‘Giant’ CdSe/CdS Core/Shell Nanocrystal Quantum Dots As Efficient Electroluminescent Materials: Strong Influence of Shell Thickness on Light-Emitting Diode Performance

We use a simple device architecture based on a poly(3,4-ethylendioxythiophene):poly(styrenesulfonate) (PEDOT:PSS)-coated indium tin oxide anode and a LiF/Al cathode to assess the effects of shell thickness on the properties of light-emitting diodes (LEDs) comprising CdSe/CdS core/shell nanocrystal quantum dots (NQDs) as the emitting layer. Specifically, we are interested in determining whether LEDs based on thick-shell nanocrystals, so-called "giant" NQDs, afford enhanced performance compared to their counterparts incorporating thin-shell systems. We observe significant improvements in device performance as a function of increasing shell thickness. While the turn-on voltage remains approximately constant for all shell thicknesses (from 4 to 16 CdS monolayers), external quantum efficiency and maximum luminance are found to be about one order of magnitude higher for thicker shell nanocrystals (≥13 CdS monolayers) compared to thinner shell structures (<9 CdS monolayers). The thickest-shell nanocrystals (16 monolayers of CdS) afforded an external quantum efficiency and luminance of 0.17% and 2000 Cd/m2, respectively, with a remarkably low turn-on voltage of ∼3.0 V.