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.     

High‐Performance Tandem Organic Solar Cells Using HSolar as the Interconnecting Layer

Tandem structure provides a practical way to realize high efficiency organic photovoltaic cells, it can be used to extend the wavelength coverage for light harvesting. The interconnecting layer (ICL) between subcells plays a critical role in the reproducibility and performance of tandem solar cells, yet the processability of the ICL has been a challenge. In this work the fabrication of highly reproducible and efficient tandem solar cells by employing a commercially available material, PEDOT:PSS HTL Solar (HSolar), as the hole transporting material used for the ICL is reported. Comparing with the conventional PEDOT:PSS Al 4083 (c‐PEDOT), HSolar offers a better wettability on the underlying nonfullerene photoactive layers, resulting in better charge extraction properties of the ICL. When FTAZ:IT‐M and PTB7‐Th:IEICO‐4F are used as the subcells, a power conversion efficiency (PCE) of 14.7% is achieved in the tandem solar cell. To validate the processability of these tandem solar cells, three other research groups have successfully fabricated tandem devices using the same recipe and the highest PCE obtained is 16.1%. With further development of donor polymers and device optimization, the device simulation results show that a PCE > 22% can be realized in tandem cells in the near future.     

Inverted Tandem Polymer Solar Cells with Polyethylenimine‐Modified MoOX/Al2O3:ZnO Nanolaminate as the Charge Recombination Layers

A new charge recombination layer for inverted tandem polymer solar cells is reported. A bilayer of MoO_X/Al₂O₃:ZnO nanolaminate is shown to enable efficient charge recombination in inverted tandem cells. A polymer surface modification on the MoO_X/Al₂O₃:ZnO nanolaminate bilayer increases the work function contrast between the two outward surfaces of the charge recombination layer, further improving the performance of tandem solar cells. An analysis of the electrical, optical, and surface properties of the charge recombination layer is presented. Inverted tandem polymer solar cells, with two photoactive layers comprising poly (3‐hexylthiophene) (P3HT):indene‐C₆₀ bisadduct (IC₆₀BA) for the bottom cell and poly[(4,8‐bis‐(2‐ethylhexyloxy)‐benzo[1,2‐b:4,5‐b']dithiophene)‐2,6‐diyl‐alt‐(4‐(2‐ethylhexanoyl)‐thieno[3,4‐b]thiophene))‐2,6‐diyl] (PBDTTT‐C):[6,6]‐phenyl C₆₁ butyric acid methyl ester (PC₆₀BM) for the top cell, yield an open‐circuit voltage of 1481 mV ± 15 mV, a short‐circuit current density of 7.1 mA cm^?2 ± 0.1 mA cm^?2, and a fill factor of 0.62 ± 0.01, resulting in a power conversion efficiency of 6.5% ± 0.1% under simulated AM 1.5G, 100 mW cm^?2 illumination.     

Spatially and Spectrally Resolved Absorptivity: New Approach for Degradation Studies in Perovskite and Perovskite/Silicon Tandem Solar Cells

Instability in perovskite solar cells is the main challenge for the commercialization of this solar technology. Here, a contactless, nondestructive approach is reported to study degradation across perovskite and perovskite/silicon tandem solar cells. The technique employs spectrally and spatially resolved absorptivity at sub‐bandgap wavelengths of perovskite materials, extracted from their luminescence spectra. Parasitic absorption in other layers, carrier diffusion, and photon smearing phenomena are all demonstrated to have negligible effects on the extracted absorptivity. The absorptivity is demonstrated to reflect real degradation in the perovskite film and is much more robust and sensitive than its luminescence spectral peak position, representing its optical bandgap, and intensity. The technique is applied to study various common factors which induce and accelerate degradation in perovskite solar cells including air and heat exposure and light soaking. Finally, the technique is employed to extract the individual absorptivity component from the perovskite layer in a monolithic perovskite/silicon tandem structure. The results demonstrate the value of this approach for monitoring degradation mechanisms in perovskite and perovskite/silicon tandem cells at early stages of degradation and various fabrication stages.     

