Abstract

Phosphorescent white organic light-emitting diodes (WOLEDs) with high efficiency and color rendering index (CRI) are demonstrated based on a macrospirocyclic oligomer matrix (TPA-PO)3, which exhibits good solution processability, stable film morphology, and excellent compatibility with phosphorescent emitters. High-efficiency blue, green, orange, and red OLEDs were demonstrated with maximum current efficiencies of 21.7, 21.9, 13.1, and 6.4 cd A−1, maximum brightness of 22475, 67757, 21232, and 8046 cd m−2, respectively. Furthermore, by simultaneously incorporating blue, green, orange, and red emitters into a single emitting layer, a quaternary doping WOLED with a maximum current efficiency of 18.9 cd A−1 (at 280 cd m−2) was realized, featuring a “warm-white” light emission with correlated color temperatures ranging from 2841 to 3514 K. Importantly, color rendering index values over 90 were obtained at practical brightness of 100 ~1000 cd m−2. Even at a high brightness of ~5000 cd m−2, the CRI was still above 88, which is among the highest CRI values achieved for solution-processed phosphorescent WOLEDs.

© 2018 Optical Society of America under the terms of the OSA Open Access Publishing Agreement

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References

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    [Crossref]
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    [Crossref]
  24. F. Meng, D. Chen, W. Xiong, H. Tan, Y. Wang, W. Zhu, and S. J. Su, “Tuning color-correlated temperature and color rendering index of phosphorescent white polymer light-emitting diodes: towards healthy solid-state lighting,” Org. Electron. 34, 18–22 (2016).
    [Crossref]
  25. M. C. Gather, A. Köhnen, and K. Meerholz, “White organic light-emitting diodes,” Adv. Mater. 23(2), 233–248 (2011).
    [Crossref] [PubMed]
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    [Crossref]
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    [Crossref]
  29. N. Li, Z. Fan, H. Zhao, Y. Quan, Q. Chen, S. Ye, S. Li, Q. Fan, and W. Huang, “A bipolar macrospirocyclic oligomer based on triphenylamine and 4,5-diazafluorene as a solution-processable host for blue phosphorescent organic light-emitting diodes,” Dyes Pigm. 134, 348–357 (2016).
    [Crossref]
  30. N. Li, Z. Fan, Y. Fang, L. Li, Y. Quan, Q. Chen, S. Ye, Q. Fan, and W. Huang, “A macrospirocyclic carbazole-fluorene oligomer as a solution-processable matrix host material for blue phosphorescent organic light-emitting diodes with low turn-on voltage and efficiency roll-off,” J. Phys. Chem. C 121(16), 8692–8702 (2017).
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    [Crossref]
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    [Crossref] [PubMed]
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    [Crossref]
  34. X. K. Liu, Z. Chen, C. J. Zheng, C. L. Liu, C. S. Lee, F. Li, X. M. Ou, and X. H. Zhang, “Prediction and design of efficient exciplex emitters for high-efficiency, thermally activated delayed-fluorescence organic light-emitting diodes,” Adv. Mater. 27(14), 2378–2383 (2015).
    [Crossref] [PubMed]
  35. W. Y. Hung, G. C. Fang, Y. C. Chang, T. Y. Kuo, P. T. Chou, S. W. Lin, and K. T. Wong, “Highly efficient bilayer interface exciplex for yellow organic light-emitting diode,” ACS Appl. Mater. Interfaces 5(15), 6826–6831 (2013).
    [Crossref] [PubMed]
  36. K. Kawasumi, T. Wu, T. Zhu, H. S. Chae, T. Van Voorhis, M. A. Baldo, and T. M. Swager, “Thermally activated delayed fluorescence materials based on homoconjugation effect of donor-acceptor triptycenes,” J. Am. Chem. Soc. 137(37), 11908–11911 (2015).
    [Crossref] [PubMed]
  37. C. F. Madigan and V. Bulović, “Solid state solvation in amorphous organic thin films,” Phys. Rev. Lett. 91(24), 247403 (2003).
    [Crossref] [PubMed]
  38. S. Ye, T. Hu, Z. Zhou, M. Yang, Q. Mei, Y. Liu, L. Liu, B. Zhai, Z. Jia, and W. Huang, “Solution processed single-emissive-layer white organic light-emitting diodes based on fluorene host: balanced consideration for color quality and electroluminescent efficiency,” Org. Electron. 33, 235–245 (2016).
    [Crossref]
  39. X. Liu, S. Wang, B. Yao, B. Zhang, C. L. Ho, W. Y. Wong, Y. Cheng, and Z. Xie, “New deep-red heteroleptic iridium complex with 3-hexylthiophene for solution-processed organic light-emitting diodes emitting saturated red and high CRI white colors,” Org. Electron. 21, 1–8 (2015).
    [Crossref]

