无氰共沉积电镀Au-Sn共晶合金工艺及其性能研究
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摘要
倒装芯片技术能够改善大功率LED出光率低和散热能力差的缺点,而倒装芯片的导热和导电均要通过凸点来实现,因此凸点性能的优劣直接影响着芯片的可靠性。Au-30at.%Sn共晶合金钎料,具有优良的力学性能和高可靠性,是倒装芯片结构凸点的理想材料。相对于蒸镀、溅射和化学镀法,电镀法制备Au-30at.%Sn共晶合金凸点具有成本低廉、工艺简单、凸点定位精确以及可制作小尺寸凸点等优点。然而,目前使用的氰化物Au-Sn镀液含有剧毒,严重污染环境和危害人身安全,因此急需开发一种无氰的Au-Sn合金电镀液。
本论文系统地研究了无氰亚硫酸盐-焦磷酸盐Au-Sn镀液体系中镀液成分和工艺参数对Au-Sn合金镀层表面形貌和镀层成分的影响；然后通过响应曲面法来精确控制Au-Sn共沉积镀层的成分；利用电化学手段分析了镀液成分对Au-Sn共沉积行为的影响规律；最后评价了Au-30at.%Sn共晶镀层的性能：对比了分层法与共沉积法制备的Au-30at.%Sn共晶合金凸点,并研究了共沉积法制备的Au-30at.%Sn共晶合金凸点与铜、镍基板间的界面反应。主要结论如下：
1、选用弱碱性的亚硫酸盐-焦磷酸盐镀液体系共沉积电镀Au-Sn合金镀层。以镀层的表面形貌和镀层成分作为评价指标优化镀液成分和工艺参数,其结果如下：Au与亚硫酸钠摩尔浓度比为1：12-1：24,Sn与焦磷酸钾摩尔浓度比为1：6-1：9,EDTA0.01-0.08mol/L,邻苯二酚0.01～0.07mol/L,抗坏血酸0.09mol/L,氯化镍0.005mol/L, pH7.5～8.5,温度35-45℃,搅拌速度200rpm,脉冲频率大于10Hz,当周期换向脉冲频率为100Hz时,正向电流导通时间不小于2ms,正向关段时间不小于4ms,负向电流导通时间不大于2ms,正反向工作电流比大于4：1。
2、采用响应曲面法对Au-Sn共沉积镀液成分和工艺参数进行调整来进一步精确控制Au-Sn合金镀层的成分。部分因子试验发现主因素及交互作用对镀层成分影响的大小顺序为C>A>E>AB>D>AD>B。以pH值、EDTA浓度和邻苯二酚浓度为因子进行中心复合试验建立响应与因子关系的模型,通过模型求解得到特定镀层成分对应的最优因子组合。利用该模型获得了对应Au-30at.%Sn共晶合金镀层的最优镀液成分和工艺参数,重复实验表明在此镀液成分和工艺参数下可以获得成分稳定的Au-30at.%Sn共晶成分镀层。共晶合金成分准确,实验具有可重复性。
3、利用电化学手段分析了镀液成分对金锡共沉积行为的影响规律。络合剂的加入使得Au、Sn沉积电位接近,有利于Au和Sn的共沉积。EDTA的加入,使得Au-Sn合金的还原峰电位正向移动；邻苯二酚的加入,使得Au-Sn合金的还原峰电位负向移动；当同时加入EDTA和邻苯二酚时,Au-Sn还原峰进一步负向移动。添加剂的加入使得Au-Sn阴极还原峰正向、负向移动,从而改变了Au-Sn共沉积行为。阴极还原峰正向移动,有利于镀层中Au含量增加,阴极还原峰负向移动,有利于镀层中Sn含量增加。Au-Sn合金的共沉积在还原峰电位下为扩散控制,随着电位的负移,将由扩散和电化学步骤混合控制。
4、对共沉积Au-30at.%Sn共晶合金镀层粗糙度、结合力、熔点和耐蚀性等性能进行评价。实验结果表明共沉积Au-30at.%Sn共晶合金镀层的粗糙度仅为几十纳米,与Si/TiW/Au基体结合力良好,其熔点为280.66℃,此外还具有良好的耐蚀性。共沉积法制备的Au-30at.%Sn共晶合金凸点与分层法制备的共晶合金凸点相比质量明显提高。共沉积的Au-30at.%Sn共晶合金镀层分别与Ni和Cu基板在310℃下钎焊反应,在Au-30at.%Sn/Ni界面处形成了(Ni,Au)3Sn2金属间化合物；在Au-30at.%Sn/Cu界面上形成了两层金属间化合物,靠近钎料的(Au,Cu)5Sn和靠近Cu基板的AuCu。Au-30at.%Sn共晶合金镀层与Ni、Cu基板形成良好连接,表明共沉积的Au-30at.%Sn共晶合金镀层具有良好的可焊性。
The flip-chip technology can improve the luminescence efficiency and thermal dissipation of high-power LEDs. Since the electric and thermal conductivities of flip-chip are carried out by solder bump, the capability of the bump has a direct impact on the chip reliability. Au-30at.%Sn eutectic solder is the idea material for flip-chip bump due to its excellent mechanical properties and high reliability. Electroplating of Au-30at.%Sn eutectic alloy bump has the advantages of low cost, simple process, precise position control and small size bump preparation compared with evaporation, sputtering and electroless. However, cyanide Au-Sn electroplating solution being currently used is highly toxic and does seriously harm to environment and personal safety, hence it is urgent to develop a non-cyanide Au-Sn electroplating solution.