High‐Performance Semitransparent Tandem Solar Cell of 8.02% Conversion Efficiency with Solution‐Processed Graphene Mesh and Laminated Ag Nanowire Top Electrodes

A high‐performance semitransparent tandem solar cell that uses solution‐processed graphene mesh and laminated Ag NW as a transparent anode and cathode, respectively, is demonstrated. The laminated top electrode can be deposited without causing any damage to the underneath organic solar cells. Power conversion efficiencies of 8.02% and 6.47% are obtained when the light is projected from the solution‐processed graphene mesh and laminated AgNW, respectively. The performance of the tandem cell is found to be comparable to a tandem solar cell fabricated using commercially available indium tin oxide. These findings offer a high‐performance device and open a new pathway in searching for a potential replacement to the frequently used transparent conducting electrodes.     

A Switchable Interconnecting Layer for High Performance Tandem Organic Solar Cell

The all‐solution‐processed switchable interconnecting layer (ICL) for both inverted and normal tandem organic solar cells (OSCs) is reported for the first time here. The fundamental challenges in the literature arise from mixing multiple functionalities into a single layer. For a widely used ICL composed of an electron transport layer (ETL)/a hole transport layer (HTL), ETL needs not only to efficiently extract electrons from an underneath photoactive layer, but also to fulfill optical, mechanical, chemical and electrical requirements to function as effective tunneling junction ICL with HTL atop. Taking on multiple functionalities for a single ETL makes ETL in ICL highly coupled and difficult to be replaced. This is also the case for HTL. Here, this study demonstrates an all‐solution‐processed switchable ICL, ETL/recombination layer (RL)/HTL and HTL/RL/ETL, for both normal and inverted tandem OSCs. In switchable ICL, ETL and HTL simply serve as carrier transport layers as they did in single OSCs. Electrical recombination, mechanical protection and chemical separation functionalities are realized by RL alone. This strategy shifts the views of ICL for tandem OSCs from conventionally complicated ETL/HTL tunneling junction ICL, where both ETL and HTL play several different roles, towards simplified ICL where ETL and HTL play a distinct decoupled role, advancing ICL for more adaptable tandem OSCs.     

Multifunctional Coatings from Scalable Single Source Precursor Chemistry in Tandem Photoelectrochemical Water Splitting

The straightforward and inexpensive fabrication of stabilized and activated photoelectrodes for application to tandem photoelectrochemical (PEC) water splitting is reported. Semiconductors such as Si, WO₃, and BiVO₄ can be coated with a composite layer formed upon hydrolytic decomposition of hetero­bimetallic single source precursors (SSPs) based on Ti and Ni, or Ti and Co in a simple single‐step process under ambient conditions. The resulting 3d‐transition metal oxide composite films are multifunctional, as they protect the semiconductor electrode from corrosion with an amorphous TiO₂ coating and act as bifunctional electrocatalysts for H₂ and O₂ evolution based on catalytic Ni or Co species. Thus, this approach enables the use of the same precursors for both photoelectrodes in tandem PEC water splitting, and SSP chemistry is thereby established as a highly versatile low‐cost approach to protect and activate photoelectrodes. In an optimized system, SSP coating of a Si photocathode and a BiVO₄ photoanode resulted in a benchmark noble metal‐free dual‐photoelectrode tandem PEC cell for overall solar water splitting with an applied bias solar‐to‐hydrogen conversion efficiency of 0.59% and a half‐life photostability of 5 h.     

