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Title Page 2

Abstract 5

Contents 7

List of Abbreviations 11

CHAPTER 1. Introduction 13

1.1. Characteristics of Metal Halide Perovskite 13

1.2. Device Architecture and Working Mechanism of PeLEDs 16

1.3. Parameters of PeLEDs 19

1.4. Types of Perovskite Materials for LEDs 23

(1) Perovskite Nanocrystals (PeNCs) 23

(2) 3D Perovskites 23

(3) Perovskite Quantum Dots (QDs) 24

(4) Quasi-2D Perovskites 26

1.5. Characteristics of Quasi-2D Perovskite 27

CHAPTER 2. Full Color Emission using Quasi-2D Perovskite Light-Emitting Diodes 31

2.1. Research Background 31

2.2. Experimental Details 33

2.2.1. Chemicals and Materials 33

2.2.2. Preparation of CsX NCs 33

2.2.3. Fabrication of Quasi-2D Perovskite Film 33

2.2.4. CsX NCs Treatment on Quasi-2D Perovskite Film 34

2.2.5. Device Fabrication 34

2.2.6. Characterization of Films and Devices 34

2.3. Results and Discussion 35

2.3.1. Optimization of Quasi-2D Perovskite Light-Emitting Diodes 35

2.3.2. Realization of Full Color based on CsX NC-treated Quasi-2D Perovskite Light-Emitting Diodes 44

2.4. Conclusion 51

REFERENCES 52

List of Tables 10

Table 2.1. Device characteristics of PeLEDs with or without L-phenylalanine 35

Table 2.2. Device characteristics of PeLEDs with or without PSS-Na 36

Table 2.3. Device characteristics of PeLEDs with or without NH₃·H₂O 37

Table 2.4. Device characteristics of PeLEDs with different thermal annealing conditions 38

Table 2.5. Device characteristics of PeLEDs with different amount of antisolvent 39

Table 2.6. Device characteristics of PeLEDs with different drop timing of antisolvent 40

Table 2.7. Device characteristics of PeLEDs with different TPBi thickness 41

Table 2.8. Device characteristics of PeLEDs with different LiF thickness 42

Table 2.9. Distribution of EQEs of PeLEDs with different TPBi and LiF thickness 43

Table 2.10. Device characteristics of the control and CsCl-treated PeLEDs with different coating... 46

Table 2.11. Device characteristics of the control and CsCl-treated PeLEDs with different film... 47

Table 2.12. Device characteristics of CsCl-treated PeLEDs with or without intermediate thermal... 47

Table 2.13. Device characteristics of the control and CsX-treated PeLEDs 50

List of Figures 8

Figure 1.1. (a) Crystal structure of metal halide perovskite ABX₃... 14

Figure 1.2. Schematic energy level diagram of metal halide perovskites 15

Figure 1.3. FWHM and dimension of perovskite, inorganic quantum dots (QDs), and organic emitters 15

Figure 1.4. Scheme of device architectures of LEDs. (Conventional structure (Left) and Inverted... 16

Figure 1.5. Schematic of energy levels of some commonly used HTL, ETL, and emissive perovskite... 17

Figure 1.6. Working mechanism of PeLEDs 18

Figure 1.7. Optical power distributions and losses in PeLEDs 22

Figure 1.8. Perovskite nanocrystal solutions under the UV lamp 23

Figure 1.9. Structure of 3D perovskite 24

Figure 1.10. Scanning electron microscopy (SEM) images of ITO/TiO₂/Perovskite samples... 24

Figure 1.11. Emission color changes depending on the size (Left) and composition (Right) 25

Figure 1.12. Illustration of quantum confinement effect 25

Figure 1.13. Bandgap calculations of quasi-2D perovskite with different number of inorganic... 26

Figure 1.14. Structure and properties of a quasi-2D perovskite 27

Figure 1.15. Crystal structure of 2D and 3D halide perovskites 28

Figure 1.16. Spectral tunability of quasi-2D perovskite 29

Figure 1.17. (a) Exciton binding energy change with different number of inorganic layers.... 30

Figure 2.1. Device characteristics of PeLEDs with or without L-phenylalanine. (a) J-V-L plot. (b) EQE-... 35

Figure 2.2. Device characteristics of PeLEDs with or without PSS-Na. (a) J-V-L plot. (b) EQE-V plot.... 36

Figure 2.3. Device characteristics of PeLEDs with or without NH₃·H₂O. (a) J-V-L plot. (b) EQE-V plot 37

Figure 2.4. Device characteristics of PeLEDs with different thermal annealing conditions. (a) J-V-L... 38

Figure 2.5. Device characteristics of PeLEDs with different amount of antisolvent. (a) J-V-L plot. (b)... 39

Figure 2.6. Device characteristics of PeLEDs with different drop timing of antisolvent. (a) J-V-L plot.... 40

Figure 2.7. Device characteristics of PeLEDs with different TPBi thickness. (a) J-V-L plot. (b) EQE-V... 41

Figure 2.8. Device characteristics of PeLEDs with different LiF thickness. (a) J-V-L plot. (b) EQE-V... 42

Figure 2.9. Schematic illustration of the fabrication of modified emissive layer with CsX nanocrystals 44

Figure 2.10. PL emission spectra of CsX-treated films(X＝I, Br, and Cl) with 365㎚ excitation 44

Figure 2.11. Schematic illustration of CsX-treated quasi-2D perovskite light-emitting diodes 45

Figure 2.12. Device characteristics of the control and CsCl-treated PeLEDs with different coating... 45

Figure 2.13. Device characteristics of the control and CsCl-treated PeLEDs with different film... 46

Figure 2.14. EL spectra for (a) control, (b) CsI, (c) CsBr, and (d) CsCl treatment with different... 48

Figure 2.15. Device characteristics of CsX-treated PeLEDs. (a) EL spectra. (b) CIE coordinates. (c) J-... 49

초록보기

 Perovskite has attracted great attention in next-generation optoelectronic devices such as light-emitting diodes (LEDs) and solar cells because of its outstanding optical and electrical properties. It can realize various luminescent properties through high absorption coefficient and carrier mobility. Moreover, it shows easy control of composition to change bandgap. In addition, it shows narrow linewidth in photoluminescence (PL) and electroluminescence (EL) spectra, and good defect tolerance. Specifically for quasi-2D perovskite, it can obtain a lot of radiative recombination by quantum confinement and dielectric confinement effect. The energy funneling effect from its unique structure can achieve high luminous efficiency and this structure can obtain high resistance to moisture and heat which is related to device stability. Furthermore, since dimensional engineering of quasi-2D perovskite can reduce the use of chlorine to make the blue emission, this material could be another candidate for light-emitting materials. With the advantages of perovskite light-emitting materials, research on LEDs has been conducted continuously. External quantum efficiencies (EQEs) of perovskite LEDs (PeLEDs) with red and green emission have already exceeded 20%. Blue emission used to lag behind these two colors, but it has recently caught up with them, reaching 21.4 % of EQE at 483 nm. Additionally, some studies have exhibited the significance of full color emission, which further increases the possibility of commercialization. Herein, we suggest the importance of device optimization and realization of full colors using quasi-2D PeLEDs. Changes in each layer that consists of the LED device were introduced by using various materials and film formation methods. With these structural conditions, quasi-2D PeLEDs were fabricated with CsX (X = I, Br, and Cl) NCs treatment to change emission color by halide exchange with CsI and CsCl. Overall, this research can provide new access for the implementation of full color LEDs.

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