2018 (4)

J. Y. Wu and S. A. Chen, “Development of a highly efficient hybrid white organic-light-emitting diode with a single emission layer by solution processing,” ACS Appl. Mater. Interfaces 10(5), 4851–4859 (2018).
[Crossref] [PubMed]

D. K. Dubey, M. Singh, S. Sahoo, and J. H. Jou, “Simple-structured efficient white organic light emitting diode via solution process,” Microelectron. Reliab. 83, 293–296 (2018).

Y. Miao, K. Wang, B. Zhao, L. Gao, P. Tao, X. Liu, Y. Hao, H. Wang, B. Xu, and F. Zhu, “High-efficiency/CRI/color stability warm white organic light-emitting diodes by incorporating ultrathin phosphorescence layers in a blue fluorescence layer,” Nanophotonics 7(1), 295–304 (2018).
[Crossref]

C. Coburn, C. Jeong, and S. R. Forrest, “Reliable, all-phosphorescent stacked white organic light emitting devices with a high color rendering index,” ACS Photonics 5(2), 630–635 (2018).
[Crossref]

2017 (7)

H. Guo, J. Zhao, Z. Tian, Y. Wu, B. Liu, F. Dang, X. Yang, G. Zhou, Z. Wu, and W. Y. Wong, “Homoleptic thiazole-based IrIII phosphorescent complexes for achieving both high EL efficiencies and an optimized trade-off among the key parameters of solution-processed WOLEDs,” J. Mater. Chem. C Mater. Opt. Electron. Devices 5(1), 208–219 (2017).
[Crossref]

Z. A. Hasan, K. L. Woon, W. S. Wong, A. Ariffin, and S. A. Chen, “Solution processed multilayer red, green and blue phosphorescent organic light emitting diodes using carbazole dendrimer as a host,” J. Lumin. 183, 150–158 (2017).
[Crossref]

K. Gao, K. Liu, X. L. Li, X. Cai, D. Chen, Z. Xu, Z. He, B. Li, Z. Qiao, D. Chen, Y. Cao, and S. J. Su, “An ideal universal host for highly efficient full-color, white phosphorescent and TADF OLEDs with a simple and unified structure,” J. Mater. Chem. C Mater. Opt. Electron. Devices 5(39), 10406–10416 (2017).
[Crossref]

F. Zhao and D. Ma, “Approaches to high performance white organic light-emitting diodes for general lighting,” Mater. Chem. Front. 1(10), 1933–1950 (2017).
[Crossref]

B. Liu, H. Nie, G. Lin, S. Hu, D. Gao, J. Zou, M. Xu, L. Wang, Z. Zhao, H. Ning, J. Peng, Y. Cao, and B. Z. Tang, “High-performance doping-free hybrid white OLEDs based on blue aggregation-induced emission luminogens,” ACS Appl. Mater. Interfaces 9(39), 34162–34171 (2017).
[Crossref] [PubMed]

G. Sarada, W. Cho, A. Maheshwaran, V. G. Sree, H. Y. Park, Y. S. Gal, M. Song, and S. H. Jin, “Deep-blue phosphorescent Ir(III) complexes with light-harvesting functional moieties for efficient blue and white PhOLEDs in solution-process,” Adv. Funct. Mater. 27(27), 1701002 (2017).
[Crossref]

