Organic and inorganic hybrid perovskites (e.g., CH(3)NH(3)PbI(3)), with advantages of facile processing, tunable bandgaps, and superior charge-transfer properties, have emerged as a new class of revolutionary optoelectronic semiconductors promising for various applications. Perovskite solar cells constructed with a variety of configurations have demonstrated unprecedented progress in efficiency, reaching about 20% from multiple groups after only several years of active research. A key to this success is the development of various solution-synthesis and film-deposition techniques for controlling the morphology and composition of hybrid perovskites. The rapid progress in material synthesis and device fabrication has also promoted the development of other optoelectronic applications including light-emitting diodes, photodetectors, and transistors. Both experimental and theoretical investigations on organic-inorganic hybrid perovskites have enabled some critical fundamental understandings of this material system. Recent studies have also demonstrated progress in addressing the potential stability issue, which has been identified as a main challenge for future research on halide perovskites. Here, we review recent progress on hybrid perovskites including basic chemical and crystal structures, chemical synthesis of bulk/nanocrystals and thin films with their chemical and physical properties, device configurations, operation principles for various optoelectronic applications (with a focus on solar cells), and photophysics of charge-carrier dynamics. We also discuss the importance of further understanding of the fundamental properties of hybrid perovskites, especially those related to chemical and structural stabilities.

Organic–inorganic hybrid lead halide perovskites for optoelectronic and electronic applications

BACKGROUND Perovskite solar cells (PSCs) have attracted intensive attention because of their ever-increasing power conversion effi­ciency (PCE), low-cost materials constituents, and simple solution fabrication process. Initi­ated in 2009 with an efficiency of 3.8%, PSCs have now achieved a lab-scale power conversion efficiency of 23.3%, rivaling the performance of commercial multicrystalline silicon solar cells, as well as copper indium gallium selenide (CIGS) and cadmium telluride (CdTe) thin-film solar cells. Thousands of articles re­lated to PSCs have been published each year since 2015, highlighting PSCs as a topic of in­tense interest in photovoltaics (PV) research. With high efficiencies achieved in lab devices, stability and remaining challenges in upscal­ing the manufacture of PSCs are two critical concerns that must be addressed on the path to PSC commercialization. ADVANCES We review recent progress in PSCs and discuss the remaining challenges along the pathway to their commercialization. Device configurations of PSCs (see the figure) include mesoscopic formal (n-i-p) and inverted (p-i-n) structures, planar formal and inverted struc­tures, and the printable triple mesoscopic structures. PCEs of devices that use these structures have advanced rapidly in the case of small-area devices (~0.1 cm 2 ). PSCs are also attracting attention as top cells for the construction of tandem solar cells with existing mature PV technologies to increase efficiency beyond the Shockley-Queisser limit of single-junction devices. The stability of PSCs has attracted much well-deserved attention of late, and notable progress has been made in the past few years. PSCs have recently achieved exhibited life­times of 10,000 hours under 1 sun (1 kW/m 2 ) illumina­tion with an ultraviolet filter at a stabilized temperature of 55°C and at short-circuit conditions for a printable triple mesoscopic PSCs. This irradiation is equivalent to the total irradiation of 10 years of outdoor use in most of Europe. However, within the PSC community, standard testing protocols require further development. In addition, transpar­ency in reporting standards on stability tests needs to be improved; this can be achieved by providing both initial photovoltaic performance and normalization parameters. The upscaling of PSCs has also progressed steadily, leading to PSC mini-modules, standard-sized modules, and power systems. PV companies have set out to manufacture large-area PSC modules (see the figure), and a 110-m 2 perovskite PV system with screen-printed triple mesoscopic PSC modules was recently debuted. Studies of these increased-area modules and systems will promote the development of PSCs toward commercializa­tion. PSC research is expanding to cover fundamental topics on materials and lab-sized cells, as well as to address issues of in­dustrial-scale manufacturing and deployment. OUTLOOK The PV market has been continu­ously expanding in recent years, bringing op­portunities for new PV technologies of which PSCs are promising candidates. It is impera­tive to achieve a low cost per watt, which means that both efficiency and lifetime need improve­ment relative to current parameters. The efficiency gap between lab cells and industrial modules has seen impressive reduc­tions in crystalline silicon; PSCs must simi­larly enlarge module areas to the panel level and need to achieve lifetimes comparable to those of legacy PV technologies. Other improvements will need to include industry-scale electronic-grade films, recycling methods to address concerns regarding lead toxicity, and the adoption of standardized testing protocols to predict the operation lifetime of PSCs. Modules will need to endure light-induced degradation, potential-induced degradation, partial-shade stress, and mechanical shock. The field can benefit from lessons learned during the development of mature PV technologies as it strives to de­fine, and overcome, the hurdles to PSC com­mercial impact.

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Challenges for commercializing perovskite solar cells.

