臺灣博碩士論文加值系統

於覆晶封裝(flip-chip technology)銲接點與三維封裝(3D packages)微銲點中，界面介金屬化合物（intermetallic compounds）之性質包括形貌、相穩定性、機械性質與晶粒結構將嚴重影響銲接點可靠度。其中，銲料合金與凸塊底層金屬材料的選擇是影響介金屬化合物微結構、相生成與機械強度的重要議題。因此，本研究開發微量鎳參雜之銲料合金與銅鋅凸塊底層金屬，並將其應用於銲接點、微銲點與暫態液相接合中，深入探討鎳與鋅元素對介金屬化合物與可靠度之影響。
本研究首先針對鎳與鋅元素對覆晶接合銲接點中介金屬化合物之影響進行探討。研究發現，參雜微量鎳元素於銲料合金中有助於抑制Cu3Sn之成長並改變界面介金屬化合物之生成形貌，而銅鋅凸塊底層金屬能有效的抑制銅錫介金屬化合物之生成。於SAC305-0.1Ni/Cu-15Zn銲接點中，更是發現鎳元素能增進鋅元素抑制介金屬化合物生長之效果。於此有效抑制生長的機制下，只有平坦的(Cu,Ni)6(Sn,Zn)5緩慢生成於銲接點界面，沒有任何的Cu3Sn與孔洞生成。
此外，SAC305-0.1Ni/Cu-15Zn銲接點於回焊後展現優異的機械可靠度，並於長時間熱處理的過程中，維持其機械強度。此結果歸因於其兩樣特性，其一，由鎳元素引起之平坦狀介金屬化合物將防止機械測試過程中，應力累積於介金屬化合物，其二，鋅元素於(Cu,Ni)6(Sn,Zn)5中能抑制高低溫相轉換，進而避免由晶體體積膨脹引起之應力生成於介金屬化合物中。因此，於鎳與鋅元素同時改善介金屬化合物之性質下，銲接點於熱處理前後皆能展現優異的機械可靠度。
本研究更進一步地將鋅元素抑制介金屬化合物之效果延伸應用於三維封裝微銲點。於微小銲點中，由於銲料體積小，介金屬化合物易大比例充斥整個銲點，其硬脆的特性將容易使銲接點在使用過程中失效，對封裝的可靠度產生莫大的威脅。另外，大片狀脆性Ag3Sn將生成於銲料之中，其與銲點本身之熱膨脹係數差異，將造成大量熱應力累積。於此研究中發現，將鋅元素參雜至銅凸塊底層金屬中能有效地抑制銅錫與銀錫化合物之生長，此抑制機制將會藉由熱力學理論與過冷效應進行解釋與深入探討。
為更深入了解鋅元素對介金屬化合物之效益，本研究於鋅元素添加之銲接點、微銲點與暫態液相接合中，針對介金屬化合物之晶粒結構進行探討。於銲料體積小之微銲點與暫態液相接合中，對接後之介金屬化合物其晶粒將呈現均勻且單一方向性，於外力衝擊下，此結構將容易使裂痕穿越銲點，造成破壞。本研究發現將傳統銅凸塊底層金屬置換為新穎銅鋅凸塊底層金屬後，鋅元素能使銲接點與微銲點中介金屬化合物之晶粒展現多方向性，進而阻止裂痕穿越行為，提升可靠度。
有趣地，於回焊後長滿介金屬化合物之暫態液相接合中，鋅元素引起之多向性介金屬化合物將形成交錯之結構，根據Hall-Petch理論，此交錯結構將能有效阻止差排滑移與裂痕穿越，進而提升整體可靠度。於長時間熱處理過程中，鋅元素仍然能使介金屬化合物仍呈現多向性之晶粒結構，並有效抑制Cu3Sn化合物之生成。此多向性結構生成之相關機制，本研究將藉由熱力學相關理論、第一原理模擬、電子顯微鏡觀察與背向散射繞射儀之結果進行深入探討。
綜合上述，鎳與鋅元素針對介金屬化合物展現優異的特性，包括抑制其生長、穩定生成相、微結構細化、韌性提升與晶粒結構改善等。本研究呈現之所有結果，有效解決覆晶封裝銲接點、三維封裝微銲點與暫態液相接合面臨之可靠度重要議題。因此，微量鎳參雜之銲料合金與銅鋅凸塊底層金屬將有機會成為電子構裝中穩定連結之理想材料。

The properties of interfacial intermetallic compound (IMC), including morphology, phase stability, mechanical properties and grain structure, significantly affect the reliability of solder joint in flip-chip technology (FCT) and micro-bump in 3D packages. The material selection for solder alloys and under bump metallurgies (UBMs) material is a critical issue to affect the microstructure, phase formation, and the mechanical strength of intermetallic compound. In this study, Ni-doped solder and Cu-Zn UBM were developed and applied on solder joints, micro-bump and transient liquid-phase (TLP) bonding. The effects of Ni and Zn on the IMCs and reliability are investigated and discussed.
