Interfacial Stabilization of Organic Electrochemical Transistors Conferred Using Polythiophene-Based Conjugated Block Copolymers with a Hydrophobic Coil Design.

The recent interest in developing low-cost, biocompatible, and lightweight bioelectronic devices has focused on organic electrochemical transistors (OECTs), which have the potential to fulfill these requirements. In this study, three types of poly(3-hexylthiophene) (P3HT)-based block copolymers (BCPs) incorporating different insulating blocks (poly(nbutyl acrylate) (PBA), polystyrene, and poly(ethylene oxide) (PEO)) were synthesized for application in OECTs. The morphological, crystallographic, and electrochemical properties of these BCPs are systematically investigated. Accordingly, P3HT-b-PBA demonstrates superior performance in the KCl-based aqueous electrolyte, with a higher product of mobility and capacitance (µC*) at 170 F s-1 cm-1 V-1 than that of the P3HT homopolymer at 58 F s-1 cm-1 V-1. P3HT-b-PBA exhibits better stability over 50 ON/OFF switching cycles than do other BCPs and P3HT homopolymers. With regard to the performance in the KPF6-based aqueous electrolyte, P3HT-b-PBA outperforms with a higher µC* of 9.2 F s-1 cm-1 V-1 than that of 8.6 F s-1 cm-1 V-1 observed from P3HT. Notably, both polymers exhibited almost no decay in device performance over 110 ON/OFF switching cycles. The strongly different performance of polymers in these two electrolytes is due to the side chain's hydrophobicity and interdigitated lamellar structures, thereby retarding the doping kinetics of the highly hydrated Cl- ions compared with the slightly hydrated PF6- ions. Concerning the improved performance of P3HT-b-PBA, this is attributed to its soft and hydrophobic backbone. Our morphological and crystallographic analyses reveal that P3HT-b-PBA experiences minimal structural disorder when swelled by the electrolyte, maintaining its original structure better than the P3HT homopolymer and the hydrophilic BCP of P3HT-b-PEO. The hydrophobic nature of P3HT-b-PBA contributes to the stability of its backbone structure, ensuring enhanced capacitance during the operation of the OECT operation. These findings provide reassurance about the stability and performance of P3HT-b-PBA in the field of OECT applications. In summary, this study represents the first exploration of P3HT-based BCPs for OECT applications and investigates their structure-performance relationships in mixed ionic-electronic conductors.

Tungsten-Doped ZnO as an Electron Transport Layer for Perovskite Solar Cells: Enhancing Efficiency and Stability.

This study delves into enhancing the efficiency and stability of perovskite solar cells (PSCs) by optimizing the surface morphologies and optoelectronic properties of the electron transport layer (ETL) using tungsten (W) doping in zinc oxide (ZnO). Through a unique green synthesis process and spin-coating technique, W-doped ZnO films were prepared, exhibiting improved electrical conductivity and reduced interface defects between the ETL and perovskite layers, thus facilitating efficient electron transfer at the interface. High-quality PSCs with superior ETL demonstrated a substantial 30% increase in power conversion efficiency (PCE) compared to those employing pristine ZnO ETL. These solar cells retained over 70% of their initial PCE after 4000 h of moisture exposure, surpassing reference PSCs by 50% PCE over this period. Advanced numerical multiphysics solvers, employing finite-difference time-domain (FDTD) and finite element method (FEM) techniques, were utilized to elucidate the underlying optoelectrical characteristics of the PSCs, with simulated results corroborating experimental findings. The study concludes with a thorough discussion on charge transport and recombination mechanisms, providing insights into the enhanced performance and stability achieved through W-doped ZnO ETL optimization.

Hysteresis-Free and Bias-Stable Organic Transistors Fabricated by Dip-Coating with a Vertical-Phase-Separation Structure.

