• Energy Research

A scalable, two-step synthesis facilitates the preparation of a polymer library of varying side chain and co-monomer, enabling rapid photovoltaic device screening. FO6-T emerged as the optimal donor achieving 15.4% PCE with L8BO as the acceptor.

The production of high-performance, solution-processed kesterite Cu2ZnSn(Sx,Se1-x)4 (CZTSSe) solar cells typically relies on high-temperature crystallization processes in chalcogen-containing atmosphere and often on the use of environmentally harmful solvents, which could hinder the widespread adoption of this technology. We report a method for processing selenium free Cu2ZnSnS4 (CZTS) solar cells based on a short annealing step at temperatures as low as 350 °C using a molecular based precursor, fully avoiding highly toxic solvents and high-temperature sulfurization. We show that a simple device structure consisting of ITO/CZTS/CdS/Al and comprising an extremely thin absorber layer (∼110 nm) achieves a current density of 8.6 mA/cm(2). Over the course of 400 days under ambient conditions encapsulated devices retain close to 100% of their original efficiency. Using impedance spectroscopy and photoinduced charge carrier extraction by linearly increasing voltage (photo-CELIV), we demonstrate that reduced charge carrier mobility is one limiting parameter of low-temperature CZTS photovoltaics. These results may inform less energy demanding strategies for the production of CZTS optoelectronic layers compatible with large-scale processing techniques.

Light-induced formation of fullerene/BCP CT complexes results in new electronic states which enable efficient electron-transport through BCP to the electrode.

Emergent bioelectronic technologies are underpinned by the organic electrochemical transistor (OECT), which employs an electrolyte medium to modulate the conductivity of its organic semiconductor channel. Here we utilize postpolymerization modification (PPM) on a conjugated polymer backbone to directly introduce glycolated or anionic side chains via fluoride displacement. The resulting polymers demonstrated increased volumetric capacitances, with subdued swelling, compared to their parent polymer in p-type enhancement mode OECTs. This increase in capacitance was attributed to their modified side chain configurations enabling cationic charge compensation for thin film electrochemical oxidation, as deduced from electrochemical quartz crystal microbalance measurements. An overall improvement in OECT performance was recorded for the hybrid glycol/ionic polymer compared to the parent, owing to its low swelling and bimodal crystalline orientation as imaged by grazing-incidence wide-angle X-ray scattering, enabling its high charge mobility at 1.02 cm2·V-1·s-1. Compromised device performance was recorded for the fully glycolated derivative compared to the parent, which was linked to its limited face-on stacking, which hindered OECT charge mobility at 0.26 cm2·V-1·s-1, despite its high capacitance. These results highlight the effectiveness of anionic side chain attachment by PPM as a means of increasing the volumetric capacitance of p-type conjugated polymers for OECTs, while retaining solid-state macromolecular properties that facilitate hole transport.

AbstractOrganic semiconductors are in general known to have an inherently lower charge carrier mobility compared to their inorganic counterparts. Bimolecular recombination of holes and electrons is an important loss mechanism and can often be described by the Langevin recombination model. Here, the device physics of bulk heterojunction solar cells based on a nonfullerene acceptor (IDTBR) in combination with poly(3‐hexylthiophene) (P3HT) are elucidated, showing an unprecedentedly low bimolecular recombination rate. The high fill factor observed (above 65%) is attributed to non‐Langevin behavior with a Langevin prefactor (β/βL) of 1.9 × 10−4. The absence of parasitic recombination and high charge carrier lifetimes in P3HT:IDTBR solar cells inform an almost ideal bimolecular recombination behavior. This exceptional recombination behavior is explored to fabricate devices with layer thicknesses up to 450 nm without significant performance losses. The determination of the photoexcited carrier mobility by time‐of‐flight measurements reveals a long‐lived and nonthermalized carrier transport as the origin for the exceptional transport physics. The crystalline microstructure arrangement of both components is suggested to be decisive for this slow recombination dynamics. Further, the thickness‐independent power conversion efficiency is of utmost technological relevance for upscaling production and reiterates the importance of understanding material design in the context of low bimolecular recombination.

AbstractElectrochemically induced volume changes in organic mixed ionic‐electronic conductors (OMIECs) are particularly important for their use in dynamic microfiltration systems, biomedical machinery, and electronic devices. Although significant advances have been made to maximize the dimensional changes that can be accomplished by OMIECs, there is currently limited understanding of how changes in their molecular structures impact their underpinning fundamental processes and their performance in electronic devices. Herein, a series of ethylene glycol functionalized conjugated polymers is synthesized, and their electromechanical properties are evaluated through a combined approach of experimental measurements and molecular dynamics simulations. As demonstrated, alterations in the molecular structure of OMIECs impact numerous processes occurring during their electrochemical swelling, with sidechain length shortening decreasing the number of incorporated water molecules, reducing the generated void volumes and promoting the OMIECs to undergo different phase transitions. Ultimately, the impact of these combined molecular processes is assessed in organic electrochemical transistors, revealing that careful balancing of these phenomena is required to maximize device performance.

Nonradiative recombination reduces the open-circuit voltage relative to its theoretical limit and leads to reduced luminescence emission at a given excitation. Therefore, it is possible to correlat...