The combined effects of Ni and Zn on interfacial IMC in solder joints were first investigated. Doping Ni in the solder joint suppressed the growth of Cu3Sn and altered the morphology of the interfacial intermetallic compounds (IMCs) from scallop type to layer type. In comparison with the Cu substrates, the Cu-Zn substrates effectively suppressed the formation of Cu-Sn IMCs. It was revealed that the presence of Ni acted to enhance the effect of Zn on the suppression of Cu-Sn IMCs in SAC305-0.1Ni/Cu-15Zn solder joint. The efficient limitation of IMCs lead to that only layer-type (Cu,Ni)6(Sn,Zn)5 formed at joint interface before and after aging.
Furthermore, it was notable that the SAC305-0.1Ni/Cu-15Zn solder joint exhibited good impact reliability after reflow and maintained the bonding strength during thermal aging for a long time. The formation of layer-type IMCs caused by Ni prevents the stress accumulation in IMCs under high speed impact test. Moreover, doping small amount of Zn into (Cu,Ni)6(Sn,Zn)5 inhibited the phase transformation (η-Cu6Sn5 to η’-Cu6Sn5) during aging and thus avoided the occurrence of stress in IMC caused by volume expansion. In SAC305-0.1Ni/Cu-15Zn solder joint, the properties of interfacial IMCs were simultaneously modified by Ni and Zn, resulting in the high bonding strength before and after aging.
Thereupon, the advantages of Zn on IMCs suppression was extended to be used in micro-bumps of 3D packages. Due to the small size of micro-bumps, Cu-Sn intermetallic compounds (IMCs) rapidly form from the Cu pads. These brittle IMCs occupy the entire joint and weaken joint reliability. Moreover, Ag3Sn tends to precipitate inside the solder in large plates, which results in the accumulation of thermal stress due to a CTE mismatch between Ag3Sn and β-Sn. It wass demonstrated that doping Zn into one of the Cu substrates effectively suppressesed the growth of Cu-Sn and Ag-Sn IMCs. The mechanisms involved were explained in detail using thermodynamic theories and undercooling effects.
To further study the Zn effects on IMC, the evolution of grain structures in IMCs in Zn-doped solder joints, micro-bumps, and TLP bondings were investigated. Due to the small size of micro-bumps and TLP bonding, the grain orientation of impinged intermetallic compounds (IMCs) tends to be homogenous and closely-grouped, allowing cracks to more easily propagate under impact experiences. Replacing the Cu substrate with Cu-Zn causes the grain orientation of Cu-Sn IMCs in both solder joints and micro-bumps to become more random and dispersed, which may hinder crack propagation and enhance the bonding strength of joint interface.
Fancifully, in the Zn-doped TLP bonding composed of IMC, the randomly-orientated IMCs formed as interfolding pattern after reflow. According to the Hall-Petch theory, this interfolded structure may inhibit the move of dislocations and propagation of cracks. Besides, Zn in the TLP bonding efficiently retained the multi-orientation structure of Cu-Sn IMCs and suppressed the formation of Cu3Sn during lone-time aging. The formation mechanisms of randomly-orientated IMCs were explained in details using thermodynamic related theories, First-principle simulation, FE-SEM observation and EBSD analyses.
In summary, Ni and Zn exhibits good ability on suppression, phase stabilization, refinement, toughness enhancement and grain structure modification of IMCs. All the results in this study provide the solutions for critical issues of reliability in solder joints, micro-bumps and TLP bondings. Therefore, Cu-Zn UBM and Ni-doped solder are expected to be two of the idea materials for stable interconnections in electronic packages.