The morphology of organic films plays a pivotal role in determining the performance of transistor devices. While the dip-coating technique is capable of producing highly oriented organic films, it often encounters challenges such as limited coverage and the presence of defects in gaps between strips, adversely affecting device performance. In this study, we address these challenges by increasing solution viscosity through the incorporation of a substantial proportion of dielectric polymers, thereby enhancing the participation of additional molecules during the film formation process when pulled up. This method produces continuous and oriented organic films with a notable absence of gaps, significantly improving the carrier mobility of transistor devices by more than twofold. Importantly, the fabricated devices exhibit remarkable reliability, showing no hysteresis even after 200 cycles of measurement. Furthermore, the current and threshold voltages of the devices demonstrate exceptional stability, maintaining steady after 10,000 s of bias measurement. This approach provides a solution for the cost-effective and large-scale production of organic transistors, contributing significantly to the advancement of organic electronics.

Efficient and Stable CuSCN-based Perovskite Solar Cells Achieved by Interfacial Engineering with Amidinothiourea.

Cuprous thiocyanate (CuSCN) emerges as a prime candidate among inorganic hole-transport materials, particularly suitable for the fabrication of perovskite solar cells. Nonetheless, there is an Ohmic contact degradation between the perovskite and CuSCN layers. This is induced by polar solvents and undesired purities, which reduce device efficiency and operational stability. In this work, we introduce amidinothiourea (ASU) as an intermediate layer between perovskites and CuSCN to overcome the above obstacles. The characterization results confirm that ASU-modified perovskites have eliminated trap-induced defects by strong chemical bonding between -NH- and C═S from ASU and under-coordinated ions in perovskites. The interfacial engineering based on the ASU also reduces the potential barrier between the perovskite and CuSCN layers. The ASU-treated perovskite solar cells (PSC) with a gold electrode obtains an improved power conversion efficiency (PCE) from 16.36 to 18.03%. Furthermore, after being stored for 1800 h in ambient air (relative humidity (RH) = 45%), the related device without encapsulation maintains over 90% of its initial efficiency. The further combination of ASU and carbon-tape electrodes demonstrates its potential to fabricate low-cost but stable carbon-based PSCs. This work finds a universal approach for the fabrication of efficient and stable PSCs with different device structures.

Emerging Trends in Electron Transport Layer Development for Stable and Efficient Perovskite Solar Cells.

Perovskite solar cells (PSCs) stand at the forefront of photovoltaic research, with current efficiencies surpassing 26.1%. This review critically examines the role of electron transport materials (ETMs) in enhancing the performance and longevity of PSCs. It presents an integrated overview of recent advancements in ETMs, like TiO2, ZnO, SnO2, fullerenes, non-fullerene polymers, and small molecules. Critical challenges are regulated grain structure, defect passivation techniques, energy level alignment, and interfacial engineering. Furthermore, the review highlights innovative materials that promise to redefine charge transport in PSCs. A detailed comparison of state-of-the-art ETMs elucidates their effectiveness in different perovskite systems. This review endeavors to inform the strategic enhancement and development of n-type electron transport layers (ETLs), delineating a pathway toward the realization of PSCs with superior efficiency and stability for potential commercial deployment.

Origin of the High Density of Oxygen Vacancies at the Back Channel of Back-Channel-Etched a-InGaZnO Thin-Film Transistors.

This study reveals the pronounced density of oxygen vacancies (Vo) at the back channel of back-channel-etched (BCE) a-InGaZnO (a-IGZO) thin-film transistors (TFTs) results from the sputtered deposition rather than the wet etching process of the source/drain metal, and they are distributed within approximately 25 nm of the back surface. Furthermore, the existence and distribution depth of the high density of Vo defects are verified by means of XPS spectra analyses. Then, the mechanism through which the above Vo defects lead to the instability of BCE a-IGZO TFTs is elucidated. Lastly, it is demonstrated that the device instability under high-humidity conditions and negative bias temperature illumination stress can be effectively alleviated by etching and thus removing the surface layer of the back channel, which contains the high density of Vo defects. In addition, this etch method does not cause a significant deterioration in the uniformity of electrical characteristics and is quite convenient to implement in practical fabrication processes. Thus, a novel and effective solution to the device instability of BCE a-IGZO TFTs is provided.

Highly Efficient and Stable ITO-Free Organic Solar Cells Based on Squaraine N-Doped Quaternary Bulk Heterojunction.

