Polar Organic Charge-Transfer Complex of the Asymmetrical Component for Flexible Piezoelectric Energy Harvesting and Self-Powered Wearable Sensors

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Organic piezomaterials have attracted much attention because of their easy processing, lightweight, and mechanic flexibility properties. Developing new smart organic piezomaterials is highly required for new-generation electronic applications. Here, we found a novel organic piezomaterial of organic charge-transfer complex (CTC) consisting of dibenzcarbazole analogue (DBCz) and tetracyanoquinodimethane (TCNQ) in the molecular-level heterojunction stacking mode. The DBCz–TCNQ complex exhibited ferroelectric properties (the saturated polarization of ∼1.23 μC/cm 2 ) at room temperature with a low coercive field. The noncentrosymmetric alignment ( Pc space group) led to a spontaneous polarization of this architecture and thus was the origin of the piezoelectric behavior. Lateral piezoelectric nanogenerators (PENGs) based on the thermal evaporated CTC thin-film exhibited significant energy conversion behavior under mechanical agitation with a calculated piezoelectric coefficient ( d 31 ) of ∼33 pC/N. Furthermore, such a binary CTC thin-film constructed single-electrode PENG could show steady-state sensing performance to external stimuli as this flexible wearable device precisely detected physiological signals (e.g., finger bending, blink movement, carotid artery, etc.) with a self-powered supply. This work provides that the polar CTCs can act as efficient piezomaterials for flexible energy harvesting, conversion, and wearable sensing devices with a self-powered supply, enabling great potential in healthcare, motion detection, human–machine interfaces, etc.