Flexible Organic Photovoltaics Research Articles

Large‐Area Flexible Organic Photovoltaic Modules on Smoothened Silver Nanowire Transparent Electrodes with Thick Electron Transporting Layer

AbstractHigh‐efficiency large‐area flexible organic photovoltaic (OPV) modules are still challenging. Electrical shunt and shortage generally occur due to surface roughness or spikes that result in low efficiency. In this work, a thick electron transporting layer (ETL) of zinc‐chelated polyethylenimine (PEI‐Zn) is introduced to smoothen the surface of silver nanowires (AgNWs) transparent electrodes. The smoothened surface of AgNWs electrodes helped to suppress the electrical leakage or shortage. Thicker PEI‐Zn layers are required to overcome the open‐circuit voltage (VOC) loss when the device area increases. For large‐area OPV modules on AgNWs electrodes, a high thickness of PEI‐Zn up to 350 nm can deliver high VOC as well as power conversion efficiency (PCE). Based on the AgNWs transparent electrode coated by thick PEI‐Zn ETL, a PCE of 12.50% is achieved for 35.2 cm2 flexible OPV modules certified by a third party. The modules exhibited good illumination stability and mechanical flexibility.

Enhancing the Efficiency of Flexible, Large-Area, ITO-Free Organic Photovoltaic Devices.

The development of flexible ITO-free devices is crucial for the industrial advancement of organic photovoltaic (OPV) technology. Here, a novel ITO-free device architecture is proposed, and ITO-free OPV devices are realized on glass substrates with performance comparable to that of ITO-based devices. It is also demonstrated that the performance of ITO-free devices on polyethylene terephthalate (PET) substrates is limited due to the higher surface roughness of PET, leading to high voltage losses, low device quantum efficiency, and high device leakage current. To address the issue of high roughness on the PET surface, a polyimide (PI) modification strategy is developed and the PI-modified PET is employed as the substrate to construct flexible ITO-free OPV devices and large-area modules with an active area of up to 16.5cm2. This approach leads to decreased trap-assisted recombination losses, enhanced exciton dissociation efficiency, and a reduced density of pinholes in flexible OPV devices, resulting in improved photovoltaic performance under both strong and weak illumination conditions. The outcomes of this work are expected to advance the industrial development of flexible organic photovoltaic technology.

Highly Efficient and Stable Organic Photovoltaic Cells for Underwater Applications.

Organic photovoltaic (OPV) technology holds tremendous promise as a sustainable power source for underwater off-grid systems. However, research on underwater OPV cells is relatively scarce. Here, this gap is addressed by focusing on the exploration and development of OPV cells specifically designed for underwater applications. An acceptor, named ITO-4Cl, with excellent water resistance, is rationally designed and synthesized. Benefiting from its low energetic disorder and an absorption spectrum well-suited to the underwater environment, the ITO-4Cl-based OPV cell achieves an unprecedented power conversion efficiency (PCE) of over 25.6% at a water depth of 1m. Additionally, under 660nm laser irradiation, the cell demonstrates a notable PCE of 31.6%, indicating its potential for underwater wireless energy transfer. Due to the mitigation of thermal effects from solar irradiation, the lifetime of the ITO-4Cl-based OPV cell exceeds 7000h. Additionally, a flexible OPV cell is fabricated that maintains its initial PCE even under exposure to high pressures of 5MPa. A 32.5cm2 flexible module achieves an excellent PCE of 17%. This work fosters a deeper understanding of underwater OPV cells and highlights the promising prospects of OPV cells for underwater applications.