In the present work, the effects of solution ingredients and process parameters of non-cyanide sulfite-pyrophosphate Au-Sn solution system on the morphology and composition of Au-Sn coating were systematically investigated, and then the response surface methodology was used to precisely control the composition of Au-Sn coating. The influence law of solution ingredients on Au-Sn co-electrodeposition behavior was analyzed by electrochemical means. Finally, the properties of the Au-30at.%Sn eutectic coating were evaluated. The Au-30at.%Sn eutectic alloy bumps prepared by co-electrodeposition were compared with those prepared by sequential electroplating. The interfacial reactions between co-electrodeposited Au-30at.%Sn eutectic alloy bumps and copper and nickel substrates were also investigated. The main conclusions are as follows:
1. The weakly alkaline sulfite-pyrophosphate Au-Sn solution system was chosen to co-electrodeposit Au-Sn alloy coating. The morphology and composition of Au-Sn coating were regarded as the evaluation indexes to optimize the solution ingredients and process parameters. The results were as follows:the molar ratio of gold to sodium sulfite and tin to potassium pyrophosphate were1:12-1:24and1:6～1:9, respectively; the concentration of EDTA, catechol, ascorbic acid and nickel chloride were0.01-0.08mol/L,0.01-0.07mol/L,0.09mol/L and0.005mol/L, respectively; the range of the pH value of the solution was restricted between7.5～8.5; the temperature range was35～45℃; the stirring speed was set at200rpm; the pulse frequency was greater than10Hz; the forward on time was not shorter than2ms, the forward off time was not shorter than4ms, the reversal on time was not longer than2ms, and the ratio of forward current to reverse current was larger than4:1when the duty ratio of periodic reversal pulse was100Hz.
2. Response surface methodology was adopted to adjust the Au-Sn co-electrodeposition solution ingredients and process parameters to precisely control the composition of Au-Sn coating. It was shown that the impact of main factors and interactions on the composition of Au-Sn coating fell in order of C>A>E>AB>D>AD>B in the fractional factorial design experiment. Central composite design experiment, containing pi I value, EDTA concentration and catechol concentration, was carried out to built the model correlating the response and the factors. Then the optimum solutions of solution ingredient and process parameter for the predicted values of Au-Sn coating can be determined based on the model. According to the model, the optimum solution for the Au-30at.%Sn eutectic coating was also determined. It was indicated that the Au-30at.%Sn eutectic alloy can be obtained under the optimum condition by repeated experiments. The eutectic alloy composition was accurate, and the experiment had repeatability.
