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Title Page 2

Abstract 5

초록 6

Contents 7

List of Abbreviations 14

Chapter 1. Introduction to Organic Solar Cells 16

1.1. Renewable energy - powering a safer future 16

1.2. Organic Solar Cells 17

1.2.1. Historical Background 17

1.3. Fundamental Principles 18

1.3.1. Device Architectures 18

1.4. Recent Strategies for efficient OSCs 25

1.4.1. Development in Acceptor Materials 25

1.5. Evaluation and Assessment 29

1.5.1. SWOT analysis for OPVs 30

References 32

Chapter 2. Morphological Optimizations in OSCs 37

Abstract 37

2.1. Introduction 39

2.1.1. Role of morphology on OSCs 39

2.1.2 Factor Affecting the Morphology of OSCs Blend Films 39

2.2. Literature Review 44

2.3. Materials 45

Experimental Section 47

2.4.1. Device Fabrication 47

2.4.2. Charge Carrier Mobility Measurements 47

2.5. Device Characterization Methods 48

2.5.1. External Quantum Efficiency (EQE) 48

2.5.2. Atomic Force Microscopy (AFM) 49

2.5.3. Transmission Electron Microscopy 49

2.5.4. Grazing Incidence Wide Angle Spectroscopy 50

2.5.5. Differential Scanning Calorimetry 51

2.5.3. Thermogravimetric analysis 51

2.5.4. Fourier transform infrared spectroscopy 51

2.5.5. UV-Vis Spectroscopy 51

2.5.6. Computational Methodology 52

2.6. Results and Discussions 53

2.6.1. Validity of Removal of Solid Additive 53

2.6.2. Formation of Eutectic Phase 54

2.6.3. Intermolecular Interaction Analysis 56

2.6.4. Photovoltaic Performance and Charge Carrier Dynamics 57

2.6.5. Influence of DHB Additives on Materials Morphology 62

2.6.6. Assessing Miscibility Changes induced by DHB Additives 64

2.6.7. Exploring Molecular Orientation in DHB Modified Systems 66

2.6.8. Theoretical Study by DFT 71

2.6.9. Universality Test 75

Conclusion 78

References 79

Chapter 3. Improving Stability in OSCs: The Role of Cathode Interlayers 85

Abstract 85

3.1. Introduction 87

3.1.1. Degradation Mechanism 87

3.2. Stability Testing Protocols 91

3.3. Device Architectures uses for Stability 91

3.4. Stability Testing Conditions 92

3.5. CILs and AILs used in OSCs 93

3.5.1. ZnO as CILs 94

3.6. ZnO Modified ETL with IL for Enhanced Efficiency/Photo-stability in OSCs 94

3.6.1. Experimental Procedure 96

3.7. Results and Discussions 97

3.7.1. Materials properties 97

3.7.2. Photovoltaic characteristics 100

3.7.3. Morphological properties 105

3.7.4. Operational stability 106

Conclusion 110

References 111

Chapter 4. Enhancing Stability in OSCs: The Role of Intermolecular Hydrogen Bonding 118

Abstract 118

4.1. Introduction 119

4.2. Random Terpolymers with hydrogen bonding moiety for enhance d stability 120

4.2.1. Experimental Procedure 122

4.3. Results and discussions 122

4.3.1. Material structures and confirmation of hydrogen bonding 122

4.3.2. Photovoltaic properties 124

4.3.3. Photo-stability 127

4.3.4. Thermal-stability 129

4.3.5. Morphological Study 130

Conclusion 136

References 137

Summary 139

List of Tables 13

Table 2.1. Photovoltaic parameters of inverted OSCs based on PM6:Y6-BO with... 58

Table 2.2. Summary of contact angles for water and diiodomethane, surface... 65

Table 2.3. The orientation distribution of PM6 depending on the DHB solid... 69

Table 2.4. The orientation distribution of Y6-BO depending on the DHB solid... 70

Table 2.5. Crystallographic parameters of PM6:Y6-BO without and with DHB... 70

Table 2.6. The orientation distribution of PM6:Y6-BO depending on the... 71

Table 2.7. Summary of binding free energy and dipole moment parameters of PM6,... 75

Table 3.1. Photovoltaic Parameters for OSC Devices with Different Interlayers... 102

Table 3.2. Fitted parameters of EIS plots for OSCs based on different ETLs 105

Table 3.3. Electron and Hole mobilities of PM6:Y6-BO devices based on ZnO and... 105

Table 3.4. Contact angel of water and diiodomethane and surface energies of... 107

Table 4.1. Photovoltaic parameters of PSCs based on polymer donor:Y6- BO... 126

Table 4.2. Photovoltaic parameters of flexible PSCs based on polymer donor: Y6-... 133

Table 4.3. Mechanical properties from pseudo free-standing tensile test of neat... 135

List of Figures 11

Figure 1.1. Renewable energy sources, such as wind and solar, emit little to no... 16

Figure 1.2. Schematic diagram of different OSCs device structures 19

Figure 1.3. Idealized J-V curve for an OPV device 20

Figure 1.4. Schematic working principle of BHJ OPVs. The bounded Frenkel... 22

Figure 1.5. Illustration of geminate and non-geminate recombination process 23

Figure 1.6. Molecular structures of NFAs materials for efficient OSCs compared... 26

Figure 1.7. Molecular structures of donor materials for efficient OSCs 27

Figure 1.8. Illustration of additive injection in OSCs 28

Figure 1.9. Possible compositions of three components constitute ternary blend... 29

Figure 2.1. BHJ film morphology. (A) PM6 and Y6 composition on the BHJ film... 41

