CN107949447B - 接合用铜糊料、接合体的制造方法及半导体装置的制造方法 - Google Patents

接合用铜糊料、接合体的制造方法及半导体装置的制造方法 Download PDF

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CN107949447B
CN107949447B CN201680051482.0A CN201680051482A CN107949447B CN 107949447 B CN107949447 B CN 107949447B CN 201680051482 A CN201680051482 A CN 201680051482A CN 107949447 B CN107949447 B CN 107949447B
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bonding
copper
particles
copper paste
copper particles
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CN107949447A (zh
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川名祐贵
蔵渊和彦
江尻芳则
中子伟夫
须镰千绘
石川大
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Lishennoco Co ltd
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Hitachi Chemical Co Ltd
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    • B22F7/06—Manufacture of composite layers, workpieces, or articles, comprising metallic powder, by sintering the powder, with or without compacting wherein at least one part is obtained by sintering or compression of composite workpieces or articles from parts, e.g. to form tipped tools
    • B22F7/062—Manufacture of composite layers, workpieces, or articles, comprising metallic powder, by sintering the powder, with or without compacting wherein at least one part is obtained by sintering or compression of composite workpieces or articles from parts, e.g. to form tipped tools involving the connection or repairing of preformed parts
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Abstract

本发明的接合用铜糊料含有金属粒子和分散介质，金属粒子含有体积平均粒径为0.12μm以上且0.8μm以下的亚微米铜粒子和体积平均粒径为2μm以上且50μm以下的微米铜粒子，亚微米铜粒子的含量及微米铜粒子的含量之和以金属粒子的总质量为基准计为80质量％以上，亚微米铜粒子的含量以亚微米铜粒子的质量及微米铜粒子的质量之和为基准计为30质量％以上且90质量％以下。

