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Transparent electrodes (TEs) are vital in optoelectronic devices, enabling the interaction of light and charges. While indium tin oxide (ITO) has traditionally served as a benchmark TE, its high cost prompts the exploration of alternatives to optimize electrode characteristics and improve device efficiencies. Conducting polymers, which combine polymer advantages with metal‐like conductivity, emerge as a promising solution for TEs. This work introduces a two‐in‐one electron transport layer (ETL) and TE based on films of polyethylenimine ethoxylated (PEIE)‐modified poly(benzodifurandione) (PBFDO). These PEIE‐modified PBFDO layers exhibit a unique combination of properties, including low sheet resistance (130 Ω sq−1), low work function (4.2 eV), and high optical transparency (>85% in the UV–vis‐NIR range). In contrast to commonly used poly(3,4‐ethylenedioxythiophene):poly(styrenesulfonate) (PEDOT:PSS), the doping level of PBFDO remains unaffected by the PEIE treatment, as verified through UV–vis‐NIR absorption and X‐ray photoelectron spectroscopy measurements. When employed as a two‐in‐one ETL/TE in organic solar cells, the PEIE‐modified PBFDO electrode exhibits performance comparable to conventional ITO electrodes. Moreover, this work demonstrates all‐organic solar cells with record‐high power conversion efficiencies of >15.1% under indoor lighting conditions. These findings hold promise for the development of fully printed, all‐organic optoelectronic devices. [ABSTRACT FROM AUTHOR]

Terahertz (THz) technologies provide opportunities ranging from calibration targets for satellites and telescopes to communication devices and biomedical imaging systems. A main component will be broadband THz absorbers with switchability. However, optically switchable materials in THz are scarce and their modulation is mostly available at narrow bandwidths. Realizing materials with large and broadband modulation in absorption or transmission forms a critical challenge. This study demonstrates that conducting polymer‐cellulose aerogels can provide modulation of broadband THz light with large modulation range from ≈ 13% to 91% absolute transmission, while maintaining specular reflection loss < −30 dB. The exceptional THz modulation is associated with the anomalous optical conductivity peak of conducting polymers, which enhances the absorption in its oxidized state. The study also demonstrates the possibility to reduce the surface hydrophilicity by simple chemical modifications, and shows that broadband absorption of the aerogels at optical frequencies enables de‐frosting by solar‐induced heating. These low‐cost, aqueous solution‐processable, sustainable, and bio‐friendly aerogels may find use in next‐generation intelligent THz devices. [ABSTRACT FROM AUTHOR]