High‐Performance,Transparent, Dye‐Sensitized Solar Cells for See‐Through Photovoltaic Windows

Dye‐sensitized solar cells (DSCs) have attracted great interest as one of the most promising photovoltaic technologies, and transparent DSCs show potential applications as photovoltaic windows. However, the competition between light absorption for photocurrent generation and light transmittance for obtaining high transparency limits the performance of transparent DSCs. Here, transparent DSCs exhibiting a high light transmittance of 60.3% and high energy conversion efficiency (3.66%) are reported. The strategy is to create a cocktail system composed of ultraviolet and near‐infrared dye sensitizers that selectively and efficiently harvest light in the invisible or low‐eye‐sensitivity region while transmitting light in high‐eye‐sensitivity regions. This new design provides a reasonable approach for realizing high efficiency and transparency DSCs that have potential applications as photovoltaic windows.     

Fully Solution‐Processed TCO‐Free Semitransparent Perovskite Solar Cells for Tandem and Flexible Applications

Semitransparent perovskite solar cells (st‐PSCs) have received remarkable interest in recent years because of their great potential in applications for solar window, tandem solar cells, and flexible photovoltaics. However, all reported st‐PSCs require expensive transparent conducting oxides (TCOs) or metal‐based thin films made by vacuum deposition, which is not cost effective for large‐scale fabrication: the cost of TCOs is estimated to occupy ≈75% of the manufacturing cost of PSCs. To address this critical challenge, this study reports a low‐temperature and vacuum‐free strategy for the fabrication of highly efficient TCO‐free st‐PSCs. The TCO‐free st‐PSC on glass exhibits 13.9% power conversion efficiency (PCE), and the four‐terminal tandem cell made with the st‐PSC top cell and c‐Si bottom cell shows an overall PCE of 19.2%. Due to the low processing temperature, the fabrication of flexible st‐PSCs is demonstrated on polyethylene terephthalate and polyimide, which show excellent stability under repeated bending or even crumbing.     

Constructing High‐Performance Organic Photovoltaics via Emerging Non‐Fullerene Acceptors and Tandem‐Junction Structure

In consideration of the unique advantages of new non‐fullerene acceptors and the tandem‐junction structure, organic photovoltaics (OPVs) based on them are very promising. Studies related to this emerging area began in 2016 with achieved power conversion efficiencies (PCEs) of 8–10%, which have now been boosted to 17%. In this essay, the construction of high‐performance OPVs is discussed, with a focus on combining the advantages of new non‐fullerene acceptors and the tandem‐junction structure. In order to achieve higher PCEs, methods to enable high short‐circuit current density, open‐circuit voltage, and fill factor are discussed. In addition, the stability and reproducibility of high‐efficiency OPVs are also addressed. Herein, it is forecast that the new non‐fullerene acceptors‐based tandem‐junction OPVs will become the next big wave in the field and achieve high PCEs over 20% in the near future. Some promising research directions on this emerging hot topic are proposed which may further push the field into the 25% high efficiency era and considerably advance the technology beyond laboratory research.     

The Role of Antireflective Coating CYTOP,Immersion Oil,and Sensitizer Selection in Fabricating a 2.3 V, 10% Power Conversion Efficiency SSM‐DSC Device

Sequential series multijunction dye‐sensitized solar cells (SSM‐DSCs) can power solar‐to‐fuel processes with a single illuminated area device. Dye selection and strategies limiting photon losses are critical in SSM‐DSC devices for higher performance systems. Herein, an efficient and readily applicable spin coating protocol on glass surfaces with an antireflective fluoropolymer (CYTOP) is applied to an SSM‐DSC architecture. Combining CYTOP with the use of an immersion oil between glass spacers in a three subcell SSM‐DSC with judiciously selected TiO₂ photoanode sensitizers and thicknesses, an overall power conversion efficiency (PCE) of 10.1% is obtained with an output of 2.3 V. Without external bias, this SSM‐DSC configuration shows an impressive overall solar‐to‐fuel conversion efficiency of 6% when powering IrO₂ and Au₂O₃ electrocatalysts for CO₂ and H₂O to CO and H₂ conversion in aqueous solution. The role of CYTOP, immersion oil, sensitizer selection, and film thickness on SSM‐DSC devices is discussed along with the stability of this system.     

