Silver-based Ultrathin Transparent Top Electrode for Organic Light Emitting Diodes
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1 SESSION 25: EMERGING CAPABILITIES Silver-based Ultrathin Transparent Top Electrode for Organic Light Emitting Diodes THURSDAY, JUNE 22, 2017 Kwan Hyun Cho*, Heui Seok Kang, Kyung Tae Kang and Yong-Cheol Jeong Center for Advanced Printed Electronics (CAPE) Korea Institute of Industrial Technology (KITECH)
2 Korea Institute of Industrial Technology (KITECH) KITECH is a government supported research institute, which has 7 regional divisions. Root Technologies* (Molding, Weldign, etc.) Incheon Capital Region Nonferrous Metal Technology GangWon Center GangWon GangWon region Gyeonggi Convergence Technologies (Micro process, Robot, Textile) Clean/smart MFG** System (Green process & materials, etc.) Automotive Components, Applied Optics & Energy related technology Chungcheong Honam Chungcheong region Honam region Dongnam region Daegu-Kyeongbuk region Dongnam Daekyeong Convergence Components & materials Mechatronics (Nano-level sensors & actuators) Root technologies : Foundry, Molding, Welding, Forming, Heat treatment, Surface treatment MFG : Manufacturing 2
3 Center for Advanced Printed Electronics (CAPE) More than 10 years research experience in printed electronics area. 10 Ph.D. s in mechanical, electrical, material majors. 3
4 Contents Transparent electrode Ag based transparent electrode Ag based electrode for transparent OLED (TrOLED) Micro-cavity simulation for high performance OLED Summary 4
5 Transparent electrode Flexible/Stretchable Electronics Materials for transparent electrode Demands for flexibility Samsung SID2017 Indium Tin Oxide Nanowire Metal mesh Metal based thin film Graphene Carbon Nanotube Conducting polymer Hybrid Flexibility High transparent High conductivity Low cost process Large area deposition Patterning Damage free to underlying films Device performance 5
6 Metal based thin film Dielectric/Metal/Dielectric (DMD) Top emission OLED Bottom emission OLED (Top) Dielectric Metal (Bottom) Dielectric Dielectric Metal Dielectric Electrode Organic Oxide/Metal/Oxide (OMO) Dielectric/Metal/Dielectric (DMD) Organic Electrode Dielectric Metal Dielectric Organic/Metal/Organic Hybrid Optical properties (transmittance, reflection) Electric properties (conductivity, charge injection) Damage free deposition Optical properties (transmittance, reflection) Electric properties (conductivity, charge injection) Easy patternability 6
7 Superiority of Ag film Electrical conductance Resistivity of metal :Handbook of Chemistry and Physics, CRC Press, (1997)/ Resistivity of ITO: NATURE PHOTONICS, VOL 6, (2012). Metal Resistivity (μμω cccc) Metal Resistivity (μμω cccc) Ag 1.6 In 8.0 Cu 1.7 Pt 10.0 Au 2.4 Pd 11.0 Al 2.8 Sn 11.5 Mg 4.6 Cr 12.6 W 5.6 Ta 15.5 Mo 5.7 Ti 39.0 Zn 5.8 ITO 200~500 Ni 7.8 Ag is praised for their excellent electrical performance. 7
8 Superiority of Ag film Optical transmittance Absorption Transmittance Ir Mg Pt Co Ag Ni Au Ti Cu Mo Cr W Ir Mg Pt Co Ag Ni Au Ti Cu Mo Cr W SiO2 ITO SiO2 ITO 10-nm-thick metal films at 550nm wavelength Product of n and k Absorption, transmittance Ag is expected to be good candidate materials for the high transmittance. 8
9 Technically challenging 3D growth mode of Ag film island-like metal clusters coalescence nanotrough network continuous film Adv. Funct. Mater. 2017, the nucleation and evolution of discrete nanoscopic clusters (I,II); complete coalescence between relatively small and regular clusters (III), followed by incomplete coalescence between large and irregular clusters (IV); the formation of a nanotrough network at the percolation threshold (V); and the transition from a nanotrough network to a continuous film (VI VIII) with increasing metal thickness. percolation threshold Coalescence mode: no electrical paths (electrical) localized surface plasmon resonance (optical) Nanotrough network mode: establishing electrical paths (electrical) the penetration depth of the incident light (optical) A reduction in metal thickness of the percolation threshold (TT pppppp tttttttttttttttt ) is important. 9
