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.

Long-Term Chemical Aging of Hybrid Halide Perovskites.

Because the power conversion efficiency (PCE) of hybrid halide perovskite solar cells (PSCs) could exceed 24%, extensive research has been focused on improving their long-term stability for commercialization in the near future. In a previous study, we reported that the addition of a number of ionized iodide (triiodide: I3-) ions during perovskite film formation significantly improved the efficiency of PSCs by reducing deep-level defects in the perovskite layer. Understanding the relationship between the concentration of these defects and the long-term chemical aging of PSCs is important not only for obtaining fundamental insight into the perovskite materials but also for studying the long-term chemical stability of PSCs. Herein we aim to identify the origin of the natural decay in PCE during long-term chemical aging of PSCs in the dark based on formamidinium lead triiodide by comparing the performance of control and low-defect (LD) devices. After aging for 200 days, the change in the PCE of the LD devices (1.3%) was found to be half that of the control devices (2.6%). We investigated this difference using grazing incidence wide-angle X-ray scattering, deep-level transient spectroscopy, scanning photoelectron microscopy, and high-resolution photoemission spectroscopy. The addition of I3- was found to reduce the amounts of hydroxide and Ox in the halide perovskites (HPs), affecting the migration of defects and the structural transformation of the HPs.

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.

Sb(2)Se(3) -sensitized inorganic-organic heterojunction solar cells fabricated using a single-source precursor.

The photovoltaic performance of Sb2 Se3 -sensitized heterojunction solar cells, which were fabricated by a simple deposition of Sb2 Se3 on mesoporous TiO2 by an approach that features multiple cycles of spin coating with a single-source precursor solution and thermal decomposition, is reported. Poly[2,6-(4,4-bis(2-ethylhexyl)-4H-cyclopenta[2,1-b;3,4-b']dithiophene)-alt-4,7(2,1,3-benzothioadiazole)] was used as the hole-transporting material. The most efficient cell exhibited a short-circuit current density of 22.3 mA cm(-2) , an open-circuit voltage of 304.5 mV, and a fill factor of 47.2 %, yielding a power conversion efficiency of 3.21 % under standard test conditions (irradiation of 1000 W m(-2) , air mass=1.5 G). The results of this study imply that the developed approach has a high potential as a simple and effective route for the fabrication of efficient and inexpensive solar cells.

Understanding how excess lead iodide precursor improves halide perovskite solar cell performance.

The presence of excess lead iodide in halide perovskites has been key for surpassing 20% photon-to-power conversion efficiency. To achieve even higher power conversion efficiencies, it is important to understand the role of remnant lead iodide in these perovskites. To that end, we explored the mechanism facilitating this effect by identifying the impact of excess lead iodide within the perovskite film on charge diffusion length, using electron-beam-induced current measurements, and on film formation properties, from grazing-incidence wide-angle X-ray scattering and high-resolution transmission electron microscopy. Based on our results, we propose that excess lead iodide in the perovskite precursors can reduce the halide vacancy concentration and lead to formation of azimuthal angle-oriented cubic α-perovskite crystals in-between 0° and 90°. We further identify a higher perovskite carrier concentration inside the nanostructured titanium dioxide layer than in the capping layer. These effects are consistent with enhanced lead iodide-rich perovskite solar cell performance and illustrate the role of lead iodide.

Spatial Distribution of Lead Iodide and Local Passivation on Organo-Lead Halide Perovskite.

We identify nanoscale spatial distribution of PbI2 on the (FAPbI3)0.85(MAPbBr3)0.15 perovskite thin film and investigate the local passivation effect using confocal based optical microscopy of steady state and time-resolved photoluminescence (PL). Different from a typical scanning electron microscope (SEM) morphology study, confocal based PL spectroscopy and microscopy allow researchers to map the morphologies of both perovskite and PbI2 grains simultaneously, by selectively detecting their characteristic fluorescent bands using band-pass filters. In this work, we compare the perovskite samples without and with excess PbI2 incorporation and unambiguously reveal PbI2 distribution for the PbI2-rich sample. In addition, using the nanoscale time-resolved PL technique we show that the PbI2-rich regions exhibit longer lifetime due to suppressed defect trapping, compared to the PbI2-poor regions. The measurement on the PbI2-rich sample indicates that the passivation effect of PbI2 in perovskite film is effective, especially in localized regions. Hence, this finding is important for further improvement of the solar cells by considering the strategy of excess PbI2 incorporation.

