phenyl (C 60 MC 12 ) demonstrates an enhanced power conversion efficiency of 16.74% with the record open circuit voltage ( V OC ) of 1.24 V, an increase by 70 mV with concomitant V OC deficit reduction to 0.47 V. This is achieved by mitigating the recombination loss through the use of highly crystalline C 60 MC 12 film compared to amorphous [6,6]-phenyl-C 61 -butyric acid methyl ester layer. The device analysis reveals the soothing of the defect activities with shallower defect states and passivation of the interface recombination centers for the device with C 60 MC 12 . We ascribe this property to the crystallinity of fullerene derivatives as ETL, which is also important for the optimization of device parameters, besides the band alignment matching of WB perovskite devices.

Low-temperature solution-processed perovskite solar cells are attracting immense interest due to their ease of fabrication and potential for mass production on flexible substrates. However, the unfavorable surface properties of planar substrates often lead to large variations in perovskite crystal size and weak charge extractions at interfaces, resulting in inferior performance. Here, we report the improved performance, reproducibility, and high stability of "p-i-n" planar heterojunction perovskite solar cells. The key fabrication process is the addition of the amine-polymer poly[(9,9-bis(3'-(N,N-dimethylamino)propyl)-2,7-fluorene)-alt-2,7-(9,9-dioctylfluorene)] (PFN-P1) to a simple spin-coating process. The PFN-P1 works as a surfactant and helps promote uniform crystallization. As a result, perovskite films with PFN-P1 have a uniform distribution of grain sizes and improved open circuit voltage. Devices with PFN-P1 showed the best efficiency (13.2%), with a small standard deviation (0.40), out of 60 cells. Moreover, ∼90% of the initial efficiency was retained over more than 6 months. Additionally, devices fabricated from PFN-P1 mixed perovskite films showed higher stability under continuous operation at maximum power point over 150 h. Our results show that this approach is simple and effective for improving device performance, reproducibility, and stability by modifying perovskite properties with PFN-P1. Because of the simplicity of the fabrication process and reliable performance increase, this approach marks important progress in low-temperature solution-processed perovskite solar cells.