N. Li, Z. Fan, Y. Fang, L. Li, Y. Quan, Q. Chen, S. Ye, Q. Fan, and W. Huang, “A macrospirocyclic carbazole-fluorene oligomer as a solution-processable matrix host material for blue phosphorescent organic light-emitting diodes with low turn-on voltage and efficiency roll-off,” J. Phys. Chem. C 121(16), 8692–8702 (2017).
[Crossref]

2016 (8)

S. Ye, T. Hu, Z. Zhou, M. Yang, Q. Mei, Y. Liu, L. Liu, B. Zhai, Z. Jia, and W. Huang, “Solution processed single-emissive-layer white organic light-emitting diodes based on fluorene host: balanced consideration for color quality and electroluminescent efficiency,” Org. Electron. 33, 235–245 (2016).
[Crossref]

T. H. Han, M. R. Choi, C. W. Jeon, Y. H. Kim, S. K. Kwon, and T. W. Lee, “Ultrahigh-efficiency solution-processed simplified small-molecule organic light-emitting diodes using universal host materials,” Sci. Adv. 2(10), e1601428 (2016).
[Crossref] [PubMed]

A. Liang, G. Huang, S. Dong, X. Zheng, J. Zhu, Z. Wang, W. Wu, J. Zhang, and F. Huang, “Novel iridium complexes as yellow phosphorescent emitters for single-layer yellow and white polymer light-emitting diodes,” J. Mater. Chem. C Mater. Opt. Electron. Devices 4(27), 6626–6633 (2016).
[Crossref]

X. Du, X. Yang, J. Zhao, H. Lin, C. Zheng, and S. Tao, “Highly efficient solution-processed small-molecule white organic light-emitting diodes,” Org. Electron. 38, 344–349 (2016).
[Crossref]

X. Ban, K. Sun, Y. Sun, B. Huang, and W. Jiang, “Design of high triplet energy electron transporting material for exciplex-type host: efficient blue and white phosphorescent OLEDs based on solution processing,” Org. Electron. 33, 9–14 (2016).
[Crossref]

Z. Wu and D. Ma, “Recent advances in white organic light-emitting diodes,” Mater. Sci. Eng. Rep. 107, 1–42 (2016).
[Crossref]

N. Li, Z. Fan, H. Zhao, Y. Quan, Q. Chen, S. Ye, S. Li, Q. Fan, and W. Huang, “A bipolar macrospirocyclic oligomer based on triphenylamine and 4,5-diazafluorene as a solution-processable host for blue phosphorescent organic light-emitting diodes,” Dyes Pigm. 134, 348–357 (2016).
[Crossref]

F. Meng, D. Chen, W. Xiong, H. Tan, Y. Wang, W. Zhu, and S. J. Su, “Tuning color-correlated temperature and color rendering index of phosphorescent white polymer light-emitting diodes: towards healthy solid-state lighting,” Org. Electron. 34, 18–22 (2016).
[Crossref]

2015 (7)

S. H. Ye, T. Q. Hu, Z. Zhou, M. Yang, M. H. Quan, Q. B. Mei, B. C. Zhai, Z. H. Jia, W. Y. Lai, and W. Huang, “Solution processed single-emission layer white polymer light-emitting diodes with high color quality and high performance from a poly(N-vinyl)carbazole host,” Phys. Chem. Chem. Phys. 17(14), 8860–8869 (2015).
[Crossref] [PubMed]

K. Chen, H. R. Zhao, Z. K. Fan, G. Yin, Q. M. Chen, Y. W. Quan, S. H. Li, and S. H. Ye, “Macrospirocyclic oligomer based on triphenylamine and diphenylphosphine oxide as a bipolar host for efficient blue electrophosphorescent organic light-emitting diodes (OLEDs),” Org. Lett. 17(6), 1413–1416 (2015).
[Crossref] [PubMed]