Biobased Thermoset Substrate for Flexible and Sustainable Organic Photovoltaics

AbstractToward a sustainable development of the flexible electronics industry, the design and facile preparation of sustainable flexible substrates with satisfactory mechanical properties and transparency is still a challenge. Herein, taking structural advantages of biobased eugenol and vanillin, a polymerizable aromatic carbonate monomer with α,ω‐diene functionality (2E), and a robust aromatic acetal monomer with α,ω‐tetraene functionality (4E), are designed and prepared. Then, they are cross‐linked with pentaerythritol tetrakis(2‐mercaptoacetate) (4SH) via thiol‐ene click reaction to generate a series of ternary poly(thioether carbonate acetal) thermosets. It is found that the introduction of 4E allows the production of thiol‐ene thermosets with higher crosslink density, which can balance their mechanical, optical, and surface properties. In addition, the thermoset shows good resistance against various natural environmental conditions and can be decomposed into recyclable small molecules under harsher conditions (3 m NaOH, 80 °C). As a result, the optimal thermoset is well‐suited for the fabrication of flexible organic solar cells (OSCs), yielding a power conversion efficiency of 15.41%, which is superior to polyethylene terephthalate‐based OSC. The results provided significant insights for the design and preparation of sustainable polymer substrates for OSCs, even flexible electronics.

Printable Flexible Organic Photovoltaic by R2R Process

Printable Flexible Organic Photovoltaic by R2R Process

Self-Powering Sensory Device with Multi-Spectrum Image Realization for Smart Indoor Environments.

The development of organic-based optoelectronic technologies for the indoor Internet of Things market, which relies on ambient energy sources, has increased, with organic photovoltaics (OPVs) and photodetectors (OPDs) considered promising candidates for sustainable indoor electronic devices. However, the manufacturing processes of standalone OPVs and OPDs can be complex and costly, resulting in high production costs and limited scalability, thus limiting their use in a wide range of indoor applications. This study uses a multi-component photoactive structure to develop a self-powering dual-functional sensory device with effective energy harvesting and sensing capabilities. The optimized device demonstrates improved free-charge generation yield by quantifying charge carrier dynamics, with a high output power density of over 81 and 76 µW cm-2 for rigid and flexible OPVs under indoor conditions (LED 1000lx (5200 K)). Furthermore, a single-pixel image sensor is demonstrated as a feasible prototype for practical indoor operating in commercial settings by leveraging the excellent OPD performance with a linear dynamic range of over 130dB in photovoltaic mode (no external bias). This apparatus with high-performance OPV-OPD characteristics provides a roadmap for further exploration of the potential, which can lead to synergistic effects for practical multifunctional applications in the real world by their mutual relevance.

Highly Efficient Flexible Roll-to-Roll Organic Photovoltaics Based on Non-Fullerene Acceptors.

The ability of organic photovoltaics (OPVs) to be deposited on flexible substrates by roll-to-roll (R2R) processes is highly attractive for rapid mass production. Many research teams have demonstrated the great potential of flexible OPVs. However, the fabrication of R2R-coated OPVs is quite limited. There is still a performance gap between the R2R flexible OPVs and the rigid OPVs. In this study, we demonstrate the promising photovoltaic characteristics of flexible OPVs fabricated from blends of low bandgap polymer poly[(2,6-(4,8-bis(5-(2-ethylhexyl)thiophen-2-yl)-benzo[1,2-b:4,5-b']dithiophene))-alt-(5,5-(1',3'-di-2-thienyl-5',7'-bis(2-ethylhexyl)benzo[1',2'-c:4',5'-c']dithiophene-4,8-dione)] (PBDB-T) and non-fullerene 3,9-bis(2-methylene-(3-(1,1-dicyanomethylene)-indanone))-5,5,11,11-tetrakis(4-hexylphenyl)-dithieno[2,3-d:2',3'-d']-s-indaceno[1,2-b:5,6-b']dithiophene (ITIC). We successfully R2R slot-die coated the flexible OPVs with high power conversion efficiency (PCE) of over 8.9% under irradiation of simulated sunlight. Our results indicate that the processing parameters significantly affect the PCE of R2R flexible OPVs. By adjusting the amount of solvent additive and processing temperature, as well as optimizing thermal annealing conditions, the high PCE of R2R slot-die coated OPVs can be obtained. These results provide significant insights into the fundamentals of highly efficient OPVs for the R2R slot-die coating process.

