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Letter
Two Host-Dopant Emitting Systems Realizing Four-Color Emission:
A Simple and Effective Strategy for Highly Efficient Warm-
White OLED with High Color-Rendering Index at High Luminance
Xuming Zhuang, Hao Zhang, Kaiqi Ye, Yu Liu, and Yue Wang
ACS Appl. Mater. Interfaces, Just Accepted Manuscript • DOI: 10.1021/acsami.6b03374 • Publication Date (Web): 22 Apr 2016
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Two Host-Dopant Emitting Systems Realizing Four-
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12 Color Emission: A Simple and Effective Strategy for
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16 Highly Efficient Warm-White OLED with High
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Color-Rendering Index at High Luminance
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Xuming Zhuang, Hao Zhang, Kaiqi Ye, Yu Liu* and Yue Wang
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29 State Key Laboratory of Supramolecular Structure and Materials, Institute of Theoretical
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31 Chemistry, Jilin University, Changchun, 130012, P. R. China
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35 KEYWORDS. white organic light-emitting diode (WOLED), four-color, warm-white, high CRI,
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37 phosphorescent material
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41 ABSTRACT. A four-color warm-white OLED employing simple adjacent two-EML structure as
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43 blue host-orange dopant/green host-red dopant has been fabricated, which exhibited stable high
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46 EL performance: the EQE of 23.3% and PE of 63.2 lm W–1 at an illumination-relevant
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48 luminance of 1000 cd m–2 with a high CRI of 92 and maintained the high levels of 21.6% and
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50 48.8 lm W−1 with the CRI range of 93 at the extremely high luminance of 5000 cd m−2. To our
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53 knowledge, this should be the best result so far for a WOLED with CRI >90, simultaneously
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55 exhibiting very high efficiencies based on high-luminance level for the solid-state lighting.
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Currently, organic light-emitting diodes (OLEDs) with high electricity-light conversion
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6 efficiency have great potential for energy saving solid-state lighting (SSL), and many research
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8 efforts have been made for high-efficiency white OLEDs (WOLEDs) by employing all the
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electrically generated excitons, thereby achieving nearly 100% internal quantum eifficiency.1-4 In
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13 addition, a high color rendering index (CRI≥80) is another important parameter for white
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illumination source.5,6 In particular, very-high CRI is essential for lighting applications in house,
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18 museums, art galleries and other commercial places, and great developments in efficient
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20 WOLEDs with the CRI values of >90 have been achieved recently.7-9 In this regard, the use of
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three or more fluorescent and/or phosphorescent emitters has been a prerequisite for realizing a
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25 broad electroluminescent (EL) spectrum. Unfortunately, in addition to the high CRI achieved at a
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27 cost of low device efficiency accompanied by significant efficiency roll-off (<20 lm W–1@1000
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30 cd m–2), such WOLEDs employing four or more emission units usually suffered from the
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32 disadvantage of device fabricating complexity due to their multi-layer or multi-dopant co-doping
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34 structure together with one or more precisely-controlled interlayer. Therefore, there is still
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37 considerable room for improving the device efficiency as well as simplifying the device structure
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39 of the WOLEDs with CRI values of greater than 90.