Contents
Lists of Table XII
Figures Caption XIV
Chapter I Introduction 1
1.1 Background 1
1.2 Motivations and Goals in this Study 2
1.2.1 Suppressing the growth of interfacial Cu-Sn intermetallic compounds in the Sn-3.0Ag-0.5Cu-0.1Ni/Cu-15Zn solder joint during thermal aging 4
1.2.2 Improving the shear strength of Sn-Ag-Cu-Ni/Cu-Zn solder joints via modifying the microstructure and phase stability of Cu-Sn intermetallic compounds 5
1.2.3 Retarding the Cu-Sn and Ag-Sn Intermetallic Compounds by Applying Cu-xZn Alloy on Micro-bump in Novel 3D-IC Technologies 6
1.2.4 Growth orientation of Cu-Sn IMC in Cu/Sn-3.5Ag/Cu-xZn micro-bumps and Zn-doped solder joints 7
1.2.5 Grain structure modification of Cu-Sn IMCs by applying Cu-Zn UBM on transient liquid-phase bonding in novel 3D-IC Technologies 8
1.2.6 Suppression of Cu3Sn layer and formation of multi-orientation IMCs during thermal aging in Cu/Sn-3.5Ag/Cu-15Zn transient liquid-phase bonding in novel 3D-IC Technologies 9
Chapter II Literature Review 11
2.1 Electronic Package 11
2.2 Flip-Chip Technology 12
2.3 Solder Bump 13
2.3.1 Pb-Free Solder 14
2.4 Under Bump Metallurgy (UBM) 15
2.4.1 Cu-Based UBM 16
2.5 Metallurgical Reactions in Pb-Free Solder Joints 16
2.5.1 Metallurgical Reactions between Pb-free Solder and Cu UBM 17
2.6 Ni Addition to Sn-Based Solder Alloy on Cu UBM 18
2.7 Zn effects on Ag-Sn and Cu-Sn IMCs in solder joint 20
2.7.1 Zn Addition to Sn-Based Solder Alloy on Cu UBM 20
2.7.2 Metallurgical Reactions between Solders and Cu-Zn UBM 22
2.8 Three Dimensional Packages (3D packages) 23
2.9 Metallurgical Reactions in Small-sized Solder Joint 25
2.9.1 Metallurgical Reactions in Cu-based Micro-bump 26
2.9.2 Metallurgical Reactions in Cu-based Transient Liquid Phase Bonding 27
2.10. Properties of Cu6Sn5 IMC at Solder/Cu Interface 28
2.10.1 Grain Structure and Preferred Orientation of Cu6Sn5 at Solder/Cu Interface 28
2.10.2 Multiple morphologies of Cu6Sn5 at Solder/Cu Interface 30
2.10.3 Phase stability of Cu6Sn5 at Solder/Cu Interface 31
Chapter III Experimental Procedures 69
3.1 Preparation and Analysis for SAC305-0.1Ni/Cu-xZn (x= 0 or 15 wt %) Solder Joints 69
3.1.1 Fabrication of SAC305-0.1Ni/Cu-xZn (x= 0 or 15 wt %) Solder Joints 69
3.1.2 Analysis Methods for SAC305-0.1Ni/Cu-xZn (x= 0 or 15 wt %) Solder Joints 70
3.2 High Speed Impact Testing and Characterization Analyzing for SAC305-0.1Ni/Cu-xZn (x= 0 or 15 wt %) Solder Joints 71
3.3 Preparation and Grain Analysis for Cu6(Sn,Zn)5 in SAC305/Cu-xZn (x=0 or 15 wt %) Solder Joint and Cu/Sn-3.5Ag/Cu-xZn Micro-bump 72
3.4 Preparation and Analysis for Cu/Sn-3.5Ag/Cu-xZn (x=0 or 15 wt%) Micro-bump after Reflow 72
3.4.1 Fabrication of Cu/Sn-3.5Ag/Cu-xZn Micro-bump 73
3.4.2 Microstructural Evaluation and Compositional Analysis of Cu/Sn-3.5Ag/Cu-xZn Micro-bump 73
3.5 Preparation and Analysis for Cu/Sn-3.5Ag/Cu-xZn (x=0 or 15 wt %) Transient Liquid Phase Bonding after Reflow 73
3.5.1 Fabrication of Cu/Sn-3.5Ag/Cu-xZn Transient Liquid Phase Bonding after Reflow 74