Simultaneously achieving high efficiency and robust device stability remains a significant challenge for organic solar cells (OSCs). Solving this challenge is highly dependent on the film morphology of the bulk heterojunction (BHJ) photoactive blends; however, there is a lack of rational control strategy. Herein, it is shown that the molecular crystallinity and nanomorphology of nonfullerene-based BHJ can be effectively controlled by a squaraine-based doping strategy, leading to an increase in device efficiency from 17.26% to 18.5% when doping 2 wt% squaraine into the PBDB-TF:BTP-eC9:PC71 BM ternary BHJ. The efficiency is further improved to 19.11% (certified 19.06%) using an indium-tin-oxide-free column-patterned microcavity (CPM) architecture. Combined with interfacial modification, CPM quaternary OSC excitingly shows an extrapolated lifetime of ≈23 years based on accelerated aging test, with the mechanism behind enhanced stability well studied. Furthermore, a flexible OSC module with a high and stable efficiency of 15.2% and an overall area of 5 cm2 is successfully fabricated, exhibiting a high average output power for wearable electronics. This work demonstrates that OSCs with new design of BHJ and device architecture are highly promising to be practical relevance with excellent performance and stability.

Achieving Ideal and Environmentally Stable n-Type Charge Transport in Polymer Field-Effect Transistors.

Realizing ideal charge transport in field-effect transistors (FETs) of conjugated polymers is crucial for evaluating device performance, such as carrier mobility and practical applications of conjugated polymers. However, the current FETs using conjugated polymers as the active layers generally show certain non-ideal transport characteristics and poor stability. Here, ideal charge transport of n-type polymer FETs is achieved on flexible polyimide substrates by using an organic-inorganic hybrid double-layer dielectric. Deposited conjugated polymer films show highly ordered structures and low disorder, which are supported by grazing-incidence wide-angle X-ray scattering, near-edge X-ray absorption fine structure, and molecular dynamics simulations. Furthermore, the organic-inorganic hybrid double-layer dielectric provides low interfacial defects, leading to excellent charge transport in FETs with high electron mobility (1.49 ± 0.46 cm2 V-1 s-1) and ideal reliability factors (102 ± 7%). Fabricated polymer FETs show a self-encapsulation effect, resulting in high stability of the FET charge transport. The polymer FETs still work with high mobility above 1 cm2 V-1 s-1 after storage in air for more than 300 days. Compared with state-of-the-art conjugated polymer FETs, this work simultaneously achieves ideal charge transport and environmental stability in n-type polymer FETs, facilitating rapid device optimization of high-performance polymer electronics.

Stepwise-Process-Controlled Ligand Management Strategy for Efficient and Stable Perovskite Quantum Dot Solar Cells.

CsPbI3 perovskite quantum dots (QDs) have attracted much attention in the field of solar cells because of their excellent photovoltaic properties. Conventional modification of long-chain insulating ligands can ensure good dispersion and film-forming stability of QDs, but the limitations of their low defect passivation ability and poor charge transport ability will make them fail to achieve high efficiency in the corresponding solar cell devices. In this study, by introducing "Benzylphosphonic acid" short-chain ligands to the surface of CsPbI3 QDs, the ligands were re-administered on the surface during the preparation of the CsPbI3 QDs as well as during the film-forming process. The strong coordination ability of Benzenephosphonic acid can effectively passivate defects on the surface of CsPbI3 QDs and inhibit non-radiative recombination and phase transition. Meanwhile, this short-chain ligand can effectively promote the charge exchange between adjacent QDs and improve the electrical transport properties of the film. The efficiency of the Benzylphosphonic acid-modified CsPbI3 QDs solar cell reaches 13.91% compared to the unmodified device (PCE of 11.4%). The storage stability and operation stability of the device are also significantly improved. (The efficiency remains at 91% of the original for 800 h of atmospheric storage; the efficiency remains at 92% of the original for 200 h of continuous light exposure.) The present strategy realizes the simultaneous improvement of photovoltaic properties and stability of CsPbI3 QD solar cells and also provides a reference for surface ligand engineering to realize highly efficient and stable perovskite quantum dot solar cells.

Isomerized Green Solid Additive Engineering for Thermally Stable and Eco-Friendly All-Polymer Solar Cells with Approaching 19% Efficiency.