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Recently, several WOLEDs based on both the host and the guest molecules acting as the
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45 emitters, which usually consisted of one fluorescent host for blue light doping with one
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47 phosphorescent guest for yellow (or orange) light, or doping with two phosphorescent guests for
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50 green and orange (or red) light respectively, have been reported.10-13 As we know, they not only
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52 achieved very high EL efficiencies by utilizing all the generated singlet and triplet excitons for
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54 light emission, but can effectively reduce the total number of emitting layers (EMLs) and
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57 constituent components within the whole emitting system, which therefore rendered the greater
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possibility of high-efficiency WOLEDs with simple device structure. But in fact, some of their
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6 EL characters such as the CRI and the efficiency values within the illumination-relevant
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8 luminance range of 1000-5000 cd m–2, still needed be further improved. In this work, a four-
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11 color WOLED employing double EMLs consisting of four emitting complexes: Bepp2 (λmax∼450
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13 nm) for blue,12,13 FPPCA (λmax∼500 nm) for green,14 BZQPG (λmax∼605 nm) for orange and
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16 BTIPG (λmax∼630 nm) for red,15 was fabricated. Here, the blue-orange (B-O) EML based on
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18 BZQPG doped in Bepp2 together with the green-red (G-R) EML based on BTIPG doped in
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FPPCA realized an excellent ROGB-type white EL through the optimization for the relative
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23 emission intensity of blue, green, orange and red. There is no specialized host molecule and
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25 interlayer being additionally introduced into this novel device architecture, avoiding complicated
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28 process for device fabrication and undesirable charge accumulation in this device.9,10,16 An
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30 optimal management of four emitting components aiming at balanced charge injection together
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32 with efficient charge/exciton confinement simultaneously, ensured that this WOLED realized a
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35 wide-cover EL spectrum as well as high and stable EL performance with respect to luminance
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37 increases as follows: very high forward-viewing EQE of 23.3% and PE of 63.2 lm W–1 at the
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39 luminance of 1000 cd m–2 with a high CRI of 92 and eye-friendly warm-white17-20 Commission
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42 Internationale de L’Eclairage (CIEx,y) coordinates of (0.433, 0.458) were realized, which
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44 maintained the high levels of 21.6% and 48.8 lm W−1 with the CRI range of 93 at the extremely
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47 high luminance of 5000 cd m−2. To our knowledge, this should be the best result so far for a
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49 WOLED with such high CRI values (>90), simultaneously exhibiting very high efficiencies
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based on high-luminance level for the solid-state lighting.
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Figure 1. a) Molecular structures of Bepp2, FPPCA, BZQPG and BTIPG. b) UV-Vis absorption
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36 of BZQPG and BTIPG in neat thin film and PL spectra of neat films of Bepp2, FPPCA, BZQPG
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38 and BTIPG, and the films of BZQPG and BTIPG doped in Bepp2 and FPPCA respectively with
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5 wt% doping concentration.
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44 The chemical structures of Bepp2, FPPCA, BZQPG and BTIPG and the absorption and
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46 photoluminescence (PL) spectra in neat and doped films are shown in Figures 1a and 1b. The
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spectral overlap between the emission peaks of Bepp2/FPPCA and the MLCT absorption band of
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51 BZQPG/BTIPG, together with their triplet energy alignment: 2.6, 2.4, 2.1 and 2.0 eV for T1 of
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53 Bepp2, FPPCA, BZQPG and BTIPG those estimated from the 0−0 band of their phosphorescence
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56 spectra respectively previous reports,13-15 suggested effective energy transfer from Bepp2 to
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BZQPG, and from FPPCA to BTIPG. This has been demonstrated in the PL spectra of
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6 Bepp2:BZQPG and FPPCA:BTIPG thin films with the concentration of 5 wt%, which show the
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8 emission only from BZQPG and BTIPG at λmax of ∼570 and 620 nm with the quantum yields of
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11 0.68±0.03 and 0.55±0.02, respectively.
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14 To obtain high efficiency and high CRI WOLED with the optimal EL spectral curve, four
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17 emitting components have been arranged elaborately in two EMLs (B-O EML and G-R EML)
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19 according to their respective charge-transporting and luminous characters, and the energy
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21 diagram of the optimized WOLED (Device I: ITO/NPB (35 nm)/Bepp2:BZQPG (2.0 wt%, 5
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24 nm)/FPPCA:BTIPG (0.8 wt%, 15 nm)/TPBi (30 nm)/LiF (0.5 nm)/Al) as shown in Figure 2a.
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26 Here, NPB and TPBi are the hole-transporting layer (HTL) and the electron-transporting layer
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(ETL), respectively. Theoretically, both singlet and triplet excitons are created with a ratio of 1:3
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31 in either of the EMLs.22 In the G-R layer based on BTIPG doped in FPPCA, all the generated
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33 excitons can produce either green emission through direct radiative decay on the host FPPCA
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molecule, or red emission from the dopant BTIPG molecules through host-guest energy transfer.