3.5.2 Analysis for the Cu/Sn-3.5Ag/Cu-xZn Transient Liquid Phase Bonding 74
3.6 Preparation and Analysis for Cu/Sn-3.5Ag/Cu-xZn (x=0 or 15 wt %) Transient Liquid Phase Bonding after Thermal Aging 75
3.6.1 Fabrication of Cu/Sn-3.5Ag/Cu-xZn Transient Liquid Phase Bonding after Thermal Aging 75
3.6.2 Microstructure and Composition Analysis of Cu/Sn-3.5Ag/Cu-xZn Transient Liquid Phase Bonding after Thermal Aging 75
Chapter IV Results and Discussion 82
4.1 Suppressing the growth of interfacial Cu-Sn intermetallic compounds in the Sn-3.0Ag-0.5Cu-0.1Ni/Cu-15Zn solder joint during thermal aging 82
4.1.1 Phase identification and microstructural variation 82
4.1.2 Quantitative analysis and elemental distribution 85
4.1.3 Mechanism of phase formation 87
4.2 Improving the shear strength of Sn-Ag-Cu-Ni/Cu-Zn solder joints via modifying the microstructure and phase stability of Cu-Sn intermetallic compounds 97
4.2.1 Interfacial reaction between the Ni-doped solder and the Cu-xZn (x=0 or 15 wt%) substrate before and after thermal aging 97
4.2.2 High speed shear testing for the SAC305-0.1Ni/Cu and SAC305-0.1Ni/Cu-15Zn solder joints before and after thermal aging 99
4.2.3 Mechanism for the improvement of impact reliability in SAC305-0.1Ni/Cu-15Zn solder joints 101
4.3 Retarding the Cu-Sn and Ag-Sn Intermetallic Compounds by Applying Cu-xZn Alloy on Micro-bump in Novel 3D-IC Technologies 114
4.3.1 Microstructure observation of interfacial Cu-Sn IMCs in Cu/Sn3.5Ag/Cu-xZn (x=0 or 15 wt%) micro-bumps 114
4.3.2 Elemental distribution in micro-bump 115
4.3.3 Formation mechanisms of Ag-Sn and Cu-Sn IMCs in Cu/Sn3.5Ag/Cu-xZn (x=0 or 15 wt%) micro-bumps 115
4.4 Growth orientation of Cu-Sn IMC in Cu/Sn-3.5Ag/Cu-xZn micro-bumps and Zn-doped solder joint 125
4.4.1 Grain structure and orientation of Cu-Sn IMC in in Cu/Sn-3.5Ag/Cu-xZn micro-bumps and Zn-doped solder joint 125
4.4.2 Possible mechanisms of randomly-orientated Cu6(Sn,Zn)5 in micro-bump 127
4.5 Grain structure modification of Cu-Sn IMCs by applying Cu-Zn UBM on transient liquid-phase bonding in novel 3D-IC Technologies 133
4.5.1 Grain structure and orientation of Cu-Sn IMC in Cu/Sn-3.5Ag/Cu-xZn (x=0 or 15 wt %) TLP bonding 133
4.5.2 Possible mechanisms of the randomly-orientated Cu6(Sn,Zn)5 in TLP bonding 135
4.5.3 Frist principle simulation for lattice lengths in Cu6(Sn,Zn)5 with various Zn concentration 137
4.6 Suppression of Cu3Sn layer and formation of multi-orientation IMCs during thermal aging in Cu/Sn-3.5Ag/Cu-15Zn transient liquid-phase bonding in novel 3D-IC Technologies 148
4.6.1 Microstructure observation of Cu-Sn IMCs in Cu/Sn-3.5Ag/Cu-xZn (x=0 or 15 wt%) TLP bonding before and after thermal aging 148
4.6.2 Possible mechanisms of Cu-Sn IMCs suppression in TLP bonding during thermal aging 149
4.6.3 Grain structure detection of Cu-Sn IMCs in TLP bonding after thermal aging 150
Chapter V Conclusions 157
References 160

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