Skip to main content

Thank you for visiting nature.com. You are using a browser version with limited support for CSS. To obtain the best experience, we recommend you use a more up to date browser (or turn off compatibility mode in Internet Explorer). In the meantime, to ensure continued support, we are displaying the site without styles and JavaScript.

  • Article
  • Published:

High-efficiency light-emitting devices based on quantum dots with tailored nanostructures

Abstract

We report a full series of blue, green and red quantum-dot-based light-emitting devices (QD-LEDs), all with high external quantum efficiencies over 10%. We show that the fine nanostructure of quantum dots—especially the composition of the graded intermediate shell and the thickness of the outer shell—plays a very important role in determining QD-LED device performance due to its effects on charge injection, transport and recombination. These simple devices have maximum current and external quantum efficiencies of 63 cd A−1 and 14.5% for green QD-LEDs, 15 cd A−1 and 12.0% for red devices, and 4.4 cd A−1 and 10.7% for blue devices, all of which are well maintained over a wide range of luminances from 102 to 104 cd m−2. All the QD-LEDs are solution-processed for ease of mass production, and have low turn-on voltages and saturated pure colours. The green and red devices exhibit lifetimes of more than 90,000 and 300,000 h, respectively.

This is a preview of subscription content, access via your institution

Access options

Buy this article

Prices may be subject to local taxes which are calculated during checkout

Figure 1: Surface elemental composition evolution with reaction time by XPS characterization, TEM characterization and photoluminescence spectra of green quantum dots.
Figure 2: Schematic of device structure, energy levels and electroluminescence performance of green QD-LEDs.
Figure 3: Electroluminescence performance of red and deep blue QD-LEDs.
Figure 4: Electroluminescence spectra, CIE coordinates and operating lifetime of QD-LEDs.
Figure 5: Monochrome active matrix QD-LED display prototypes.

Similar content being viewed by others

References

  1. Ekimov, A. I. & Onushchenko, A. A. Quantum size effect in 3-dimensional microscopic semiconductor crystals. J. Exp. Theor. Phys. Lett. 34, 345–349 (1981).

    Google Scholar 

  2. Efros, A. L. Interband absorption of light in a semiconductor sphere. Sov. Phys. Semicond. 16, 772–775 (1982).

    Google Scholar 

  3. Brus, L. E. A simple model for the ionization potential, electron affinity, and aqueous redox potentials of small semiconductor crystallites. J. Chem. Phys. 79, 5566–5571 (1983).

    Article  ADS  Google Scholar 

  4. Brus, L. Electronic wave-functions in semiconductor clusters—experiment and theory. J. Phys. Chem. 90, 2555–2560 (1986).

    Article  Google Scholar 

  5. Alivisatos, A. P. Semiconductor clusters, nanocrystals, and quantum dots. Science 271, 933–937 (1996).

    Article  ADS  Google Scholar 

  6. Lim, J. et al. Perspective on synthesis, device structures, and printing processes for quantum dot displays. Opt. Mater. Express 2, 594–628 (2012).

    Article  ADS  Google Scholar 

  7. Shirasaki, Y., Supran, G. J., Bawendi, M. G. & Bulovic, V. Emergence of colloidal quantum-dot light-emitting technologies. Nature Photon. 7, 13–23 (2012).

    Article  ADS  Google Scholar 

  8. Coe, S., Woo, W. K., Bawendi, M. & Bulovic, V. Electroluminescence from single monolayers of nanocrystals in molecular organic devices. Nature 420, 800–803 (2002).

    Article  ADS  Google Scholar 

  9. Sun, Q. et al. Bright, multicoloured light-emitting diodes based on quantum dots. Nature Photon. 1, 717–722 (2007).

    Article  ADS  Google Scholar 

  10. Caruge, J. M., Halpert, J. E., Wood, V., Bulovic, V. & Bawendi, M. G. Colloidal quantum-dot light-emitting diodes with metal-oxide charge transport layers. Nature Photon. 2, 247–250 (2008).

    Article  Google Scholar 

  11. Cho, K. S. et al. High-performance crosslinked colloidal quantum-dot light-emitting diodes. Nature Photon. 3, 341–345 (2009).

    Article  ADS  Google Scholar 

  12. Kim, T. H. et al. Full-colour quantum dot displays fabricated by transfer printing. Nature Photon. 5, 176–182 (2011).

    Article  ADS  Google Scholar 

  13. Qian, L., Zheng, Y., Xue, J. & Holloway, P. H. Stable and efficient quantum-dot light-emitting diodes based on solution-processed multilayer structures. Nature Photon. 5, 543–548 (2011).

    Article  ADS  Google Scholar 

  14. Kwak, J. et al. Bright and efficient full-color colloidal quantum dot light-emitting diodes using an inverted device structure. Nano Lett. 12, 2362–2366 (2012).

    Article  ADS  Google Scholar 

  15. Lee, K. H. et al. Highly efficient, color-pure, color-stable blue quantum dot light-emitting devices. ACS Nano 7, 7295–7302 (2013).