10 Well known approaches (1) Bottom dielectric layer Interfacial adhesion Adv. Funct. Mater. 2017, TT pppppp tttttttttttttttt on ZnO < TT pppppp tttttttttttttttt on TiO2 The Zn O bonding in ZnO is one of the weakest among the oxide candidates, whereas the Ti O bonding in TiO2, similar to SiO2, is among the strongest. Ag atoms adsorbed on ZnO can form a strong bond to the oxygens at the topmost surface of ZnO. Surface energy Adv. Funct. Mater. 2015, 25, (2015) TT pppppp tttttttttttttttt on ZnS < < < TT pppppp tttttttttttttttt on MoO3 TT pppppp tttttttttttttttt on WO3 TT pppppp tttttttttttttttt on Glass 10
11 Well known approaches (2) Seed layer Metal seed layer Surf. Sci. 2008, 602, L49./ Adv. Energy Mater. 2013, 3, 438./ Adv. Funct. Mater. 2017, kinetic approach the activation energy barrier for the surface diffusion of Ag metals is expected to increase on the metallic seed layer compared to pristine oxide substrates. thermodynamic approach the reduction in the driving force for the surface diffusion of Ag metals to lower the difference in the surface free energy between the Ag metals and the substrate. Change in the number density of Ag clusters as a function of the thickness of the Sn surfactant number density of Ag clusters Polymer seed layer 1 nm seed layer/ Ag with a thickness of 7 nm. Adv. Mater. 2014, 26, / Adv. Energy Mater. 2014, 4,
12 Well known approaches (3) Co-deposition Adv. Mater. 2014, 26, / Adv. Funct. Mater. 2017, Ag:Al co-deposition Ca:Ag co-deposition Change in the number density of Ag clusters as a function of the thickness of the Sn surfactant c) 9-nm pure Ag fi lm, d) 9-nm Al-doped Ag fi lm. Even without any seed layer, the Ca:Ag blend electrode shows a high mean transmittance of 79.5% 12
13 Top electrode for TrOLED Transmittance spectra Organic Electronics 33 (2016) Ag-only cathode shows a substantial difference compared with the theoretical calculation. Al/Ag bilayer cathode transmission clearly exhibits an increased transmittance, and the shape of the spectrum is similar to those of the calculated theoretical transmission. 13
14 Top electrode for TrOLED SEM images Organic Electronics 33 (2016) Ag-only cathodes show separately island-like Ag films, and the sample of thickness with 8 nm show starting to become continuous Ag film. Al/Ag bilayer show the continuous bulk-like Ag film. 14
15 Top electrode for TrOLED Sheet resistance & Figure of merit (FOM) Organic Electronics 33 (2016) Luminous transmittance Sheet resistance Figure of merit (FOM) Ag(measurement) Al/Ag(measurement) Ag(calculation) Ag (measurement) Al/Ag (measurement) Ag (calculation) Al/Ag (calculation) Luminous transmittance Maximum T lum value of 86% was obtained for the Al/Ag bilayer cathode (@ 4 nm thickness). The FOM of the Al/Ag cathode based on the calculated values is high and similar to the ITO. 15
16 Top electrode for TrOLED Transmittance of the TrOLED Device structure Transmittance of TrOLED Alq3 (60nm) Ag (x nm) Al (1nm) LiF (1nm) Alq3 (40nm) NPB (60nm) PEDOT:PSS (50nm) ITO Glass The transmittance of the TrOLED devices decreased as the Ag layer thickness increased. The maximum value was 72 % at 550nm wavelength with the 4 nm Ag thickness. 16
