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[Display omitted] • Indium tin oxide was hybrid modified with MoO 3 and self-assembled monolayer. • Self-assembled monolayer was used to adjust oxygen vacancies in MoO 3. • Solution-processed hole transport layer-free OLED achieved EQE max of 18.18% Compared with current vacuum-deposited multilayer organic light-emitting diodes (OLEDs), solution-processed simplified-structured OLEDs are more appealing by merits of low costs and promising potentials in large-area OLEDs. Nevertheless, it remains challenging due to intermixing between adjacent organic layers. Herein, indium tin oxide (ITO) surface was deposited with molybdenum trioxide (MoO 3) and then modified with self-assembled monolayer (SAM) of pentafluorobenzyl phosphonic acid. The SAM modification process made the MoO x film rich in oxygen vacancies, which ensured effective hole injection from the hybrid modified ITO directly to the emitting layer. This strategy facilitates HTL-free OLEDs and then completely avoids interlayer intermixing. Using the hybrid modified ITO as anode, HTL-free solution-processed green phosphorescent OLED was prepared and achieved a maximum current efficiency of 63.24 cd A−1 and a maximum external quantum efficiency of 18.18%. Meanwhile, preferable operational stability than standard multilayer OLEDs was obtained. For red phosphorescent OLED, a maximum external quantum efficiency of 17.49% was achieved. This work proposed a new way of adjusting cation valence to improve hole injection, contributing to solution-processed OLED fabrication. [ABSTRACT FROM AUTHOR]

• Two vinyl-based cross-linkable hole transporting materials are synthesized. • Cross-linking temperature is markedly lowered by doping photoinitiator. • Hole mobility is also enhanced by doping photoinitiator. • The highest external quantum efficiencies are 15.5% (green) and 15.0% (red). Recently, developing insoluble cross-linkable functional layers plays a vital role for solution-processed organic light emitting diodes (OLEDs). Here, two vinyl-based cross-linkable hole transporting materials V-TPAVTPD and V-TPAVCBP are designed and synthesized. Additionally, cationic photoinitiator 4-octyloxydiphenyliodonium hexafluoroantimonate (OPPI) is first introduced to chemically induce vinyl-based photo cross-linking process, aiming at lowering cross-linking temperature and enhancing hole mobility. As a result, cross-linking can occur at expressly low temperature of 120 °C with >95% solvent resistance. Moreover, hole mobility is markedly enhanced with the value higher than 10−3 cm2 V−1 s−1. When applying hole transporting layers (HTLs) to solution-processed green and red phosphorescent OLEDs, devices exhibit excellent properties. Particularly, the maximum current efficiency of 54.0 cd A−1 (green), 9.8 cd A−1 (red) and external quantum efficiency of 15.5% (green), 15.0% (red) are obtained when OPPI doped V-TPAVCBP serves as HTL. This low temperature feasible cross-linking process to prepare HTLs with preferable hole mobility promotes the development of OLEDs. [ABSTRACT FROM AUTHOR]