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.     

A New Interconnecting Layer of Metal Oxide/Dipole Layer/Metal Oxide for Efficient Tandem Organic Solar Cells

A new metal‐oxide‐based interconnecting layer (ICL) structure of all‐solution processed metal oxide/dipole layer/metal oxide for efficient tandem organic solar cell (OSC) is demonstrated. The dipole layer modifies the work function (WF) of molybdenum oxide (MoO _x ) to eliminate preexisted counter diode between MoO _x and TiO₂. Three different amino functionalized water/alcohol soluble conjugated polymers (WSCPs) are studied to show that the WF tuning of MoO _x is controllable. Importantly, the results show that S‐shape current density versus voltage (J–V) characteristics form when operation temperature decreases. This implies that thermionic emission within the dipole layer plays critical role for helping recombination of electrons and holes. Meanwhile, the insignificant homotandem open‐circuit voltage (V _oc) loss dependence on dipole layer thickness shows that the quantum tunneling effect is weak for efficient electron and hole recombination. Based on this ICL, poly(3‐hexylthiophene) (P3HT)‐based homotandem OSC with 1.20 V V _oc and 3.29% power conversion efficiency (PCE) is achieved. Furthermore, high efficiency poly(4,8‐bis(5‐(2‐ethylhexyl)‐thiophene‐2‐yl)‐benzo[1,2‐b54,5‐b9]dithiophene‐alt alkylcarbonylthieno[3,4‐b]thiophene) (PBDTTT‐C‐T)‐based homotandem OSC with 1.54 V V _oc and 8.11% PCE is achieved, with almost 15.53% enhancement compared to its single cell. This metal oxide/dipole layer/metal oxide ICL provides a new strategy to develop other qualified ICL with different hole transporting layer and electron transporting layer in tandem OSCs.     

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.     

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.     

All‐Oxide MoOx/SnOx Charge Recombination Interconnects for Inverted Organic Tandem Solar Cells

Multijunction solar cells are designed to improve the overlap with the solar spectrum and to minimize losses due to thermalization. Aside from the optimum choice of photoactive materials for the respective sub‐cells, a proper interconnect is essential. This study demonstrates a novel all‐oxide interconnect based on the interface of the high‐work‐function (WF) metal oxide MoO_x and low‐WF tin oxide (SnO_x). In contrast to typical p‐/n‐type tunnel junctions, both the oxides are n‐type semiconductors with a WF of 5.2 and 4.2 eV, respectively. It is demonstrated that the electronic line‐up at the interface of MoO_x and SnO_x comprises a large intrinsic interface dipole (≈0.8 eV), which is key to afford ideal alignment of the conduction band of MoO_x and SnO_x, without the requirement of an additional metal or organic dipole layer. The presented MoO_x/SnO_x interconnect allows for the ideal (loss‐free) addition of the open circuit voltages of the two sub‐cells.     

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.     

Improvement of Transparent Metal Top Electrodes for Organic Solar Cells by Introducing a High Surface Energy Seed Layer

We present highly transparent and conductive silver thin films in a thermally evaporated dielectric/metal/dielectric (DMD) multilayer architecture as top electrode for efficient small molecule organic solar cells. DMD electrodes are frequently used for optoelectronic devices and exhibit excellent optical and electrical properties. Here, we show that ultrathin seed layers such as calcium, aluminum, and gold of only 1 nm thickness strongly influence the morphology of the subsequently deposited silver layer used as electrode. The wetting of silver on the substrate is significantly improved with increasing surface energy of the seed material resulting in enhanced optical and electrical properties. Typically thermally evaporated silver on a dielectric material forms rough and granular layers which are not closed and not conductive below thicknesses of 10 nm. With gold acting as seed layer, the silver electrode forms a continuous, smooth, conductive layer down to a silver thickness of 3 nm. At 7 nm silver thickness such an electrode exhibits a sheet resistance of 19 Ω/□ and a peak transmittance of 83% at 580 nm wavelength, both superior compared to silver electrodes without seed layer and even to indium tin oxide (ITO). Top‐illuminated solar cells using gold/silver double layer electrodes achieve power conversion efficiencies of 4.7%, which is equal to 4.6% observed in bottom‐illuminated reference devices employing conventional ITO. The top electrodes investigated here exhibit promising properties for semitransparent solar cells or devices fabricated on opaque substrates.     

Semi‐Transparent Tandem Organic Solar Cells with 90% Internal Quantum Efficiency

Semi‐transparent (ST) organic solar cells with potential application as power generating windows are studied. The main challenge is to find proper transparent electrodes with desired electrical and optical properties. In this work, this is addressed by employing an amphiphilic conjugated polymer PFPA‐1 modified ITO coated glass substrate as the ohmic electron‐collecting cathode and PEDOT:PSS PH1000 as the hole‐collecting anode. For active layers based on different donor polymers, considerably lower reflection and parasitic absorption are found in the ST solar cells as compared to solar cells in the standard geometry with an ITO/PEDOT:PSS anode and a LiF/Al cathode. The ST solar cells have remarkably high internal quantum efficiency at short circuit condition (～90%) and high transmittance (～50%). Hence, efficient ST tandem solar cells with enhanced power conversion efficiency (PCE) compared to a single ST solar cell can be constructed by connecting the stacked two ST sub‐cells in parallel. The total loss of photons by reflection, parasitic absorption and transmission in the ST tandem solar cell can be smaller than the loss in a standard solar cell based on the same active materials. We demonstrate this by stacking five separately prepared ST cells on top of each other, to obtain a higher photocurrent than in an optimized standard solar cell.     