Indium Zinc Tin Oxide Bottom Electrode‐Based Flexible Indoor Organic Photovoltaics with Remarkably High Mechanical Stability

Indium Zinc Tin Oxide Bottom Electrode‐Based Flexible Indoor Organic Photovoltaics with Remarkably High Mechanical Stability

Indium Zinc Tin Oxide Bottom Electrode‐Based Flexible Indoor Organic Photovoltaics with Remarkably High Mechanical Stability

The demand for flexible indoor organic photovoltaic cells (OPVs) is growing dramatically due to their simple and practical use as a powering aid for various electronic gadgets connected to the Internet of Things. Due to the brittleness of inorganic material‐based transparent bottom electrodes and their incompatibility with flexible organic substrates, it is extremely difficult to limit the influence of mechanical stress on the stability of flexible OPV. In this regard, choosing a mechanically stable and highly conductive transparent conducting oxide (TCO) is crucial. Therefore, flexible OPVs are fabricated onto a flexible (polyimide) substrate coated with mechanically stable TCO indium zinc tin oxide (IZTO). Sheet resistance measurements and observations of scanning electron microscope images of IZTO film after 100 000 bending repetitions (bending radius: 5 mm) confirm the ultrahigh mechanical stability of the TCO. The sheet resistance of flexible IZTO electrode layers is increased by 9%, from 17.42 to 19.12 Ω sq−1. In addition, the impact of a large number of bending repetitions on film transmittance is minimal. The OPV shows ≈69% and ≈20% of its initial power conversion efficiency value after 100 000 bending repetitions for 1000 lx LED illumination and 1 sun conditions, respectively.

Self‐Powered e‐Skin Based on Integrated Flexible Organic Photovoltaics and Transparent Touch Sensors

There is a growing interest in the large area, lightweight, low‐power electronic skin (e‐Skin), consisting of a multitude of sensors over conformable surfaces. The use of multifunctional sensors is always challenging, especially when their energy requirements are considered. Herein, the heterogeneous integration of custom‐made flexible organic photovoltaic (OPV) cells is demonstrated with a large area touch sensor array. The OPV can offer power density of more than 0.32 μW cm−2 at 1500 lux, which is sufficient to meet the instantaneous demand of the array of touch sensors. In addition to energy harvesting, it is shown that the OPVs can perform shadow sensing for proximity and gesture recognition, which are crucial features needed in the e‐Skin, particularly for safe interaction in the industrial domain. Along with pressure sensing (sensitivity of up to 0.26 kPa−1 in the range of 1–10 kPa) and spatial information, the touch sensors made of indium tin oxide and monolayer graphene have shown >70% transparency, which allow light to pass through them to reach the bottom OPV layer. With better resource management and space utilization, the presented stacked integration of transparent touch‐sensing layer and OPVs can evolve into a futuristic energy‐autonomous e‐Skin that can “see” and “feel.”

Lab-to-Fab development and long-term greenhouse test of stable flexible semitransparent organic photovoltaic module

The Lab-to-Fab transfer from cell to large-area flexible semitransparent organic photovoltaic (OPV) module by the slot-die coating based on halogen-free host solvent and under ambient air environment is developed. The bulk heterojunction structure (BHJ) and formation mechanism of slot-die-coated active layer on flexible substrate are different from those usually reported. The relationship among processing, film thickness/BHJ morphology, transmittance and performance for the slot-die-coated module, and the optimum strategy are studied in this article. The flexible semitransparent modules with active areas of 45 and 22.5 cm2 have the average visible transmittance of 21.3%–16.7%. The corresponding average power conversion efficiency (PCE) values are 4%–6.2%. The highest PCE can achieve 7.8%. Compared to all large-area flexible semitransparent slot-die-coated OPV modules reported with PCEs (usually ≤5%), the modules prepared here have the best PCE. The electric behavior and stability of these OPV modules and a Si-PV panel under the greenhouse test are studied. Among the stability data (usual T80 lifetime ≤100 days) reported for semitransparent flexible OPV modules under greenhouse test, the T80 lifetime of the OPV modules prepared here can reach 200 days and also remain the highest PCE with the least burn-in loss.

