Advancing perovskite solar cell technologies toward their theoretical power conversion efficiency (PCE) requires delicate control over the carrier dynamics throughout the entire device. By controlling the formation of the perovskite layer and careful choices of other materials, we suppressed carrier recombination in the absorber, facilitated carrier injection into the carrier transport layers, and maintained good carrier extraction at the electrodes. When measured via reverse bias scan, cell PCE is typically boosted to 16.6% on average, with the highest efficiency of ~19.3% in a planar geometry without antireflective coating. The fabrication of our perovskite solar cells was conducted in air and from solution at low temperatures, which should simplify manufacturing of large-area perovskite devices that are inexpensive and perform at high levels.

http://science.sciencemag.org/content/sci/345/6196/542.full.pdf

Interface engineering of highly efficient perovskite solar cells

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%.

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High-performance photovoltaic perovskite layers fabricated through intramolecular exchange

Three-dimensional organic-inorganic perovskites have emerged as one of the most promising thin-film solar cell materials owing to their remarkable photophysical properties, which have led to power conversion efficiencies exceeding 20 per cent, with the prospect of further improvements towards the Shockley-Queisser limit for a single‐junction solar cell (33.5 per cent). Besides efficiency, another critical factor for photovoltaics and other optoelectronic applications is environmental stability and photostability under operating conditions. In contrast to their three-dimensional counterparts, Ruddlesden-Popper phases--layered two-dimensional perovskite films--have shown promising stability, but poor efficiency at only 4.73 per cent. This relatively poor efficiency is attributed to the inhibition of out-of-plane charge transport by the organic cations, which act like insulating spacing layers between the conducting inorganic slabs. Here we overcome this issue in layered perovskites by producing thin films of near-single-crystalline quality, in which the crystallographic planes of the inorganic perovskite component have a strongly preferential out-of-plane alignment with respect to the contacts in planar solar cells to facilitate efficient charge transport. We report a photovoltaic efficiency of 12.52 per cent with no hysteresis, and the devices exhibit greatly improved stability in comparison to their three-dimensional counterparts when subjected to light, humidity and heat stress tests. Unencapsulated two-dimensional perovskite devices retain over 60 per cent of their efficiency for over 2,250 hours under constant, standard (AM1.5G) illumination, and exhibit greater tolerance to 65 per cent relative humidity than do three-dimensional equivalents. When the devices are encapsulated, the layered devices do not show any degradation under constant AM1.5G illumination or humidity. We anticipate that these results will lead to the growth of single-crystalline, solution-processed, layered, hybrid, perovskite thin films, which are essential for high-performance opto-electronic devices with technologically relevant long-term stability.

High-efficiency two-dimensional Ruddlesden–Popper perovskite solar cells

Metal-halide perovskites are crystalline materials originally developed out of scientific curiosity. Unexpectedly, solar cells incorporating these perovskites are rapidly emerging as serious contenders to rival the leading photovoltaic technologies. Power conversion efficiencies have jumped from 3% to over 20% in just four years of academic research. Here, we review the rapid progress in perovskite solar cells, as well as their promising use in light-emitting devices. In particular, we describe the broad tunability and fabrication methods of these materials, the current understanding of the operation of state-of-the-art solar cells and we highlight the properties that have delivered light-emitting diodes and lasers. We discuss key thermal and operational stability challenges facing perovskites, and give an outlook of future research avenues that might bring perovskite technology to commercialization.

Metal-halide perovskites for photovoltaic and light-emitting devices

Lead halide perovskite solar cells have recently attracted tremendous attention because of their excellent photovoltaic efficiencies. However, the poor stability of both the perovskite material and the charge transport layers has so far prevented the fabrication of devices that can withstand sustained operation under normal conditions. Here, we report a solution-processed lead halide perovskite solar cell that has p-type NiOx and n-type ZnO nanoparticles as hole and electron transport layers, respectively, and shows improved stability against water and oxygen degradation when compared with devices with organic charge transport layers. Our cells have a p–i–n structure (glass/indium tin oxide/NiOx/perovskite/ZnO/Al), in which the ZnO layer isolates the perovskite and Al layers, thus preventing degradation. After 60 days storage in air at room temperature, our all-metal-oxide devices retain about 90% of their original efficiency, unlike control devices made with organic transport layers, which undergo a complete degradation after just 5 days. The initial power conversion efficiency of our devices is 14.6 ± 1.5%, with an uncertified maximum value of 16.1%. Using metal oxides for both the hole- and electron-transport layers in perovskite solar cells significantly improves their stability compared with devices containing organic transport layers.

