Tuning Ambipolarity of the Conjugated Polymer Channel Layers of Floating-Gate Free Transistors: From Volatile Memories to Artificial Synapses.

Three-terminal synaptic transistor has drawn significant research interests for neuromorphic computation due to its advantage of facile device integrability. Lately, bulk-heterojunction-based synaptic transistors with bipolar modulation are proposed to exempt the use of an additional floating gate. However, the actual correlation between the channel's ambipolarity, memory characteristic, and synaptic behavior for a floating-gate free transistor has not been investigated yet. Herein, by studying five diketopyrrolopyrrole-benzotriazole dual-acceptor random conjugated polymers, a clear correlation among the hole/electron ratio, the memory retention characteristic, and the synaptic behavior for the polymer channel layer in a floating-gate free transistor is described. It reveals that the polymers with balanced ambipolarity possess better charge trapping capabilities and larger memory windows; however, the high ambipolarity results in higher volatility of the memory characteristics, namely poor memory retention capability. In contrast, the polymer with a reduced ambipolarity possesses an enhanced memory retention capability despite showing a reduced memory window. It is further manifested that this enhanced charge retention capability enables the device to present artificial synaptic characteristics. The results highlight the importance of the channel's ambipolarity of floating-gate free transistors on the resultant volatile memory characteristics and synaptic behaviors.

Solution-Processable Anion-doped Conjugated Polymer for Nonvolatile Organic Transistor Memory with Synaptic Behaviors.

Brain-inspired synaptic transistors have been considered as a promising device for next-generation electronics. To mimic the behavior of a biological synapse, both data processing and nonvolatile memory capability are simultaneously required for a single electronic device. In this work, a simple approach to realize a synaptic transistor with improved memory characteristics is demonstrated by doping an ionic additive, tetrabutylammonium perchlorate (TBAP), into an active polymer semiconductor without using any extra charge storage layer. TBAP doping is first revealed to improve the memory window of a derived transistor memory device from 19 to 32 V (∼68% enhancement) with an on/off current ratio over 103 at VG = -10 V. Through morphological analysis and theoretical calculations, it is revealed that the association of anion with polymers enhances the charge retention capability of the polymer and facilitates the interchain interactions to result in improved memory characteristics. More critically, the doped device is shown to successfully mimic the synaptic behaviors, such as paired-pulse facilitation (PPF), excitatory and inhibitory postsynaptic currents, and spike-rate dependent plasticity. Notably, the TBAP-doped device is shown to deliver a PPF index of up to 204% in contrast to the negligible value of an undoped device. This study describes a novel approach to prepare a synaptic transistor by doping conjugated polymers, which can promote the future development of artificial neuromorphic systems.