Electrochemically-stable ligands bridge the photoluminescence-electroluminescence gap of quantum dots

Abstract

Colloidal quantum dots are promising emitters for quantum-dot-based light-emitting-diodes. Though quantum dots have been synthesized with efficient, stable, and high colour-purity photoluminescence, inheriting their superior luminescent properties in light-emitting-diodes remains challenging. This is commonly attributed to unbalanced charge injection and/or interfacial exciton quenching in the devices. Here, a general but previously overlooked degradation channel in light-emitting-diodes, i.e., operando electrochemical reactions of surface ligands with injected charge carriers, is identified. We develop a strategy of applying electrochemically-inert ligands to quantum dots with excellent luminescent properties to bridge their photoluminescence-electroluminescence gap. This material-design principle is general for boosting electroluminescence efficiency and lifetime of the light-emitting-diodes, resulting in record-long operational lifetimes for both red-emitting light-emitting-diodes (T 95 > 3800 h at 1000 cd m −2 ) and blue-emitting light-emitting-diodes (T 50 > 10,000 h at 100 cd m −2 ). Our study provides a critical guideline for the quantum dots to be used in optoelectronic and electronic devices.

Full text

Its licence does not allow us to show the full text. Read it at PubMed Central:

References 50

1. 1.

   Steigerwald ML, Brus LE. Semiconductor crystallites: a class of large molecules. Acc. Chem. Res. 1990;23:183-188.

   Not in our library10.1021/ar00174a003

2. 2.

   Chen O, et al. Compact high-quality CdSe-CdS core-shell nanocrystals with narrow emission linewidths and suppressed blinking. Nat. Mater. 2013;12:445-451.

   Not in our library10.1038/nmat3539

3. 3.

   Cao HJ, et al. Design and synthesis of antiblinking and antibleaching quantum dots in multiple colors via wave function confinement. J. Am. Chem. Soc. 2016;138:15727-15735.

   Not in our library10.1021/jacs.6b10102

4. 4.

   Zhou JH, Zhu MY, Meng RY, Qin HY, Peng XG. Ideal CdSe/CdS core/shell nanocrystals enabled by entropic ligands and their core size-, shell thickness-, and ligand-dependent photoluminescence properties. J. Am. Chem. Soc. 2017;139:16556-16567.

   Not in our library10.1021/jacs.7b07434

5. 5.

   Park YS, Lim J, Klimov VI. Asymmetrically strained quantum dots with non-fluctuating single-dot emission spectra and subthermal room-temperature linewidths. Nat. Mater. 2019;18:249-255.

   Not in our library10.1038/s41563-018-0254-7

6. 6.

   Hanifi DA, et al. Redefining near-unity luminescence in quantum dots with photothermal threshold quantum yield. Science. 2019;363:1199-1202.

   Not in our library10.1126/science.aat3803

7. 7.

   Colvin VL, Schlamp MC, Alivisatos AP. Light-emitting-diodes made from cadmium selenide nanocrystals and a semiconducting polymer. Nature. 1994;370:354-357.

   Not in our library10.1038/370354a0

8. 8.

   Coe S, Woo WK, Bawendi M, Bulovic V. Electroluminescence from single monolayers of nanocrystals in molecular organic devices. Nature. 2002;420:800-803.

   Not in our library10.1038/nature01217

9. 9.

   Dai XL, et al. Solution-processed, high-performance light-emitting diodes based on quantum dots. Nature. 2014;515:96-99.

   Not in our library10.1038/nature13829

10. 10.

    Yang YX, et al. High-efficiency light-emitting devices based on quantum dots with tailored nanostructures. Nat. Photonics. 2015;9:259-266.

    Not in our library10.1038/nphoton.2015.36

11. 11.

    Oh NR, et al. Double-heterojunction nanorod light-responsive LEDs for display applications. Science. 2017;355:616-619.

    Not in our library10.1126/science.aal2038

12. 12.

    Lin X, et al. Electrically-driven single-photon sources based on colloidal quantum dots with near-optimal antibunching at room temperature. Nat. Commun. 2017;8:1132.

    Not in our library10.1038/s41467-017-01379-6

13. 13.

    Lim J, Park YS, Klimov VI. Optical gain in colloidal quantum dots achieved with direct-current electrical pumping. Nat. Mater. 2018;17:42-49.

    Not in our library10.1038/nmat5011

14. 14.

    Li XY, et al. Bright colloidal quantum dot light-emitting diodes enabled by efficient chlorination. Nat. Photonics. 2018;12:159-165.

    Not in our library10.1038/s41566-018-0105-8

15. 15.
    Highly stable QLEDs with improved hole injection via quantum dot structure tailoring · 2018

    No notice
16. 16.

    Zhang ZX, et al. High-performance, solution-processed, and insulating-layer-free light-emitting diodes based on colloidal quantum dots. Adv. Mater. 2018;30:1801387.

    Not in our library10.1002/adma.201801387

17. 17.

    Lim J, Park YS, Wu KF, Yun HJ, Klimov VI. Droop-free colloidal quantum dot light-emitting diodes. Nano Lett. 2018;18:6645-6653.

    Not in our library10.1021/acs.nanolett.8b03457

18. 18.

    Shirasaki Y, Supran GJ, Bawendi MG, Bulovic V. Emergence of colloidal quantum-dot light-emitting technologies. Nat. Photonics. 2013;7:13-23.

    Not in our library10.1038/nphoton.2012.328

19. 19.