    Article  Google Scholar 

  16. Mashford, B. S. et al. High-efficiency quantum-dot light-emitting devices with enhanced charge injection. Nature Photon. 7, 407–412 (2013).

    Article  ADS  Google Scholar 

  17. Lee, K. H. et al. Over 40 cd/A efficient green quantum dot electroluminescent device comprising uniquely large-sized quantum dots. ACS Nano 8, 4893–4901 (2014).

    Article  Google Scholar 

  18. Dai, X. et al. Solution-processed, high-performance light-emitting diodes based on quantum dots. Nature 515, 86–89 (2014).

    Article  ADS  Google Scholar 

  19. Adachi, C., Baldo, M. A., Thompson, M. E. & Forrest, S. R. Nearly 100% internal phosphorescence efficiency in an organic light-emitting device. J. Appl. Phys. 90, 5048–5051 (2001).

    Article  ADS  Google Scholar 

  20. Baldo, M. A., Lamansky, S., Burrows, P. E., Thompson, M. E. & Forrest, S. R. Very high-efficiency green organic light-emitting devices based on electrophosphorescence. Appl. Phys. Lett. 75, 4–6 (1999).

    Article  ADS  Google Scholar 

  21. Baldo, M. A. et al. Highly efficient phosphorescent emission from organic electroluminescent devices. Nature 395, 151–154 (1998).

    Article  ADS  Google Scholar 

  22. Wang, X. et al. Non-blinking semiconductor nanocrystals. Nature 459, 686–689 (2009).

    Article  ADS  Google Scholar 

  23. Mahler, B. et al. Towards non-blinking colloidal quantum dots. Nature Mater. 7, 659–664 (2008).

    Article  ADS  Google Scholar 

  24. Chen, O. et al. Compact high-quality CdSe–CdS core–shell nanocrystals with narrow emission linewidths and suppressed blinking. Nature Mater. 12, 445–451 (2013).

    Article  ADS  Google Scholar 

  25. Li, J. et al. Large-scale synthesis of nearly monodisperse CdSe/CdS core/shell nanocrystals using air-stable reagents via successive ion layer adsorption and reaction. J. Am. Chem. Soc. 125, 12567–12575 (2003).

    Article  Google Scholar 

  26. Shen, H. et al. High quality synthesis of monodisperse zinc-blende CdSe and CdSe/ZnS nanocrystals with a phosphine-free method. CrystEngComm 11, 1733–1738 (2009).

    Article  Google Scholar 

  27. Pal, B. N. et al. ‘Giant’ CdSe/CdS core/chell nanocrystal quantum dots as efficient electroluminescent materials: strong influence of shell thickness on light-emitting diode performance. Nano Lett. 12, 331–336 (2011).

    Article  ADS  Google Scholar 

  28. Jha, P. P. & Guyot-Sionnest, P. Photoluminescence switching of charged quantum dot films. J. Phys. Chem. C 111, 15440–15445 (2007).

    Article  Google Scholar 

  29. Woo, W. K. et al. Reversible charging of CdSe nanocrystals in a simple solid-state device. Adv. Mater. 14, 1068–1071 (2002).

    Article  Google Scholar 

  30. Htoon, H. et al. Highly emissive multiexcitons in steady-state photoluminescence of individual ‘giant’ CdSe/CdS core/shell nanocrystals. Nano Lett. 10, 2401–2407 (2010).

    Article  ADS  Google Scholar 

  31. Jin, S., Song, N. & Lian, T. Suppressed blinking dynamics of single QDs on ITO. ACS Nano 4, 1545–1552 (2010).

    Article  Google Scholar 

  32. Wu, X. & Yeow, E. K. L. Charge-transfer processes in single CdSe/ZnS quantum dots with p-type NiO nanoparticles. Chem. Commun. 46, 4390–4392 (2010).

    Article  Google Scholar 

  33. Bae, W. K., Char, K., Hur, H. & Lee, S. Single-step synthesis of quantum dots with chemical composition gradients. Chem. Mater. 20, 531–539 (2008).

    Article  Google Scholar 

  34. Li, S., Steigerwald, M. L. & Brus, L. E. Surface states in the photoionization of high-quality CdSe core/shell nanocrystals. ACS Nano 3, 1267–1273 (2009).

    Article  Google Scholar 

  35. Cherniavskaya, O., Chen, L. W., Islam, M. A. & Brus, L. Photoionization of individual CdSe/CdS core/shell nanocrystals on silicon with 2-nm oxide depends on surface band bending. Nano Lett. 3, 497–501 (2003).

    Article  ADS  Google Scholar 

  36. Wei, S. & Zunger, A. Calculated natural band offsets of all IIVI and IIIV semiconductors: chemical trends and the role of cation d orbitals. Appl. Phys. Lett. 72, 2011–2013 (1998).

    Article  ADS  Google Scholar 

  37. Bae, W. K., Nam, M. K., Char, K. & Lee, S. Gram-scale one-pot synthesis of highly luminescent blue emitting Cd1−xZnxS/ZnS nanocrystals. Chem. Mater. 20, 5307–5313 (2008).

