Direct Photopatterning of Colloidal Quantum Dots with Electronically Optimized Diazirine Cross-Linkers.

Colloidal quantum dots (QDs) with a wide color gamut and high luminescent efficiency are promising for next-generation electronic and photonic devices. However, precise and scalable patterning of QDs without degrading their properties and their integration into commercially relevant devices, such as digitally addressable QD light-emitting diode (QLED) displays, remain challenging. Here, we develop electronically optimized diazirine-based cross-linkers for nondestructive, direct photopatterning of QDs and, ultimately, building the active-matrix QLED displays. The key to the cross-linker design is the introduction of electron-donating substituents that permit the formation of ground-state singlet carbenes for air-stable and benign QD photopatterning. Under ambient conditions, these cross-linkers enable the patterning of heavy metal-free QDs at a resolution of over 13,000 pixels per inch using commercial i-line photolithography. The patterned QD layers fully preserved their optical and optoelectronic properties. Pixelated electroluminescent devices with patterned InP/ZnSe/ZnS QD layers show a peak external quantum efficiency of 15.3% and a maximum luminance of about 40,000 cd m-2, outperforming those made by existing QD patterning approaches. We further show the seamless integration of patterned QLEDs with thin-film transistor circuits and the fabrication of dual-color active-matrix displays. These results underscore the importance of designing photochemistry for QD patterning, and promise the implementation of direct photopatterning methods in manufacturing commercial QLED displays and other integrated QD device platforms.

Beyond a Linker: The Role of Photochemistry of Crosslinkers in the Direct Optical Patterning of Colloidal Nanocrystals.

Surface chemistry mediated direct optical patterning represents an emerging strategy for incorporating colloidal nanocrystals (NCs) in integrated optoelectronic platforms including displays and image sensors. However, the role of photochemistry of crosslinkers and other photoactive species in patterning remains elusive. Here we show the design of nitrene- and carbene-based photocrosslinkers can strongly affect the patterning capabilities and photophysical properties of NCs, especially quantum dots (QDs). Their role beyond physical linkers stems from structure-dictated electronic configuration, energy alignment and associated reaction kinetics and thermodynamics. Patterned QD layers with designed carbene-based crosslinkers fully preserve their photoluminescent and electroluminescent properties. Patterned light emitting diodes (QLEDs) show a maximum external quantum efficiency of ≈12 % and lifetime over 4800 h, among the highest for reported patterned QLEDs. These results would guide the rational design of photoactive species in NC patterning and create new possibilities in the monolithic integration of NCs in high-performance device platforms.