鋅黃錫礦太陽能電池之銀合金化及前介面鈍化研究

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研究生：	黃韋智 Huang, Wei-Chih
論文名稱：	鋅黃錫礦太陽能電池之銀合金化及前介面鈍化研究 Investigation of Ag-alloying and front interface passivation of kesterite solar cells
指導教授：	賴志煌 Lai, Chih-Huang
口試委員:	黃瑜 Huang, Yu 謝東坡 Hsieh, Tung-Po 闕郁倫 Chueh, Yu-Lun 林姿瑩 Lin, Tzu-Ying
學位類別：	博士 Doctor
系所名稱：	工學院 - 材料科學工程學系 Materials Science and Engineering
論文出版年：	2022
畢業學年度：	110
語文別：	英文
論文頁數：	150
中文關鍵詞：	鋅黃錫礦、硒硫化銀銅鋅錫、噴霧熱裂解、銅鋅錯位、點接觸、鈍化
外文關鍵詞：	kesterite, (Cu, Ag)2ZnSn(S, Se)4, spray pyrolysis, Cu_Zn antisite, point contact, passivation
相關次數：	點閱：2 下載：0
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硒硫化銅鋅錫為鋅黃錫礦結構，是地表多豐且組成便宜的材料，有高吸收係數使其具潛力作為低成本高效率的薄膜太陽能電池。然而其光電轉換效率仍停滯於12.6%，遠低於硒硫化銅銦鎵太陽能電池的23.35%。本博士論文針對鋅黃錫礦薄膜太陽能電池的開路電壓不足採取對策，以改善光電轉換效率。銀的合金化形成新穎的硒硫化銀銅鋅錫化合物，被認為能夠減少銅鋅錯位，減少能帶尾端態並提升開路電壓。然而引入銀將使本已複雜的四/五元化合物變成更複雜的五/六元素化合物，在製程上更具挑戰性。首先我們研發以低成本，環境友善，具有大面積塗佈能力的噴霧熱裂解製程，製作含銀的銀-銅-鋅-錫-硫前驅物並探討形成硒硫化銀銅鋅錫薄膜的過程。選擇溶解度較高的金屬鹽類以及適當的添加順序，我們能夠配製透明均質的前驅物水溶液，噴霧塗佈後形成成分均勻的硫化物前驅物薄膜，製作出成分均勻，高銀含量且較少二次相的硒硫化銀銅鋅錫化合物。接著我們深入探討此製程製備的硒硫化銀銅鋅錫薄膜太陽能電池。銀合金化幫助晶粒成長、提高能隙、減少銅鋅錯位以及能帶尾端態，但伴隨高溫相穩定性問題，低載子濃度及缺鈉的介面載子復合。充分考慮以上因素後，我們能在較低的製程溫度，額外添加鈉改善性質，在Ag/(Ag+Cu)~ 35%的鋅黃錫礦太陽能電池達到10 %的光電轉換效率，是高銀含量(Ag/(Ag+Cu)> 30%)鋅黃錫礦的效率紀錄。為解決鋅黃錫礦介面載子復合問題，在前介面引入介電鈍化層搭配點接觸結構為一理想方法。然而在硫系化物前介面形成點接觸結構，因表面粗糙且額外圖案化製程可能損傷吸收層表面，非常具挑戰性。利用在硒化過程中原位形成的硫化鋅二次相奈米粒子作為舉離製程的遮罩，我們首次在前介面形成具點接觸的氧化鉭薄膜鈍化結構，減少介面載子復合，有效提升開路電壓以及光電轉換效率，為硫系化物太陽能電池的表面鈍化帶來更多可能。

