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We suggest phase transition-induced surface passivation of alkylammonium formates for effective defect passivation of perovskite, achieving significantly improved efficiency and thermal stability.

With the unprecedented development of perovskite solar cells (PSCs), various interlayers have been investigated. Interlayers have diverse roles in shifting the energy levels, attracting and extracting charges, and passivating surface traps. These can improve the stability of PSCs, as well as their power conversion efficiency (PCE). In this study, a small molecular self-assembled monolayer (2-[carbamimidoyl(methyl)amino]acetic acid) is introduced on a SnO2 layer. The acetic acid is known as creatine, existing naturally in the human body. It is eatable and dosed by athletes for energy. Due to its structural properties, creatine can be anchored on a SnO2 layer, thus, it can strengthen the charge extraction from a perovskite layer by forming interface dipoles and reducing the work function. Also, it can passivate the defects in the perovskite layer. These properties are comprehensively investigated via various experimental techniques. With the creatine layer as a cathode interfacial layer on the SnO2 layer, the PSC employing a triple cation-based perovskite achieves the highest PCE of 20.8% and retained 90% of it after 50 days. Furthermore, 22.1% of PCE is obtained from the formamidinium-based perovskite. This report represents an interesting application of creatine as an interlayer in PSCs and suggests the possible application of other essential amino acids.

Organic–inorganic perovskites are crystalline light absorbers which are gaining great attraction from the photovoltaic community. Surprisingly, the power conversion efficiencies of these perovskite solar cells have rapidly increased by over 25% in 2019, which is comparable to silicon solar cells. Despite the many advances in efficiency, there are still many areas to be improved to increase the efficiency and stability of commercialization. For commercialization and enhancement of applicability, the development of electron transport layer (ETL) and its interface for low temperature processes and efficient charge transfer are very important. In particular, understanding the ETL and its interface is of utmost importance, and when this understanding has been made enough, excellent research results have been published that can improve the efficiency and stability of the device. Here, we review the progress of perovskite solar cells. Especially we discuss recent important development of perovskite deposition method and its engineering as well as the electron transport layer.

We report a simple post annealing-free (PAF) method for making uniform, large grain-sized, and highly crystalline triple cation perovskite films. In this simple process, a perovskite precursor solution was spin-coated onto a TiO 2 mesoporous substrate and as an antisolvent, diethyl ether (DEE) was subsequently dripped onto the film during spinning to produce an intermediate phase (IP) of perovskite film. This IP was immediately immersed into a DEE bath at room temperature for only 1 min in replacement of the conventional post annealing (PA) treatment. The as-prepared PAF film was characterized by X-ray powder diffraction, UV–vis absorption spectroscopy, fourier transform infrared spectroscopy, scanning electron microscopy, atomic-force microscopy, and photoluminescence spectroscopy. The overall power conversion efficiency (PCE) of the PAF devices was in the range of 18.8–19.5%, which is comparable with the reported PA devices (17.2–18.1%), mainly due to the J SC and the FF values, caused by the high absorption ability and the large crystal size with better surface smoothness in the PAF film. This efficiency is the highest reported for perovskite deposition by PAF methods. This new method enables reducing the device fabrication time at room temperature, which will reduce the cost of manufacturing efficient perovskite solar cells.

We introduce 1 step pin-hole free CH3NH3PbI3−xClx perovskite layers by using heated airflow during the nucleation stage of the perovskite. Upon employing heated air, we stimulate uniformly distributed nuclei growth, resulting in a pin-hole free planar perovskite layer. We find an optimized heated airflow of 100 °C as the optimized condition. The resulting planar device employing a conventional TiO2 electron transporting layer exhibits 17.6% average power conversion efficiency with 14.3% maximum powerpoint (MPP) efficiency. In addition, our method gives a very reproducible perovskite layer. Thus, our pin-hole free perovskite layer allows for 14.9% efficiency in a larger area device (0.71 cm2) that is generally prone to shunting paths.

Hybrid perovskites form an extremely attractive class of materials for large scale, low-cost photovoltaic applications. Fullerene-based charge extraction layers have emerged as a viable n-type charge collection layer, and in “inverted” p–i–n device architectures the solar cells are approaching efficiencies of 20%. However, the regular n–i–p devices employing fullerenes still lag behind in performance. Here, we show that partial solubility of fullerene derivatives in the aprotic solvents used for the perovskites makes it challenging to retain integral films in multilayer solution processing. To overcome this issue we introduce cross-linkable fullerene derivatives as charge collection layers in n–i–p planar junction perovskite solar cells. The cross-linked fullerene layers are insolubilized and deliver improved performance in solar cells enabled by a controllable film thickness.