    Acharya KP, Titov A, Ying CY, Hyvonen J, Holloway PH. High-performance quantum dot light emitting diodes and their challenges. SID Symp. Dig. Tech. Pap. 2018;49:969-972.

    Not in our library10.1002/sdtp.12207

20. 20.

    Singh S, et al. Colloidal CdSe nanoplatelets, a model for surface chemistry/optoelectronic property relations in semiconductor nanocrystals. J. Am. Chem. Soc. 2018;140:13292-13300.

    Not in our library10.1021/jacs.8b07566

21. 21.

    Zhang J, et al. Identification of facet-dependent coordination structures of carboxylate ligands on CdSe nanocrystals. J. Am. Chem. Soc. 2019;141:15675-15683.

    Not in our library10.1021/jacs.9b07836

22. 22.

    Pu CD, Peng XG. To battle surface traps on CdSe/CdS core/shell nanocrystals: shell isolation versus surface treatment. J. Am. Chem. Soc. 2016;138:8134-8142.

    Not in our library10.1021/jacs.6b02909

23. 23.

    Shim M, Guyot-Sionnest P. N-type colloidal semiconductor nanocrystals. Nature. 2000;407:981-983.

    Not in our library10.1038/35039577

24. 24.

    Simon T, et al. Redox shuttle mechanism enhances photocatalytic H-2 generation on Ni-decorated CdS nanorods. Nat. Mater. 2014;13:1013-1018.

    Not in our library10.1038/nmat4049

25. 25.

    Neyts KA. Simulation of light emission from thin-film microcavities. J. Opt. Soc. Am. A. 1998;15:962-971.

    Not in our library10.1364/josaa.15.000962

26. 26.

    Zhao J, Holmes MA, Osterloh FE. Quantum confinement controls photocatalysis: a free energy analysis for photocatalytic proton reduction at CdSe nanocrystals. ACS Nano. 2013;7:4316-4325.

    Not in our library10.1021/nn400826h

27. 27.

    Hartley CL, Dempsey JL. Electron-promoted X-type ligand displacement at CdSe quantum dot surfaces. Nano Lett. 2019;19:1151-1157.

    Not in our library10.1021/acs.nanolett.8b04544

28. 28.

    Boles MA, Ling D, Hyeon T, Talapin DV. The surface science of nanocrystals. Nat. Mater. 2016;15:141-153.

    Not in our library10.1038/nmat4526

29. 29.

    Shirasaki Y, Supran GJ, Tisdale WA, Bulovic V. Origin of efficiency roll-off in colloidal quantum-dot light-emitting diodes. Phys. Rev. Lett. 2013;110:217403.

    Not in our library10.1103/physrevlett.110.217403

30. 30.

    Impellizzeri S, et al. Structural implications on the electrochemical and spectroscopic signature of CdSe-ZnS core-shell quantum dots. J. Phys. Chem. C. 2010;114:7007-7013.

    Not in our library10.1021/jp1021032

31. 31.

    Amelia M, Lincheneau C, Silvi S, Credi A. Electrochemical properties of CdSe and CdTe quantum dots. Chem. Soc. Rev. 2012;41:5728-5743.

    Not in our library10.1039/c2cs35117j

32. 32.

    Hoener CF, et al. Demonstration of a shell core structure in layered CdSe-ZnSe Small particles by X-ray photoelectron and Auger spectroscopies. J. Phys. Chem. 1992;96:3812-3817.

    Not in our library10.1021/j100188a045

33. 33.

    Sen P, Hegde MS, Rao CNR. Surface oxidation of cadmium, indium, tin and antimony by photoelectron and Auger spectroscopy. Appl. Surf. Sci. 1982;10:63-74.

    Not in our library10.1016/0378-5963(82)90135-0

34. 34.

    Anderson NC, Hendricks MP, Choi JJ, Owen JS. Ligand exchange and the stoichiometry of metal chalcogenide nanocrystals: spectroscopic observation of facile metal-carboxylate displacement and binding. J. Am. Chem. Soc. 2013;135:18536-18548.

    Not in our library10.1021/ja4086758

35. 35.

    Owen J. The coordination chemistry of nanocrystal surfaces. Science. 2015;347:615-616.

    Not in our library10.1126/science.1259924

36. 36.

    Saniepay M, Mi CJ, Liu ZH, Abel EP, Beaulac R. Insights into the structural complexity of colloidal CdSe nanocrystal surfaces: correlating the efficiency of nonradiative excited-state processes to specific defects. J. Am. Chem. Soc. 2018;140:1725-1736.

    Not in our library10.1021/jacs.7b10649

37. 37.

    Lee KH, et al. Over 40 cd/A efficient green quantum dot electroluminescent device comprising uniquely large-sized quantum dots. ACS Nano. 2014;8:4893-4901.

    Not in our library10.1021/nn500852g

38. 38.

    Lee KH, et al. Highly efficient, color-pure, color-stable blue quantum dot light-emitting devices. ACS Nano. 2013;7:7295-7302.

    Not in our library10.1021/nn402870e

39. 39.

    Mashford BS, et al. High-efficiency quantum-dot light-emitting devices with enhanced charge injection. Nat. Photonics. 2013;7:407-412.

    Not in our library10.1038/nphoton.2013.70

40. 40.

    Tan R, et al. Monodisperse hexagonal pyramidal and bipyramidal wurtzite CdSe-CdS core-shell nanocrystals. Chem. Mater. 2017;29:4097-4108.

    Not in our library10.1021/acs.chemmater.7b00968

Reads

A person counts once a day per paper. We keep no cookie and no address: a reader is a hash that changes every day. Any month under five reads shows no number.