Jangwon Seo

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.

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.

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.

A White-Light-Emitting Molecule: Frustrated Energy Transfer between Constituent Emitting Centers

White-light-emitting single molecules are promising materials for use in a new generation of displays and light sources because they offer the possibility of simple fabrication with perfect color reproducibility and stability. To realize white-light emission at the molecular scale, thereby eliminating the detrimental concentration- or environment-dependent energy transfer problem in conventional fluorescent or phosphorescent systems, energy transfer between a larger band-gap donor and a smaller band-gap acceptor must be fundamentally blocked. Here, we present the first example of a concentration-independent ultimate white-light-emitting molecule based on excited-state intramolecular proton transfer materials. Our molecule is composed of covalently linked blue- and orange-light-emitting moieties between which energy transfer is entirely frustrated, leading to the production of reproducible, stable white photo- and electroluminescence.

Colloidally prepared La-doped BaSnO3 electrodes for efficient, photostable perovskite solar cells

Transporter layers for greater stability Although perovskite solar cells (PSCs) can have power conversion efficiencies exceeding 20%, they can have limited stability under ultraviolet irradiation. This is in part because the mesoporous TiO2 used as an electron-transporting layer can photocatalyze unwanted reactions in the perovskite layer. Shin et al. report a low-temperature colloidal method for depositing La-doped BaSnO3 films as a replacement for TiO2 to reduce such ultraviolet-induced damage. Solar cells retained over 90% of their initial performance after 1000 hours of full sun illumination. Science, this issue p. 167 Ultraviolet damage in perovskite photovoltaics induced by TiO2 in the electron-transporting layer can be avoided with La-doped BaSnO3. Perovskite solar cells (PSCs) exceeding a power conversion efficiency (PCE) of 20% have mainly been demonstrated by using mesoporous titanium dioxide (mp-TiO2) as an electron-transporting layer. However, TiO2 can reduce the stability of PSCs under illumination (including ultraviolet light). Lanthanum (La)–doped BaSnO3 (LBSO) perovskite would be an ideal replacement given its electron mobility and electronic structure, but LBSO cannot be synthesized as well-dispersible fine particles or crystallized below 500°C. We report a superoxide colloidal solution route for preparing a LBSO electrode under very mild conditions (below 300°C). The PSCs fabricated with LBSO and methylammonium lead iodide (MAPbI3) show a steady-state power conversion efficiency of 21.2%, versus 19.7% for a mp-TiO2 device. The LBSO-based PSCs could retain 93% of their initial performance after 1000 hours of full-Sun illumination.

Efficient CH3NH3PbI3 Perovskite Solar Cells Employing Nanostructured p‐Type NiO Electrode Formed by a Pulsed Laser Deposition

Highly transparent and nanostructured nickel oxide (NiO) films through pulsed laser deposition are introduced for efficient CH3 NH3 PbI3 perovskite solar cells. The (111)-oriented nanostructured NiO film plays a key role in extracting holes and preventing electron leakage as hole transporting material. The champion device exhibits a power conversion efficiency of 17.3% with a very high fill factor of 0.813.

Rational Strategies for Efficient Perovskite Solar Cells

A long-standing dream in the large scale application of solar energy conversion is the fabrication of solar cells with high-efficiency and long-term stability at low cost. The realization of such practical goals depends on the architecture, process and key materials because solar cells are typically constructed from multilayer heterostructures of light harvesters, with electron and hole transporting layers as a major component. Recently, inorganic-organic hybrid lead halide perovskites have attracted significant attention as light absorbers for the fabrication of low-cost and high-efficiency solar cells via a solution process. This mainly stems from long-range ambipolar charge transport properties, low exciton binding energies, and suitable band gap tuning by managing the chemical composition. In our pioneering work, a new photovoltaic platform for efficient perovskite solar cells (PSCs) was proposed, which yielded a high power conversion efficiency (PCE) of 12%. The platform consisted of a pillared architecture of a three-dimensional nanocomposite of perovskites fully infiltrating mesoporous TiO2, resulting in the formation of continuous phases and perovskite domains overlaid with a polymeric hole conductor. Since then, the PCE of our PSCs has been rapidly increased from 3% to over 20% certified efficiency. The unprecedented increase in the PCE can be attributed to the effective integration of the advantageous attributes of the refined bicontinuous architecture, deposition process, and composition of perovskite materials. Specifically, the bicontinuous architectures used in the high efficiency comprise a layer of perovskite sandwiched between mesoporous metal-oxide layer, which is a very thinner than that of used in conventional dye-sensitized solar cells, and hole-conducting contact materials with a metal back contact. The mesoporous scaffold can affect the hysteresis under different scan direction in measurements of PSCs. The hysteresis also greatly depends on the cell architecture and perovskite composition. In this Account, we will describe what we do with major aspects including (1) the film morphology through the development of intermediate chemistry retarding the rapid reaction between methylammonium or formamidinium iodide and lead halide (PbI2) for improved perovskite film formation; (2) the phase stability and band gap tuning of the perovskite layer through the materials engineering; (3) the development of electron and hole transporting materials for carrier-selective contacting layers; and (4) the adoption of p-i-n and n-i-p architectures depending on the position of the electron or hole conducting layer in front of incident light. Finally, we will summarize the recent incredible achievements in PSCs, and finally provide challenges facing the future development and commercialization of PSCs.