S. Wang, B. Zhang, X. Wang, J. Ding, Z. Xie, and L. Wang, “Ultrahigh color-stable, solution-processed, white OLEDs using a dendritic binary host and long-wavelength dopants with different charge trapping depths,” Adv. Opt. Mater. 3(10), 1349–1354 (2015).
[Crossref]

X. K. Liu, Z. Chen, C. J. Zheng, C. L. Liu, C. S. Lee, F. Li, X. M. Ou, and X. H. Zhang, “Prediction and design of efficient exciplex emitters for high-efficiency, thermally activated delayed-fluorescence organic light-emitting diodes,” Adv. Mater. 27(14), 2378–2383 (2015).
[Crossref] [PubMed]

D. Sun, X. Zhou, J. Liu, X. Sun, H. Li, Z. Ren, D. Ma, M. R. Bryce, and S. Yan, “Solution-processed blue/deep blue and white phosphorescent organic light-emitting diodes (PhOLEDs) hosted by a polysiloxane derivative with pendant mCP (1,3-bis(9-carbazolyl)benzene),” ACS Appl. Mater. Interfaces 7(51), 27989–27998 (2015).
[Crossref] [PubMed]

X. Liu, S. Wang, B. Yao, B. Zhang, C. L. Ho, W. Y. Wong, Y. Cheng, and Z. Xie, “New deep-red heteroleptic iridium complex with 3-hexylthiophene for solution-processed organic light-emitting diodes emitting saturated red and high CRI white colors,” Org. Electron. 21, 1–8 (2015).
[Crossref]

K. Kawasumi, T. Wu, T. Zhu, H. S. Chae, T. Van Voorhis, M. A. Baldo, and T. M. Swager, “Thermally activated delayed fluorescence materials based on homoconjugation effect of donor-acceptor triptycenes,” J. Am. Chem. Soc. 137(37), 11908–11911 (2015).
[Crossref] [PubMed]

2014 (2)

Z. Fan, N. Li, Y. Quan, Q. Chen, S. Ye, Q. Fan, W. Huang, and H. Xu, “A solution-processable triphenylamine-fluorene host for exciplex based white phosphorescent organic light-emitting diodes,” J. Mater. Chem. C Mater. Opt. Electron. Devices 2(45), 9754–9759 (2014).
[Crossref]

C. C. Fan, M. H. Huang, W. C. Lin, H. W. Lin, Y. Chi, H. F. Meng, T. C. Chao, and M. R. Tseng, “Single-emission-layer white organic light-emitting devices: chromaticity and colour-rendering consideration,” Org. Electron. 15(2), 517–523 (2014).
[Crossref]

2013 (4)

W. Y. Hung, G. C. Fang, Y. C. Chang, T. Y. Kuo, P. T. Chou, S. W. Lin, and K. T. Wong, “Highly efficient bilayer interface exciplex for yellow organic light-emitting diode,” ACS Appl. Mater. Interfaces 5(15), 6826–6831 (2013).
[Crossref] [PubMed]

J. Li, T. Zhang, Y. Liang, and R. Yang, “Solution-processible carbazole dendrimers as host materials for highly efficient phosphorescent organic light-emitting diodes,” Adv. Funct. Mater. 23(5), 619–628 (2013).
[Crossref]

Q. Fu, J. Chen, H. Zhang, C. Shi, and D. Ma, “Solution-processed single-emitting-layer white organic light-emitting diodes based on small molecules with efficiency/CRI/color-stability trade-off,” Opt. Express 21(9), 11078–11085 (2013).
[Crossref] [PubMed]

M. Y. Zhang, F. F. Wang, N. Wei, P. C. Zhou, K. J. Peng, J. N. Yu, Z. X. Wang, and B. Wei, “High color rending index and high-efficiency white organic light-emitting diodes based on the control of red phosphorescent dye-doped hole transport layer,” Opt. Express 21(S1), A173–A178 (2013).
[Crossref] [PubMed]

2012 (1)

W. Jiang, Z. Ge, P. Cai, B. Huang, Y. Dai, Y. Sun, J. Qiao, L. Wang, L. Duan, and Y. Qiu, “Star-shaped dendritic hosts based on carbazole moieties for highly efficient blue phosphorescent OLEDs,” J. Mater. Chem. 22(24), 12016–12022 (2012).
[Crossref]

