SCALABLE COATING OF HYBRID PEROVSKITE FOR HIGH EFFICIENCY SOLAR MODULES

Solar cells have experienced a rapid performance enhancement and price reduction in recent years, thanks to the technology innovation and governments’ incentives. However, the growth of solar cell installation annually is still slow and it only accounts for 1~2% of electricity generation globally. The slow processing and high capital cost limit the rapid expansion of solar cell market based on current technologies. Solution processable perovskite solar cells developed in the most recent decade hold the premise of low cost and rapid fabrication. Its efficiency increases dramatically from 3% in 2009 to 23.7% in 2018, being the record for all kinds of thin film solar cells. However, the high performance is obtained from tiny sized devices ( 10 cm2) could go beyond 17.0% with efficiency loss from increased series resistance of larger sized transparent conductive electrode, being at the same level as commercialized silicon solar modules. In this dissertation, studies are focused on blade coating of perovskite films. Blade coating is one kind scalable coating method. It is compatible with other scalable coating process such as slot die coating, gravure coating, but it also has the advantages of simple set-up and freely tunable coating parameters (speed, temperature, thickness, etc.). Therefore, it is very suitable for preliminary study of perovskite scalable coating.Doctor of Philosoph

Fast Growth of Thin MAPbI\u3csub\u3e3\u3c/sub\u3e Crystal Wafers on Aqueous Solution Surface for Efficient Lateral-Structure Perovskite Solar Cells

Solar-grade single or multiple crystalline wafers are needed in large quantities in the solar cell industry, and are generally formed by a top-down process from crystal ingots, which causes a significant waste of materials and energy during slicing, polishing, and other processing. Here, a bottom-up technique that allows the growth of wafer-size hybrid perovskite multiple crystals directly from aqueous solution is reported. Single-crystalline hybrid perovskite wafers with centimeter size are grown at the top surface of a perovskite precursor solution. As well as saving raw materials, this method provides unprecedented advantages such as easily tunable thickness and rapid growth of the crystals. These crystalline wafers show high crystallinity, broader light absorption, and a long carrier recombination lifetime, comparable with those of bulk single crystals. Lateral-structure perovskite solar cells made of these crystals demonstrate a record power conversion efficiency of 5.9%. Includes supplementary materials

Low Temperature Solution-Processed Sb:SnO\u3csub\u3e2\u3c/sub\u3e Nanocrystals for Efficient Planar Perovskite Solar Cells

Inorganic metal oxide electron-transport layers (ETLs) have the potential to yield perovskite solar cells with improved stability, but generally need high temperature to form conductive and defect-less forms, which is not compatible with the fabrication of flexible and tandem solar cells. Here, we demonstrate a facile strategy for developing efficient inorganic ETLs by doping SnO2 nanocrystals (NCs) with a small amount of Sb using a low-temperature solution-processed method. The electrical conductivity was remarkably enhanced by Sb-doping, which increased the carrier concentration in Sb:SnO2 NCs. Moreover, the upward shift of the Fermi level owing to doping results in improved energy level alignment, which led to reduced charge recombination, and thus longer electron recombination lifetime and improved open-circuit voltage (VOC). Therefore, Sb-doping of SnO2 significantly enhanced the photovoltaic performance of planar perovskite devices by increasing the fill factor and VOC, and reducing photocurrent hysteresis, extending the potential application of low-temperature-processed ETLs in future flexible and tandem solar cells

Strained hybrid perovskite thin films and their impact on the intrinsic stability of perovskite solar cells

Organic-inorganic hybrid perovskite (OIHP) solar cells have achieved comparable efficiencies to those of commercial solar cells, although their instability hinders their commercialization. Although encapsulation techniques have been developed to protect OIHP solar cells from external stimuli such as moisture, oxygen, and ultraviolet light, understanding of the origin of the intrinsic instability of perovskite films is needed to improve their stability. We show that the OIHP films fabricated by existing methods are strained and that strain is caused by mismatched thermal expansion of perovskite films and substrates during the thermal annealing process. The polycrystalline films have compressive strain in the out-of-plane direction and in-plane tensile strain. The strain accelerates degradation of perovskite films under illumination, which can be explained by increased ion migration in strained OIHP films. This study points out an avenue to enhance the intrinsic stability of perovskite films and solar cells by reducing residual strain in perovskite films

Strained hybrid perovskite thin films and their impact on the intrinsic stability of perovskite solar cells

Organic-inorganic hybrid perovskite (OIHP) solar cells have achieved comparable efficiencies to those of commercial solar cells, although their instability hinders their commercialization. Although encapsulation techniques have been developed to protect OIHP solar cells from external stimuli such as moisture, oxygen, and ultraviolet light, understanding of the origin of the intrinsic instability of perovskite films is needed to improve their stability. We show that the OIHP films fabricated by existing methods are strained and that strain is caused by mismatched thermal expansion of perovskite films and substrates during the thermal annealing process. The polycrystalline films have compressive strain in the out-of-plane direction and in-plane tensile strain. The strain accelerates degradation of perovskite films under illumination, which can be explained by increased ion migration in strained OIHP films. This study points out an avenue to enhance the intrinsic stability of perovskite films and solar cells by reducing residual strain in perovskite films

