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In this paper, an extensive investigation of hybrid molecular/Si field-effect memories is presented, where redox ferrocene (Fc) molecules play the role of the memory charge storage nodes. Engineering of the organic linkers between Fc and Si is achieved by grafting Fc with different linker lengths. The study shows a clear correlation between results from atomistic computational density functional theory, electrochemical measurements (cyclic voltammetry) and electrical data obtained by a detailed study on capacitors and pseudo-MOS devices. Physical-chemical analyses (atomic force microscopy, high-resolution transmission electron microscopy, and X-ray photoelectron spectroscopy), corroborate the quality of molecular layers on devices.