Laboratory-scale all-polymer solar cells (all-PSCs) have exhibited remarkable power conversion efficiencies (PCEs) exceeding 19%. However, the utilization of hazardous solvents and nonvolatile liquid additives poses challenges for eco-friendly commercialization, resulting in the trade-off between device efficiency and operation stability. Herein, an innovative approach based on isomerized solid additive engineering is proposed, employing volatile dithienothiophene (DTT) isomers to modulate intermolecular interactions and facilitate molecular stacking within the photoactive layers. Through elucidating the underlying principles of the DTT-induced polymer assembly on molecular level, a PCE of 18.72% is achieved for devices processed with environmentally benign solvents, ranking it among the highest record values for eco-friendly all-PSCs. Significantly, such superiorities of the DTT-isomerized strategy afford excellent compatibility with large-area blade-coating techniques, offering a promising pathway for industrial-scale manufacturing of all-PSCs. Moreover, these devices demonstrate enhanced thermal stability with a promising extrapolated T80 lifetime of 14 000 h, further bolstering their potential for sustainable technological advancement.

Solution-Processed Semiconductor Materials as Cathode Interlayers for Organic Solar Cells.

Cathode interlayers (CILs) play a crucial role in improving the photovoltaic efficiency and stability of OSCs. CILs generally consists of two kinds of materials, interfacial dipole-based CILs and SPS-based CILs. With good charge transporting ability, excellent compatibility with large-area processing methods, and highly tunable optoelectronic properties, the SPS-based CILs exhibit remarkable superiorities to their interfacial dipole-based counterparts in practical use, making them promising candidate in developing efficient CILs for OSCs. This mini-review highlights the great potential of SPS-based CILs in OSC applications and elucidates the working mechanism and material design strategy of SPS materials. Afterward, the SPS-based CIL materials are summarized and discussed in four sections, including organic small molecules, conjugated polymers, nonconjugated polymers, and TMOs. The structure-property-performance relationship of SPS-based CIL materials is revealed, which may provide readers new insight into the molecular design of SPS-based CILs. The mechanisms to endow SPS-based CILs with thickness insensitivity, resistance to environmental erosion, and photo-electric conversion ability are also elucidated. Finally, after a brief summary, the remaining issues and the prospects of SPS-based CILs are suggested.

Improving the Performance of Layer-by-Layer Organic Solar Cells by n-Doping of the Acceptor Layer.

Molecular dopants can effectively improve the performance of organic solar cells (OSCs). Here, PM6/BTP-eC9-4Cl-based OSCs are fabricated by a layer-by-layer (LbL) deposition method, and the electron acceptor BTP-eC9-4Cl layer is properly doped by n-type dopant benzyl viologen (BV) or [4-(1,3-dimethyl-2,3-dihydro-1H-benzoimidazol-2-yl)phenyl]dimethyl-amine (N-DMBI-H). The power conversion efficiency (PCE) of OSCs increases from 16.80 to 17.61 or 17.84% when the acceptor layer is doped by BV (0.01 wt %) or N-DMBI-H (0.01 wt %), respectively. At the optimal doping concentration, the device exhibits more balanced charge transport, fewer bimolecular recombinations, faster charge separation and transfer, and better stability. This doping strategy has good universality; when the acceptor layer L8-BO of LbL OSCs is doped by 0.01 wt % BV or 0.01 wt % N-DMBI-H, the PCE increases from 17.49 to 18.35 or 18.25%, respectively. All in all, our studies have demonstrated that the doping strategy is effective in enhancing the performance of OSCs.

Surface Passivation of Perovskite Solar Cells with Oxalic Acid: Increased Efficiency and Device Stability.

Solution processed perovskite films usually exhibit numerous defect states on the surfaces of the films. Here in this work, oxalic acid (H2 C2 O4 ), which has two C=O groups, is selected and used to passivate the surface defects of the two-step deposited perovskite films via post-treatment. Strong interaction between H2 C2 O4 molecule and the Pb2+ ions located on the surface of perovskite film has been confirmed via Fourier transform infrared spectroscopy and X-ray photoelectron spectroscopy, which can result in an effective suppress of the surface defects. Furthermore, time-resolved PL spectrum indicates that carrier lifetime is prolonged in the H2 C2 O4 passivated perovskite film. After optimizing the H2 C2 O4 concentration, the target perovskite solar cells can demonstrate superior power conversion efficiencies (21.67 % from reverse measurement and 21.54 % from forward measurement) and superior device-stability.

