Increased Brightness and Reduced Efficiency Droop in Perovskite Quantum Dot Light-Emitting Diodes using Carbazole-Based Phosphonic Acid Interface Modifiers

Abstract

We demonstrate the use of [2-($\textit{9H}$-carbazol-9-yl)ethyl]phosphonic acid (2PACz) and [2-(3,6-di-$\textit{tert}$-butyl-$\textit{9H}$-carbazol-9-yl)ethyl]phosphonic acid (t-Bu-2PACz) as anode modification layers in metal-halide perovskite quantum dot light-emitting diodes (QLEDs). Compared to conventional QLED structures with PEDOT:PSS (poly(3,4-ethylenedioxythiophene) polystyrene sulfonate)/PVK (poly(9-vinylcarbazole)) hole-transport layers, QLEDs made with phosphonic acid (PA)-modified indium tin oxide (ITO) anodes show an over 7-fold increase in brightness, achieving a brightness of 373,000 cd m$^{-2}$, one of the highest brightnesses reported to date for colloidal perovskite QLEDs. Importantly, the onset of efficiency roll-off, or efficiency droop, occurs at ~1000-fold higher current density for QLEDs made with PA-modified anodes compared to control QLEDs made with conventional PEDOT:PSS/PVK hole transport layers, allowing the devices to sustain significantly higher levels of external quantum efficiency at a brightness of >10$^{5}$ cd m$^{-2}$. Steady-state and time-resolved photoluminescence measurements indicate these improvements are due to a combination of multiple factors, including reducing quenching of photoluminescence at the PEDOT:PSS interface and reducing photoluminescence efficiency loss at high levels of current density.