Efficient perovskite solar cells via improved carrier management.

Metal halide perovskite solar cells (PSCs) are an emerging photovoltaic technology with the potential to disrupt the mature silicon solar cell market. Great improvements in device performance over the past few years, thanks to the development of fabrication protocols1-3, chemical compositions4,5 and phase stabilization methods6-10, have made PSCs one of the most efficient and low-cost solution-processable photovoltaic technologies. However, the light-harvesting performance of these devices is still limited by excessive charge carrier recombination. Despite much effort, the performance of the best-performing PSCs is capped by relatively low fill factors and high open-circuit voltage deficits (the radiative open-circuit voltage limit minus the high open-circuit voltage)11. Improvements in charge carrier management, which is closely tied to the fill factor and the open-circuit voltage, thus provide a path towards increasing the device performance of PSCs, and reaching their theoretical efficiency limit12. Here we report a holistic approach to improving the performance of PSCs through enhanced charge carrier management. First, we develop an electron transport layer with an ideal film coverage, thickness and composition by tuning the chemical bath deposition of tin dioxide (SnO2). Second, we decouple the passivation strategy between the bulk and the interface, leading to improved properties, while minimizing the bandgap penalty. In forward bias, our devices exhibit an electroluminescence external quantum efficiency of up to 17.2 per cent and an electroluminescence energy conversion efficiency of up to 21.6 per cent. As solar cells, they achieve a certified power conversion efficiency of 25.2 per cent, corresponding to 80.5 per cent of the thermodynamic limit of its bandgap.

Efficient, stable and scalable perovskite solar cells using poly(3-hexylthiophene).

Perovskite solar cells typically comprise electron- and hole-transport materials deposited on each side of a perovskite active layer. So far, only two organic hole-transport materials have led to state-of-the-art performance in these solar cells1: poly(triarylamine) (PTAA)2-5 and 2,2',7,7'-tetrakis(N,N-di-p-methoxyphenylamine)-9,9'-spirobifluorene (spiro-OMeTAD)6,7. However, these materials have several drawbacks in terms of commercialization, including high cost8, the need for hygroscopic dopants that trigger degradation of the perovskite layer9 and limitations in their deposition processes10. Poly(3-hexylthiophene) (P3HT) is an alternative hole-transport material with excellent optoelectronic properties11-13, low cost8,14 and ease of fabrication15-18, but so far the efficiencies of perovskite solar cells using P3HT have reached only around 16 per cent19. Here we propose a device architecture for highly efficient perovskite solar cells that use P3HT as a hole-transport material without any dopants. A thin layer of wide-bandgap halide perovskite is formed on top of the narrow-bandgap light-absorbing layer by an in situ reaction of n-hexyl trimethyl ammonium bromide on the perovskite surface. Our device has a certified power conversion efficiency of 22.7 per cent with hysteresis of ±0.51 per cent; exhibits good stability at 85 per cent relative humidity without encapsulation; and upon encapsulation demonstrates long-term operational stability for 1,370 hours under 1-Sun illumination at room temperature, maintaining 95 per cent of the initial efficiency. We extend our platform to large-area modules (24.97 square centimetres)-which are fabricated using a scalable bar-coating method for the deposition of P3HT-and achieve a power conversion efficiency of 16.0 per cent. Realizing the potential of P3HT as a hole-transport material by using a wide-bandgap halide could be a valuable direction for perovskite solar-cell research.

Quantum barriers engineering toward radiative and stable perovskite photovoltaic devices.

Efficient photovoltaic devices must be efficient light emitters to reach the thermodynamic efficiency limit. Here, we present a promising prospect of perovskite photovoltaics as bright emitters by harnessing the significant benefits of photon recycling, which can be practically achieved by suppressing interfacial quenching. We have achieved radiative and stable perovskite photovoltaic devices by the design of a multiple quantum well structure with long (∼3 nm) organic spacers with oleylammonium molecules at perovskite top interfaces. Our L-site exchange process (L: barrier molecule cation) enables the formation of stable interfacial structures with moderate conductivity despite the thick barriers. Compared to popular short (∼1 nm) Ls, our approach results in enhanced radiation efficiency through the recursive process of photon recycling. This leads to the realization of radiative perovskite photovoltaics with both high photovoltaic efficiency (in-lab 26.0%, certified to 25.2%) and electroluminescence quantum efficiency (19.7 % at peak, 17.8% at 1-sun equivalent condition). Furthermore, the stable crystallinity of oleylammonium-based quantum wells enables our devices to maintain high efficiencies for over 1000 h of operation and >2 years of storage.

Metal-Free Phthalocyanine as a Hole Transporting Material and a Surface Passivator for Efficient and Stable Perovskite Solar Cells.

Perovskite solar cells in an n-i-p structure record high power conversion efficiency, but issues of insufficient thermal stability and the high cost of p-type hole transporting materials have been raised as drawbacks. H2 -phthalocyanine (Pc) is introduced as a hole transport material to ensure the thermal stability and simultaneously have served surface passivation effects on hybrid halide perovskites as a Lewis base. Pyrrolic nitrogen in the Pc reacts with uncoordinated Pb2+ ions on the perovskite surface. Upon enhancing the interfacial interaction between phthalocyanine and the perovskite, the open circuit voltage in devices increases as compared to that of devices using a metal-phthalocyanine complex. While the phthalocyanine-applied device maintains superior thermal long-term stability, the power conversion efficiency also exceeds 20%.

Transparent Electrodes with Enhanced Infrared Transmittance for Semitransparent and Four-Terminal Tandem Perovskite Solar Cells.

This report addresses indium oxide doped with titanium and tantulum with high near-infrared transparency to potentially replace the conventional indium tin oxide transparent electrode used in semitransparent perovskite devices and top cells of tandem devices. The high near-infrared transparency of this electrode is possibly explained by the lower carrier concentration, suggesting less defect sites that may sacrifice its optical transparency. Incorporating this transparent electrode into semitransparent perovskite solar cells for both the top and bottom electrodes improved the device performance through possible reduction of interfacial defect sites and modification in energy alignment. With this indium oxide-based semitransparent perovskite top cell, we also demonstrated four-terminal perovskite-silicon tandem configurations with improved photocurrent response in the bottom silicon cell.

Simultaneous Ligand Exchange Fabrication of Flexible Perovskite Solar Cells using Newly Synthesized Uniform Tin Oxide Quantum Dots.

Halide perovskite solar cells (HPSCs) have a significant potential for future photovoltaic systems because of a high power conversion efficiency (PCE) exceeding 23% using solution processing methods. A low-temperature processed oxide layer is a challenging issue for large-scale manufacture of flexible and low-cost HPSCs. Here, we propose a simple reverse micelle-water injection method for highly dispersed ligand-capped ultrafine SnO2 quantum dots (QD). Interestingly, we observed that the ligands, which help in the formation of a uniform SnO2 QD thin film, spontaneously exchange for halide through a perovskite solution, and finally we form a suitable SnO2 QD-halide junction for high-performance HPSCs. The flexible HPSC with the SnO2 QD-halide junction formed via the ligand exchange exhibits a high PCE of 17.7% using a flexible substrate. It also shows an excellent flexibility, where the initial PCE is maintained within 92% after 1000 bending cycles with a bending radius of 18 mm.