The synthesis of three novel phosphonate-substituted aromatic diimides is described: N,N '-bis(2-phosphonoethyl)pyromellitimide (PPMI), N,N '-bis(2-phosphonoethyl)-1,4,5,8-naphthalenediimide (PNDI) and N,N '-bis(2-phosphonoethyl)-3,4,9,10-perylenediimide (PPDI). The imides are water-soluble, allowing spectroscopical studies to be performed in water. PPMI and PNDI exist in the monomeric form in water, but PPDI formed dimers. Self-assembled thin films of the three compounds were gown on phosphonate-primed silicon and quartz substrates by the zirconium phosphonate method. Film growth was followed by ellipsometry (silicon) and ultraviolet/visible absorption spectroscopy (quartz). The films obtained were highly thermally and solvolitically stable for all the three imides, making them excellent candidates for applications in nanotechnological devices. (c) 2005 Elsevier B.V All rights reserved.