Stable and Highly Efficient PbS Quantum Dot Tandem Solar Cells Employing a Rationally Designed Recombination Layer

This study reports the fabrication of stable, high‐performance, simple structured tandem solar cells based on PbS colloidal quantum dots (CQDs) under ambient air. This study also reveals detailed device engineering to deposit each functional layer in the subcells at low temperature to avoid damage to the PbS CQDs and meanwhile makes the fabrication process compatible to flexible plastic substrate. Two efficient recombination layers (RLs) are rationally designed to connect the two subcells in series. The use of solution‐processed RL with an organic PEDOT:PSS (poly(3,4‐ethylenedioxythiophene): polystyrene sulfonate) interlayer leads to the fabrication of the tandem devices in solution process. The use of robust inorganic RL containing an ultrathin Au interlayer results in more efficient device performance and remarkably improved device lifetime. The optimal PbS CQDs tandem cells based on inorganic RL demonstrate a high power conversion efficiency approaching 9%. This efficiency is more than two times higher than the previous record of 4.2%, which has been kept for more than five years. The remarkable stability, high performance, and low‐temperature processing of these tandem devices may provide insight into the commercialization of flexible and large‐area CQDs tandem solar cells in the near future.     

Photoluminescence‐Based Characterization of Halide Perovskites for Photovoltaics

Photoluminescence spectroscopy is a widely applied characterization technique for semiconductor materials in general and halide perovskite solar cell materials in particular. It can give direct information on the recombination kinetics and processes as well as the internal electrochemical potential of free charge carriers in single semiconductor layers, layer stacks with transport layers, and complete solar cells. The correct evaluation and interpretation of photoluminescence requires the consideration of proper excitation conditions, calibration and application of the appropriate approximations to the rather complex theory, which includes radiative recombination, non‐radiative recombination, interface recombination, charge transfer, and photon recycling. In this article, an overview is given of the theory and application to specific halide perovskite compositions, illustrating the variables that should be considered when applying photoluminescence analysis in these materials.     

Upscaling of Perovskite Solar Cells: Fully Ambient Roll Processing of Flexible Perovskite Solar Cells with Printed Back Electrodes

A scaling effort on perovskite solar cells is presented where the device manufacture is progressed onto flexible substrates using scalable techniques such as slot‐die roll coating under ambient conditions. The printing of the back electrode using both carbon and silver is essential to the scaling effort. Both normal and inverted device geometries are explored and it is found that the formation of the correct morphology for the perovskite layer depends heavily on the surface upon which it is coated and this has significant implications for manufacture. The time it takes to form the desired layer morphology falls in the range of 5–45 min depending on the perovskite precursor, where the former timescale is compatible with mass production and the latter is best suited for laboratory work. A significant loss in solar cell performance of around 50% is found when progressing to using a fully scalable fabrication process, which is comparable to what is observed for other printable solar cell technologies such as polymer solar cells. The power conversion efficiency (PCE) for devices processed using spin coating on indium tin oxide (ITO)‐glass with evaporated back electrode yields a PCE of 9.4%. The same device type and active area realized using slot‐die coating on flexible ITO‐polyethyleneterphthalate (PET) with a printed back electrode gives a PCE of 4.9%.     

Highly Efficient Tandem Organic Solar Cell Enabled by Environmentally Friendly Solvent Processed Polymeric Interconnecting Layer

In the field of organic solar cells (OSCs), tandem structure devices exhibit very attractive advantages for improving power conversion efficiency (PCE). In addition to the well researched novel pair of active layers in different subcells, the construction of interconnecting layer (ICL) also plays a critical role in achieving high performance tandem devices. In this work, a new way of achieving environmentally friendly solvent processed polymeric ICL by adopting poly[(9,9‐bis(3′‐(N,N‐dimethylamino)propyl)‐2,7‐fluorene)‐alt‐5,5′‐bis(2,2′‐thiophene)‐2,6‐naphthalene‐1,4,5,8‐tetracaboxylic‐N,N′‐di(2‐ethylhexyl)imide] (PNDIT‐F3N) blended with poly(ethyleneimine) (PEI) as the electron transport layer (ETL) and PEDOT:PSS as the hole transport layer is reported. It is found that the modification ability of PNDIT‐F3N on PEDOT can be linearly tuned by the incorporation of PEI, which offers the opportunity to study the charge recombination behavior in ICL. At last, tandem OSC with highest PCE of 12.6% is achieved, which is one of the best tandem OSCs reported till now. These results offer a new selection for constructing efficient ICL in high performance tandem OSCs and guide the way of design new ETL materials for ICL construction, and may even be integrated in future printed flexible large area module device fabrication with the advantages of environmentally friendly solvent processing and thickness insensitivity.     