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38 In the B-O EML consisting of Bepp2 doped BZQPG, the Bepp2 molecules not only generate blue
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40 singlet emission, but also sensitize the emission of BZQPG in this EML, leading to the increase
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43 in both blue and orange emission intensity. As we known, Bepp2 is an effective electron-
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48 s−1.12,21 Normally, this could prevent the recombination zone confined in this Bepp2-EML from
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50 the excitons generating in another EML, leading to higher blue and/or orange intensity in the
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52 whole EL spectrum that suffered from the low CRI. However, a rather thin Bepp2-based B-O
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55 EML (5 nm) adopted here would effectively induce more recombination taken place in G-R
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EML with the thicker thickness of 15 nm, which dramatically decreased the relative EL intensity
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45 Figure 2. a) Proposed energy diagram of the materials used in OLEDs. b) EL spectra and the
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47 corresponding CRI values of Device I at different luminances (L). Inset: a photograph of Device
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50 I illuminating at 5000 cd m−2 with a CRI of 93.
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53 Figure 2b showed the white EL spectra and the corresponding CRIs of Device I at different
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55 luminance levels. These spectral curves covered all visible wavelengths from 400 to 750 nm due
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58 to the simultaneous fluorescent blue from Bepp2 (~450 nm), and phosphorescent green, orange
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and red from FPPCA (~510 nm) and BZQPG (~570 nm) and BTIPG (~620 nm) respectively.
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6 Clearly, they are primarily due to the red emitter BTIPG, with the moderate intensities of green
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8 FPPCA and orange BZQPG as well as the weakest blue Bepp2. This strongly supports the
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hypothesis above that the recombination zone mainly occurred in the G-R EML, where the more
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13 EL-efficient all-phosphor host-guest emitting system14 would facilitate the desirable CRI values
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15 as well as the very high EL efficiency. Furthermore, it can be seen that the relative contribution
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18 of the green and red emission slightly increased compared to the blue and orange emission as the
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20 driving voltages (equivalent to the luminance) gradually increased. This is due to the inherent
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22 hole- and exciton-blocking character of Bepp2-based EML, although its thickness has been
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25 controlled at a very low level as thin as 5 nm, which still had the ability to confine the certain
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27 holes within this layer. Thus, the increased driving voltage can actuate more holes flowing into
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the G-R EML through the B-O EML, leading to the more recombination of holes and electrons
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32 in G-R EML, where both the green and red emission increased gradually.
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35 Figure 3a show the efficiency-luminance (PE/EQE-L) characteristics of Device I, and the
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38 detailed data are summarized in Table 1. Device I exhibit rather excellent EL performance with
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40 turn-on voltage at 2.5 V, and the driving voltages for the luminances of 1000 and 5000 cd m−2
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are 3.7 and 4.8 V respectively. The corresponding CIEx,y coordinates changed only marginally
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45 from (0.431, 0.449) at 1000 cd m−2 to (0.433, 0.458) at 5000 cd m−2, with the correlated color
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47 temperature (CCT) of 3230 K and 3290 K, corresponding to the warm-white color emission at
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50 these illumination-relevant luminance levels. At a luminance of 1000 cd m−2 this WOLED with
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55 efficiencies slightly rolled off to 21.6% and 48.8 lm W−1 at a critical luminance level of 5000 cd
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EQEs and PEs represented the highest reported to date among WOLEDs exhibiting the decent
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49 Figure 3. a) Power efficiency (PE)-luminance (L)-external quantum efficiency (EQE) curves of
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51 Devices I, II, III and IV. b) EL spectra and the corresponding CIE coordinates of Devices I, II,
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54 III and IV at the luminance of 5000 cd m−2
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In addition, three exploratory devices with the same configuration as Device I were fabricated
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6 by using the single doping films of Bepp2:BZQPG (2.0 wt%, 20 nm) and FPPCA:BTIPG (0.8
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8 wt%, 20 nm) and the double doping films of Bepp2:BZQPG (2.0 wt%, 10 nm)/FPPCA:BTIPG
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(0.8 wt%, 10 nm) as the EML for Device II, III and IV respectively (see Figure S1 in ESI file).