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

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.

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

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.

Tailoring of Electron-Collecting Oxide Nanoparticulate Layer for Flexible Perovskite Solar Cells.

Low-temperature-processed perovskite solar cells (PSCs), especially those fabricated on flexible substrates, exhibit device performance that is worse than that of high-temperature-processed PSCs. One of the main reasons for the inferior performance of low-temperature-processed PSCs is the loss of photogenerated electrons in the electron collection layer (ECL) or related interfaces, i.e., indium tin oxide/ECL and ECL/perovskite. Here, we report that tailoring of the energy level and electron transporting ability in oxide ECLs using Zn2SnO4 nanoparticles and quantum dots notably minimizes the loss of photogenerated electrons in the low-temperature-fabricated flexible PSC. The proposed ECL with methylammonium lead halide [MAPb(I0.9Br0.1)3] leads to fabrication of significantly improved flexible PSCs with steady-state power conversion efficiency of 16.0% under AM 1.5G illumination of 100 mW cm(-2) intensity. These results provide an effective method for fabricating high-performance, low-temperature solution-processed flexible PSCs.

Thermal Stability of CuSCN Hole Conductor-Based Perovskite Solar Cells.

Although perovskite solar cells (PSCs) surpassing 20 % in certified power conversion efficiency (PCE) have been demonstrated with organic hole-transporting layers (HTLs), thermal degradation remains one of the key issues for practical applications. We fabricated PSCs using low temperature solution-processed CuSCN as the inorganic hole-transport layer (HTL), which possesses a highly stable crystalline structure and is robust even at high temperatures. The best-performing cell delivers a PCE of 18.0 %, with 15.9 % measured at the stabilized power output. Here we report the thermal stability of PSCs based on CuSCN in comparison with commonly used 2,2',7,7'-tetrakis-(N,N-di-4-methoxyphenylamino)-9,9'-spirobifluorene (spiro-OMeTAD). The PSC fabricated with organic spiro-OMeTAD degrades to 25 % of initial PCE after annealing for 2 h at 125 °C in air under 40 % average relative humidity. However, CuSCN-based PSCs maintain approximately 60 % of the initial value, exhibiting superior thermal stability under identical conditions. This work demonstrates that high efficiency and improved thermal stability are simultaneously achieved when CuSCN is used as an HTL in PSCs.

SOLAR CELLS. High-performance photovoltaic perovskite layers fabricated through intramolecular exchange.

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%.

High-performance flexible perovskite solar cells exploiting Zn2SnO4 prepared in solution below 100 °C.

Fabricating inorganic-organic hybrid perovskite solar cells (PSCs) on plastic substrates broadens their scope for implementation in real systems by imparting portability, conformability and allowing high-throughput production, which is necessary for lowering costs. Here we report a new route to prepare highly dispersed Zn2SnO4 (ZSO) nanoparticles at low-temperature (<100 °C) for the development of high-performance flexible PSCs. The introduction of the ZSO film significantly improves transmittance of flexible polyethylene naphthalate/indium-doped tin oxide (PEN/ITO)-coated substrate from ∼75 to ∼90% over the entire range of wavelengths. The best performing flexible PSC, based on the ZSO and CH3NH3PbI3 layer, exhibits steady-state power conversion efficiency (PCE) of 14.85% under AM 1.5G 100 mW·cm(-2) illumination. This renders ZSO a promising candidate as electron-conducting electrode for the highly efficient flexible PSC applications.