Enhanced and balanced efficiency of white bi-directional organic light-emitting diodes

We report on the characteristics of enhanced and balanced whitelight emission from bi-directional organic light-emitting diodes (BiOLEDs) enabled by the introduction of micro-cavity effects. The insertion of an additional metal layer between the indium tin oxide anode and the hole transporting layer results in similar light output of our BiOLEDs in both top and bottom direction and in reduced distortion of the electroluminescence spectrum. Furthermore, we find that by utilizing MC effects, the overall current efficiency can be improved by 26.2% compared to that of a conventional device. ©2013 Optical Society of America OCIS codes: (230.3670) Light-emitting diodes; (230.4170) Multilayers; (310.6845) Thin film devices and applications. References and links 1. S. Reineke, F. Lindner, G. Schwartz, N. Seidler, K. Walzer, B. Lüssem, and K. Leo, “White organic lightemitting diodes with fluorescent tube efficiency,” Nature 459(7244), 234–238 (2009). 2. M. C. Gather, A. Köhnen, and K. Meerholz, “White organic light-emitting diodes,” Adv. Mater. 23(2), 233–248 (2011). 3. S. Chen, L. Deng, J. Xie, L. Peng, L. Xie, Q. Fan, and W. Huang, “Recent developments in top-emitting organic light-emitting diodes,” Adv. Mater. 22(46), 5227–5239 (2010). 4. H. W. Chang, J.-H. Lee, S. Hofmann, Y. H. Kim, L. Müller-Meskamp, B. Lüssem, C.-C. Wu, K. Leo, and M. C. Gather, “Nano-particle based scattering layers for optical efficiency enhancement of organic light-emitting diodes and organic solar cells,” J. Appl. Phys. 113(20), 204502 (2013). 5. K. S. Yook, S. O. Jeon, C. W. Joo, and J. Y. Lee, “Transparent organic light emitting diodes using a multilayer oxide as a low resistance transparent cathode,” Appl. Phys. Lett. 93(1), 013301 (2008). 6. H. Cho, J.-M. Choi, and S. Yoo, “Highly transparent organic light-emitting diodes with a metallic top electrode: the dual role of a Cs2CO3 layer,” Opt. Express 19(2), 1113–1121 (2011). 7. J.-H. Lee, S. Lee, J.-B. Kim, J. Jang, and J.-J. Kim, “A high performance transparent inverted organic light emitting diode with 1,4,5,8,9,11-hexaazatriphenylenehexacarbonitrile as an organic buffer layer,” J. Mater. Chem. 22(30), 15262–15266 (2012). 8. J. W. Huh, J. Moon, J. W. Lee, D.-H. Cho, J.-W. Shin, J.-H. Han, J. Hwang, C. W. Joo, H. Y. Chu, and J.-I. Lee, “Directed emissive high efficient white transparent organic light emitting diodes with double layered capping layer,” Org. Electron. 13(8), 1386–1391 (2012). 9. J. Lee, S. Hofmann, M. Furno, M. Thomschke, Y. H. Kim, B. Lüssem, and K. Leo, “Influence of organic capping layers on the performance of transparent organic light-emitting diodes,” Opt. Lett. 36(8), 1443–1445 (2011). 10. J. Lee, S. Hofmann, M. Thomschke, M. Furno, Y. H. Kim, B. Lüssem, and K. Leo, “Increased and balanced light emission of transparent organic light-emitting diodes by enhanced microcavity effects,” Opt. Lett. 36(15), 2931–2933 (2011). 11. J. Lee, S. Hofmann, M. Thomschke, M. Furno, Y. H. Kim, B. Lüssem, and K. Leo, “Highly efficient bidirectional organic light-emitting diodes by strong micro-cavity effects,” Appl. Phys. Lett. 99(7), 073303 (2011). 12. J. Lee, J. -I. Lee, J. -W. Lee, and H. Y. Chu, “Interlayer engineering with different host material properties in blue phosphorescent organic light-emitting diodes” ETRI. J. 32, 32-38 (2011). #198448 $15.00 USD Received 27 Sep 2013; revised 28 Oct 2013; accepted 29 Oct 2013; published 7 Nov 2013 (C) 2013 OSA 18 November 2013 | Vol. 21, No. 23 | DOI:10.1364/OE.21.028040 | OPTICS EXPRESS 28040 13. J.-I. Lee, J. Lee, J.-W. Lee, D.-H. Cho, J.-W. Shin, J.-H. Han, and H. Y. Chu, “Dependence of light-emitting characteristics of blue phosphorescent organic light-emitting diodes on electron injection and transport materials,” ETRI J. 34(5), 690–695 (2012). 14. S. Olthof, W. Tress, R. Meerheim, B. Lüssem, and K. Leo, “Photoelectron spectroscopy study of systematically varied doping concentrations in an organic semiconductor layer using a molecular p-dopant,” J. Appl. Phys. 106(10), 103711 (2009). 15. M. Agrawal, Y. Sun, S. R. Forrest, and P. Peumans, “Enhanced outcoupling from organic light-emitting diodes using aperiodic dielectric mirrors,” Appl. Phys. Lett. 90(24), 241112 (2007). 16. S. Hofmann, M. Thomschke, P. Freitag, M. Furno, B. Lüssem, and K. Leo, “Top-emitting organic light-emitting diodes: Influence of cavity design,” Appl. Phys. Lett. 97(25), 253308 (2010). 17. R. Meerheim, M. Furno, S. Hofmann, B. Lüssem, and K. Leo, “Quantification of energy loss mechanisms in organic light-emitting diodes,” Appl. Phys. Lett. 97(25), 253305 (2010). 18. T. Schwab, S. Schubert, S. Hofmann, M. Fröbel, M. Thomschke, L. Müller-Meskamp, K. Leo, and M. C. Gather, “Highly efficient color stable inverted white top-emitting OLEDs with ultra-thin wetting layer top electrodes,” Adv. Opt. Mater. in press., doi:10.1002/adom.201300241. 19. C.-W. Chen, C.-L. Lin, and C.-C. Wu, “An effective cathode structure for inverted top-emitting organic light emitting devices,” Appl. Phys. Lett. 85(13), 2469–2471 (2004). 20. M. Furno, R. Meerheim, S. Hofmann, B. Lüssem, and K. Leo, “Efficiency and rate of spontaneous emission in organic electroluminescent devices,” Phys. Rev. B 85(11), 115205 (2012). 21. W. Brütting, J. Frischeisen, T. D. Schmidt, B. J. Scholz, and C. Mayr, “Device efficiency of organic lightemitting diodes: Progress by improved light outcoupling,” Phys. Status Solidi A 210(1), 44–65 (2013). 22. “ENERGY STAR ® Program Requirements for Solid State Lighting Luminaires Eligibility Criteria – Version 1.1” 1–23 (2008). 23. M. Furno, T. C. Rosenow, M. C. Gather, B. Lüssem, and K. Leo, “Analysis of the external and internal quantum efficiency of multi-emitter, white organic emitting diodes,” Appl. Phys. Lett. 101(14), 143304 (2012).


