Interface dipoles formed at an electrolyte/electrode interface have been widely studied and interpreted using the "double dipole step" model, where the dipole vector is determined by the size and/or range of motion of the charged ions. Some electron transport materials (ETMs) with lone pairs of electrons on heteroatoms exhibit a similar interfacial behavior. However, the origin of the dipoles in such materials has not yet been explored in great depth. Herein, we systematically investigate the influence of the lone pair of electrons on the interface dipole through three pyridine derivatives B2-B4PyMPM. Experiments show that different positions of nitrogen atoms in the three materials give rise to different hydrogen bonds and molecular orientations, thereby affecting the areal density and direction of the lone pair of electrons. The interface dipoles of the three materials predicted by the "double dipole step" model are in good agreement with the ultraviolet photoelectron spectroscopy results both in spin-coated and vacuum-deposited films. These findings help to better understand the ETMs/electrode interfacial behaviors and provide new guidelines for the molecular design of the interlayer.

The mass implementation of renewable energies is limited by the absence of efficient and affordable technology to store electrical energy. Thus, the development of new materials is needed to improve the performance of actual devices such as batteries or supercapacitors. Herein, the facile consecutive chemically oxidative polymerization of poly(1-amino-5-chloroanthraquinone) (PACA) and poly(3,4-ethylenedioxythiophene (PEDOT) resulting in a water dispersible material PACA-PEDOT is shown. The water-based slurry made of PACA-PEDOT nanoparticles can be processed as film coated in ambient atmosphere, a critical feature for scaling up the electrode manufacturing. The novel redox polymer electrode is a nanocomposite that withstands rapid charging (16 A g−1) and delivers high power (5000 W kg−1). At lower current density its storage capacity is high (198 mAh g−1) and displays improved cycling stability (60% after 5000 cycles). Its great electrochemical performance results from the combination of the redox reversibility of the quinone groups in PACA that allows a high amount of charge storage via Faradaic reactions and the high electronic conductivity of PEDOT to access to the redox-active sites. These promising results demonstrate the potential of PACA-PEDOT to make easily organic electrodes from a water-coating process, without toxic metals, and operating in non-flammable aqueous electrolyte for large scale pseudocapacitors. 

Due to the rapid development of non-fullerene acceptors (NFAs), the efficiency of organic solar cells is steadily being improved. The stability of organic solar cells also is expected to be enhanced with the introduction of the NFAs, yet the stability of NFAs themselves have been less investigated to date. In this paper, the stability of a set of typical NFAs was studied in situ employing photoelectron spectroscopy. The studied molecules show higher resistance to water vapor and thermal stress compared to fullerenes. For water vapor exposure, the highest occupied molecular orbital (HOMO) of NFAs undergoes only minor and reversible changes and the NFAs/substrate work function stays constant. Exposure to oxygen gas significantly modified the electronic structure of the NFAs and the effect was only partially reversible by annealing. However, the presence of water vapor was shown to slow down the degradation caused by oxygen. This is in stark contrast to fullerenes that undergo irreversible degradation upon water vapor exposure.

The fast evolution of metal halide perovskite solar cells has opened a new chapter in the field of renewable energy. High-quality perovskite films as the active layers are essential for both high efficiency and long-term stability. Here, the perovskite films with enlarged crystal grain size and decreased defect density are fabricated by introducing the extremely low-cost and green polymer, ethyl cellulose (EC), into the perovskite layer. The addition of EC triggers hydrogen bonding interactions between EC and the perovskite, passivating the charge defect traps at the grain boundaries. The long chain of EC further acts as a scaffold for the perovskite structure, eliminating the annealing-induced lattice strain during the film fabrication process. The resulting devices with the EC additive exhibit a remarkably enhanced average power conversion efficiency from 17.11 to 19.27% and an improvement of all device parameters. The hysteresis index is found to decrease by three times from 0.081 to 0.027, which is attributed to suppressed ion migration and surface charge trapping. In addition, the defect passivation by EC significantly improves the environmental stability of the perovskite films, yielding devices that retain 80% of their initial efficiency after 30 days in ambient air at 45% relative humidity, whereas the pristine devices without EC fully degrade. This work provides a low-cost and green avenue for passivating defects that improves both the efficiency and operational stability of perovskite solar cells.