High‐Efficiency Polymer Homo‐Tandem Solar Cells with Carbon Quantum‐Dot‐Doped Tunnel Junction Intermediate Layer

The tunnel junction (TJ) intermediate connection layer (ICL), which is the most critical component for high‐efficient tandem solar cell, generally consists of hole conducting layer and polyethyleneimine (PEI) polyelectrolyte. However, because of the nonconducting feature of pristine PEI, photocurrent is open‐restricted in ICL even with a little thick PEI layer. Here, high‐efficiency homo‐tandem solar cells are demonstrated with enhanced efficiency by introducing carbon quantum dot (CQD)‐doped PEI on TJ–ICL. The CQD‐doped PEI provides substantial dynamic advantages in the operation of both single‐junction solar cells and homo‐tandem solar cells. The inclusion of CQDs in the PEI layer leads to improved electron extraction property in single‐junction solar cells and better series connection in tandem solar cells. The highest efficient solar cell with CQD‐doped PEI layer in between indium tin oxide (ITO) and photoactive layer exhibits a maximum power conversion efficiency (PCE) of 9.49%, which represents a value nearly 10% higher than those of solar cells with pristine PEI layer. In the case of tandem solar cells, the highest performing tandem solar cell fabricated with C‐dot‐doped PEI layer in ICL yields a PCE of 12.13%; this value represents an ≈15% increase in the efficiency compared with tandem solar cells with a pristine PEI layer.     

Scaling Up ITO‐Free Solar Cells

Indium‐tin‐oxide‐free (ITO‐free) polymer solar cells with composite electrodes containing current‐collecting grids and a semitransparent poly(3,4‐ethylenedioxythiophene):polystyrenesulfonate) (PEDOT:PSS) conductor are demonstrated. The up‐scaling of the length of the solar cell from 1 to 6 cm and the effect of the grid line resistance are explored for a series of devices. Laser‐beam‐induced current (LBIC) mapping is used for quality control of the devices. A theoretical modeling study is presented that enables the identification of the most rational cell dimension for the grids with different resistances. The performance of ITO‐free organic solar cells with different dimensions and different electrode resistances are evaluated for different light intensities. The current generation and electric potential distribution are found to not be uniformly distributed in large‐area devices at simulated 1 Sun illumination. The generated current uniformity increases with decreasing light intensities.     

Slot‐Die and Roll‐to‐Roll Processed Single Junction Organic Photovoltaic Cells with the Highest Efficiency

The record efficiency of the state‐of‐the‐art polymer solar cells (PSCs) is rapidly increasing, due to the discovery of high‐performance photoactive donor and acceptor materials. However, strong questions remain as to whether such high‐efficiency PSCs can be produced by scalable processes. This paper reports a high power conversion efficiency (PCE) of 13.5% achieved with single‐junction ternary PSCs based on PTB7‐Th, PC₇₁BM, and COi8DFIC fabricated by slot‐die coating, which shows the highest PCE ever reported in PSCs fabricated by a scalable process. To understand the origin of the high performance of the slot‐die coated device, slot‐die coated photoactive films and devices are systematically investigated. These results indicate that the good performance of the slot‐die PSCs can be due to a favorable molecule‐structure and film‐morphology change by introducing 1,8‐diiodooctane and heat treatment, which can lead to improved charge transport with reduced carrier recombination. The optimized condition is then used for the fabrication of large‐area modules and also for roll‐to‐roll fabrication. The slot‐die coated module with 30 cm² active‐area and roll‐to‐roll produced flexible PSC has shown 8.6% and 9.6%, respectively. These efficiencies are the highest in each category and demonstrate the strong potential of the slot‐die coated ternary system for commercial applications.     

Nonaromatic Green‐Solvent‐Processable,Dopant‐Free,and Lead‐Capturable Hole Transport Polymers in Perovskite Solar Cells with High Efficiency

With the recent developments in the efficiency of perovskite solar cells (PSCs), diverse functionalities are necessary for next‐generation charge‐transport layers. Specifically, the hole‐transport layer (HTL) in the various synthesized materials modified with functional groups is explored. A novel donor–acceptor type polymer, alkoxy‐PTEG, composed of benzo[1,2‐b:4,5:b′]dithiophene and tetraethylene glycol (TEG)‐substituted 2,1,3‐benzothiadiazole is reported. The alkoxy‐PTEG exhibits high solubility even in nonaromatic solvents, such as 3‐methylcyclohexanone (3‐MC), and can prevent possible lead leakage via chelation. The optical and electronic properties of alkoxy‐PTEG are thoroughly analyzed. Finally, a dopant‐free alkoxy‐PTEG device processed with 3‐MC exhibits 19.9% efficiency and a device with 2‐methyl anisole, which is a reported aromatic food additive, exhibits 21.2% efficiency in a tin oxide planar structure. The PSC device shows 88% stability after 30 d at ambient conditions (40–50% relative humidity and room temperature). In addition, nuclear magnetic resonance reveals that TEG groups can chelate lead ions with moderate strength (K_binding = 2.76), and this strength is considered to be nondestructive to the perovskite lattice to prevent lead leakage. This is the first report to consider lead leakage and provide solutions to reduce this problem.     