Introduction
White organic light-emitting diodes (OLEDs) are attracting widespread attention as nextgeneration low-cost and high-efficiency thin-film electroluminescent devices for both flat panel displays and lighting applications [1][2][3] due to recent rapid technical evolution.The uniqueness of these light-emitting devices can for example be demonstrated in transparent or bi-directional OLEDs (TOLEDs or BiOLEDs), where light is emitted from both the bottom and the top side of the device; this intrinsic bi-directional emission capability of OLEDs clearly distinguishes them from other light-emitting devices [4][5][6][7][8][9][10][11].
To improve the light-emitting performance of TOLEDs/BiOLEDs, many approaches have been used, such as the modification of electrode components [5][6][7] and the introduction of a capping layer [8,9].More recently, we reported systematic studies on the influence of microcavity (MC) effects on BiOLEDs in which a thin metal layer is inserted in between organic and transparent conductive oxide (TCO) layers [10,11].Although these previous studies were successful in enhancing the efficiency of monochromatic OLEDs, limitations remain in the application of these methods to white-light BiOLEDs.This is mainly due to the spectral dependence of the cavity resonance condition that makes it very challenging to control the optical characteristics of MC-OLEDs such that the cavity resonance enhancement is achieved over a wide range of emission wavelengths.Fortunately, BiOLEDs rely inherently on top and bottom electrodes that are both relatively transparent.Hence it might be plausible to assume that the MC effect in BiOLEDs is "weak" at best and that the issue of spectral sensitivity is therefore of less concern for white BiOLEDs.However, questions still remain whether such a low degree of MC effect, if any, can still lead to efficiency enhancement in white BiOLEDs.

