While the external quantum efficiency (EQE) of iridium(III) (Ir(III)) phosphor based near-infrared organic light-emitting diodes (NIR OLEDs) has been limited to 5.7% to date, there is no significant EQE improvement for these types of OLEDs due to the lack of efficient Ir(III) emitters. Here, a convenient approach within three synthetic steps is developed to afford two novel and efficient deep-red to near-infrared (DR-NIR) emitting phosphors (CNIr and TCNIr), in which a cyano group is added into a commercial red emitter named Ir(piq)₂(acac) to significantly stabilize the lowest unoccupied molecular orbitals of the newly designed Ir(III) complexes. They emit strong DR-NIR phosphorescence emissions at a wavelength of around 700 nm, with relatively high absolute quantum efficiencies of around 45% for their doped films. DR-NIR OLEDs made using CNIr and TCNIr exhibit high-efficiencies, affording peak EQEs of 10.62% and 9.59% with emission peak wavelengths of 690 and 706 nm, respectively. All these devices represent the most efficient Ir(III)-based DR-NIR OLEDs with a similar color gamut. The simplified synthesis procedure of the DR-NIR-emitting phosphors in conjunction with their excellent performance in OLEDs confirms our efficient strategy to achieve the DR-NIR-emitting Ir(III) phosphors.

Integrating together two dissimilar π-conjugated molecules into controlled complex topological configurations remains a largely unsolved problem owing to the diversity of organic species and their respective different assembly features. Here, we find that two structurally similar organic semiconductors, 9,10-bis(phenylethynyl)anthracene (BA) and 5,12-bis(phenylethynyl)naphthacene (BN), co-assemble into two-component helices by control of the growth kinetics as well as the molar ratio of BA/BN. The helical superstructures made of planar and twisted bis(phenylethynyl) derivatives can be regarded as (BA)_x(BN)_1−x alloys, which are formed due to compatible structural relationship between BA and BN. Moreover, epitaxial growth of (BA)_x(BN)_1−x alloy layer on the surface of BA tube to form BA@(BA)_x(BN)_1−x core-shell structure is also achieved via a solute exchange process. The precise control over composition and morphology towards organic alloy helices and core-shell microstructures opens a door for understanding the complex co-assembly features of two or more different material partners with similar structures.