Abstract:The morphology control of CH 3 NH 3 PbI 3 (MAPbI 3 ) thin-film is crucial for the high-efficiency perovskite solar cells, especially for their planar structure devices. Here, a feasible and effective post-treatment method is presented to improve the quality of MAPbI 3 films by using methylamine (CH 3 NH 2 ) vapor. This post-treatment process is studied thoroughly, and the perovskite films with smooth surface, high preferential growth orientation and large crystals are obtained after 10 s treatment in MA atmosphere. It enhances the light absorption, and increases the recombination lifetime. Ultimately, the power conversion efficiency (PCE) of 15.3% for the FTO/TiO 2 /MAPbI 3 /spiro-OMeTAD/Ag planar architecture solar cells is achieved in combination with this post-treatment method. It represents a 40% improvement in PCE compared to the best control cell. Moreover, the whole post-treatment process is simple and cheap, which only requires some CH 3 NH 2 solution in absolute ethanol. It is beneficial to control the reaction rate by changing the volume of the solution. Therefore, we are convinced that the post-treatment method is a valid and essential approach for the fabrication of high-efficiency perovskite solar cells.

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The energy extracted from solar radiation is the most abundant and accessible source of renewable energy, which will become progressively more important as time goes on. Solar cells are regarded as one of the most promising candidates for generating renewable clean energy. Recently, a new class of semiconducting material called organic-inorganic halide perovskite has received great attention of academia, and the record power conversion efficiency (PCE) of perovskite solar cell (PSC) rapidly increased from 3.8% in 2009 to 22.7% in late 2017 through intensive research due to some advantages as follows. 1) Excellent optoelectronic property. Perovskite materials exhibit excellent properties, including long diffusion length, high carrier mobility, and high absorption coefficient. 2) Low cost. The ingredients of perovskite materials are cheap, and PSCs can be manufactured by a solution process. 3) Tunable bandgap. Perovskite materials have highly tunable bandgap (1.2-2.2 eV), contributing to the further improvement in PCE of single junction PSCs by realizing the ideal bandgap (1.3-1.4 eV) as demonstrated by the Shockley-Queisser detailed balanced calculation. The basic architectures of PSCs are divided mainly into mesoscopic and planar heterojunction structures. Compared with the former configuration, the later configuration combined with low-temperature processable interlayers provides a method of fabricating flexible PSCs and tandem PSCs. Furthermore, the nonuse of the mesoscopic structure simplifies the structure of PSCs and reduces the cost and time of fabrication. The key requirement to achieve an efficient and reproducible planar heterojunction PSCs is that the perovskite layer should be uniform, continuous, and pinhole free to minimize shunting pathways. So, significant research effort is being devoted to the quality management of perovskite films with the goal of achieving the controllable preparation, including the optimization of their morphology (uniformity, coverage, roughness) and microstructure (grain size/distribution, texture), and the elimination of defects (voids, pinholes, grain boundaries), which influence the PSC performance directly. Especially for the one-step solution coating method, the film quality of perovskite on different planar substrates under varied deposition conditions exhibits a large difference, due to the complex crystallization process and the heightened sensitivity to environmental conditions. In this paper, the characteristics of perovskite materials, the nucleation-growth mechanism of films in the one-step solution method, and the evolution of cell structures are described briefly. The latest quality control methods of high-quality perovskite films prepared by solution method are then discussed emphatically. Finally, to provide references for the future research, the development and existing problems of PSCs are addressed and prospected.

Inorganic-organic metal halide perovskite solar cells (PSCs) have drawn tremendous attention as a promising next-generation solar-cell technology because of their high efficiencies and low production cost. Since the first report in 2009, the recorded power conversion efficiency (PCE) of PSCs has rapidly risen to 22.1% by using 2, 2', 7, 7'-tetrakis (N,Ndi-p-methoxyphenyl-amine) 9,9-spirobifluorene (spiro-MeoTAD) as hole transport material (HTM), with the efforts devoted to the device architecture optimization, material compositional engineer and interface engineering. Nevertheless, the synthesis and cost of the organic HTM (OHTM) become a major challenging issue and therefore alternative materials are required. In the past few years, the applications of inorganic HTMs (IHTMs) in PSCs have shown large improvement in PCE and stability. For example, PSCs with CuOx as IHTM reached a PCE of 19.0% with better stability. Even more exciting, the theoretical PCE of PSC based on Cu2O HTM reaches 24.4%. So, Cu2O is a promising IHTM for future optimized PSC and the large area uniform preparation is very important. In this paper, Cu2O films have been successfully prepared using electron beam evaporation followed by air annealing. The influences of annealing temperature and time on the composition, structure, and photoelectric characteristics of film are investigated in detail. It is found that the as-deposited film is a mixture of Cu2O and Cu. With the increase of annealing temperature, material composition is transformed from mixture to pure Cu2O phase, and then to CuO, due to the oxidation in air. In an annealing temperature between 100℃ to 150℃, pure Cu2O film can be obtained with an average transmission rate over 70%, optical band-gap of 2.5 eV, HOMO level of -5.32 eV, and a carrier mobility of 30 cm2·V-1·s-1. When the film is treated with a UV lamp, the structure and composition of the film can be changed more easily because of the enhancement of oxidation. Finally, reverted planar PSCs with the structure of Ag/PCBM/CH3NH3PbI3/HTMs/ITO are constructed and compared carefully based on HTMs of Cu2O, with poly(3,4-ethylenedioxythiophene)-poly(styrenesulfonate)(PEDOT:PSS), and Cu2O/PEDOT:PSS layers, respectively. An optimum thickness of 40 nm of Cu2O HTM is achieved with high carrier extraction rate. However, the performances of all of the PSCs are inferior to those of PEDOT:PSS-based devices, due to the formation of pinholesin absorber layer resulting from the strong hydrophobicity of Cu2O film. However, the efficiency of PSC based on Cu2O/PEDOT:PSS double-HTM is deteriorated because of the chemical interaction between PEDOT:PSS and Cu2O. These findings provide some important guidelines for the design of HTMs.