3. The influence law of solution ingredients on Au-Sn co-electrodeposition behavior was analyzed by electrochemical means. After adding complexing agent into the solution, the deposition potential of Au was close to that of Sn, which was benefit for the co-electrodeposition of Au-Sn alloy. After adding EDTA into the solution, the reduction peak potential of Au-Sn moved towards positive direction; after adding catechol into the solution, the reduction peak potential of Au-Sn was shifted negatively; the reduction peak potential of Au-Sn was further shifted to negative direction with the addition of both EDTA and catechol. The additives made the Au-Sn eathodie reduction peaks move towards to positive or negative position, which changed the co-electrodeposition behavior of Au-Sn. The Au content in the coating increased when the eathodie reduction peak moved towards to positive direction, while the Sn content in the coating increased when the eathodie reduction peak moved towards to negative direction. The co-electrodcposition of Au-Sn under the eathodie peak potential was controlled by diffusion step. With cathodic potential towards to negative direction, the co-electrodeposition process was controlled by both diffusion and electrochemical step.
4. The properties of the co-electrodeposiled Au-30at.%Sn eutectic coatings were evaluated, such as roughness, bonding force, melting point, corrosion resistance and so on. The results showed that the roughness of the co-electrodeposited Au-30at.%Sn eutectic alloy coatings was only tens of nanometer, and the bonding force between the Au-30at.%Sn alloy eutectic coating and Si/TiW/Au substrate was good. The melt point was280.66℃. Moreover, the co-electrodeposited Au-30at.%Sn eutectic alloy coatings had good corrosion resistance. It is obvious that the quality of the Au-30at.%Sn eutectic bump prepared by co-electrodeposition was improved compared with that prepared by sequential electroplating. After the co-electrodeposited Au-30at.%Sn coatings reacted with Ni and Cu substrates at310oC, it was shown that (Ni,Au)3Sn2intermetallic compound formed at the interface of Au-30at.%Sn/Ni, while two-layer intermetallic compound, i.e.,(Au,Cu)5Sn close to the matrix of solder and AuCu close to the Cu substrate, formed at the interface of Au-30at.%Sn/Cu. The good bonding between the Au-30at.%Sn eutectic alloy coatings and Ni and Cu substrates indicated that the co-electrodeposited Au-30at.%Sn eutectic coating had good solderability.
