N-type organic mixed ionic electronic conductors
(n-OMIECs) struggle to match the performance of p-type counterparts,
particularly in bioelectronics' flagship device, the organic electrochemical
transistor. Enhancing n-type transistor performance typically necessitates the
synthesis of new materials. More sustainable post-synthetic treatments, known
to improve organic devices in dry and oxygen-free conditions, are not applied
to n-OMIECs. This study introduces thermal annealing to enhance n-OMIECs' electron
mobility without sacrificing their ability to take up ionic charges. Annealing
increases the crystallinity of p(gNDI-gT2), the first designed n-OMIEC,
enhancing its transistor performance to compete with new-generation NDI-based
materials. Annealing reduces passive and in operando electrolyte uptake without
compromising the device threshold voltage, keeping the device power demand low.
The microstructure obtained by annealing, combined with the film's strong
near-infrared (NIR) absorption and reduced water swelling, enables the creation
of a device that retains photocurrent generated upon frequency-dependent light
training. This leads to a microscale, water-compatible memory device that
emulates the learning process of biological neurons triggered by light. This
simple device can be implemented in artificial neural networks and face
recognition platforms and achieve vector-matrix multiplication when fabricated
in an array form, showcasing the potential for innovative applications in
bioelectronics.