Improved Optics in Monolithic Perovskite/Silicon Tandem Solar Cells with a Nanocrystalline Silicon Recombination Junction

Perovskite/silicon tandem solar cells are increasingly recognized as promi­sing candidates for next‐generation photovoltaics with performance beyond the single‐junction limit at potentially low production costs. Current designs for monolithic tandems rely on transparent conductive oxides as an intermediate recombination layer, which lead to optical losses and reduced shunt resistance. An improved recombination junction based on nanocrystalline silicon layers to mitigate these losses is demonstrated. When employed in monolithic perovskite/silicon heterojunction tandem cells with a planar front side, this junction is found to increase the bottom cell photocurrent by more than 1 mA cm^?2. In combination with a cesium‐based perovskite top cell, this leads to tandem cell power‐conversion efficiencies of up to 22.7% obtained from J–V measurements and steady‐state efficiencies of up to 22.0% during maximum power point tracking. Thanks to its low lateral conductivity, the nanocrystalline silicon recombination junction enables upscaling of monolithic perovskite/silicon heterojunction tandem cells, resulting in a 12.96 cm² monolithic tandem cell with a steady‐state efficiency of 18%.     

Progress in Tandem Solar Cells Based on Hybrid Organic–Inorganic Perovskites

Owing to their high efficiency, low‐cost solution‐processability, and tunable bandgap, perovskite solar cells (PSCs) made of hybrid organic‐inorganic perovskite (HOIP) thin films are promising top‐cell candidates for integration with bottom‐cells based on Si or other low‐bandgap solar‐cell materials to boost the power conversion efficiency (PCE) beyond the Shockley‐Quiesser (S‐Q) limit. In this review, recent progress in such tandem solar cells based on the emerging PSCs is summarized and reviewed critically. Notable achievements for different tandem solar cell configurations including mechanically‐stacked, optical coupling, and monolithically‐integrated with PSCs as top‐cells are described in detail. Highly‐efficient semitransparent PSC top‐cells with high transmittance in near‐infrared (NIR) region are critical for tandem solar cells. Different types of transparent electrodes with high transmittance and low sheet‐resistance for PSCs are reviewed, which presents a grand challenge for PSCs. The strategies to obtain wide‐bandgap PSCs with good photo‐stability are discussed. The PCE reduction due to reflection loss, parasitic absorption, electrical loss, and current mismatch are analyzed to provide better understanding of the performance of PSC‐based tandem solar cells.     

Self‐Assembled 2D Perovskite Layers for Efficient Printable Solar Cells

2D organic–inorganic hybrid Ruddlesden–Popper perovskites have emerged recently as candidates for the light‐absorbing layer in solar cell technology due largely to their impressive operational stability compared with their 3D‐perovskite counterparts. The methods reported to date for the preparation of efficient 2D perovksite layers for solar cells involve a nonscalable spin‐coating step. In this work, a facile, spin‐coating‐free, directly scalable drop‐cast method is reported for depositing precursor solutions that self‐assemble into highly oriented, uniform 2D‐perovskite films in air, yielding perovskite solar cells with power conversion efficiencies (PCE) of up to 14.9% (certified PCE of 14.33% ± 0.34 at 0.078 cm²). This is the highest PCE to date for a solar cell with 2D‐perovskite layers fabricated by nonspin‐coating method. The PCEs of the cells display no evidence of degradation after storage in a nitrogen glovebox for more than 5 months. 2D‐perovskite layer deposition using a slot‐die process is also investigated for the first time. Perovskite solar cells fabricated using batch slot‐die coating on a glass substrate or R2R slot‐die coating on a flexible substrate produced PCEs of 12.5% and 8.0%, respectively.     

