Abstract

A rational implementation and optimization of thermally activated delayed fluorescent (TADF) dendrimer emitters in light-emitting electrochemical cells (LECs) sets in the Dendri-LEC family. They feature outstanding stabilities (90/1050 h for green/yellow devices) that are comparable to the best green/yellow Ir(III)-complexes (450/500 h) and conjugated polymers (33/5500 h), while offering benefits of low-cost synthesis and easy upscaling. In particular, a fundamental molecular design that capitalizes on exchanging peripheral substituents (tert-butyl vs methoxy) to tune photophysical, electrochemical, morphological, and ion conductivity features in thin films is rationalized by temperature-dependent steady-state and time-resolved emission spectroscopy, cyclic voltammetry, atomic force microscopy, and electrochemical impedance spectroscopy techniques. Herein, a TADF mechanism associated to a reduced photoluminescence quantum yield, but an enhanced electrochemical stability and ion conductivity enables to clarify the reduced device efficiency and brightness (4.0 lm W−1@110 cd m−2 vs 3.2 lm W−1@55 cd m−2) and increased stability (90 vs 1050 h) upon using methoxy groups. What is more, this substitution enables an excellent compatibility with biogenic electrolytes keeping device performances (1.9 lm W−1@35 cd m−2 and 1300 h), while graphene-devices achieve on par figures to traditional indium–tin oxide-devices. Overall, this work establishes the bright future of dendrimer emitters toward highly stable and truly sustainable lighting sources.

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