本论文系统地研究了无氰亚硫酸盐-焦磷酸盐Au-Sn镀液体系中镀液成分和工艺参数对Au-Sn合金镀层表面形貌和镀层成分的影响；然后通过响应曲面法来精确控制Au-Sn共沉积镀层的成分；利用电化学手段分析了镀液成分对Au-Sn共沉积行为的影响规律；最后评价了Au-30at.%Sn共晶镀层的性能：对比了分层法与共沉积法制备的Au-30at.%Sn共晶合金凸点,并研究了共沉积法制备的Au-30at.%Sn共晶合金凸点与铜、镍基板间的界面反应。主要结论如下：
1、选用弱碱性的亚硫酸盐-焦磷酸盐镀液体系共沉积电镀Au-Sn合金镀层。以镀层的表面形貌和镀层成分作为评价指标优化镀液成分和工艺参数,其结果如下：Au与亚硫酸钠摩尔浓度比为1：12-1：24,Sn与焦磷酸钾摩尔浓度比为1：6-1：9,EDTA0.01-0.08mol/L,邻苯二酚0.01～0.07mol/L,抗坏血酸0.09mol/L,氯化镍0.005mol/L, pH7.5～8.5,温度35-45℃,搅拌速度200rpm,脉冲频率大于10Hz,当周期换向脉冲频率为100Hz时,正向电流导通时间不小于2ms,正向关段时间不小于4ms,负向电流导通时间不大于2ms,正反向工作电流比大于4：1。
2、采用响应曲面法对Au-Sn共沉积镀液成分和工艺参数进行调整来进一步精确控制Au-Sn合金镀层的成分。部分因子试验发现主因素及交互作用对镀层成分影响的大小顺序为C>A>E>AB>D>AD>B。以pH值、EDTA浓度和邻苯二酚浓度为因子进行中心复合试验建立响应与因子关系的模型,通过模型求解得到特定镀层成分对应的最优因子组合。利用该模型获得了对应Au-30at.%Sn共晶合金镀层的最优镀液成分和工艺参数,重复实验表明在此镀液成分和工艺参数下可以获得成分稳定的Au-30at.%Sn共晶成分镀层。共晶合金成分准确,实验具有可重复性。
3、利用电化学手段分析了镀液成分对金锡共沉积行为的影响规律。络合剂的加入使得Au、Sn沉积电位接近,有利于Au和Sn的共沉积。EDTA的加入,使得Au-Sn合金的还原峰电位正向移动；邻苯二酚的加入,使得Au-Sn合金的还原峰电位负向移动；当同时加入EDTA和邻苯二酚时,Au-Sn还原峰进一步负向移动。添加剂的加入使得Au-Sn阴极还原峰正向、负向移动,从而改变了Au-Sn共沉积行为。阴极还原峰正向移动,有利于镀层中Au含量增加,阴极还原峰负向移动,有利于镀层中Sn含量增加。Au-Sn合金的共沉积在还原峰电位下为扩散控制,随着电位的负移,将由扩散和电化学步骤混合控制。
4、对共沉积Au-30at.%Sn共晶合金镀层粗糙度、结合力、熔点和耐蚀性等性能进行评价。实验结果表明共沉积Au-30at.%Sn共晶合金镀层的粗糙度仅为几十纳米,与Si/TiW/Au基体结合力良好,其熔点为280.66℃,此外还具有良好的耐蚀性。共沉积法制备的Au-30at.%Sn共晶合金凸点与分层法制备的共晶合金凸点相比质量明显提高。共沉积的Au-30at.%Sn共晶合金镀层分别与Ni和Cu基板在310℃下钎焊反应,在Au-30at.%Sn/Ni界面处形成了(Ni,Au)3Sn2金属间化合物；在Au-30at.%Sn/Cu界面上形成了两层金属间化合物,靠近钎料的(Au,Cu)5Sn和靠近Cu基板的AuCu。Au-30at.%Sn共晶合金镀层与Ni、Cu基板形成良好连接,表明共沉积的Au-30at.%Sn共晶合金镀层具有良好的可焊性。
The flip-chip technology can improve the luminescence efficiency and thermal dissipation of high-power LEDs. Since the electric and thermal conductivities of flip-chip are carried out by solder bump, the capability of the bump has a direct impact on the chip reliability. Au-30at.%Sn eutectic solder is the idea material for flip-chip bump due to its excellent mechanical properties and high reliability. Electroplating of Au-30at.%Sn eutectic alloy bump has the advantages of low cost, simple process, precise position control and small size bump preparation compared with evaporation, sputtering and electroless. However, cyanide Au-Sn electroplating solution being currently used is highly toxic and does seriously harm to environment and personal safety, hence it is urgent to develop a non-cyanide Au-Sn electroplating solution.