Strained hybrid perovskite thin films and their impact on the intrinsic stability of perovskite solar cells

Organic-inorganic hybrid perovskite (OIHP) solar cells have achieved comparable efficiencies to those of commercial solar cells, although their instability hinders their commercialization. Although encapsulation techniques have been developed to protect OIHP solar cells from external stimuli such as moisture, oxygen, and ultraviolet light, understanding of the origin of the intrinsic instability of perovskite films is needed to improve their stability. We show that the OIHP films fabricated by existing methods are strained and that strain is caused by mismatched thermal expansion of perovskite films and substrates during the thermal annealing process. The polycrystalline films have compressive strain in the out-of-plane direction and in-plane tensile strain. The strain accelerates degradation of perovskite films under illumination, which can be explained by increased ion migration in strained OIHP films. This study points out an avenue to enhance the intrinsic stability of perovskite films and solar cells by reducing residual strain in perovskite films

Enhancing stability and efficiency of perovskite solar cells with crosslinkable silane-functionalized and doped fullerene

The instability of hybrid perovskite materials due to water and moisture arises as one major challenge to be addressed before any practical application of the demonstrated high efficiency perovskite solar cells. Here we report a facile strategy that can simultaneously enhance the stability and efficiency of p–i–n planar heterojunction-structure perovskite devices. Crosslinkable silane molecules with hydrophobic functional groups are bonded onto fullerene to make the fullerene layer highly water-resistant. Methylammonium iodide is introduced in the fullerene layer for n-doping via anion-induced electron transfer, resulting in dramatically increased conductivity over 100-fold. With crosslinkable silane-functionalized and doped fullerene electron transport layer, the perovskite devices deliver an efficiency of 19.5% with a high fill factor of 80.6%. A crosslinked silane-modified fullerene layer also enhances the water and moisture stability of the non-sealed perovskite devices by retaining nearly 90% of their original efficiencies after 30 days’ exposure in an ambient environment

Excess charge-carrier induced instability of hybrid perovskites

Identifying the origin of intrinsic instability for organic–inorganic halide perovskites (OIHPs) is crucial for their application in electronic devices, including solar cells, photodetectors, radiation detectors, and light-emitting diodes, as their efficiencies or sensitivities have already been demonstrated to be competitive with commercial available devices. Here we show that free charges in OIHPs, whether generated by incident light or by current-injection from electrodes, can reduce their stability, while efficient charge extraction effectively stabilizes the perovskite materials. The excess of both holes and electrons reduce the activation energy for ion migration within OIHPs, accelerating the degradation of OIHPs, while the excess holes and electrons facilitate the migration of cations or anions, respectively. OIHP solar cells capable of efficient charge-carrier extraction show improved light stability under regular operation conditions compared to an open-circuit condition where the photo-generated charges are confined in the perovskite layers

Molecular doping enabled scalable blading of efficient hole-transport-layer-free perovskite solar cells

The efficiencies of perovskite solar cells (PSCs) are now reaching such consistently high levels that scalable manufacturing at low cost is becoming critical. However, this remains challenging due to the expensive hole-transporting materials usually employed, and difficulties associated with the scalable deposition of other functional layers. By simplifying the device architecture, hole-transport-layer-free PSCs with improved photovoltaic performance are fabricated via a scalable doctor-blading process. Molecular doping of halide perovskite films improved the conductivity of the films and their electronic contact with the conductive substrate, resulting in a reduced series resistance. It facilitates the extraction of photoexcited holes from perovskite directly to the conductive substrate. The bladed hole-transport-layerfree PSCs showed a stabilized power conversion efficiency above 20.0%. This work represents a significant step towards the scalable, cost-effective manufacturing of PSCs with both high performance and simple fabrication processes

Fast Growth of Thin MAPbI\u3csub\u3e3\u3c/sub\u3e Crystal Wafers on Aqueous Solution Surface for Efficient Lateral-Structure Perovskite Solar Cells

Solar-grade single or multiple crystalline wafers are needed in large quantities in the solar cell industry, and are generally formed by a top-down process from crystal ingots, which causes a significant waste of materials and energy during slicing, polishing, and other processing. Here, a bottom-up technique that allows the growth of wafer-size hybrid perovskite multiple crystals directly from aqueous solution is reported. Single-crystalline hybrid perovskite wafers with centimeter size are grown at the top surface of a perovskite precursor solution. As well as saving raw materials, this method provides unprecedented advantages such as easily tunable thickness and rapid growth of the crystals. These crystalline wafers show high crystallinity, broader light absorption, and a long carrier recombination lifetime, comparable with those of bulk single crystals. Lateral-structure perovskite solar cells made of these crystals demonstrate a record power conversion efficiency of 5.9%. Includes supplementary materials