Roll‐to‐Roll Printed Large‐Area All‐Polymer Solar Cells with 5% Efficiency Based on a Low Crystallinity Conjugated Polymer Blend

The challenge of continuous printing in high‐efficiency large‐area organic solar cells is a key limiting factor for their widespread adoption. A materials design concept for achieving large‐area, solution‐coated all‐polymer bulk heterojunction solar cells with stable phase separation morphology between the donor and acceptor is presented. The key concept lies in inhibiting strong crystallization of donor and acceptor polymers, thus forming intermixed, low crystallinity, and mostly amorphous blends. Based on experiments using donors and acceptors with different degree of crystallinity, the results show that microphase separated donor and acceptor domain sizes are inversely proportional to the crystallinity of the conjugated polymers. This methodology of using low crystallinity donors and acceptors has the added benefit of forming a consistent and robust morphology that is insensitive to different processing conditions, allowing one to easily scale up the printing process from a small‐scale solution shearing coater to a large‐scale continuous roll‐to‐roll (R2R) printer. Large‐area all‐polymer solar cells are continuously roll‐to‐roll slot die printed with power conversion efficiencies of 5%, with combined cell area up to 10 cm². This is among the highest efficiencies realized with R2R‐coated active layer organic materials on flexible substrate.     

Ternary Blended Fullerene‐Free Polymer Solar Cells with 16.5% Efficiency Enabled with a Higher‐LUMO‐Level Acceptor to Improve Film Morphology

Ternary approaches to solar cell design utilizing a small bandgap nonfullerene acceptor as the near infrared absorber to increase the short‐circuit current density always decreases the open‐circuit voltage. Herein, a highly efficient polymer solar cell with an impressive efficiency of 16.28 ± 0.20% enabled by an effective voltage‐increased ternary blended fullerene‐free material approach is reported. In this approach, the structural similarity between the host and the higher‐LUMO‐level guest enables the two acceptors to be synergized, obtaining increased open‐circuit voltage and fill factor and a small increase of short‐circuit current density. The same beneficial effects are demonstrated by using two host binary systems. The homogeneous fine film morphologies and the π–π stacking patterns of the host blend are well maintained, while larger donor and acceptor phases and increased lamellar crystallinity, increased charge mobilities, and reduced monomolecular recombination can be achieved upon addition of the guest nonfullerene acceptor. The increased charge mobilities and reduced monomolecular recombination not only contribute to the improved fill factor but also enable the best devices to be fabricated with a relatively thicker ternary blended active layer (110 vs 100 nm). This, combined with the absorption from the added guest acceptor, contribute to the increased short‐circuit current.     

Development of Next‐Generation Organic‐Based Solar Cells: Studies on Dye‐Sensitized and Perovskite Solar Cells

Next‐generation organic solar cells such as dye‐sensitized solar cells (DSSCs) and perovskite solar cells (PSCs) are studied at the National Institute of Advanced Industrial Science and Technology (AIST), and their materials, electronic properties, and fabrication processes are investigated. To enhance the performance of DSSCs, the basic structure of an electron donor, π‐electron linker, and electron acceptor, i.e., D–π–A, is suggested. In addition, special organic dyes containing coumarin, carbazole, and triphenylamine electron donor groups are synthesized to find an effective dye structure that avoids charge recombination at electrode surfaces. Meanwhile, PSCs are manufactured using both a coating method and a laser deposition technique. The results of interfacial studies demonstrate that the level of the conduction band edge (CBE) of a compact TiO₂ layer is shifted after TiCl₄ treatment, which strongly affects the solar cell performance. Furthermore, a special laser deposition system is developed for the fabrication of the perovskite layers of PSCs, which facilitates the control over the deposition rate of methyl ammonium iodide used as their precursor.     

