A class
of solution-processable, donor–acceptor-decorated dithienophosphole
oxide derivatives has been successfully synthesized and employed to
fabricate solution-processed resistive memory devices with a simple
indium–tin oxide/active layer/aluminum structure. The intramolecular
charge transfer (ICT) characters of the donor–acceptor dithienophosphole
oxide derivatives were established from photophysical, solvatochromic,
and computational studies. The number of conductance states in the
organic memory devices was found to be altered by slight changes in
molecular structures. The mechanism for the tristable memory property
of the devices was proposed based on the correlation of the extent
of ICT characters and the computed structural parameters of the compounds,
current–voltage characteristics of the devices and the fitting
to theoretical conduction models. These findings offer important insights
for the realization of multilevel resistive memory devices through
the modification of the ICT character of the active compounds.