Figure 2.2. Detailed crystal information of DR3TBDTT:PC71BM blend films... 42

Figure 2.3. Related chemical structures of processing solvents and additives 43

Figure 2.4. Chemical structure of photoactive material and solid additives 46

Figure 2.5. Device architecture of inverted OSC 46

Figure 2.6. Morphologies of organic film with size scale 50

Figure 2.7. FTIR spectra of (a) DIB, BHJ, BHJ+DIB, (b) DBrB, BHJ, BHJ+... 53

Figure 2.8. DSC thermograms (a, b) cooling and (c, d) heating process of (a, c)... 55

Figure 2.9. FTIR spectra of (a) PM6, PM6: DHB and (b) Y6-BO, Y6-BO: DHB... 57

Figure 2.10. (a) J-V characteristics, (b) EQE and integrated JSC curves, and (c)... 57

Figure 2.11. Dark J-V plots of (a) electron-only and (b) hole-only devices based... 60

Figure 2.12. (a) AFM height, (b) phase, and (c) TEM images of optimized blend... 62

Figure 2.13. AFM (a, c) height and (b, d) phase images of (a, b) PM6, PM6:DHB... 63

Figure 2.14. Contact angles of (a, c) water and (b, d) diiodomethane droplets on... 64

Figure 2.15. 2D-GIWAXS pattern images of PM6:Y6-BO blend film with (a)... 67

Figure 2.16. 2D-GIWAXS scattering pattern images of (a) PM6, PM6+DHB and... 68

Figure 2.17. Azimuthal cut plots of (010) scattering peaks for (a) PM6, PM6:... 69

Figure 2.18. ESP patterns of neat PM6 donor, Y6-BO acceptor and DHB solid... 72

Figure 2.19. EPS distribution of (a-c) PM6: DHB and (d-f) Y6-BO: DHB in the... 73

Figure 2.20. Optimized structures for (a) PM6: DHB and (b) Y6-BO: DHB... 74

Figure 2.21. Molecular structure of Y6-HU. (b) J-V curves and (c) EQE spectra... 76

Figure 2.22. Chemical structure of IT-4F. (b) Best J-V curves of OSCs based on... 77

Figure 3.1. Summary of ISOS test guidelines 92

Figure 3.2. Illustration of the dipole formation over ZnO ETL in SAMs based 95

Figure 3.3. (a) UV-vis absorption and optical transmittance of ZnO and ZnO/IL (b)... 98

Figure 3.4. (a) Device configuration of the inverted OSC and chemical of PM6,... 101

Figure 3.5. Electron and hole mobilities devices of PM6:Y6-BO based on... 105

Figure 3.6. Surface topographic AFM images of (a) fresh and (b) photo-aged OSC... 106

Figure 3.7. Contact angle of water and diiodomethane films of (a)... 107

Figure 3.8. Normalized photovoltaic parameters of (a) VOC, (b) JSC, (c) FF, and... 108

Figure 4.1. Intermolecular H-bonding and F...S, O...S interactions enhances the... 121

Figure 4.2. (a) Chemical structures of polymer donors and Y6-BO acceptor. (b)... 123

Figure 4.3. a) Best J-V characteristics, (b) EQE curves, and (c) Jph versus Veff... 125

Figure 4.4. Evolution of the J-V characteristics of the PSCs based on (a) PM6, (b)... 128

Figure 4.5. Normalized photovoltaic parameters of (a) VOC, (b) JSC, (c) FF, and (d)...[이미지참조] 129

Figure 4.6. Thermal stability and AFM of the polymer donor:Y6-BO acceptor PSCs as a... 129

Figure 4.7. Normalized photovoltaic parameters of (a) JSC, (b) VOC, and (c) FF...[이미지참조] 131

Figure 4.8. (a) The picture of flexible PSC. (b) The best J-V curves, (c) bending... 132

초록보기

유기 태양전지(OSC)는 유기 물질의 고유한 장점을 활용하여 지속 가능한 태양 에너지 활용을 위해 발전되어 왔다. 그러나 이러한 잠재력에도 불구하고 다양한 장애물이 OSC의 상용화를 가로막고 있다. 고효율, 안정성, 재현성을 달성하는 것이 주요 과제이며, 이를 위해 전 세계적으로 지속적인 연구가 진행되고 있다. 연구자들은 새로운 도너 또는 억셉터 재료, 첨가제, 층간 엔지니어링 등 다양한 전략을 모색하여 OSC 성능 향상을 위해 노력했다. 이러한 접근 방식 중 휘발성 고체 첨가제를 활성층에 통합하는 방법은 비용 효율성, 처리 용이성, 효율성과 안정성을 모두 향상시킬 수 있는 잠재력으로 인해 특히 유망한 방법으로 부상하고 있다. 이 논문에서는 비 할로겐 용매인 오 쏘-자일렌 (o-xylene)과 함께 폴리머 공여체 및 수용체를 사용하여 OSC에서 휘발성 고체 첨가제의 역할을 연구한다. 또한 음극 중간층 재료(CIL)로서 효율적인 이온 성 액체(IL)를 탐구하여 OSC 효율과 장기 안정성이 크게 개선됨을 보였다. 또한 분자 간 수소 결합이 OSC 소자 성능과 안정성에 미치는 영향에 대한 종합적인 분석을 수행했다. 이 연구는 도너 삼성분계 활용하여 캐리어의 재결합 손실을 완화하면서 효율적인 전하 수송 및 생성에 도움이 되는 형태를 밝혀냈다. 또한, 기계적 특성을 포함한 광 전 효율과 장기 안정성을 향상시켰다. 이러한 연구 결과는 OSC에 대한 이해를 심화할 뿐만 아니라 효율성과 내구성이 향상된 차세대 태양전지 기술 개발의 토대를 마련할 것으로 기대한다.

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