There are only few semiconducting materials that have been shaping the progress of third generation photovoltaic cells as much as perovskites. Although they are deceivingly simple in structure, the archetypal AMX3-type perovskites have built-in potential for complex and surprising discoveries. Since 2009, a small and somewhat exotic class of perovskites, which are quite different from the common rock-solid oxide perovskite, have turned over a new leaf in solar cell research. Highlighted as one of the major scientific breakthroughs of the year 2013, the power conversion efficiency of the title compound hybrid organic–inorganic perovskite has now exceeded 18%, making it competitive with thin-film PV technology. In this minireview, a brief history of perovskite materials for photovoltaic applications is reported, the current state-of-the-art is distilled and the basic working mechanisms have been discussed. By analyzing the attainable photocurrent and photovoltage, realizing perovskite solar cells with 20% efficiency for a single junction, and 30% for a tandem configuration on a c-Si solar cell would be realistic.

Organohalide lead perovskites for photovoltaic applications

In the past few years, organic-inorganic halide perovskites have rapidly emerged as promising materials for photovoltaic applications, but simultaneously achieving high performance and long-term stability has proved challenging. Here, we show a one-step solution-processing strategy using phosphonic acid ammonium additives that results in efficient perovskite solar cells with enhanced stability. We modify the surface of methylammonium lead triiodide (CH3NH3PbI3) perovskite by spin-coating its precursor solution in the presence of butylphosphonic acid 4-ammonium chloride. Morphological, structural and elemental analyses show that the phosphonic acid ammonium additive acts as a crosslink between neighbouring grains in the perovskite structure, through strong hydrogen bonding of the -PO(OH)2 and -NH3(+) terminal groups to the perovskite surface. The additives facilitate the incorporation of the perovskite within a mesoporous TiO2 scaffold, as well as the growth of a uniform perovskite layer at the surface, enhancing the material's photovoltaic performance from 8.8 to 16.7% as well as its resistance to moisture.

Improved performance and stability of perovskite solar cells by crystal crosslinking with alkylphosphonic acid ω-ammonium chlorides.

This review article examines the current state of understanding in how metal halide perovskite solar cells can degrade when exposed to moisture, oxygen, heat, light, mechanical stress, and reverse bias. It also highlights strategies for improving stability, such as tuning the composition of the perovskite, introducing hydrophobic coatings, replacing metal electrodes with carbon or transparent conducting oxides, and packaging. The article concludes with recommendations on how accelerated testing should be performed to rapidly develop solar cells that are both extraordinarily efficient and stable.

Understanding Degradation Mechanisms and Improving Stability of Perovskite Photovoltaics.

By the introduction of an organic silane self-assembled monolayer, an interface-engineering approach is demonstrated for hole-conductor-free, fully printable mesoscopic perovskite solar cells based on a carbon counter electrode. The self-assembled silane monolayer is incorporated between the TiO2 and CH3NH3PbI3, resulting in optimized interface band alignments and enhanced charge lifetime. The average power conversion efficiency is improved from 9.6% to 11.7%, with a highest efficiency of 12.7%, for this low-cost perovskite solar cell.

Fully Printable Mesoscopic Perovskite Solar Cells with Organic Silane Self-Assembled Monolayer

Hole-Conductor-Free Fully Printable Mesoscopic Solar Cell with Mixed-Anion Perovskite CH3NH3PbI(3−x)(BF4)x

Solvent effect on the hole-conductor-free fully printable perovskite solar cells

An alcohol-dispersed conducting polymer complex for fully printable organic solar cells with improved stability

The control of film morphology is crucial in achieving high-performance perovskite solar cells (PSCs). Herein, the crystals of the perovskite films are reconstructed by post-treating the MAPbI3 devices with methylamine gas, yielding a homogeneous nucleation and crystallization of the perovskite in the triple mesoscopic inorganic layers structured PSCs. As a result, a uniform, compact, and crystalline perovskite layer is obtained after the methylamine gas post-treatment, yielding high power conversion efficiency (PCE) of 15.26%, 128.8% higher than that of the device before processing. More importantly, this post-treatment process allows the regeneration of the photodegraded PSCs via the crystal reconstruction and the PCE can recover to 91% of the initial value after two cycles of the photodegradation-recovery process. This simple method allows for the regeneration of perovskite solar cells on site without reconstruction or replacing any components, thus prolonging the service life of the perovskite solar cells and distinguishing from any other photovoltaic devices in practice.

Pei Jiang

Papers

Fully Printable Mesoscopic Perovskite Solar Cells with Organic Silane Self-Assembled Monolayer

Hole-Conductor-Free Fully Printable Mesoscopic Solar Cell with Mixed-Anion Perovskite CH3NH3PbI(3−x)(BF4)x

Solvent effect on the hole-conductor-free fully printable perovskite solar cells

An alcohol-dispersed conducting polymer complex for fully printable organic solar cells with improved stability

Improvement and Regeneration of Perovskite Solar Cells via Methylamine Gas Post-Treatment