Sang Il Seok

High-performance photovoltaic perovskite layers fabricated through intramolecular exchange

Taking in more sun Most efforts to grow superior films of organic-inorganic perovskites for solar cells have focused on methylammonium lead iodide (MAPbI3). However, formamidinium lead iodide (FAPbI3) has a broader solar absorption spectrum that could ultimately lead to better performance. Yang et al. grew high-quality FAPbI3 films by starting with a film of lead iodide and dimethylsulfoxide (DMSO) and then exchanging the DMSO with formamidinium iodide. Their best devices achieved power conversion efficiencies exceeding 20%. Science, this issue p. 1234 An intramolecular exchange process enables growth of high-quality organic perovskite films with greater solar spectral range. The band gap of formamidinium lead iodide (FAPbI3) perovskites allows broader absorption of the solar spectrum relative to conventional methylammonium lead iodide (MAPbI3). Because the optoelectronic properties of perovskite films are closely related to film quality, deposition of dense and uniform films is crucial for fabricating high-performance perovskite solar cells (PSCs). We report an approach for depositing high-quality FAPbI3 films, involving FAPbI3 crystallization by the direct intramolecular exchange of dimethylsulfoxide (DMSO) molecules intercalated in PbI2 with formamidinium iodide. This process produces FAPbI3 films with (111)-preferred crystallographic orientation, large-grained dense microstructures, and flat surfaces without residual PbI2. Using films prepared by this technique, we fabricated FAPbI3-based PSCs with maximum power conversion efficiency greater than 20%.

Iodide management in formamidinium-lead-halide–based perovskite layers for efficient solar cells

Healing defects with triiodide ions Deep-level defects in organic-inorganic perovskites decrease the performance of solar cells through unproductive recombination of charge carriers. Yang et al. show that introducing additional triiodide ions during the formation of layers of formamidinium lead iodide, which also contain small amounts of methylammonium lead bromide, suppresses the formation of deep-level defects. This process boosts the certified efficiency of 1-cm2 solar cells to almost 20%. Science, this issue p. 1376 Deep-level defect states in formamidinium lead perovskite layers can be minimized by the addition of triiodide ions. The formation of a dense and uniform thin layer on the substrates is crucial for the fabrication of high-performance perovskite solar cells (PSCs) containing formamidinium with multiple cations and mixed halide anions. The concentration of defect states, which reduce a cell’s performance by decreasing the open-circuit voltage and short-circuit current density, needs to be as low as possible. We show that the introduction of additional iodide ions into the organic cation solution, which are used to form the perovskite layers through an intramolecular exchanging process, decreases the concentration of deep-level defects. The defect-engineered thin perovskite layers enable the fabrication of PSCs with a certified power conversion efficiency of 22.1% in small cells and 19.7% in 1-square-centimeter cells.

Solvent engineering for high-performance inorganic–organic hybrid perovskite solar cells

Organolead trihalide perovskite materials have been successfully used as light absorbers in efficient photovoltaic cells. Two different cell structures, based on mesoscopic metal oxides and planar heterojunctions have already demonstrated very impressive advances in performance. Here, we report a bilayer architecture comprising the key features of mesoscopic and planar structures obtained by a fully solution-based process. We used CH3NH3 Pb(I(1-x)Br(x))3 (x = 0.1-0.15) as the absorbing layer and poly(triarylamine) as a hole-transporting material. The use of a mixed solvent of γ-butyrolactone and dimethylsulphoxide (DMSO) followed by toluene drop-casting leads to extremely uniform and dense perovskite layers via a CH3NH3I-PbI2-DMSO intermediate phase, and enables the fabrication of remarkably improved solar cells with a certified power-conversion efficiency of 16.2% and no hysteresis. These results provide important progress towards the understanding of the role of solution-processing in the realization of low-cost and highly efficient perovskite solar cells.

Compositional engineering of perovskite materials for high-performance solar cells

Of the many materials and methodologies aimed at producing low-cost, efficient photovoltaic cells, inorganic–organic lead halide perovskite materials appear particularly promising for next-generation solar devices owing to their high power conversion efficiency. The highest efficiencies reported for perovskite solar cells so far have been obtained mainly with methylammonium lead halide materials. Here we combine the promising—owing to its comparatively narrow bandgap—but relatively unstable formamidinium lead iodide (FAPbI3) with methylammonium lead bromide (MAPbBr3) as the light-harvesting unit in a bilayer solar-cell architecture. We investigated phase stability, morphology of the perovskite layer, hysteresis in current–voltage characteristics, and overall performance as a function of chemical composition. Our results show that incorporation of MAPbBr3 into FAPbI3 stabilizes the perovskite phase of FAPbI3 and improves the power conversion efficiency of the solar cell to more than 18 per cent under a standard illumination of 100 milliwatts per square centimetre. These findings further emphasize the versatility and performance potential of inorganic–organic lead halide perovskite materials for photovoltaic applications.

Chemical Management for Colorful, Efficient, and Stable Inorganic− Organic Hybrid Nanostructured Solar Cells

Chemically tuned inorganic-organic hybrid materials, based on CH3NH3(═MA)Pb(I(1-x)Br(x))3 perovskites, have been studied using UV-vis absorption and X-ray diffraction patterns and applied to nanostructured solar cells. The band gap engineering brought about by the chemical management of MAPb(I(1-x)Br(x))3 perovskites can be controllably tuned to cover almost the entire visible spectrum, enabling the realization of colorful solar cells. We demonstrate highly efficient solar cells exhibiting 12.3% in a power conversion efficiency of under standard AM 1.5, for the most efficient device, as a result of tunable composition for the light harvester in conjunction with a mesoporous TiO2 film and a hole conducting polymer. We believe that the works highlighted in this paper represent one step toward the realization of low-cost, high-efficiency, and long-term stability with colorful solar cells.