Flexible Solution-Processed Electron-Transport-Layer-Free Organic Photovoltaics for Indoor Application

Organic photovoltaics (OPVs) have unique advantages of low weight, mechanical flexibility, and solution processability, which make them exceptionally suitable for integrating low-power Internet of Things devices. However, achieving improved operational stability together with solution processes that are applicable to large-scale fabrication remains challenging. Their major limitation arises due to the instable factors that occur both inside the thick active film and from the ambient environment, which cannot be completely resolved via the current encapsulation techniques used for flexible OPVs. Additionally, thin active layers are highly vulnerable to point defects, which result in low yield rates and impede the laboratory-to-industry translation. In this study, flexible fully solution-processed OPVs with improved indoor efficiency and long-term operational stability than that of conventional OPVs with evaporated electrodes are achieved. Benefiting from the oxygen and water vapor permeation barrier of the spontaneously formed gallium oxide layers on the exposed eutectic gallium-indium surface, fast degradation of the OPVs with thick active layers is prevented, maintaining 93% of its initial Pmax after 5000 min of indoor operation under 1000 lx light-emitting diode (LED) illumination. Additionally, by using the thick active layer, spin-coated silver nanowires could be directly used as bottom electrodes without complicated flattening processes, thereby substantially simplifying the fabrication process and proposing a promising manufacturing technique for devices with high-throughput energy demands.

Surface-Energy-Mediated Interfacial Adhesion for Mechanically Robust Ultraflexible Organic Photovoltaics.

Insufficient interfacial adhesion is a widespread problem across multilayered devices that undermines their reliability. In flexible organic photovoltaics (OPVs), poor interfacial adhesion can accelerate degradation and failure under mechanical deformations due to the intrinsic brittleness and mismatching mechanical properties between functional layers. We introduce an argon plasma treatment for OPV devices, which yields 58% strengthening in interfacial adhesion between an active layer and a MoOX hole transport layer, thus contributing to mechanical reliability. The improved adhesion is attributed to the increased surface energy of the active layer that occurred after the mild argon plasma treatment. The mechanically stabilized interface retards the flexible device degradation induced by mechanical stress and maintains a power conversion efficiency of 94.8% after 10,000 cycles of bending with a radius of 2.5 mm. In addition, a fabricated 3 μm thick ultraflexible OPV device shows excellent mechanical robustness, retaining 91.0% of the initial efficiency after 1000 compressing-stretching cycles with a 40% compression ratio. The developed ultraflexible OPV devices can operate stably at the maximum power point under continuous 1 sun illumination for 500 min with an 89.3% efficiency retention. Overall, we validate a simple interfacial linking strategy for efficient and mechanically robust flexible and ultraflexible OPVs.

Oxidized Carbon Materials as Hole Transport Layers for High‐Performance Organic Photovoltaics

Flexible Organic Photovoltaics In article number 2200908, Dong-Yu Kim and co-workers introduced an oxidized carbon soot (OCS)-based hole-transporting layer to improve charge transport without charge recombination, finally enhancing the device performance up to 15.04%. Due to the functionalization of OCS with octadecylamine, the largesized and flexible organic photovoltaics prepared by blade coating exhibited high storage stability (71% retention) and mechanical stability (78% retention).

Mechanically Stable Flexible Organic Photovoltaics with Silver Nanomesh for Indoor Applications.