Cu2ZnSn(S, Se)4, with kesterite crystal structure, is an earth abundant and cheap material which possesses high absorption coefficient and make it a potential candidate for low cost high efficiency thin film solar cells. However, the efficiency is still staggered around 12.6 %, which is still far lower than the Cu(In, Ga)(S, Se)2 of 23.35%.This dissertation aims to take action to solve VOC-deficit problem of kesterite solar cells to improve the efficiency. Incorporation of Ag to form novel (Ag, Cu)2ZnSn(S,Se)4 (ACZTSSe) compounds has been regarded as an approach to reducing Cu-Zn disorder and tailing states. However, Ag incorporation makes the materials more complicated with five or six elements, which is even more challenging for processing.
First, we fabricate ACZTSSe films through low-cost, environment-friendly, and scalable aqueous spray pyrolysis process. The formation mechanism is discussed and compared with CZTSSe. With proper choices of chemicals and addition sequence, clear Ag-containing solution can be formed, which was utilized to deposit ACZTSSe films with high Ag content and less secondary phases in 2015.
Next, we further discuss ACZTSSe solar cells through the process. Ag incorporation helps grain growth, increases bandgap, reduces Cu-Zn antisites and Urbach tail energy, but accompanied by the phase stability problem, low carrier concentration and interface recombination due to Na-deficient. Considering the factors above, we reached 10% efficiency with Ag/(Ag+Cu) ~0.35, which is processed at lower temperature with improved properties by extra Na. This is the record of kesterite solar cells with high Ag content (Ag/(Ag+Cu) ≥ 30%).
Introducing a dielectric passivation layer with point contacts is an ideal way to solve interface recombination. However, forming point contacts at front surface of chalcogenide solar cells is even challenging because extra patterning process may damage the absorber surface. With the help of in-situ formed ZnS nanoparticles to act as a mask for lift-off process, we first demonstrated the TaOx film with point contact openings at front interface to reduce interface recombination, resulting in the improved VOC and efficiency, which bring more opportunity for the developments of chalcogenide solar cells.

Abstract                                                i
中文摘要                                                 ii
Acknowledgements                                        iii
Contents                                                iv
List of Figures                                         vii
List of Tables                                          xiii
Chapter 1                                                  1
General introduction                                       1
Chapter 2                                                  4
Background                                                 4
2.1 Physics of photovoltaics                               4
2.1.1 P-N junction                                         4
2.1.2 Current density (J) -voltage (V) characteristics of p-n junction and solar cells.                                  5
2.1.3 Recombination mechanism in solar cells               9
2.2 Introduction to kesterite solar cells                 11
2.2.1 General properties of Cu2ZnSn(S, Se)4               11
2.2.2 Process of kesterite solar cells                    15
2.3 Cation substitution of kesterite                      30
2.3.1 Concepts of cation substitution                     30
2.3.2 Ge substitution for Sn                              31
2.3.3 Cd substitution for Zn                              34
2.3.4 Ag substitution for Cu                              36
2.4 Front surface dielectric passivation                  39
2.4.1 Materials for front surface passivation layers      39
2.4.2 Point contacts                                      42
Chapter 3                                                 45
Experimental techniques                                   45
3.1 Sample preparation                                    45
3.1.1 Absorber preparation                                45
3.1.2 Sputtering                                          47
3.1.3 Backend process                                     48
3.2 Material analysis                                     49
3.2.1 X-ray diffraction                                   49
3.2.2 Scanning electron microscopy (SEM) and energy-dispersive X-ray spectroscopy (EDX)                                    50
3.2.3 Raman spectroscopy                                  51
3.2.4 Photoluminescence (PL) and time-resolved photoluminescence (TRPL)                                                    52
3.2.5 X-ray photoelectron spectroscopy                    53
3.2.6 Transmission electron microscopy (TEM)              55
3.2.7 Atomic force microscopy                             56
3.3 Electrical characterization                           57
3.3.1 Current density-voltage measurements                57
3.3.2 External quantum efficiency (EQE)                   59
3.3.3 Capacitance-based measurements                      60
Chapter 4                                                 63
Formation of Ag-alloyed kesterite by using spray pyrolysis63
4.1 Introduction                                          64
4.2 Experimental                                          65
4.3 Results and discussion                                67
4.3.1 Evolution of sprayed Cu-Zn-Sn-S precursor during selenization                                              67
4.3.2. Solution formation and evolution of Ag-Cu-Zn-Sn-S precursor
70
4.4 Conclusions                                           76
Chapter 5                                                 78
The role of Ag in aqueous solution processed (Ag,Cu)2ZnSn(S,Se)4 kesterite solar cells                                     78
5.1 Introduction                                          79
5.2 Experimental                                          80
5.3 Results and discussion                                82
5.4 Conclusions                                           99
Chapter 6                                                 101
ALD-TaOx layer with point contacts enabled by in-situ formed nanoparticles for front interface passivation of kesterite solar cells                                                     101
6.1 Introduction                                          102
6.2 Experimental                                          105
6.3 Results and discussion                                107
6.3.1. Formation of point openings using in-situ formed nanoparticles
107
6.3.2 Characterization of kesterite solar cells with point contact openings of TaOx passivation layer                        113
6.4 Conclusion                                            120
Chapter 7                                                 121
Conclusion and outlooks                                   121
References                                                124
Appendix                                                  148

                                

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