Here we study perovskite solar cells based on mesoporous alumina scaffold infiltrated and capped with a perovskite absorber layer, which are devoid of a discrete n-type electron collection layer. We employ ethoxylated polyethylenimine (PEIE) to modify the interface between the perovskite absorber layer and the metallic transparent fluorine-doped SnO 2 (FTO) electrode. Surprisingly, the PEIE interlayer obviates the requirement for the conventional dense-TiO 2 (d-TiO 2 ) compact layer (or organic fullerene layer), usually required to selectively extract electrons from the perovskite film. The self-organized PEIE interlayer produced a strong induced dipole moment at the perovskite-FTO interface, with our results indicating that electrons accumulate within the perovskite film at this interface. The resultant “n-type” contact region within the perovskite absorber layer, progressing to an intrinsic (i) region within the bulk of the perovskite layer, represents an n-i homojunction and favorably enables selective electron extraction at the FTO electrode. Resulting solar cells deliver current-voltage measured power conversion efficiencies (η) of over 15.0% and a substantial stabilized efficiency (η) of 9.1%. Although our solar cell performance remains lower than the highest reported efficiencies for perovskite solar cells employing discrete charge selective extraction layers, it indicates significant potential for “homo-junction” perovskite solar cells, once the metallic-to-perovskite contact is fully controlled. Additionally, our work identifies the potential impact of modifying the interface between the perovskite absorber and the subsequent contact materials with dipolar organic compounds, which may be applicable to optimizing contact at perovskite-semiconductor heterojunctions.

Nanoporous network polymer nanocomposites with tunable pore size for size-dependent selective ion transport are successfully prepared via the surface-induced cross-linking polymerization of methyl methacrylate (MMA) and 1,6-hexanediol diacrylate (HDDA) on the surfaces of nanocrystalline TiO2 particles. The morphologies of the porous network polymer layer and nanopores were investigated by transmission electron microscopy (TEM), field emission scanning electron microscopy (FE-SEM), and Brunauer–Emmett–Teller (BET) experiments. The porous layer size-selectively screened the ions that contacted the nanocrystalline TiO2 particles, as demonstrated by ion conductivity measurements, electrochemical impedance spectroscopy (EIS), and transient absorption spectroscopy (TAS).

Compact TiO2 is widely used as an electron transport material in planar-perovskite solar cells. However, TiO2-based planar-perovskite solar cells exhibit low efficiencies due to intrinsic problems such as the unsuitable conduction band energy and low electron extraction ability of TiO2. Herein, the planar TiO2 electron transport layer (ETL) of perovskite solar cells is modified with ionic salt CuI via a simple one-step spin-coating process. The p-type nature of the CuI islands on the TiO2 surface leads to modification of the TiO2 band alignment, resulting in barrier-free contacts and increased open-circuit voltage. It is found that the polarity of the CuI-modified TiO2 surface can pull electrons to the interface between the perovskite and the TiO2, which improves electron extraction and reduces nonradiative recombination. The CuI solution concentration is varied to control the electron extraction of the modified TiO2 ETL, and the optimized device shows a high efficiency of 19.0%. In addition, the optimized device shows negligible hysteresis, which is believed to be due to the removal of trap sites and effective electron extraction by CuI-modified TiO2. These results demonstrate the hitherto unknown effect of p-type ionic salts on electron transport material.

A series of liquid junction dye-sensitized solar cells (DSCs) was fabricated based on polymer membrane-encapsulated dye-sensitized TiO2 nanoparticles, prepared using a surface-induced cross-linking polymerization reaction, to investigate the dependence of the solar cell performance on the encapsulating membrane layer thickness. The ion conductivity decreased as the membrane thickness increased; however, the long term-stability of the devices improved with increasing membrane thickness. Nanoparticles encapsulated in a thick membrane (ca. 37 nm), obtained using a 90 min polymerization time, exhibited excellent pore filling among TiO2 particles. This nanoparticle layer was used to fabricate a thin-layered, quasi-solid state DSC. The thick membrane prevented short-circuit paths from forming between the counter and the TiO2 electrode, thereby reducing the minimum necessary electrode separation distance. The quasi-solid state DSC yielded a high power conversion efficiency (7.6 → 8.1%) and excellent stability during heating at 65 °C over 30 days. These performance characteristics were superior to those obtained from a conventional DSC (7.5 → 3.5%) prepared using a TiO2 active layer with the same thickness. The reduced electrode separation distance shortened the charge transport pathways, which compensated for the reduced ion conductivity in the polymer gel electrolyte. Excellent pore filling on the TiO2 particles minimized the exposure of the dye to the liquid and reduced dye detachment.