Inkjet printing, a highly promising
technique for the cost-effective
fabrication of large-scale organic light-emitting devices (OLEDs),
typically necessitates the intricate alignment of precisely patterned
insulating layers. Recently, we introduced a unique single-step inkjet
printing process that produces well-patterned microinlaid spots of
functional compounds through insulating polymer layers. This approach
exploits lateral phase separation between the solute of functional
compounds and the polymer, allowing the simultaneous spatial etching
of the polymer and the infilling of the solute using a single inkjet-printed
sessile droplet. Here, we demonstrate that the interaction between
the solvent and polymer, as well as the solute and polymer, critically
determines the precision and efficiency of printing. This is particularly
evident when using either the insulating poly(vinylpyridine) isomer
of poly(4-vinylpyridine) (P4VP) or poly(2-vinylpyridine) (P2VP) with
chloroform as a solvent, which allows for a detailed examination of
these interactions based on certain solubility parameters. Micro-Raman
spectroscopy reveals that the self-organizing capability of the microinlaid
spots with P4VP is superior to that with P2VP. This is due to the
fact that P2VP shows higher affinity to the solvent and causes imperfect
phase separation as compared to P4VP. As a result, a performance evaluation
demonstrates enhanced device performance for inkjet-printed green
micro-OLEDs with P4VP, exhibiting a higher external quantum efficiency
of 3.3% compared to that of 2.3% achieved with P2VP. These findings
elucidate the important roles of solvent–polymer and solute–polymer
interactions in the inkjet printing process, leading to interfacial
control of inkjet printing technique for the cost-effective production
of high-performance and high-resolution micro-OLEDs.