A Cross‐Linked Interconnecting Layer Enabling Reliable and Reproducible Solution‐Processing of Organic Tandem Solar Cells

The performance of tandem organic solar cells (OSCs) is directly related to the functionality and reliability of the interconnecting layer (ICL). However, it is a challenge to develop a fully functional ICL for reliable and reproducible fabrication of solution‐processed tandem OSCs with minimized optical and electrical losses, in particular for being compatible with various state‐of‐the‐art photoactive materials. Although various ICLs have been developed to realize tandem OSCs with impressively high performance, their reliability, reproducibility, and generic applicability are rarely analyzed and reported so far, which restricts the progress and widespread adoption of tandem OSCs. In this work, a robust and fully functional ICL is developed by incorporating a hydrolyzed silane crosslinker, (3‐glycidyloxypropyl)trimethoxysilane (GOPS), into poly(3,4‐ethylenedioxythiophene):poly(styrenesulfonate) (PEDOT:PSS), and its functionality for reliable and reproducible fabrication of tandem OSCs based on various photoactive materials is validated. The cross‐linked ICL can successfully protect the bottom active layer against penetration of high boiling point solvents during device fabrication, which widely broadens the solvent selection for processing photoactive materials with high quality and reliability, providing a great opportunity to continuously develop the tandem OSCs towards future large‐scale production and commercialization.     

Highly Efficient Polymer Tandem Cells and Semitransparent Cells for Solar Energy

Highly efficient tandem and semitransparent (ST) polymer solar cells utilizing the same donor polymer blended with [6,6]‐phenyl‐C₆₁‐butyric acid methyl ester (PC₆₁BM) and [6,6]‐phenyl‐C₇₁‐butyric acid methyl ester (PC₇₁BM) as active layers are demonstrated. A high power conversion efficiency (PCE) of 8.5% and a record high open‐circuit voltage of 1.71 V are achieved for a tandem cell based on a medium bandgap polymer poly(indacenodithiophene‐co‐phananthrene‐quinoxaline) (PIDT‐phanQ). In addition, this approach can also be applied to a low bandgap polymer poly[2,6‐(4,4‐bis(2‐ethylhexyl)‐4H‐cyclopenta[2,1‐b;3,4‐b′]dithiophene)‐alt‐4,7‐(5‐fluoro‐2,1,3‐benzothia‐diazole)] (PCPDTFBT), and PCEs up to 7.9% are achieved. Due to the very thin total active layer thickness, a highly efficient ST tandem cell based on PIDT‐phanQ exhibits a high PCE of 7.4%, which is the highest value reported to date for a ST solar cell. The ST device also possesses a desirable average visible transmittance (≈40%) and an excellent color rendering index (≈100), permitting its use in power‐generating window applications.     

Hybrid Perovskite‐Organic Flexible Tandem Solar Cell Enabling Highly Efficient Electrocatalysis Overall Water Splitting

Perovskite‐organic tandem solar cells are attracting more attention due to their potential for highly efficient and flexible photovoltaic device. In this work, efficient perovskite‐organic monolithic tandem solar cells integrating the wide bandgap perovskite (1.74 eV) and low bandgap organic active PBDB‐T:SN6IC‐4F (1.30 eV) layer, which serve as the top and bottom subcell, respectively, are developed. The resulting perovskite‐organic tandem solar cells with passivated wide‐bandgap perovskite show a remarkable power conversion efficiency (PCE) of 15.13%, with an open‐circuit voltage (V_oc) of 1.85 V, a short‐circuit photocurrent (J_sc) of 11.52 mA cm^?2, and a fill factor (FF) of 70.98%. Thanks to the advantages of low temperature fabrication processes and the flexibility properties of the device, a flexible tandem solar cell which obtain a PCE of 13.61%, with V_oc of 1.80 V, J_sc of 11.07 mA cm^?2, and FF of 68.31% is fabricated. Moreover, to demonstrate the achieved high V_oc in the tandem solar cells for potential applications, a photovoltaic (PV)‐driven electrolysis system combing the tandem solar cell and water splitting electrocatalysis is assembled. The integrated device demonstrates a solar‐to‐hydrogen efficiency of 12.30% and 11.21% for rigid, and flexible perovskite‐organic tandem solar cell based PV‐driven electrolysis systems, respectively.     