Ultraviolet photoelectron spectroscopy (UPS) and cyclic voltammetry (CV) are employed to measure energy levels for charge transport in organic semiconductor films. A series of classical molecules/polymers used in organic bulk heterojunction solar cells are deposited on platinum substrates/electrodes to form thin films and a linear relationship of vertical ionization potential (IP) measured by UPS and relative oxidation potential (Eox) obtained by CV is found, with a slope equal to unity. The intercept varies with the different reference redox couples and repeated potential sweep numbers during experiment processes. The relationship provides for an easy conversion of values obtained by the two techniques and correlates well with device parameters. The precision in the CV-derived IP values is not sufficient, however, to enable precise design of energy level alignment at heterojunction and the approach does not improve upon the current ?best practice? for obtaining donor ionization potential?acceptor electron affinity gaps at heterojunctions.

The interface energetics and intermixing effects of the donor/acceptor bulk heterojunction (BHJ) blends of poly[2,3‐bis‐(3‐octyloxyphenyl) quinoxaline‐5, 8‐dilyl‐alt‐thiophene‐2, 5‐diyl]: [6,6]‐phenyl C71butyric acid methyl ester (TQ1:PC71BM) have been investigated using ultraviolet photoemission spectroscopy (UPS) in combination with the integer charge transfer model. The TQ1:PC71BM represents the useful model system for BHJ organic photovoltaics featuring effective charge generation and transport. It finds out that the positive integer charge state of TQ1 are equal in energy to the negative integer charge state of PC71BM, leading to a negligible potential step at TQ1:PC71BM interface and thus the vacuum level alignment. It is observed that the TQ1 accumulates on the top of TQ1:PC71BM BHJ and UPS spectra as function of various blend ratios suggest that the TQ1 mixes finely with PC71BM with the little work function modification in a wide range. In addition, no significant influence of the long‐range Coulomb interactions or the intermolecular hybridization on the occupied electronic structures is present for the well‐intermixed TQ1:PC71BM BHJs. These findings provide deep insights into the properties of BHJ blends and are beneficial for the performance optimization in organic photovoltaics.

The semiconductor-electrode interface impacts the function and the performance of (opto) electronic devices. For printed organic electronics the electrode surface is not atomically clean leading to weakly interacting interfaces. As a result, solution-processed organic ultrathin films on electrodes typically form islands due to dewetting. It has therefore been utterly difficult to achieve homogenous ultrathin conjugated polymer films. This has made the investigation of the correct energetics of the conjugated polymer-electrode interface impossible. Also, this has hampered the development of devices including ultrathin conjugated polymer layers. Here, LangmuirShafer-manufactured homogenous mono-and multilayers of semiconducting polymers on metal electrodes are reported and the energy level bending using photoelectron spectroscopy is tracked. The amorphous films display an abrupt energy level bending that does not extend beyond the first monolayer. These findings provide new insights of the energetics of the polymer-electrode interface and opens up for new high-performing devices based on ultrathin semiconducting polymers.

In electronics, the field-effect transistor (FET) is a crucial cornerstone and successful integration of this semiconductor device into circuit applications requires stable and ideal electrical characteristics over a wide range of temperatures and environments. Solution processing, using printing or coating techniques, has been explored to manufacture organic field-effect transistors (OFET) on flexible carriers, enabling radically novel electronics applications. Ideal electrical characteristics, in organic materials, are typically only found in single crystals. Tiresome growth and manipulation of these hamper practical production of flexible OFETs circuits. To date, neither devices nor any circuits, based on solution-processed OFETs, has exhibited an ideal set of characteristics similar or better than todays FET technology based on amorphous silicon. Here, bar-assisted meniscus shearing of dibenzo-tetrathiafulvalene to coat-process self-organized crystalline organic semiconducting domains with high reproducibility is reported. Including these coatings as the channel in OFETs, electric field and temperature-independent charge carrier mobility and no bias stress effects are observed. Furthermore, record-high gain in OFET inverters and exceptional operational stability in both air and water are measured.

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Regular energetics at a conjugated electrolyte/electrode modifier are found and controlled by equilibration of the Fermi level and an additional interface double dipole step induced by ionic functionality. Based on the results, design rules for conjugated electrolyte/electrode modifiers to achieve the smallest charge injection/exaction barrier and break through the current thickness limitation are proposed.