Molecular Stacking and Aggregation Optimization of Photoactive Layer through Solid Additive Enables High-Performance Organic Solar Cells.

Regulating molecular packing and aggregation of photoactive layer is a critical but challenging issue in developing high-performance organic solar cells. Herein, two structurally similar analogues of anthra[2,3-b : 6,7-b']dithiophene (ADT) and naphtho[1,2-b : 5,6-b']dithiophene (NDT) are developed as solid additive to exploit their effect in regulating the molecular aggregation and π-stacking of photoactive layer. We clarify that the perpendicular arrangements of NDT can enlarge the molecular packing space and improve the face-on stacking of Y6 during the film formation, favoring a more compact and ordered long-range π-π stacking in the out-of-plane direction after the removal of NDT under thermal annealing. The edge-to-face stacked herringbone-arrangement of ADT along with its non-volatilization under thermal annealing can induce the coexistence of face-on and edge-on stacking of blend film. As a result, the NDT treatment shows encouraging effect in improving the photovoltaic performance of devices based on various systems. Particularly, a remarkable PCE of 18.85 % is achieved in the PM6 : L8-BO-based device treated by NDT additive, which is a significant improvement with regard to the PCE of 16.41 % for the control device. This work offers a promising strategy to regulate the molecular packing and aggregation of photoactive layer towards significantly improved performance and stability of organic solar cells.

Manipulating the Alkyl Chains of Naphthodithiophene Imide-Based Polymers to Concurrently Boost the Efficiency and Stability of Organic Solar Cells.

Morphology instability holds the major responsibility for efficiency degradation of organic solar cells (OSCs). However, how to develop polymer donors simultaneously with high efficiency and excellent morphology stability remains challenging. Herein, we reported naphtho[2,1-b:3,4-b']dithiophene-5,6-imide (NDTI)-based new polymers PNDT1 and PNDT2. The alkyl chain engineering leads to high crystallinity, high hole mobility (>10-3 cm2 V-1 S-1), and nanofibrous film morphology, which enable PNDT2 to exhibit an efficiency of 18.13% and a remarkable FF value of 0.80. Moreover, the NDTIs have short π-π stacking and abundant short interactions, and their polymers exhibit superior morphological stability. Therefore, the PNDT2-based OSCs exhibit much better device stability than that of PNDT1, PAB-α, and benchmark polymers PM6 and D18. This work suggests the great importance of the large conjugated backbone of the monomer and alkyl chain engineering to develop high-performance and morphology-stable polymers for OSCs.

Photoelectric Conversion and Device Stability of PM6:PY-IT Solar Cells Based on a Water Solution-Processed MoO3 Hole Transport Layer.

To enhance the power conversion efficiency (PCE) and stability of all-polymer solar cells (all-PSCs), a new precursor solution based on an in situ chemical reaction of nanomolybdenum powder (Mo), hydrogen peroxide (H2O2), and ammonia (NH3·H2O) was developed for preparing a MoO3 hole transport layer (HTL) for all-PSCs. The results showed that the PCE and stability of PM6:PY-IT solar cells based on the MoO3 HTL were better than those based on a PEDOT:PSS layer. To further understand the relationship between the HTL and the device performance, ultrafast photophysical processes of all-PSCs based on different HTLs were contrastively analyzed. Our research indicated that the micromorphology of active layers could be influenced by the interfacial layer material, consequently determining the photoelectric conversion process of all-PSCs. The MoO3-based all-PSCs had longer charge lifetime, higher charge mobility, and lower charge recombination characteristics compared with the devices based on the PEDOT:PSS layer during the operation time. As a result, the MoO3-based PM6:PY-IT solar cells achieved an initial PCE of 15.2%, and they still maintained more than 80% of their initial efficiency after 1000 h.

Thermal Properties of Polymer Hole-Transport Layers Influence the Efficiency Roll-off and Stability of Perovskite Light-Emitting Diodes.