High-Performance Nanostructured Inorganic−Organic Heterojunction Solar Cells

We report all solid-state nanostructured inorganic-organic heterojunction solar cells fabricated by depositing Sb(2)S(3) and poly(3-hexylthiophene) (P3HT) on the surface of a mesoporous TiO(2) layer, where Sb(2)S(3) acts as an absorbing semiconductor and P3HT acts as both a hole conductor and light absorber. These inorganic-organic light harvesters perform remarkably well with a maximum incident-photon-to-current efficiency (IPCE) of 80% and power conversion efficiency of 5.13% under air-mass 1.5 global (AM 1.5G) illumination with the intensity of 100 mW cm(-2). These devices are highly stable under room light in air, even without encapsulation. The present findings offer novel directions for achieving high-efficiency solid-state solar cells by hybridization of inorganic-organic light harvesters and hole transporters.

Voltage output of efficient perovskite solar cells with high open-circuit voltage and fill factor

Besides the generated photocurrent as a key factor that impacts the efficiency of solar cells, the produced photovoltage and fill factor are also of critical importance. Therefore, understanding and optimization of the open-circuit voltage (Voc) of perovskite solar cells, especially with an architecture consisting of mesoporous (mp)-TiO2/perovskite/hole transporting materials (HTMs), are required to further improve the conversion efficiency. In this work, we study the effects of the energy level between CH3NH3(= MA)PbI3 and MAPbBr3 and a series of triarylamine polymer derivatives containing fluorene and indenofluorene, which have different highest occupied molecular orbital (HOMO) levels, in terms of the photovoltaic behaviour. The voltage output of the device is found to be dependent on the higher energy level of perovskite solar absorbers as well as the HOMO level of the HTMs. The combination of MAPbBr3 and a deep-HOMO HTM leads to a high photovoltage of 1.40 V, with a fill factor of 79% and an energy conversion efficiency of up to 6.7%, which is the highest value reported to date for MAPbBr3 perovskite solar cells.

o-Methoxy Substituents in Spiro-OMeTAD for Efficient Inorganic–Organic Hybrid Perovskite Solar Cells

Three spiro-OMeTAD derivatives have been synthesized and characterized by (1)H/(13)C NMR spectroscopy and mass spectrometry. The optical and electronic properties of the derivatives were modified by changing the positions of the two methoxy substituents in each of the quadrants, as monitored by UV-vis spectroscopy and cyclic voltammetry measurements. The derivatives were employed as hole-transporting materials (HTMs), and their performances were compared for the fabrication of mesoporous TiO2/CH3NH3PbI3/HTM/Au solar cells. Surprisingly, the cell performance was dependent on the positions of the OMe substituents. The derivative with o-OMe substituents showed highly improved performance by exhibiting a short-circuit current density of 21.2 mA/cm(2), an open-circuit voltage of 1.02 V, and a fill factor of 77.6% under 1 sun illumination (100 mW/cm(2)), which resulted in an overall power conversion efficiency (PCE) of 16.7%, compared to ~15% for conventional p-OMe substituents. The PCE of 16.7% is the highest value reported to date for perovskite-based solar cells with spiro-OMeTAD.

Benefits of very thin PCBM and LiF layers for solution-processed p–i–n perovskite solar cells

Highly efficient p–i–n perovskite solar cells employing a flat and thick CH3NH3PbI3 film and a thin PCBM film are fabricated by the solution-process at low temperature. Through attainment of optimized PCBM thickness and insertion of the LiF interlayer, the unit cell shows 14.1% of overall power conversion efficiency (PCE) with a Jsc of 20.7 mA cm−2, a Voc of 0.866 V, and a FF of 78.3% under AM 1.5G 100 mW cm−2 conditions, while a larger area 10 cell serially connected module (10 × 10 cm2) shows an 8.7% PCE. These PCE values are the highest reported to date for the planar perovskite–PCBM solar cells.

Efficient Inorganic–Organic Hybrid Perovskite Solar Cells Based on Pyrene Arylamine Derivatives as Hole-Transporting Materials

A set of three N,N-di-p-methoxyphenylamine-substituted pyrene derivatives have successfully been synthesized and characterized by (1)H/(13)C NMR spectroscopy, mass spectrometry, and elemental analysis. The optical and electronic structures of the pyrene derivatives were adjusted by controlling the ratio of N,N-di-p-methoxyphenylamine to pyrene, and investigated by UV/vis spectroscopy and cyclic voltammetry. The pyrene derivatives were employed as hole-transporting materials (HTMs) in fabricating mesoporous TiO2/CH3NH3PbI3/HTMs/Au solar cells. The pyrene-based derivative Py-C exhibited a short-circuit current density of 20.2 mA/cm(2), an open-circuit voltage (Voc) of 0.886 V, and a fill factor of 69.4% under an illumination of 1 sun (100 mW/cm(2)), resulting in an overall power conversion efficiency of 12.4%. The performance is comparable to that of the well-studied spiro-OMeTAD, even though the Voc is slightly lower. Thus, this newly synthesized pyrene derivative holds promise as a HTM for highly efficient perovskite-based solar cells.