Correlating Stiffness,Ductility, and Morphology of Polymer:Fullerene Films for Solar Cell Applications

The development of flexible and physically robust organic solar cells requires detailed knowledge of the mechanical behavior of the heterogeneous material stack. However, in these devices there has been limited research on the mechanical properties of the active organic layer. Here, two critical mechanical properties, stiffness and ductility, of a widely studied organic solar cell active layer, a blend film composed of poly(3‐hexylthiophene) (P3HT) and [6,6]‐phenyl C61‐butyric acid methyl ester (PCBM) are reported. Processing conditions are varied to produce films with differing morphology and correlations are developed between the film morphology, mechanical properties and photovoltaic device performance. The morphology is characterized by fitting the absorption of the P3HT:PCBM films to a weakly interacting H‐aggregate model. The elastic modulus is determined using a buckling metrology approach and the crack onset strain is determined by observing the film under tensile strain using optical microscopy. Both the elastic modulus and crack onset strain are found to vary significantly with processing conditions. Processing methods that result in improved device performance are shown to decrease both the compliance and ductility of the film.     

Environmentally Printing Efficient Organic Tandem Solar Cells with High Fill Factors: A Guideline Towards 20% Power Conversion Efficiency

The tandem concept involves stacking two or more cells with complementary absorption spectra in series or parallel connection, harvesting photons at the highest possible potential. It is strongly suggested that the roll‐to‐roll production of organic solar cells will employ the tandem concept to enhance the power conversion efficiency (PCE). However, due to the undeveloped deposition techniques, the challenges in ink formulation as well as the lack of commercially available high performance active materials, roll‐to‐roll fabrication of highly efficient organic tandem solar cells currently presents a major challenge. The reported high PCE values from lab‐scale spin‐coated devices are, of course, representative, but not helpful for commercialization. Here, organic tandem solar cells with exceptionally high fill factors and PCE values of 7.66% (on glass) and 5.56% (on flexible substrate), which are the highest values for the solution‐processed tandem solar cells fabricated by a mass‐production compatible coating technique under ambient conditions, are demonstrated. To predict the highest possible performance of tandem solar cells, optical simulation based on experimentally feasible values is performed. A maximum PCE of 21% is theoretically achievable for an organic tandem solar cell based on the optimized bandgaps and achieved fill factors.     

Self‐Assembly Atomic Stacking Transport Layer of 2D Layered Titania for Perovskite Solar Cells with Extended UV Stability

A novel atomic stacking transporting layer (ASTL) based on 2D atomic sheets of titania (Ti_1?δO₂) is demonstrated in organic–inorganic lead halide perovskite solar cells. The atomically thin ASTL of 2D titania, which is fabricated using a solution‐processed self‐assembly atomic layer‐by‐layer deposition technique, exhibits the unique features of high UV transparency and negligible (or very low) oxygen vacancies, making it a promising electron transporting material in the development of stable and high‐performance perovskite solar cells. In particular, the solution‐processable atomically thin ASTL of 2D titania atomic sheets shows superior inhibition of UV degradation of perovskite solar cell devices, compared to the conventional high‐temperature sintered TiO₂ counterpart, which usually causes the notorious instability of devices under UV irradiation. The discovery opens up a new dimension to utilize the 2D layered materials with a great variety of homostructrual or heterostructural atomic stacking architectures to be integrated with the fabrication of large‐area photovoltaic or optoelectronic devices based on the solution processes.