In the present work, the effects of solution ingredients and process parameters of non-cyanide sulfite-pyrophosphate Au-Sn solution system on the morphology and composition of Au-Sn coating were systematically investigated, and then the response surface methodology was used to precisely control the composition of Au-Sn coating. The influence law of solution ingredients on Au-Sn co-electrodeposition behavior was analyzed by electrochemical means. Finally, the properties of the Au-30at.%Sn eutectic coating were evaluated. The Au-30at.%Sn eutectic alloy bumps prepared by co-electrodeposition were compared with those prepared by sequential electroplating. The interfacial reactions between co-electrodeposited Au-30at.%Sn eutectic alloy bumps and copper and nickel substrates were also investigated. The main conclusions are as follows:
1. The weakly alkaline sulfite-pyrophosphate Au-Sn solution system was chosen to co-electrodeposit Au-Sn alloy coating. The morphology and composition of Au-Sn coating were regarded as the evaluation indexes to optimize the solution ingredients and process parameters. The results were as follows:the molar ratio of gold to sodium sulfite and tin to potassium pyrophosphate were1:12-1:24and1:6～1:9, respectively; the concentration of EDTA, catechol, ascorbic acid and nickel chloride were0.01-0.08mol/L,0.01-0.07mol/L,0.09mol/L and0.005mol/L, respectively; the range of the pH value of the solution was restricted between7.5～8.5; the temperature range was35～45℃; the stirring speed was set at200rpm; the pulse frequency was greater than10Hz; the forward on time was not shorter than2ms, the forward off time was not shorter than4ms, the reversal on time was not longer than2ms, and the ratio of forward current to reverse current was larger than4:1when the duty ratio of periodic reversal pulse was100Hz.
2. Response surface methodology was adopted to adjust the Au-Sn co-electrodeposition solution ingredients and process parameters to precisely control the composition of Au-Sn coating. It was shown that the impact of main factors and interactions on the composition of Au-Sn coating fell in order of C>A>E>AB>D>AD>B in the fractional factorial design experiment. Central composite design experiment, containing pi I value, EDTA concentration and catechol concentration, was carried out to built the model correlating the response and the factors. Then the optimum solutions of solution ingredient and process parameter for the predicted values of Au-Sn coating can be determined based on the model. According to the model, the optimum solution for the Au-30at.%Sn eutectic coating was also determined. It was indicated that the Au-30at.%Sn eutectic alloy can be obtained under the optimum condition by repeated experiments. The eutectic alloy composition was accurate, and the experiment had repeatability.
3. The influence law of solution ingredients on Au-Sn co-electrodeposition behavior was analyzed by electrochemical means. After adding complexing agent into the solution, the deposition potential of Au was close to that of Sn, which was benefit for the co-electrodeposition of Au-Sn alloy. After adding EDTA into the solution, the reduction peak potential of Au-Sn moved towards positive direction; after adding catechol into the solution, the reduction peak potential of Au-Sn was shifted negatively; the reduction peak potential of Au-Sn was further shifted to negative direction with the addition of both EDTA and catechol. The additives made the Au-Sn eathodie reduction peaks move towards to positive or negative position, which changed the co-electrodeposition behavior of Au-Sn. The Au content in the coating increased when the eathodie reduction peak moved towards to positive direction, while the Sn content in the coating increased when the eathodie reduction peak moved towards to negative direction. The co-electrodcposition of Au-Sn under the eathodie peak potential was controlled by diffusion step. With cathodic potential towards to negative direction, the co-electrodeposition process was controlled by both diffusion and electrochemical step.
4. The properties of the co-electrodeposiled Au-30at.%Sn eutectic coatings were evaluated, such as roughness, bonding force, melting point, corrosion resistance and so on. The results showed that the roughness of the co-electrodeposited Au-30at.%Sn eutectic alloy coatings was only tens of nanometer, and the bonding force between the Au-30at.%Sn alloy eutectic coating and Si/TiW/Au substrate was good. The melt point was280.66℃. Moreover, the co-electrodeposited Au-30at.%Sn eutectic alloy coatings had good corrosion resistance. It is obvious that the quality of the Au-30at.%Sn eutectic bump prepared by co-electrodeposition was improved compared with that prepared by sequential electroplating. After the co-electrodeposited Au-30at.%Sn coatings reacted with Ni and Cu substrates at310oC, it was shown that (Ni,Au)3Sn2intermetallic compound formed at the interface of Au-30at.%Sn/Ni, while two-layer intermetallic compound, i.e.,(Au,Cu)5Sn close to the matrix of solder and AuCu close to the Cu substrate, formed at the interface of Au-30at.%Sn/Cu. The good bonding between the Au-30at.%Sn eutectic alloy coatings and Ni and Cu substrates indicated that the co-electrodeposited Au-30at.%Sn eutectic coating had good solderability.
引文
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