    Article  Google Scholar 

  38. Bae, W. K. et al. Highly efficient green-light-emitting diodes based on CdSe@ZnS quantum dots with a chemical-composition gradient. Adv. Mater. 21, 1690–1694 (2009).

    Article  Google Scholar 

  39. Dabbousi, B. O. et al. (CdSe)ZnS core–shell quantum dots: synthesis and characterization of a size series of highly luminescent nanocrystallites. J. Phys. Chem. B 101, 9463–9475 (1997).

    Article  Google Scholar 

  40. Qian, L. et al. Electroluminescence from light-emitting polymer/ZnO nanoparticle heterojunctions at sub-bandgap voltages. Nano Today 5, 384–389 (2010).

    Article  Google Scholar 

  41. Pandey, A. K. & Nunzi, J. M. Rubrene/fullerene heterostructures with a half-gap electroluminescence threshold and large photovoltage. Adv. Mater. 19, 3613–3617 (2007).

    Article  Google Scholar 

  42. Pechstedt, K., Whittle, T., Baumberg, J. & Melvin, T. Photoluminescence of colloidal CdSe/ZnS quantum dots: the critical effect of water molecules. J. Phys. Chem. C 114, 12069–12077 (2010).

    Article  Google Scholar 

  43. Cordero, S. R., Carson, P. J., Estabrook, R. A., Strouse, G. F. & Buratto, S. K. Photo-activated luminescence of CdSe quantum dot monolayers. J. Phys. Chem. B 104, 12137–12142 (2000).

    Article  Google Scholar 

  44. Dembski, S. et al. Photoactivation of CdSe/ZnS quantum dots embedded in silica colloids. Small 4, 1516–1526 (2008).

    Article  Google Scholar 

  45. Zhang, J., Li, D., Wu, W., Wu, H. & Zhu, W. Lifetime prediction of white OLED based on MLE under lognormal distribution. J. Test. Eval. 41, 398–402 (2013).

    Google Scholar 

  46. Kim, L. et al. Contact printing of quantum dot light-emitting devices. Nano Lett. 8, 4513–4517 (2008).

    Article  ADS  Google Scholar 

  47. Haverinen, H. M., Myllyla, R. A. & Jabbour, G. E. Inkjet printed RGB quantum dot-hybrid LED. J. Disp. Technol. 6, 87–89 (2010).

    Article  ADS  Google Scholar 

  48. Forrest, S. R., Bradley, D. D. C. & Thompson, M. E. Measuring the efficiency of organic light-emitting devices. Adv. Mater. 15, 1043–1048 (2003).

    Article  Google Scholar 

Download references

Acknowledgements

This work was supported financially by the US National Science Foundation (NSF; SBIR Phase I award no. 1248863 and Phase II award no. 1353411) and the Florida High-Tech Corridor Council (FHTCC). Assistance with data collection and reduction by R. Zhou and J. Mudrick (Materials Science and Engineering, University of Florida) is acknowledged. The authors also acknowledge Shanghai Tianma Micro-Electronics Group for assistance with AM QD-LED fabrication. J.X. acknowledges financial support from the NSF Major Research Instrumentation Program for the acquisition of the PHI XPS instrument.

Author information

Authors and Affiliations

Authors

Contributions

Y.Y. and Y.Z. synthesized material, fabricated devices, collected performance data and postulated mechanisms to explain the performance of the QD-LEDs. W.C. carried out the TEM and XPS measurements. A.T. and J.H. carried out the lifetime test and fabrication of the 4.3-inch AM QD-LED prototypes. J.R.M. carried out the XRD measurement and device efficiency distribution statistics. J.X., P.H.H. and L.Q. supervised the synthesis of materials and devices, directed the collection of performance data, designed tests for the postulated mechanism, and finalized the manuscript.

Corresponding authors

Correspondence to Jiangeng Xue, Paul H. Holloway or Lei Qian.

Ethics declarations

Competing interests

The authors declare competing financial interests. Y.Y., A.T., J.H. and J.R.M. are employees of NanoPhotonica Inc., and Y.Z. and L.Q. are Founders of NanoPhotonica Inc., which is the provider of the QD-LEDs display technique and related materials.

Supplementary information

Supplementary information

Supplementary information (PDF 865 kb)

Rights and permissions

Reprints and permissions

About this article

Check for updates. Verify currency and authenticity via CrossMark

Cite this article

Yang, Y., Zheng, Y., Cao, W. et al. High-efficiency light-emitting devices based on quantum dots with tailored nanostructures. Nature Photon 9, 259–266 (2015). https://doi.org/10.1038/nphoton.2015.36

Download citation

  • Received:

  • Accepted:

  • Published:

  • Issue Date:

  • DOI: https://doi.org/10.1038/nphoton.2015.36

This article is cited by

Search

Quick links

Nature Briefing

Sign up for the Nature Briefing newsletter — what matters in science, free to your inbox daily.

Get the most important science stories of the day, free in your inbox. Sign up for Nature Briefing