Layer‐by‐Layer Solution‐Processed Low‐Bandgap Polymer‐PC61BM Solar Cells with High Efficiency

Polymer solar cells (PSCs) are fabricated without solvent additives using a low‐bandgap polymer, PBDTTT‐C‐T, as the donor and [6,6]‐phenyl‐C61‐butyric‐acid‐methyl‐ester (PC₆₁BM) as the acceptor. Donor‐acceptor blend and layer‐by‐layer (LL) solution process are used to form active layers. Relative to the blend devices, the LL devices exhibit stronger absorption, better vertical phase separation, higher hole and electron mobilities, and better charge extraction at correct electrodes. As a result, after thermal annealing the LL devices exhibit an average power conversion efficiency (PCE) of 6.86%, which is much higher than that of the blend devices (4.31%). The best PCE of the LL devices is 7.13%, which is the highest reported for LL processed PSCs and among the highest reported for PC₆₁BM‐based single‐junction PSCs.     

Efficient Indium‐Doped TiOx Electron Transport Layers for High‐Performance Perovskite Solar Cells and Perovskite‐Silicon Tandems

In addition to a good perovskite light absorbing layer, the hole and electron transport layers play a crucial role in achieving high‐efficiency perovskite solar cells. Here, a simple, one‐step, solution‐based method is introduced for fabricating high quality indium‐doped titanium oxide electron transport layers. It is shown that indium‐doping improves both the conductivity of the transport layer and the band alignment at the ETL/perovskite interface compared to pure TiO₂, boosting the fill‐factor and voltage of perovskite cells. Using the optimized transport layers, a high steady‐state efficiency of 17.9% for CH₃NH₃PbI₃‐based cells and 19.3% for Cs_0.05(MA_0.17FA_0.83)_0.95Pb(I_0.83Br_0.17)₃‐based cells is demonstrated, corresponding to absolute efficiency gains of 4.4% and 1.2% respectively compared to TiO₂‐based control cells. In addition, a steady‐state efficiency of 16.6% for a semi‐transparent cell is reported and it is used to achieve a four‐terminal perovskite‐silicon tandem cell with a steady‐state efficiency of 24.5%.     

One‐Pot Gram‐Scale,Eco‐Friendly,and Cost‐Effective Synthesis of CuGaS2/ZnS Nanocrystals as Efficient UV‐Harvesting Down‐Converter for Photovoltaics

It is presented for the first time nontoxic CuGaS₂/ZnS quantum dots (QDs) with free‐self‐reabsorption losses and large Stokes shift (>190 nm) synthesized on an industrially gram‐scale as an alternative for Cd‐based energy‐downshift (EDS)‐QD layers. The QDs exhibit a typical EDS that absorbs only UV light (<407 nm) and emits the whole range of visible light (400–800 nm) with a high photoluminescence‐quantum yield of ≈76%. The straightforward application of these EDS‐QDs on the front surface of a monocrystalline p‐type silicon solar cell significantly enhances the short‐circuit current density by ≈1.64 mA cm^?2 (+4.20%); thereby, improving the power‐conversion‐efficiency by ≈4.11%. The significant improvement in the external quantum efficiency increases by ≈35.7% and that in the surface reflectance decreases by ≈14.1% in the UV region (300–450 nm) clearly manifest the photovoltaic enhancement. Such promising results together with the simple (one‐pot core/shell synthesis), cost‐effective (reduction in a bill of material–system by ≈2.62%), and scalable (2000 mL three‐neck flask, 11 g of QDs) preparation process might encourage the manufacturers of solar cells and other optoelectronic applications to apply these EDS‐QDs to different broader eco‐friendly applications.     

Molecular Engineered Hole‐Extraction Materials to Enable Dopant‐Free,Efficient p‐i‐n Perovskite Solar Cells

Two hole‐extraction materials (HEMs), TPP‐OMeTAD and TPP‐SMeTAD, have been developed to facilitate the fabrication of efficient p‐i‐n perovskite solar cells (PVSCs). By replacing the oxygen atom on HEM with sulfur (from TPP‐OMeTAD to TPP‐SMeTAD), it effectively lowers the highest occupied molecular orbital of the molecule and provides stronger Pb? S interaction with perovskites, leading to efficient charge extraction and surface traps passivation. The TPP‐SMeTAD‐based PVSCs exhibit both improved photovoltaic performance and reduced hysteresis in p‐i‐n PVSCs over those based on TPP‐OMeTAD. This work not only provides new insights on creating perovskite‐HEM heterojunction but also helps in designing new HEM to enable efficient organic–inorganic hybrid PVSCs.