Enhanced device performance of flexible organic solar cells (FOSCs) was achieved according to the development of organic solar cells (OSCs). OSCs are promising candidates as energy sources for low-power supply systems such as the Internet of Things (IoT) under indoor lighting environments. To apply FOSCs to flexible or wearable applications, they must be mechanically stable. In this study, we fabricated FOSCs with silver nanomesh (AgNM) as the bottom transparent conductive electrode (TCE). Instead of indium tin oxide (ITO), AgNMs were prepared using three pitches of 25, 50, and 100 μm with a square pattern, using a poly(ethylene terephthalate) (PET) substrate. Notably, the device using AgNMs with a pitch of 25 μm exhibited a power conversion efficiency (PCE) of 14.93% under 1 sun illumination and 17.91% under 1000 lux of light-emitting diode (LED) light conditions. Flexible devices using AgNMs maintained over 92% of their initial PCE under 1 sun illumination (PCE decreased to 12.98 from 14.04%) and over 92% when tested under 1000 lux of LED light illumination (PCE decreased to 16.57 from 17.91%) after 1000 instances of bending. These results demonstrate the advantages of using AgNMs as an alternative TCE under both 1 sun and indoor lightning environments and are promising candidates for flexible applications.

Enhanced Performance of Flexible Organic Photovoltaics Based on MoS2 Micro-Nano Array.

In this work, we investigated the influence of MoS2 functioning as an electron transport layer (ETL) on the inverted flexible organic photovoltaics (FOPVs). Three ETLs, including MoS2, lithium quinolate (Liq), and a MoS2/Liq bilayer, were evaporated onto ITO-integrated polyethylene terephthalate substrates (PET-ITO), and the properties of transmittance, water contact angle, and reflectivity of the films were analyzed. The results revealed that MoS2 was helpful to improve the lipophilicity of the surface of the ETL, which was conducive to the deposition of the active layer. In addition, the reflectivity of MoS2 to the light ranging from 400 to 600 nm was the largest among the pristine PET-ITO substrate and the PET-ITO coated with three ETLs, which promoted the efficient use of the light. The efficiency of the FOPV with MoS2/Liq ETL was 73% higher than that of the pristine device. This was attributed to the nearly two-fold amplification of the MoS2 array to the light field, which promoted the FOPV to absorb more light. Moreover, the efficiency of the FOPV with MoS2 was maintained under different illumination angles and bending angles. The results demonstrate the promising applications of MoS2 in the fabrication of FOPVs.

Oxidized Carbon Materials as Hole Transport Layers for High‐Performance Organic Photovoltaics

Organic photovoltaics (OPVs) have recently advanced as promising solar cells owing to their many advantages, including the possibility of a low‐temperature solution process, lightweight, and flexibility. In OPVs, the role of the interlayer is important for efficient charge transport from the photoactive layer to electrodes. However, as a hole‐transporting layer (HTL), molybdenum oxide and poly(3,4‐ethylenedioxythiophene)–poly(styrenesulfonate) are still used for commercialization despite their drawbacks. The development of novel materials with suitable energy levels and solvent orthogonality is required to enhance hole extraction and optimize the film morphology. Herein, oxidized carbon soot (OCS) and OCS‐functionalized octadecylamine (OCS‐ODA) nanoparticles as HTL materials are synthesized. As a large number of oxygen functional groups are produced via Hummer's method, the devices with the OCS‐ODA exhibit high hole extraction ability. The ODA long alkyl chains functionalized by facile process also improve film morphology to minimize contact resistance and charge recombination. The small‐area (SA), large‐area, and flexible (F) OPVs with OCS‐ODA show power conversion efficiencies of 15.04%, 14.57%, and 12.73%, respectively. In particular, OPVs with OCS‐ODA are further demonstrated to possess storage stability in SA‐OPVs (71% retention after 450 h) and mechanical stability in F‐OPVs (78% retention after 1000 bendings).