17 Transmittance calculation of TrOLED Transmittance of TrOLEDs (ITO vs WAW) WAW based TrOLED Encap. glass(incoherent) Air(incoherent) CPL(70nm) LiF(1nm)/Al(1nm)/Ag(8nm) Alq3(50nm) NPB(50nm) WO3(y) ITO(x) Glass (incoherent) ITO based TrOLED calculated using Setfos (Fluxim) Encap. glass(incoherent) Air(incoherent) CPL(70nm) LiF(1nm)/Al(1nm)/Ag(8nm) Alq3(50nm) NPB(50nm) WO3(y) Al(1nm)/Ag(x) WO3(50nm) Glass(incoherent) WO3 WAW based TrOLED: thickness variation from 0 to 50 nm (Ag), 0 to 200 nm (WO3). ITO based TrOLED: thickness variation from 0 to 200 nm (ITO), 0 to 200 nm (WO3). 17
18 Transmittance calculation of TrOLED Transmittance spectra (ITO vs WAW) calculated using Setfos (Fluxim) 80 Transmittance (%) Transmittance of TrOLEDs WAW based TrOLED ITO based TrOLED Wavelength (nm) Max. transmittance of WAW based TrOLED: 76.4% Ag 12nm and WO3 13nm). Max. transmittance of ITO based TrOLED: 74% 150nm and WO3 101nm). 18
19 Micro-cavity simulation Micro-cavity effect calculated using Setfos (Fluxim) Reflector(Al, Ag) ff FFPP : Multiple beam interference (= Fabry-Perot effect) d Z 0 ff TTII : Two beam interference Semitransparent (ITO, Ag, Al) Substrate Micro-cavity effect in OLED GG ccaavv (λ) =ff FFPP (λ) ff TTII (λ) I out (λ) = GG ccaavv (λ) I EML (λ) Optical length(organic layer thickness, d) and semitransparent electrode thickness is important for the micro-cavity. 19
20 Micro-cavity simulation Device structure for micro-cavity simulation calculated using Setfos (Fluxim) Device 1 -reflector: Al -semitransparent: ITO Device 2 -reflector: Al -semitransparent: : Ag Device 3 -reflector: Ag -semitransparent: Al Device 4 -reflector: Ag -semitransparent: Ag Top emission Encap Glass Encap Glass Al (100 nm) LiF (1 nm) Alq3 (50 nm) NPB (50 nm) WO 3 (y nm) ITO (x nm) Al (100 nm) LiF (1 nm) Alq3 (50 nm) NPB (50 nm) WO 3 (y nm) Ag (x nm) WO 3 (50 nm) CPL (70 nm) Al (x nm) LiF (1 nm) Alq3 (50 nm) NPB (50 nm) WO 3 (y nm) Ag (150 nm) CPL (70 nm) Al/Ag (1/x nm) LiF (1 nm) Alq3 (50 nm) NPB (50 nm) WO 3 (y nm) Ag (150 nm) Glass Glass Glass Glass Bottom emission 20
21 Micro-cavity simulation_current efficiency Device 1 Device 2 WO3 Thickness WO3 Thickness WO3 Thickness WO3 Thickness ITO Thickness Ag Thickness Device 3 Device 4 Al Thickness 21 Ag Thickness
22 Micro-cavity simulation Max. current efficiency Max. emission Max. current efficiency Emission (W*m-2*nm-1*sr-1) Wavelength (nm) Device 1 Device 2 Device 3 Device 4 Current Efficiency (cd/a) Device1 Device2 Device3 Device4 Max. emission and current the thickness of Device1: (ITO: 1~11 nm, WO3: 96 nm) Device2: (Ag: 27 nm, WO3: 11 nm) Device3: (Al: 9 nm, WO3: 6 nm) Device4: (Ag: 25, WO3: 6 nm) Electrode material for micro-cavity effect: Ag > Al> ITO 22
23 Poster Session Title: The hybrid blue organic light-emitting diodes and quantum dot color converter for flexible white lighting Schematics of hybrid red QD/blue OLED LiF/Al (100nm) Bphen (30 nm) DPVBi (30nm) NPB (70nm) WO 3 (x nm) ITO (150nm) Glass Quantum Dot LiF (100nm) LiF/Al (100nm) Bphen (30nm) DPVBi (30nm) NPB (70nm) Inner WO 3 (x nm) Al/Ag (16nm) Outer WO 3 (70nm) Glass Quantum Dot Cavity enhancement factor The CIE 1931 color coordinate of the hybrid QD/OLED WAW100 WAW80 WAW120 ITOW120 WAW60 ITOW60 ITOW80 ITOW100 We achieved a wide variation of color coordinates, including blue, near-green, and near-white regions, with a simple architecture of a blue OLED and red QD. 23
24 Summary Demands for transparent electrode; damage free deposition, device performance and low cost process are important. Ag film have high superiority of electrical conductance and optical transmittance. We demonstrate the enhanced optical and electrical properties of an ultrathin silver (Ag) film by applying an aluminum (Al) seed layer. The transparent OLED devices that employed the Al/Ag cathode showed a transmittance of 72% at a 550 nm wavelength. In the micro-cavity simulation, OLED device having Ag based top and bottom electrode was obtained the maximized current efficiency. 24
25 Center for Advanced Printed Electronics 25
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