Remotely Modulating the Optical Properties of Organic Charge-Transfer Crystallites via Molecular Packing

Organic charge-transfer complex (CTC) formation has emerged as an effective molecular engineering strategy for achieving the desired optical properties via intermolecular interactions. By synthesizing organic CTCs with carbazole-based electron donors and a 7,7,8,8-tetracyanoquinodimethane acceptor and adopting a molecular linker located remotely from the charge-transfer interface within the donors, we were able to modulate near-infrared absorptive and short-wavelength infrared emissive properties. Structural characterizations performed by using single-crystal X-ray diffraction confirmed that the unique molecular arrangements induced by the steric hindrance from the remotely located linker significantly influence the electronic interactions between the donor and acceptor molecules, resulting in different photophysical properties. Our findings offer an improved understanding of the interplay between molecular packing and optoelectronic properties, providing a foundation for designing advanced materials for optoelectronic applications.