Key progresses of MOE Key Laboratory of Macromolecular Synthesis and Functionalization in 2020

In just over a decade, the power conversion efficiency of metal‐halide perovskite solar cells has increased from 3.9% to 25.5%, suggesting this technology might be ready for large‐scale exploitation in industrial applications. Photovoltaic devices based on perovskite single crystals are emerging as a viable alternative to polycrystalline materials. Perovskite single crystals indeed possess lower trap state densities, higher carrier mobilities, and longer diffusion lengths, and potentially can achieve higher performance with respect to those fabricated with polycrystalline films, although their integration in a complete device needs particular attention and the use of specifically tailored growth techniques. In this review, recent advances on single‐crystal halide perovskites are reported. First, crystalline structure and fundamental properties of 3D perovskites are discussed, including the emerging mixed‐anion cation perovskites, and then the most popular growth methods with a focus on techniques that enable the implementation in photovoltaic devices are presented. Architectures and materials used to produce lateral and vertical solar cells are further introduced and recent improvements in device design and fabrication are summarized. Finally, the strategies used to solve the still open challenge on these materials regarding stability under environmental conditions are critically discussed and the view on the opportunities offered by halide perovskites is reflected.

https://onlinelibrary.wiley.com/doi/pdfdirect/10.1002/solr.202101085

Perovskite Single‐Crystal Solar Cells: Advances and Challenges

Flexible, stable, and self-powered photodetectors embedded with chemical vapor deposited lead-free bismuth mixed halide perovskite films

Conventional electronic devices powered by lithium-ion batteries or supercapacitors face the challenge of offering long-term and self-sustaining operations. Self-powered devices based on emerging energy harvesting technologies can help of the development of long-lasting transducers with a small form factor. Organolead halide perovskites due to their excellent electro-optical properties are promising photosensitive materials for the development of such self-powered devices. The following review aims at summarizing recent developments made in the field of organolead halide perovskite based self-powered applications. The underlying mechanism driving the self-powered operation in electronic devices such as photodetectors, tactile sensors, and gas sensors is discussed in detail. Finally, the current challenges and prospects of these perovskite based optoelectronic applications are highlighted.

/pdf/organolead-halide-perovskites-beyond-solar-cells-self-1xyx3liu8c.pdf

Organolead halide perovskites beyond solar cells: self-powered devices and the associated progress and challenges

Assembling perovskites into heterojunctions is an effective approach to achieve high‐performance photodetectors. Compared with vertical heterojunctions, in lateral heterojunction‐based photodetectors, the reflection loss is reduced because the active layer is in direct contact with light resulting in higher performance and better stability. However, lateral perovskite–perovskite heterojunctions are difficult to achieve using solution methods because the first formed film is easily dissolved by the solvent of the second precursor. In this study, a two‐step imprinting method is developed to fabricate lateral MAPbI3–MAPbBr3 microwire heterojunctions and realize a high‐performance photodetector with a responsivity and detectivity of 1207 A W−1 and 2.78 × 1013 Jones, respectively. At 0 V bias, the device exhibits a responsivity of up to 233 A W−1, which is more than double the previously reported best results. The high‐quality heterojunction endows the photodetectors with ultra‐high polarization sensitivity (Imax/Imin = 8.2) and long‐term stability, retaining 88.2% of its initial performance even after being exposed to air for 391 d.

Self‐Powered and Flexible Photodetector with High Polarization Sensitivity Based on MAPbBr3–MAPbI3 Microwire Lateral Heterojunction

The rigid and brittle nature of methylammonium lead iodide (MAPbI3) polycrystalline films limits their application in stretchable devices due to rapid deterioration in performance on cycling. By incorporation of polymer chains in the MAPbI3 films, a strategy to alter the mechanical modulus and the viscoelastic nature of the films has been developed. Combining this with flexible nanochain electrodes, highly stretchable and stable perovskite devices have been fabricated. The resultant polymer-MAPbI3 photodetector exhibits ultralow dark currents (∼10-11 A) and high light switching ratios (∼103) and maintains 75% of performance after 30 days. The viscoelastic nature and lower modulus of the polymer improve the energy dissipation in the polymer-MAPbI3 devices; as a result, they maintain 52% of the device performance after 10000 stretching cycles at 50% strain. The difference in the mechanical behavior is clearly observed in the failure mode of the two films. While rapid catastrophic cracking is observed in MAPbI3 films, the intensity and size of such crack formation are highly limited in polymer-MAPbI3 films, which prevent their failure.

Soft Polymer-Organolead Halide Perovskite Films for Highly Stretchable and Durable Photodetectors with Pt-Au Nanochain-Based Electrodes.

The integration of polymer chains with organolead halide perovskite (MAPbI3) films, leading to enhanced stability and electro-optical performance, is critically affected by the molecular weight of chains. The molecular weight determines the mobility and volume of the chains, which affects the crystallization kinetics and, hence, perovskite grain size. The insulating nature of the chains is another critical factor that affects both ion migration and conduction of electronic charge. The combined effect of these factors leads to optimal performance with the use of medium-length chains. A simple model integrating the two effects accurately fits the response of the polymer-perovskite composite. Further characterization results show that the polymer-perovskite films have a three-layer architecture consisting of nanoscale polymer-rich top and bottom layers. These combined results show that the optimization of performance in polymer-perovskite devices depends critically on the size of the chains due to their multiple effects on the perovskite matrix.

Nanoscale Architecture of Polymer-Organolead Halide Perovskite Films and the Effect of Polymer Chain Mobility on Device Performance.

A commodity-scale polymer is used for controlling the nucleation and growth of single crystals of organolead halide perovskite. The polymer [polystyrene (PS)] cross-links and strongly interacts with PbI2 and MAI (MAPbI3 perovskite precursors) resulting in the control of the crystallization process. The PS concentration modulates the nucleation time, crystal size, and the number of perovskite single crystals. In addition, the PS-based MAPbI3 crystals show an enhanced performance as well as improved thermal and environmental stability. Specifically, the PS-MAPbI3 crystals show 3 times higher photocurrent than plain MAPbI3 crystals and maintain a stable structure for more than 50 days (1200 h) under continuous 0.1 sun illumination in the air with a relative humidity of 40-45%. The improved performance and stability are attributed to the direct interaction between the PS and perovskite, which greatly reduces the ion migration, defect traps, and charge recombination and improves the carrier mobility and lifetime.

Polymer-Controlled Growth and Wrapping of Perovskite Single Crystals Leading to Better Device Stability and Performance.

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Organolead halide perovskites beyond solar cells: self-powered devices and the associated progress and challenges

Soft Polymer-Organolead Halide Perovskite Films for Highly Stretchable and Durable Photodetectors with Pt-Au Nanochain-Based Electrodes.

Nanoscale Architecture of Polymer-Organolead Halide Perovskite Films and the Effect of Polymer Chain Mobility on Device Performance.

Polymer-Controlled Growth and Wrapping of Perovskite Single Crystals Leading to Better Device Stability and Performance.