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13 The PE/EQE-L curves of Device II, III and IV and the EL spectral comparison of Device I-IV at
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15 the luminance of 5000 cd m−2 are shown in Figures 3a and 3b respectively. Clearly, the EMLs in
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18 Device II and III adopted the same doping concentration as the B-O and G-R layers respectively
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20 in Device I, thus they could generally reflect the EL processes occurred in Device I. In the EL
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spectra of Devices II and III, the emission peaks originating from both the host and dopant
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25 molecules are observed, due to suppression of energy transfer of singlet/triplet excitons at such
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27 low doping concentrations as 2.0 or 0.8 wt%. Since Bepp2 is an effective electron-
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30 transporting/hole-blocking material,12 the recombination zone in this Bepp2-based EML of
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32 Device II should be confined in the interface of NPB/Bepp2, which led to the decrease of carrier
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34 utilization and increase of the triplet-triplet annihilation (TTA) process evidently in the narrow
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37 exciton generation zone, especially under high current density. Indeed, the relatively low EL
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39 efficiency and obvious efficiency roll-off has been observed for this device. This double-color
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fluorescent/phosphorescent hybrid device just showed the moderate EL efficiency with the EQEs
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44 and PEs of 17.1, 14.0% and 31.8, 20.6 lm W−1 at 1000 and 5000 cd m−2 respectively, as shown in
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46 Figures 3a and Table 1. For Device III, The bipolar charge transport ability of the host FPPCA
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49 will effectively eliminate the accumulated carriers,14 resulting in balanced and sufficient charge
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51 fluxes within this EML, where the low-content of BTIPG (0.8 wt%) could not have the
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substantial effect on the inherent charge transport property of FPPCA. Thus, the resulting exciton
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better similarity in their molecular structure and lots of optoelectric properties between two
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6 phosphors compared with the conventional doping cases based on fluorescent host and
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8 phosphorescent dopant, are indeed the advantages of the well-matched FPPCA:BTIPG
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combination, where all the electrically generated excitons could be utilized, leading to very high
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13 EL efficiencies at high luminance levels: 23.6% and 23.3% for EQE and 65.5 lm W−1 and 51.1
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lm W−1 for PE at 1000 and 5000 cd m−2 respectively, also rendering this all-phosphorescent host-
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18 guest system remarkably efficient in nature.
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21 Table 1. Summary of EL performance for Devices I, II, III and IV.
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23 Device Va [V] ηpb [lm W−1] ηextb [%] CIEx,y b/CRIb
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25 I 2.5, 3.7, 4.8 63.2, 48.8 22.5, 21.6 (0.431, 0.449)/92, (0.433, 0.458)/93
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27 II 2.7, 4.5, 5.6 31.8, 20.6 17.1, 14.0 (0.416, 0.422)/--, (0.404, 0.413)/--
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29 III 2.3, 3.6, 4.6 65.5, 51.1 23.6, 23.3 (0.518, 0.447)/--, (0.493, 0.467)/--
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31 IV 2.6, 4.0, 5.5 52.7, 37.8 20.5, 19.1 (0.348, 0.360)/76, (0.375, 0.382)/79
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33 Applied voltage recorded at 1, 1000 and 5000 cd m−2, respectively. bValues at 1000 and 5000
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36 Besides, it is apparent that as the relative thickness of B-O layer increased, Device IV showed
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different-quality white emission from Device I, where the EL intensities of blue (~450 nm) and
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41 orange (~570 nm) emission being assigned to Bepp2 and BZQPG respectively, were significantly
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43 enhanced, becoming the dominant emission peaks as shown in the Figures 3b. This should be
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because the host Bepp2 is a typical hole-blocking material, which could block a majority of holes
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48 at this B-O layer in Device IV due to its thicker thickness (10 nm) than that (5 nm) in Device I.
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50 While electrons can easily enter this EML and consequently recombine with the confined holes,
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53 resulting in that the charge carriers mainly recombined in the less EL-efficient B-O layer based
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55 on fluorescent/phosphorescent hybrid host-dopant emitting system,9 causing the lower EL
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57 efficiency and CRI of Device IV than those of Device I. Compared with Device I, the variation
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of the relative spectral intensity for four emission peaks in Device IV, corresponded to a
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6 considerable decease in the EL efficiencies: 20.5% and 19.1% for EQE, 52.7 lm W−1 and 37.8 lm
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8 W−1 for PE, and its rather low CRI values of 76 and 79 at 1000 and 5000 cd m−2 respectively (see
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11 Figures 3a and Table 1), indicated that it can not provide adequate quality for illumination,
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13 although it possessed rather pure-white CIEx,y coordinates.