Improved air stability of perovskite solar cells via solution-processed metal oxide transport layers

P.-W. Liang, C.-Y. Liao, Dr. C.-C. Chueh, Dr. F. Zuo, S. T. Williams, Dr. X.-K. Xin, Prof. A. K.-Y. Jen Department of Materials Science and Engineering University of Washington Seattle , WA 98195 , USA E-mail: ajen@u.washington.edu Prof. A. K.-Y. Jen Department of Chemistry University of Washington Seattle , WA 98195 , USA C.-Y. Liao, Prof. J. J. Lin Institute of Polymer Science and Engineering National Taiwan University Taipei 106 , Taiwan

Additive Enhanced Crystallization of Solution‐Processed Perovskite for Highly Efficient Planar‐Heterojunction Solar Cells

A comprehensive morphological study was used to elucidate chloride’s role in CH3NH3PbI3–xClx film evolution on a conducting polymer, PEDOT:PSS. Complex ion equilibria and aggregation in solution, as well as the role they play in nucleation, are found to ultimately be responsible for the unique morphological diversity observed in perovskite films grown in the presence of the chloride ion. An intermediate phase that is generated upon deposition and initial annealing templates continued self-assembly in the case of CH3NH3PbI3–xClx. In the absence of chloride, the film growth of CH3NH3PbI3 is directed by substrate interfacial energy. By employing the through-plane TEM analysis, we gain detailed insight into the unique crystallographic textures, grain structures, and elemental distributions across the breadth of films grown from precursor solutions with different chemistries. The lattice coherence seen in morphologies generated under the influence of chloride provides a physical rational for the enhancement in...

Role of Chloride in the Morphological Evolution of Organo-Lead Halide Perovskite Thin Films

A simple, low temperature solution process for Pb/Sn binary-metal perovskite planar-heterojunction solar cells is demonstrated. Sn inclusion substantially influences the band-gap, crystallization kinetics, and thin-film formation leading to a broadened light absorption and enhanced film coverage on ITO/PEDOT:PSS. As a result, the optimized device shows a PCE exceeding 10%, which is the best result for binary-metal perovskite solar cells so far.

Binary‐Metal Perovskites Toward High‐Performance Planar‐Heterojunction Hybrid Solar Cells

Alkyl halide additives have been investigated to elucidate their effects in enhancing perovskite solar cell performance. We found that the additives can participate in the perovskite formation via dissociated halides, suggesting that molecular structure of alkyl halide additives plays multiple roles in modulating the dynamics of perovskite crystal growth.

The roles of alkyl halide additives in enhancing perovskite solar cell performance

DOI: 10.1002/aenm.201400960 red-shift beyond 1000 nm by partially replacing Pb 2+ with Sn 2+ . [ 12,13 ] Notably, the Sn 2+ cation has the tendency to oxidize to Sn 4+ and thus p-dope the perovskite, displaying metal-like conductivity. [ 12a ] However, the PCEs of the Sn-based perovskite solar cells encounter great losses when increasing the fraction of Sn 2+ due to poor perovskite fi lm formation and the instability of Sn 2+ . [ 12–15 ] Currently, successful demonstrations of Pb 2+

Chien-Yi Liao

Papers

Additive Enhanced Crystallization of Solution‐Processed Perovskite for Highly Efficient Planar‐Heterojunction Solar Cells

Role of Chloride in the Morphological Evolution of Organo-Lead Halide Perovskite Thin Films

Binary‐Metal Perovskites Toward High‐Performance Planar‐Heterojunction Hybrid Solar Cells

The roles of alkyl halide additives in enhancing perovskite solar cell performance

High‐Performance Planar‐Heterojunction Solar Cells Based on Ternary Halide Large‐Band‐Gap Perovskites