Experiment
The current density-voltage-luminance (J-V-L) characteristics of the devices were measured with a source measure unit (Keithley 2400), and the spectral radiant intensity was determined by a calibrated spectroradiometer (Instrument Systems GmbH CAS140). Figure 2 shows the J-V-L characteristics of our 3-color white BiOLEDs (Device B) with and without a 10-nm-thick Ag layer (B1: without Ag, B2: with Ag).The J-V curves as well as the EL onset voltages of the OLEDs are nearly identical because doped MeO-TPD layer deposited onto Ag or ITO can realize ohmic contacts.By using a moderate doped transporting layer, interface effects as well as the work function of electrode only play a minor role for the energy alignment [14].As a result, it is demonstrated that the additional Ag layer does not alter the electrical characteristics of our BiOLEDs.However, noticeable differences in the L-V curves are observed for both the top and bottom emission, depending on the presence of the Ag layer.As has been discussed in several previous reports, the bottom emission (black symbols) is much stronger than the top emission (red symbols) in Device B1 because the reflectance of the thin metal cathode is higher than that of the ITO anode [4][5][6][7][8][9][10][11].On the other hand, in Device B2 the bottom emission (green symbols) and the top emission (blue symbol) are nearly identical due to a significant enhancement in the top emission.This can be understood by the reflectance of the bottom electrode that increases when one introduces the Ag layer on top of the ITO electrode.It is noteworthy that the top/bottom balancing effect due to the insertion of the Ag layer in Device B2 is achieved without a significant compromise in the bottom emission, as shown in Fig. 3 and Table 1.In fact, the current efficiency (CE) for bottom emission decreases only slightly from 17.8 cd/A to 15.7 cd/A at J of 15 mA/cm 2 , when the Ag layer is added.The CE for top emission, on the other hand, increases significantly by a factor of 2.65 from 4.8 cd/A to 12.8 cd/A, resulting in an overall enhancement in the CE for total emission by more than 25%.

Results and discussions
To better understand the experimental results, a micro-cavity (MC) OLED model [10,[15][16][17][18][19][20][21][22] has been adopted to analyze the optical properties of the proposed white BiOLEDs.The precise treatment of the MC effect should consider dipole emitters embedded vertically or horizontally within OLEDs, which are optically a multilayer stack consisting of dielectric and/or metallic layers, and the environment-induced change in their radiative lifetime as well as coupling to various modes such as waveguide modes and surface plasmon polariton (SPP) modes [20,21].For the emission in forward-direction (θ = 0), however, the Fabry-Perot (FP) formulation which uses a plane-wave approximation is also popular for simplicity's sake and can still be useful in illustrating various phenomena in MC-OLEDs [18,19].Within the framework of the FP formulation, one can describe the emission intensity of an OLED in a simplified structure of front electrode/ organic layer/ rear electrode with a sheet-like emission zone by [18,19]: in which ( ) ( ) ( ) , where n org and d org are the refractive index and thickness of the organic layer, T f(r) and R f(r) are the transmittance and reflectance, respectively, of the front (rear) electrode, i.e. of the electrode that is facing the observer (front) or opposite of the observer (rear), and z EM is the distance between the emission zone and its interface with a rear electrode.φ f(r) is a phase shift occurring upon reflection at the organic/ front (rear) electrode interface and I 0 (λ) refers to the free-space emission intensity of the emitter.From the result of optical analysis shown in Fig. 4, we can attribute the observed enhancement to the multiple-beam cavity resonance enhancement as well as to constructive two-beam interference that can occur efficiently in both emission directions as the reflectance of the bottom Ag layer (anode side) is comparable to that of the top Ag layer (cathode side) [11].For top emission, the ratio of g res (λ) obtained for devices with the inserted Ag [ = g res (Ag) (λ) ] to that for devices without it [ = g res (no Ag) (λ) ] indicates that there is indeed a resonance-induced enhancement centered around λ of 550 nm with the peak enhancement ratio of 1.56.However, the two-beam interference effect appears to be more important by comparison; as can be seen in Fig. 4, the enhancement ratio for f TB (λ) ranges from 1.75 to 2.20 throughout the visible spectral range.
For bottom emission, on the other hand, the two-beam interference effect remains unchanged because there is no change in the reflectance from the top electrode.The multiplebeam cavity resonance enhancement given by the denominator in Eq. ( 2) is same as that in the top-emission case, but it is over shadowed by the reduced transmittance due to the Ag layer, which leads to a decrease in the 'g res (Ag) / g res (no Ag) '-ratio by a factor of T bot (Ag) /T bot (no Ag) (shown as a dashed gray line in Fig. 4) at a given wavelength.This reduced transmittance leads to a small net decrease in light output for the bottom direction.In addition, we observe that the bottom-to-top CE ratio (γ CE = CE for bottom-emission / CE for top-emission) is strongly influenced by the inserted Ag layer.The γ CE values of the reference Devices A1 and B1 without Ag are 3.89 and 3.67, respectively, implying imbalanced emissions in these devices, with the bottom emission being much stronger than the top emission.In contrast, the γ CE values of Devices A2 and B2 with the Ag layer are 1.20 and 1.23, respectively.The introduction of the Ag layer on top of the ITO can thus achieve a good balance between the bottom emission and the top emission.As mentioned previously, spectrally balanced broadband white emission is of great importance for practical applications of white MC-OLEDs but achieving such characteristics has turned out to be very challenging, especially for unidirectional bottom-or top-emitting white MC-OLEDs.For the BiOLEDs investigated here, the EL spectra shown in Fig. 5 indicate that balanced broadband white emission is emitted in the top and bottom direction.Although introducing the additional Ag layer tends to increase MC effects, the EL spectra of Devices A2 and B2 do not exhibit significant distortions compared to the respective reference (Devices A1 and B1).As a result, the color rendering index (CRI), the Commission Internationale del'Eclairage (CIE) color coordinates, and the correlated color temperature (CCT), of the devices with additional Ag layer are comparable to the values for the reference devices.CRI, CIE and CCT are summarized in Table 1.For instance, for bottom emission, Device B2 exhibits a CRI of 74.8, CIE coordinates of (0.43, 0.44), and a CCT of 3404 K (at a current density of 15 mA/cm 2 ).These values are near the values necessary to satisfy the Energy Star requirements for solid-state lighting applications [22].As can be seen in Fig. 6(a), the simulation results obtained under a full classical electromagnetic formalism describing dipole emitters in a cavity structure [20,21,23] show a good match to the experimental data obtained for Devices A, and it indicates that the intensity enhancement ratio between those with and without the bottom Ag layers follows a broad spectral envelope with the full-width half-maximum (FWHM) even comparable to the full visible spectral range, being consistent with the spectrally balanced enhancement in the proposed white BiOLEDs.(See Fig. 6(a)) The simulation results presented in Fig. 6(b) and 6(c) for top-emission direction further show that increasing the MC effect by making both of the Ag layers too thick indeed reduce the spectral width of the cavity-induced intensity enhancement, which may then cause undesirable side effects such as spectral distortion or reduced CRI.Nevertheless, the proposed white BiOLEDs are expected to exhibit spectrally balanced enhancement over the entire visible spectral range provided that the thickness of top and bottom Ag layers is maintained within the range of approximately 10 nm -20 nm.