2011 (1)

M. C. Gather, A. Köhnen, and K. Meerholz, “White organic light-emitting diodes,” Adv. Mater. 23(2), 233–248 (2011).
[Crossref] [PubMed]

2009 (1)

2005 (1)

X. Gong, S. Wang, D. Moses, G. C. Bazan, and A. J. Heeger, “Multilayer polymer light-emitting diodes: white-light emission with high efficiency,” Adv. Mater. 17(17), 2053–2058 (2005).
[Crossref]

2003 (1)

C. F. Madigan and V. Bulović, “Solid state solvation in amorphous organic thin films,” Phys. Rev. Lett. 91(24), 247403 (2003).
[Crossref] [PubMed]

2001 (1)

C. Adachi, M. A. Baldo, M. E. Thompson, and S. R. Forrest, “Nearly 100% internal phosphorescence efficiency in an organic light-emitting device,” J. Appl. Phys. 90(10), 5048–5051 (2001).
[Crossref]

1995 (1)

J. Kido, M. Kimura, and K. Nagai, “Multilayer white light-emitting organic electroluminescent device,” Science 267(5202), 1332–1334 (1995).
[Crossref] [PubMed]

Adachi, C.

C. Adachi, M. A. Baldo, M. E. Thompson, and S. R. Forrest, “Nearly 100% internal phosphorescence efficiency in an organic light-emitting device,” J. Appl. Phys. 90(10), 5048–5051 (2001).
[Crossref]

Ariffin, A.

Z. A. Hasan, K. L. Woon, W. S. Wong, A. Ariffin, and S. A. Chen, “Solution processed multilayer red, green and blue phosphorescent organic light emitting diodes using carbazole dendrimer as a host,” J. Lumin. 183, 150–158 (2017).
[Crossref]

Baldo, M. A.

K. Kawasumi, T. Wu, T. Zhu, H. S. Chae, T. Van Voorhis, M. A. Baldo, and T. M. Swager, “Thermally activated delayed fluorescence materials based on homoconjugation effect of donor-acceptor triptycenes,” J. Am. Chem. Soc. 137(37), 11908–11911 (2015).
[Crossref] [PubMed]

C. Adachi, M. A. Baldo, M. E. Thompson, and S. R. Forrest, “Nearly 100% internal phosphorescence efficiency in an organic light-emitting device,” J. Appl. Phys. 90(10), 5048–5051 (2001).
[Crossref]

Ban, X.

X. Ban, K. Sun, Y. Sun, B. Huang, and W. Jiang, “Design of high triplet energy electron transporting material for exciplex-type host: efficient blue and white phosphorescent OLEDs based on solution processing,” Org. Electron. 33, 9–14 (2016).
[Crossref]

Bazan, G. C.

X. Gong, S. Wang, D. Moses, G. C. Bazan, and A. J. Heeger, “Multilayer polymer light-emitting diodes: white-light emission with high efficiency,” Adv. Mater. 17(17), 2053–2058 (2005).
[Crossref]

Bryce, M. R.

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Jeong, C.

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[Crossref]

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[Crossref]

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Zhang, T.

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K. Chen, H. R. Zhao, Z. K. Fan, G. Yin, Q. M. Chen, Y. W. Quan, S. H. Li, and S. H. Ye, “Macrospirocyclic oligomer based on triphenylamine and diphenylphosphine oxide as a bipolar host for efficient blue electrophosphorescent organic light-emitting diodes (OLEDs),” Org. Lett. 17(6), 1413–1416 (2015).
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[Crossref]

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Zhou, X.