High-Efficiency and Mechanically Robust All-Polymer Organic Photovoltaic Cells Enabled by Optimized Fibril Network Morphology.

All-polymer organic photovoltaic (OPV) cells possessing high photovoltaic performance and mechanical robustness are promising candidates for flexible wearable devices. However, developing photoactive materials with good mechanical properties and photovoltaic performance so far remains challenging. In this work, a polymer donor PBDB-TF with a high weight-average molecular weight (Mw ) is introduced to enable highly efficient all-polymer OPV cells featuring excellent mechanical reliability. By incorporating the high-Mw PBDB-TF as a third component into the PBQx-TF:PY-IT blend, the bulk heterojunction morphology is finely tuned with a more compact π-π stacking distance, affording efficient pathways for charge transport as well as mechanical stress dissipation. Hence, all-polymer OPV cells based on the ternary blend film demonstrate a maximum power conversion efficiency (PCE) of 18.2% with an outstanding fill factor of 0.796. The flexible OPV cell delivers a decent PCE of 16.5% with high mechanical stability. These results present a promising strategy to address the mechanical properties and boost the photovoltaic performance of all-polymer OPV cells.

Low-Cost Silicon Phthalocyanine as a Non-Fullerene Acceptor for Flexible Large Area Organic Photovoltaics.

We demonstrate large-area (1 cm2) organic photovoltaic (OPVs) devices based on bis(tri-n-butylsilyl oxide) silicon phthalocyanine (3BS)2-SiPc as a non-fullerene acceptor (NFA) with low synthetic complexity paired with poly(3-hexylthiophene) (P3HT) as a donor polymer. Environment-friendly nonhalogenated solvents were used to process large area OPVs on flexible indium tin oxide (ITO)-coated polyethylene terephthalate (PET) substrates. An alternate sequentially (Alt-Sq) blade-coated active layer with bulk heterojunction-like morphology is obtained when using (3BS)2-SiPc processing with o-xylene/1,3,5-trimethylbenzene solvents. The sequential (Sq) active layer is prepared by first blade-coating (3BS)2-SiPc solution followed by P3HT coated on the top without any post-treatment. The conventional sequentially (Sq) blade-coated active layer presents very low performance due to the (3BS)2-SiPc bottom layer being partially washed off by processing the top layer of P3HT. In contrast, alternate sequentially (Alt-Sq) blade-coated layer-by-layer film shows even better device performance compared to the bulk heterojunction (BHJ) active layer. Time-of-flight secondary ion mass spectroscopy (TOF-SIMS) and atomic force microscopy (AFM) reveal that the Alt-Sq processing of the active layer leads to a BHJ-like morphology with a well-intermixed donor-acceptor component in the active layer while providing a simpler processing approach to low-cost and large-scale OPV production.

On-the-Fly Short-Pulse R2R Laser Patterning Processes for the Manufacturing of Fully Printed Semitransparent Organic Photovoltaics.

Ultrafast laser patterning is an essential technology for the low-cost and large area production of flexible Organic Electronic (OE) devices, such as Organic Photovoltaics (OPVs). In order to unleash the potential of ultrafast laser processing to perform the selective and high precision removal of complex multilayers from printed OPV stacks without affecting the underlying nanolayers, it is necessary to optimize its parameters for each nanolayer combination. In this work, we developed an efficient on-the-fly picosecond (ps) laser scribing process (P1, P2 and P3) using single wavelength and single step/pass for the precise and reliable in-line patterning of Roll-to-Roll (R2R) slot-die-coated nanolayers. We have investigated the effect of the key process parameters (pulse energy and overlap) on the patterning quality to obtain high selectivity on the ablation of each individual nanolayer. Finally, we present the implementation of the ultrafast laser patterning process in the manufacturing of fully R2R printed flexible semitransparent OPV modules with a 3.4% power conversion efficiency and 91% Geometric Fill Factor (GFF).