While the performance of metal halide perovskite light-emitting diodes (PeLEDs) has rapidly improved in recent years, their stability remains a bottleneck to commercial realization. Here, we show that the thermal stability of polymer hole-transport layers (HTLs) used in PeLEDs represents an important factor influencing the external quantum efficiency (EQE) roll-off and device lifetime. We demonstrate a reduced EQE roll-off, a higher breakdown current density of approximately 6 A cm-2, a maximum radiance of 760 W sr-1 m-2, and a longer device lifetime for PeLEDs using polymer HTLs with high glass-transition temperatures. Furthermore, for devices driven by nanosecond electrical pulses, a record high radiance of 1.23 MW sr-1 m-2 and an EQE of approximately 1.92% at 14.6 kA cm-2 are achieved. Thermally stable polymer HTLs enable stable operation of PeLEDs that can sustain more than 11.7 million electrical pulses at 1 kA cm-2 before device failure.

Improving the Stability of Non-fullerene-Based Organic Photovoltaics through Sequential Deposition and Utilization of a Quasi-orthogonal Solvent.

The development of organic photovoltaic (OPV) devices based on non-fullerene acceptors (NFAs) has led to a rapid improvement in their efficiency. Despite these improvements, significant performance degradation in the early stages of operation, known as burn-in, remains a challenge for NFA-based OPVs. To address this challenge, this study demonstrates a stable NFA-based OPV fabricated using sequential deposition (SqD) and a quasi-orthogonal solvent. The quasi-orthogonal solvent, which is prepared by incorporating 1-chloronaphthalene (1-CN) into dichloromethane (DCM), reduces the vapor pressure of the solvent and allows for the efficient dissolution and penetration of the Y6 (one of efficient NFAs) into a PM6 polymer-donor layer without damaging the latter. The resulting bulk heterojunction (BHJ) is characterized by a higher degree of crystallinity in the PM6 domains than that prepared using a conventional single-step deposition (SD) process. The OPV fabricated using the SqD process exhibits a PCE of 14.1% and demonstrates superior thermal stability to the SD-processed OPV. This study conclusively reveals that the formation of a thermally stable interface between the photoactive layer and the electron-transport layer (ETL) is the primary factor contributing to the high thermal stability observed in the SqD-processed OPV.

Understanding Causalities in Organic Photovoltaics Device Degradation in a Machine-Learning-Driven High-Throughput Platform.

Organic solar cells (OSCs) now approach power conversion efficiencies of 20%. However, in order to enter mass markets, problems in upscaling and operational lifetime have to be solved, both concerning the connection between processing conditions and active layer morphology. Morphological studies supporting the development of structure-process-property relations are time-consuming, complex, and expensive to undergo and for which statistics, needed to assess significance, are difficult to be collected. This work demonstrates that causal relationships between processing conditions, morphology, and stability can be obtained in a high-throughput method by combining low-cost automated experiments with data-driven analysis methods. An automatic spectral modeling feeds parametrized absorption data into a feature selection technique that is combined with Gaussian process regression to quantify deterministic relationships linking morphological features and processing conditions with device functionality. The effect of the active layer thickness and the morphological order is further modeled by drift-diffusion simulations and returns valuable insight into the underlying mechanisms for improving device stability by tuning the microstructure morphology with versatile approaches. Predicting microstructural features as a function of processing parameters is decisive know-how for the large-scale production of OSCs.

Review on Chemical Stability of Lead Halide Perovskite Solar Cells.

Lead halide perovskite solar cells (PSCs) have become a promising next-generation photovoltaic technology due to their skyrocketed power conversion efficiency. However, the device stability issues may restrict their commercial applications, which are dominated by various chemical reactions of perovskite layers. Hence, a comprehensive illustration on the stability of perovskite films in PSCs is urgently needed. In this review article, chemical reactions of perovskite films under different environmental conditions (e.g., moisture, oxygen, light) and with charge transfer materials and metal electrodes are systematically elucidated. Effective strategies for suppressing the degradation reactions of perovskites, such as buffer layer introduction and additives engineering, are specified. Finally, conclusions and outlooks for this field are proposed. The comprehensive review will provide a guideline on the material engineering and device design for PSCs.