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S. Ye, T. Hu, Z. Zhou, M. Yang, Q. Mei, Y. Liu, L. Liu, B. Zhai, Z. Jia, and W. Huang, “Solution processed single-emissive-layer white organic light-emitting diodes based on fluorene host: balanced consideration for color quality and electroluminescent efficiency,” Org. Electron. 33, 235–245 (2016).
[Crossref]

S. H. Ye, T. Q. Hu, Z. Zhou, M. Yang, M. H. Quan, Q. B. Mei, B. C. Zhai, Z. H. Jia, W. Y. Lai, and W. Huang, “Solution processed single-emission layer white polymer light-emitting diodes with high color quality and high performance from a poly(N-vinyl)carbazole host,” Phys. Chem. Chem. Phys. 17(14), 8860–8869 (2015).
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Zhu, F.

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Figures (7)

Fig. 1
Fig. 1 (a) Molecular structures of materials, (b) energy level alignment of the devices.
Fig. 2
Fig. 2 Current density-voltage characteristics of (a) hole-only and (b) electron-only devices based on (TPA-PO)3:TCTA mixed films.
Fig. 3
Fig. 3 (a) UV-vis absorption and (b) PL spectra of (TPA-PO)3:TCTA mixed films with different ratios; (c) comparison of UV-vis absorption spectra of FIrpic, Ir(ppy)2(acac), Ir(bt)2(acac), Ir(piq)2(acac) emitters and PL spectra of (TPA-PO)3 and TCTA films; (d) PL spectra of solution-processed (TPA-PO)3:TCTA mixed film doped with FIrpic, Ir(ppy)2(acac), Ir(bt)2(acac), and Ir(piq)2(acac) emitters. Note: PO represents (TPA-PO)3 in the legend of the figures.
Fig. 4
Fig. 4 AFM images of the solution-processed films: (a)/(a’), (b)/(b’), (c)/(c’), and (d)/(d’) correspond to PO:TCTA, PO:TCTA:15 wt% FIrpic, PO:TCTA:15 wt% FIrpic:0.3 wt% Ir(ppy)2(acac):0.5 wt% Ir(bt)2(acac), and PO:TCTA:15 wt% FIrpic:0.3 wt% Ir(ppy)2(acac):0.5 wt% Ir(bt)2(acac):0.5 wt% Ir(piq)2(acac) mixed films before/after annealing, respectively. Note: the weight ratio of PO:TCTA is 5:5; the annealing temperature and time are 120 °C, 1 h.
Fig. 5
Fig. 5 Performance of the blue, green, orange, and red phosphorescent OLEDs: (a) current density-voltage-brightness and (b) current efficiency-brightness characteristics. Inset: EL spectra of representative devices at varying driving voltages, with main peak at 472, 524, 564, and 632 nm for blue, green, orange, and red phosphorescent OLEDs, respectively.
Fig. 6
Fig. 6 Performance of the binary and ternary doping WOLEDs: (a) current density-voltage-brightness and (b) current efficiency-brightness characteristics; EL spectra of (c) binary and (d) ternary doping WOLEDs. Device structure: ITO/PEDOT:PSS (25 nm)/(TPA-PO)3:TCTA:15 wt% FIrpic:0.3wt% Ir(ppy)2(acac): x Ir(bt)2(acac) (35 nm)/TPBi (35 nm) /Ca (10 nm)/Ag (100 nm). Note: x = 0 for device WB, and x = 0.5 wt% for device WT.
Fig. 7
Fig. 7 Performance of WOLED device WQ-3: (a) current density-voltage-brightness, (b) current efficiency-brightness-power efficiency characteristics, (c) EL spectra, and (d) CIE 1931 chromaticity diagram as well as the emission photograph (at 7 V, ~1000 cd m-2). Device structure: ITO/PEDOT:PSS (25 nm)/(TPA-PO)3:TCTA:15 wt% FIrpic:0.3wt% Ir(ppy)2(acac):0.5 wt% Ir(bt)2(acac): 0.5 wt% Ir(piq)2(acac) (35 nm)/TPBi (35 nm) /Ca (10 nm)/Ag (100 nm). Inset: photograph of the emitting device WQ-3.

Tables (2)

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Table 1 Performance of the Solution-Processed Blue, Green, Orange, and Red OLEDs.

Tables Icon

Table 2 Performance of the Solution-Processed Phosphorescent WOLEDs.

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