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.     

Solution‐Processable Conjugated Polymers as Anode Interfacial Layer Materials for Organic Solar Cells

In recent years, solution‐processed conjugated polymers have been extensively used as anode interfacial layer (AIL) materials in organic solar cells (OSCs) due to their excellent film‐forming property and low‐temperature processing advantages. In this review, the authors focus on the recent advances in conjugated polymers as AIL materials in OSCs. Several of the main classes of solution‐processable conjugated polymers, including poly(3,4‐ethylenedioxythiophene):(styrenesulfonate), polyaniline, polythiophene, conjugated polyelectrolytes, sulfonated poly(diphenylamine), and crosslinked polymers as AIL materials are discussed in depth, and the mechanisms of these AIL materials in enhancing OSC performances are also elucidated. The structure–property relationships of various conjugated polymer AIL materials are analyzed, and some important design rules for such materials toward high efficiencies and stable OSCs are presented. In addition, some chemical and physical approaches to optimize the photoelectronic and physic properties of conjugated polymer AIL materials, which improve their performance in modifying OSCs, are also highlighted. Considering the significance of tandem OSCs, the relevant applications of conjugated polymer AIL materials in constructing interconnection layers for tandem OSCs are also mentioned. Finally, a brief summary is presented and some perspectives to help researchers understand the current challenges and opportunities in this area are proposed.     

Understanding the External Quantum Efficiency of Organic Homo‐Tandem Solar Cells Utilizing a Three‐Terminal Device Architecture

A fundamental analysis of the external quantum efficiency (EQE) of organic tandem solar cells with equal absorbers in both subcells (homo‐tandem solar cells) is presented. Providing direct access to both subcells by introducing a conductive intermediate polymer electrode into the recombination zone, without changing the optical and electric device properties, the three‐terminal device becomes a proxy to the two‐terminal tandem solar cell properties. From the spectrally resolved EQE of the subcells in three‐terminal configuration wavelength and intensity of suitable bias light as well as bias voltage are determined that in turn allow for accurate EQE measurements of the common two‐terminal tandem solar cells. Theoretic considerations allow the prediction of the tandem solar cell's EQE from its subcells' EQEs as well as the prediction of the tandem cell EQE under monochromatic bias light illumination being in excellent agreement with experimental results. All findings discussed herein can be applied to more common hetero‐tandem solar cell architectures likewise.     

Interface Modification of Tin Oxide Electron-Transport Layer for the Efficiency and Stability Enhancement of Organic Solar Cells

A small molecular phenanthroline derivative Phen-NaDPO (3-[6-(diphenylphosphinyl)-2-naphthalenyl]-1,10-Phenanthroline) to modify tin oxide (SnO₂) electron-transport layer (ETL) in organic solar cells is employed. Quantum chemistry calculations and experimental results show that Phen-NaDPO can interact with SnO₂, thereby effectively passivating the surface defects, reducing the work function and improving the electrical conductivity of SnO₂, leading to more efficient electron extraction and transport in the organic solar cells (OSCs). Moreover, upon the Phen-NaDPO modification, the decreased surface energy of SnO₂ ETL accounts for enhanced exciton dissociation and charge transport, due to the more ordered molecular organizations of the active layers. Consequently, the inverted OSCs involving Phen-NaDPO/SnO₂ ETLs exhibit an enhanced power conversion efficiency of 17.06% (PM6:Y6) and 18.31% (PM6:L8-BO), which is the highest efficiency for SnO₂ ETL-based binary solar cells to date. Furthermore, the devices based on Phen-NaDPO/SnO₂ ETL show better device stability (storage stability, photostability and humid stability), with T₈₀ exceeding 200 h encapsulated under light irradiation and 400 h without encapsulation in high-humidity ambient condition. These results demonstrate that the modification of SnO₂ using wide-band highly stable conjugated small molecules is very promising for simultaneously improve the efficiencies and device stability of OSCs.     

15% Efficiency Tandem Organic Solar Cell Based on a Novel Highly Efficient Wide‐Bandgap Nonfullerene Acceptor with Low Energy Loss

A tandem organic solar cell (OSC) is a valid structure to widen the photon response range and suppress the transmission loss and thermalization loss. In the past few years, the development of low‐bandgap materials with broad absorption in long‐wavelength region for back subcells has attracted considerable attention. However, wide‐bandgap materials for front cells that have both high short‐circuit current density (J_SC) and open‐circuit voltage (V_OC) are scarce. In this work, a new fluorine‐substituted wide‐bandgap small molecule nonfullerene acceptor TfIF‐4FIC is reported, which has an optical bandgap of 1.61 eV. When PBDB‐T‐2F is selected as the donor, the device offers an extremely high V_OC of 0.98 V, a high J_SC of 17.6 mA cm^?2, and a power conversion efficiency of 13.1%. This is the best performing acceptor with such a wide bandgap. More importantly, the energy loss in this combination is 0.63 eV. These properties ensure that PBDB‐T‐2F:TfIF‐4FIC is an ideal candidate for the fabrication of tandem OSCs. When PBDB‐T‐2F:TfIF‐4FIC and PTB7‐Th:PCDTBT:IEICO‐4F are used as the front cell and the back cell to construct tandem solar cells, a PCE of 15% is obtained, which is one of best results reported to date in the field of organic solar cells.