The highly efficient single-junction bulk-heterojunction (BHJ) PM6:Y6 system can achieve high open circuit voltages (V OC) while maintaining exceptional fill-factor (FF) and short-circuit current (J SC) values. With a low energetic offset, the blend system was found to exhibit radiative and nonradiative recombination losses that are among the lower reported values in the literature. Recombination and extraction dynamic studies revealed that the device shows moderate nongeminate recombination coupled with exceptional extraction throughout the relevant operating conditions. Several surface and bulk characterization techniques were employed to understand the phase separation, long-range ordering, as well as donor:acceptor (D:A) inter-and intramolecular interactions at an atomic-level resolution. This was achieved using photo-conductive atomic force microscopy (pc-AFM), grazing incidence wide angle x-ray scattering (GIWAXS), and solid-state 19 F Magic-Angle Spinning (MAS) NMR spectroscopy. The synergy of multifaceted characterization and device physics was used to uncover key insights, for the first time, on the structure-property relationships of this high performing BHJ blend. Detailed information about atomically resolved D:A interactions and packing revealed that the high performance of over 15% efficiency in this blend can be correlated to a beneficial morphology that allows high J SC and FF to be retained despite the low energetic offset.

Some fundamental questions in the organic solar cell (OSC) community are related to the role of bulk and interfacial morphology on key processes such as charge generation, recombination, and extraction...

Even though significant breakthroughs with over 17% power conversion efficiencies (PCEs) in polymer:non-fullerene acceptor (NFA) bulk heterojunction organic solar cells (OSCs) have been achieved, not many studies have focused on acquiring a comprehensive understanding of the underlying mechanisms governing these systems. This is because it can be challenging to delineate device photophysics in polymer:NFA blends comprehensively, and even more complicated to trace the origins of the differences in device photophysics to the subtle differences in energetics and morphology. Here, a systematic study of a series of polymer:NFA blends was conducted to unify and correlate the cumulative effects of i) voltage losses ii) charge generation efficiencies, iii) nongeminate recombination and extraction dynamics, and iv) nuanced morphological differences with device performances. Most importantly, a deconvolution of the major loss processes in polymer:NFA blends and their connections to the complex BHJ morphology and energetics were established. An extension to advanced morphological techniques, such as solid-state NMR (for atomic level insights on the local ordering and donor:acceptor π-π interactions) and resonant soft x-ray scattering (for donor and acceptor interfacial area and domain spacings), provided detailed insights on how efficient charge generation, transport, and extraction processes can outweigh increased voltage losses to yield high PCEs.

Continuously enhanced photoresponsivity and suppressed dark/noise current combinatorially lead to the recent development of high-detectivity organic photodetectors with broadband sensing competence. Despite the achievements, reliable photosensing enabled by organic photodetectors (OPDs) still faces challenges. Herein, we call for heed over a universal phenomenon of detrimental sensitivity of dark current to illumination history in high-performance inverted OPDs. The phenomenon, unfavorable to the attainment of high sensitivity and consistent figures-of-merit, is shown to arise from exposure of the commonly used electron transport layer in OPDs to high-energy photons and its consequent loss of charge selectivity via systematic studies. To solve this universal problem, “double” layer tin oxide as an alternative electron transport layer is demonstrated, which not only eliminates the inconsistency between the initial and after-illumination dark current characteristics but also preserves the low magnitude of dark current, good external quantum efficiency, and rapid transient response.

PCPDTBT-SO3K (CPE-K), a conjugated polyelectrolyte, is presented as a mixed conductor material which can be used to fabricate high transconductance accumulation mode organic electrochemical transistors (OECTs). OECTs have been utilized in a wide range of applications such as analyte This article is protected by copyright. All rights reserved. 2 detection, neural interfacing, impedance sensing and neuromorphic computing. We demonstrate the use of interdigitated contacts to enable high transconductance in a relatively small device area in comparison to standard contacts. Such characteristics are highly desired in applications such as neural activity sensing, where device area must be minimized to reduce invasiveness. The physical and electrical properties of CPE-K have been fully characterized to allow a direct comparison to other top performing OECT materials. CPE-K demonstrates an electrical performance that is among the best that have been reported in the literature for OECT materials. In addition, CPE-K OECTs operate in the accumulation mode, which allows for much lower energy consumption in comparison to commonly used depletion mode devices.

The environmental impact of solution processed organic solar cells (OSCs) can be mitigated by introducing so‐called green solvents during the fabrication processes. However, the effects of such green solvents on the molecular‐level structures and optoelectronic properties lack in‐depth characterization. Here, insights into the structure–processing–property correlation of a PPDT2FBT:PC61BM bulk‐heterojunction (BHJ) system processed from a green solvent, ortho‐xylene (o‐XY), is investigated in comparison with the same blend processed from a traditional halogenated solvent, chlorobenzene (CB). The BHJ blends are characterized with various techniques probing at difference length scales, and an increased donor:acceptor (D:A) interfacial area as well as well‐mixed features in the bulk morphologies of the active layer are observed for the o‐XY processed BHJ blend. Furthermore, molecular‐level differences in the D–A intermolecular interactions at the BHJ interfaces in o‐XY and CB cast films are elucidated by 2‐dimensional solid‐state nuclear magnetic resonance (ssNMR) measurements and analysis. These results are consistent with the device properties, suggesting that the green‐solvent‐processed devices have longer charge carrier lifetimes and faster charge carrier extraction. The optimized PPDT2FBT:PC61BM devices processed from o‐XY can achieve a noteworthy higher power conversion efficiency (PCE) owing to a higher short‐circuit current density and fill factor.

Tetracyanoquinodimethane leads to trap-enhanced photoconductive gain and highly efficient broadband sensing for bulk heterojunction organic photodetectors.