Breaking the Trade-Off Between Polymer Dielectric Constant and Loss Via Aluminum Oxo Macrocycle Dopants for High-Performance Neuromorphic Electronics.

The dielectric layer is crucial in regulating the overall performance of field-effect transistors (FETs), the key component in central processing units, sensors, and displays. Despite considerable efforts being devoted to developing high-permittivity (k) dielectrics, limited progress has been made due to the inherent trade-off between dielectric constant and loss. Here, we present a solution by designing a monodispersed disk-shaped Ce-Al-O-macrocycle as a dopant in polymer dielectrics. The molecule features a central Ce(III) core connected with eight Al atoms through sixteen bridging hydroxyls and eight 3-aminophenyl peripheries. The incorporation of this macrocycle in polymer dielectrics results in an up to 7-fold increase in dielectric constants and up to 89% reduction in dielectric loss at low frequencies. Moreover, the leakage-current densities decrease, and the breakdown strengths are improved by 63%. Relying on the above merits, FETs bearing cluster-doped polymer dielectrics give near three-orders source-drain current increments while maintaining low-level leakage/off currents, resulting in much higher charge-carrier mobilities (up to 2.45 cm 2 V -1 s -1 ) and on/off ratios. This cluster-doping strategy is generalizable and shows great promise for ultralow-power photoelectric synapses and neuromorphic retinas. This work successfully breaks the trade-off between dielectric constant and loss and offers a unique design for polymer composite dielectrics. This article is protected by copyright. All rights reserved.