Organic photodetectors (OPDs) are promising candidates for next-generation digital imaging and wearable sensors due to their low cost, tuneable optoelectrical properties combined with high-level performance, and solution-processed fabrication techniques. However, OPD detection is often limited to shorter wavelengths, whereas photodetection in the near-infrared (NIR) region is increasingly being required for wearable electronics and medical device applications. NIR sensing suffers from low responsivity and high dark currents. A common approach to enhance NIR photon detection is lowering the optical band gap via donor−acceptor (D−A) molecular engineering. Herein, we present the synthesis of two novel indacenodithiophene (IDT)based D−A conjugated polymers, namely, PDPPy-IT and PSNT-IT via palladium-catalyzed Stille coupling reactions. These novel polymers exhibit optical band gaps of 1.81 and 1.27 eV for PDPPy-IT and PSNT-IT, respectively, with highly desirable visible and NIR light detection through energy-level manipulation. Moreover, excellent materials' solubility and thin-film processability allow easy incorporation of these polymers as an active layer into OPDs for light detection. In the case of PSNT-IT devices, a photodetection up to 1000 nm is demonstrated with a peak sensitivity centered at 875 nm, whereas PDPPy-IT devices are efficient in detecting the visible spectrum with the highest sensitivity at 660 nm. Overall, both OPDs exhibit spectral responsivities up to 0.11 A W −1 and dark currents in the nA cm −2 range. With linear dynamic ranges exceeding 140 dB and fast response times recorded below 100 μs, the use of novel IDT-based polymers in OPDs shows great potential for wearable optoelectronics.

The versatile nature of organic conjugated materials renders their flawless integration into a diverse family of optoelectronic devices with light-harvesting, photodetection, or light-emitting capabilities. Classes of materials that offer the possibilities of two or more distinct optoelectronic functions are particularly attractive as they enable smart applications while providing the benefits of the ease of fabrication using low-cost processes. Here, we develop a novel, multipurpose conjugated small molecule by combining boron-azadipyrromethene (aza-BODIPY) as electron acceptor with triphenylamine (TPA) as end-capping donor units. The implemented donor-acceptor-donor (D-A-D) configuration, in the form of TPA-azaBODIPY-TPA, preserves ideal charge transfer characteristics with appropriate excitation energy levels, with the additional ability to be used as either a charge transporting interlayer or light-sensing semiconducting layer in optoelectronic devices. To demonstrate its versatility, we first show that TPA-azaBODIPY-TPA can act as an excellent hole transport layer in methylammonium lead triiodide (MAPbI 3 )-based perovskite solar cells with measured power conversion efficiencies exceeding 17%, outperforming control solar cells with PEDOT:PSS by nearly 60%. Furthermore, the optical bandgap of 1.49 eV is shown to provide significant photodetection in the wavelength range of up to 800 nm where TPA-azaBODIPY-TPA functions as donor in

This cover (DOI: 10.1002/inf2.12345) shows a multifunctional TPA‐azaBODIPY‐TPA small molecule with superior optoelectronic and photophysical properties. Material is shown to function as an efficient hole transport layer in perovskite solar cells reaching a power conversion efficiency of 17.4%, and as a robust electron donor in near‐infrared organic photodetectors absorbing light in the wavelength range of up to 800 nm. Offering two distinct optoelectronic functions, TPA‐azaBODIPY‐TPA is particularly attractive as it enables multi‐purpose applications while maintaining the ease of fabrication. image