%0 Journal Article %A Alonso-Navarro, Matías J. %A Suárez-Blas, Fátima %A Martínez, jose Ignacio %A Ramos, M. Mar %A Segura Castedo, José Luis %T Giant fully-fused tetrapodal rylenimides: Design, synthesis and optoelectrochemical characterization via alkyl chain and core engi-neering strategies %D 2025 %U https://hdl.handle.net/20.500.14352/123763 %X In this work, we report the synthesis and comprehensive characterization of a new series of fully fused three-dimensional rylenimide-based derivatives featuring extended π-conjugation through core-fusion strategies and tailored side-chain engineering at the imide nitrogen, resulting in molecular architectures with up to 19 fused rings. The effects of π-extension and alkyl/aryl imide substituents on the optical and electrochemical behavior were systematically studied using UV–vis spectroscopy, cyclic voltammetry, and density functional theory calculations. The results demonstrate that combining π-extension with bulky solubilizing groups effectively suppresses undesired π–π interactions, enhances electronic delocalization, and improves device-relevant properties. This molecular design strategy offers a promising platform for the development of next-generation functional n-type organic semiconductors. %~