Conclusions
In summary, the performance of white-emitting BiOLEDs has been enhanced and the balance between bottom-and top-emission has been improved by controlled introduction of MC effects.We find that the overall current efficacy of BiOLEDs can be increased without significant distortion of the white EL spectra when the reflectance of the electrodes in the BiOLED is carefully managed.

Fig. 1 .
Fig. 1.Device structures of the bi-directional OLEDs tested in this study.

Fig. 3 .
Fig. 3. Current efficiency of bottom-and top-emission versus current density of (a) Devices A1 and A2 and (b) Devices B1 and B2.

Fig. 4 .
Fig. 4. Calculated enhancement in multiple-beam resonance [g res (λ)] and two-beam interference [f TB (λ)] terms due to the additional Ag layer in the bottom electrode of the white BiOLEDs under study.Calculation was based on Fabry-Perot formalism in a simplified structure of front electrode/ organic layer/ rear electrode using Eqs.(1)-(3).

Fig. 5 .
Fig. 5. Electroluminescence spectra emitted in bottom and top-direction for (a) Devices A1 and A2 and (b) Devices B1 and B2 at a driving current density of 15 mA/cm 2 .

Fig. 6 .
Fig. 6.(a) The overall enhancement ratio of the forward intensity I(λ) due to the additional Ag layer in the bottom electrode of white BiOLEDs: comparison between experimental data (Device A) and simulation results.(b)-(c) Simulated intensity for various thickness values of the bottom Ag layer ( = d Ag(bott.) ) for the thickness of the top Ag layer of 15 nm (b) and 30 nm (c).Shown in (b) and (c) are the values obtained for top-emission direction.Simulation in Fig. 6 was done using the full classical electromagnetic model considering dipole emitters embedded in a microcavity structure as described in Ref. 20 with the unity radiative quantum efficiency assumed.