As a fascinating information storage device, organic transistor memory based on molecular charge storage elements (MCSEs) has attracted great research interest. However, the charge storage mechanism of MCSEs is ambiguous due to their complex charge dynamic behaviors. Herein, the dipole moment effects on the charge trapping process and the performance of transistor memory are revealed based on cruciform spiro[fluorene-9,9′-xanthene] (SFXs), incorporating cyano moieties, as the typical electronwithdrawing substitution. The characterization of electrostatic potential (ESP) calculation, UV−vis, photoluminescence, and crystallography of SFXs shows the SFXs MCSEs with weaker dipole moment through symmetrical substitution. A series of prototype transistor memories based on SFXs exhibit an erasable type feature with smart photoresponsive behavior. The weaker dipole moment ones possess larger memory window (∼40 V), higher charge trapping density (>1 × 10 13 cm −2 ), and higher programming speed (10 14 −10 11 cm −2 s −1 ). The hole trapping process is dominated by the dipole moment rather than the charge dissipation when compared with different SFXs at the same HOMO level. Rather good charge retention property (>10 4 s) and large on/off ratio (∼10 4 ) are obtained by blending SFXs with polymer dielectrics in optimized devices. The dipole moment effects on the charge trapping behavior provide not only the design of high performance transistor memory but also the smart information encryption in future data storage.
■ INTRODUCTIONOrganic memory devices have attracted extensive attention for the future information storage toward the era of big data and flexible electronics on account of their good scalability, light weight, and low-cost fabrication process. 1−4 The nonvolatile organic field-effect transistor (OFET) memory is one of the most striking devices with nondestructive read-out and multibit storage property, whose conductivity can be easily manipulated by tuning the charge behavior between the channels. 5−7 Furthermore, the open channel of FET configuration facilitates the charge tuning through the external stimulation such as light irradiation and gas or biomaterial exposure, leading to remarkable smart responsive behavior. 8−11 The thorny challenge in OFET memory is the design of trapping element and getting deep insight into the trapping mechanism with high density and long-term charge maintenance.The molecular charge storage elements (MCSEs) have great superiority in charge density over the well-investigated nanofloating gate 12−15 with a designable molecular structure, flexible synthesis, and tunable bandgap. 16,17 However, the memory performance is dominated not only by the F−N (Fowler−Nordheim) tunneling barrier between the transport layer and MCSEs but also by several other factors. 18−20 Because of the polymorphic behavior in the condensed state, the polymer-based MCSEs are ambiguous in charge trapping mechanism; meanwhile, they have several drawbacks such as multistep synthesis and uncontrollable molecular we...