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17 As we can see, the obviously difference in the EL spectra, colorimetric parameters as well as
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19 the efficiencies between Device I and IV, together with the systemic comparison for the EL
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21 characters of all the four devices above, illustrated that the color and EL performance of each
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24 white device (I and IV) can be easily and effectively tuned by adjusting the relatively thickness
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26 of the B-O and G-R EMLs, according to their respective emitting and charge-transporting
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characteristics. Actually, it is more importantly, the desirable EL performance of Device I
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31 demonstrated that the ROGB four-color white EL emission can be realized by utilizing a simple
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33 and novel two-layer emitting system, where four emitters had been employed as two host and
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two dopant materials, and radiated the light respectively based on their own emission color,
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38 through either the direct charge carrier recombination on the host emitters (Bepp2 and FPPCA),
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40 or the energy transfer to the dopant dye (BZQPG and BTIPG). This strategy avoided introducing
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43 any additional host molecule into the emitting system and the corresponding problems about the
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45 host choice and matching. Furthermore, this free recombination zone consisting of double EMLs
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47 without an interlayer in Device I, effectively reduced the undesirable charge accumulation as
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50 well as the resulting triplet-polaron and/or polaron-polaron quenching processes in the device.23
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52 Thus, it is well understood that the surplus excitons could easily diffuse into the adjacent EML
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and sensitize the emitters with a lower energy, allowing all the excitons to decay radiatively. Of
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location in both EMLs as we expected, is the essential factor for maximizing our WOLED
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6 overall quantum efficiency and simultaneously achieving the high-quality white light for lighting.
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8 Actually, this is also the optimal result obtained through the more detailed optimizing processes
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(shown in ESI file) for the emitting systems based on these four complexes.
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14 In summary, using two host-dopant emitting systems based on blue, green, orange and red
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16 dyes achieving a ROBG four-color white EL emission, which showed almost excellent
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19 performances including its efficiency and color characters, is indeed a novel and effective
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21 approach to realize the adequate white OLED for illumination sources. It is more important that,
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23 such simple adjacent two-EML structure as blue host-orange dopant/green host-red dopant
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26 adopted here, without any interlayer and specialized host introduced additionally, could
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28 effectively reduce the total number of constituent components and layers within the whole
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system, which enabled not only the simplified device fabrication process, but also the favorable
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33 charge-transporting and energy transfer processes, leading to very high EL efficiency through
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35 reducing exciton/charge accumulation as much as possible. These desirable EL performances of
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38 this WOLED are commonly believed to be the prerequisites for its use in future solid-state
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40 lighting.
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47 ASSOCIATED CONTENT
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50 Supporting Information.
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Figure S1. Configurations for Devices I, II, III and IV;
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57 Figure S2. Current density-voltage-luminance (J-V-L) of Devices I, II, III and IV;
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Figure S3. PL spectra and PLQY values of the doping films of BZQPG doped in Bepp2 (2.0
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6 wt%) and BTIPG doped in FPPCA (0.8 wt%);
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9 Figure S4. Configurations for two reference Devices V and VI;
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13 Figure S5. EL spectra and the corresponding CIE coordinates and CRI values of two reference
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15 Device V and VI at the luminance of 5000 cd m−2;
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18 Figure S6. Power efficiency (PE)-luminance (L)-external quantum efficiency (EQE) curves of
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21 two reference Devices V and VI;
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24 This material is available free of charge via the Internet at http://pubs.acs.org.
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30 AUTHOR INFORMATION
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33 Corresponding Author
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35 *E-mail: [email protected].
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39 Notes
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41 Any additional relevant notes should be placed here.
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47 ACKNOWLEDGMENT
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This work was supported by National Basic Research Program of China (973 Program,
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52 2013CB834805), Natural Science Foundation of China (91333201, 21221063, 51373062,
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54 51473028), the key scientific and technological project of Jilin province (20150204011GX).
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REFERENCES
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