Design of High‐Performance Organic Semiconductors by Intra‐ and Intermolecular Charge Transfer Interaction

Charge transfer (CT) interactions have rarely been used to organize supramolecules and cross‐linked objects. However, the ever‐increasing understanding of CT interactions opens up new avenues for the design of innovative materials with tailored electronic properties. Herein, several molar ratios of highly crystalline π‐conjugated n %TCNQ@Sq‐1,6Py oligomers ( n equal molar ratio of tetracyanoquinodimethane (TCNQ) to 1,6‐diaminopyrene (1,6Py) moiety) with simultaneously stable intra‐ and intermolecular CT mechanisms are prepared. As a result, the π ‐conjugated 200%TCNQ@Sq‐1,6Py CT complex indicates stable intra‐ and intermolecular CT interactions resulting in extremely high electrical conductivity of 8.7 × 10 −2 S cm −1 at room temperature, a charge‐distance capacitance of 70.62 F g −1 at the current density of 0.625 A g −1 which significantly increases to 968.7 F g −1 by doping of polyaniline (PANI) at a current density of 0.312 A g −1 . Finally, it exhibits a capacitance retention of 70% of the initial specific capacitance after 1000 cycles at room temperature. This type of π ‐conjugated oligomer CT complex can be used to improve existing CT‐based energy storage devices, such as capacitors.