Tuning the performance of hybrid organic/inorganic quantum dot light-emitting devices

The luminescence of inorganic core-shell semiconductor nanocrystal quantum dots (QDs) can be tuned across much of the visible spectrum by changing the size of the QDs while preserving a spectral full width at half maximum (FWHM) as narrow as 30 nm and photoluminescence efficiency of 50% [Journal of Physical Chemistry B 101 (46) (1997) 9463] [1]. Organic capping groups, surrounding the QD lumophores, facilitate processing in organic solvents and their incorporation into organic thin film light-emitting device (LED) structures [Nature 370 (6488) (1994) 354] [2]. A recent study has shown that hybrid organic/inorganic QD-LEDs can indeed be fabricated with high brightness and small spectral FWHM, utilizing a phase segregation process which self-assembles CdSe(ZnS) core(shell) QDs onto an organic thin film surface [Nature 420 (6917) (2002) 800] [3]. We now demonstrate that the phase segregation process can be generally applied to the fabrication of QD-LEDs containing a wide range of CdSe particle sizes and ZnS overcoating thicknesses. By varying the QD core diameter from 32 Angstrom to 58 Angstrom, we show that peak electroluminescence is tuned from 540 nm to 635 nm. Increase in the QD shell thickness to 2.5 monolayers (similar to0.5 nm) improves the LED external quantum efficiency, consistent with a Forster energy transfer mechanism of generating QD excited states. In this work we also identify the challenges in designing devices with very thin (similar to5 nm thick) emissive layers [Chemical Physics Letters 178 (5-6) (1991) 488] [4], emphasizing the increased need for precise exciton confinement. In both QD-LEDs and archetypical all-organic LEDs with thin emissive layers, we show that there is an increase in the exciton recombination region width as the drive current density is increased. Overall, our study demonstrates that integration of QDs into organic LEDs has the potential to enhance the performance of thin film light emitters, and promises to be a rich field of scientific endeavor. (C) 2003 Elsevier B.V. All rights reserved.