Description

接合用铜糊料、接合体的制造方法及半导体装置的制造方法
技术领域
本发明涉及接合用铜糊料、使用了该接合用铜糊料的接合体的制造方法及半导体装置的制造方法、以及接合体及半导体装置。
背景技术
制造半导体装置时，为了将半导体元件与引线框等(支撑构件)接合，使用各种各样的接合材料。半导体装置中，在150℃以上的高温下工作的功率半导体、LSI等的接合中，作为接合材料使用高熔点铅钎料。近年来，由于半导体元件的高容量化及省空间化，工作温度上升至高熔点铅钎料的熔点附近，变得难以确保连接可靠性。另一方面，随着RoHS管制强化，需求不含铅的接合材料。
在此之前，探讨了使用铅钎料以外的材料的半导体元件的接合。例如，下述专利文献1中提出了使银纳米粒子低温烧结而形成烧结银层的技术。已知这种烧结银针对动力循环的连接可靠性高(非专利文献1)。
作为其他的材料，还提出了使铜粒子烧结而形成烧结铜层的技术。例如，下述专利文献2中公开了作为用于将半导体元件与电极接合的接合材料的含有氧化铜粒子及还原剂的接合用糊料。另外，下述专利文献3中公开了含有铜纳米粒子、铜微米粒子或铜亚微米粒子或者它们两者的接合材料。
现有技术文献
专利文献
专利文献1：日本专利第4928639号
专利文献2：日本专利第5006081号
专利文献3：日本特开2014-167145号公报
非专利文献
非专利文献1：R.Khazaka，L.Mendizabal，D.Henry：J.ElecTron.Mater，43(7)，2014，2459-2466
发明内容
发明要解决的技术问题
上述专利文献1所记载的方法由于为了获得高连接可靠性、烧结银层的致密化是必须的，因此伴随加压的热压接工艺变得必要。进行伴随加压的热压接工艺时，有生产效率降低、合格率下降等课题。进而，使用银纳米粒子时，由于银所导致的材料成本的显著增加等成为问题。
上述专利文献2所记载的方法通过热压接工艺避免了由氧化铜还原成铜时的体积收缩。但是，在热压接工艺中存在上述课题。
上述专利文献3所记载的方法是在无加压下进行烧结，但在以下方面供至实用仍有不足。即，铜纳米粒子为了抑制氧化及提高分散性，需要利用保护剂对表面进行修饰，但由于铜纳米粒子的比表面积较大，因此在以铜纳米粒子为主成分的接合材料中，有表面保护剂的配合量增加的倾向。另外，为了确保分散性，有分散介质的配合量增加的倾向。因而，上述专利文献3所记载的接合材料为了保管、涂饰等的供给稳定性，有增多表面保护剂或分散介质的比例、烧结时的体积收缩易于增大、而且烧结后的致密度易于降低的倾向，变得难以确保烧结体强度。
本发明的目的在于提供即便是进行无加压下的接合时也可获得充分的接合强度的接合用铜糊料。本发明的另一个目的还在于提供使用接合用铜糊料的接合体的制造方法及半导体装置的制造方法、以及接合体及半导体装置。
用于解决技术问题的手段
本发明提供一种接合用铜糊料，其为含有金属粒子和分散介质的接合用铜糊料，其中，金属粒子含有体积平均粒径为0.12μm以上且0.8μm以下的亚微米铜粒子和体积平均粒径为2μm以上且50μm以下的微米铜粒子，亚微米铜粒子的含量及微米铜粒子的含量之和以金属粒子的总质量为基准计为80质量％以上，亚微米铜粒子的含量以亚微米铜粒子的质量及微米铜粒子的质量之和为基准计为30质量％以上且90质量％以下。
根据本发明的接合用铜糊料，即便是进行无加压下的接合时，也可获得充分的接合强度。对于获得这种效果的理由而言，认为通过以特定比例含有上述亚微米铜粒子和上述微米铜粒子，可以在维持充分的烧结性的同时充分抑制因表面保护剂或分散介质所引起的烧结时的体积收缩，可实现确保烧结体强度及提高与被接合面的接合力。另外，本发明的接合用铜糊料由于可以通过亚微米铜粒子及微米铜粒子获得上述效果，因此与以高价的铜纳米粒子为主成分的接合材料相比，具有可以更为廉价且稳定地供给的优点。由此，例如可以在制造半导体装置等接合体时进一步提高生产稳定性。
上述接合用铜糊料中，微米铜粒子可以是薄片状。使用薄片状的微米铜粒子时，例如可以更容易地提高半导体装置的芯片剪切强度及连接可靠性。此外，作为获得这种效果的理由，认为如下：接合用铜糊料内的微米铜粒子通过相对于接合面大致平行地进行取向，可以抑制对接合用铜糊料进行烧结时的体积收缩；由于薄片状微米铜粒子的重叠面积增大而接合力有所提高；以及薄片状微米铜粒子对亚微米铜粒子进行直线对准，可获得增强效果。
本发明的接合用铜糊料可以是无加压接合用。本说明书中，“无加压”是指进行接合的构件的自重、或者在受到此自重的基础上还受到0.01MPa以下的压力的状态。
本发明还提供一种接合体的制造方法，其具备以下工序：准备层叠有第一构件、以及在该第一构件的自重作用方向一侧上依次为上述接合用铜糊料及第二构件的层叠体，在第一构件的自重、或者在受到第一构件的自重及0.01MPa以下的压力的状态下对接合用铜糊料进行烧结。
根据本发明接合体的制造方法，通过使用上述接合用铜糊料，可以制造通过无加压接合、构件之间以充分的接合力进行了接合的接合体。
本发明还提供一种半导体装置的制造方法，其具备以下工序：准备层叠有第一构件、以及在该第一构件的自重作用方向一侧上依次为上述接合用铜糊料及第二构件的层叠体，在第一构件的自重、或者在受到第一构件的自重及0.01MPa以下的压力的状态下对接合用铜糊料进行烧结，第一构件及第二构件中的至少一个为半导体元件。
根据本发明半导体装置的制造方法，通过使用上述接合用铜糊料，可以制造通过无加压接合、芯片剪切强度优异的半导体装置。另外，通过本发明半导体装置的制造方法所制造的半导体装置的连接可靠性可变得优异。
本发明还提供一种接合体，其具备第一构件、第二构件、以及将第一构件和第二构件接合的上述接合用铜糊料的烧结体。本发明的接合体的第一构件及第二构件通过具有充分接合力的铜的烧结体进行接合。另外，本发明的接合体通过具备导热率优异的铜的烧结体，构件的散热性可变得优异。
上述接合体中，第一构件及第二构件中的至少一个可以在与烧结体相接触的面中含有选自铜、镍、银、金及钯中的至少1种金属。此时，可以进一步提高第一构件及第二构件中的至少一个与烧结体的粘接性。
本发明还提供一种半导体装置，其具备第一构件、第二构件、以及将第一构件和第二构件接合的上述接合用铜糊料的烧结体，第一构件及第二构件中的至少一个为半导体元件。本发明的半导体装置通过具备具有充分的接合力、导热率及熔点高的铜的烧结体，可以成为具有充分的芯片剪切强度、连接可靠性优异、同时动力循环耐受性也优异的半导体装置。
发明效果
根据本发明，可以提供即便是进行无加压的接合时也可获得充分的接合强度的接合用铜糊料。本发明进一步可以提供使用接合用铜糊料的接合体的制造方法及半导体装置的制造方法、以及接合体及半导体装置。
附图说明
图1为表示使用本实施方式的接合用铜糊料所制造的接合体之一例的示意截面图。
图2为表示使用本实施方式的接合用铜糊料所制造的半导体装置之一例的示意截面图。
图3为表示使用本实施方式的接合用铜糊料所制造的半导体装置之一例的示意截面图。
图4为表示使用本实施方式的接合用铜糊料所制造的半导体装置之一例的示意截面图。
图5为表示使用本实施方式的接合用铜糊料所制造的半导体装置之一例的示意截面图。
图6为表示使用本实施方式的接合用铜糊料所制造的半导体装置之一例的示意截面图。
图7为表示使用本实施方式的接合用铜糊料所制造的半导体装置之一例的示意截面图。
图8为表示使用本实施方式的接合用铜糊料所制造的半导体装置之一例的示意截面图。
图9为表示使用本实施方式的接合用铜糊料所制造的半导体装置之一例的示意截面图。
图10表示实施例1的接合体的截面的SEM图像。
图11表示实施例12的接合体的截面的SEM图像。
图12表示实施例13的接合体的截面的SEM图像。
图13表示比较例2的接合体的截面的SEM图像。
具体实施方式
以下对用于实施本发明的方式(以下也称作“本实施方式”)详细地进行说明。本发明并非限定于以下的实施方式。
＜接合用铜糊料＞
本实施方式的接合用铜糊料为含有金属粒子和分散介质的接合用铜糊料，其中金属粒子包含亚微米铜粒子及微米铜粒子。
(金属粒子)
作为本实施方式的金属粒子，可举出亚微米铜粒子、微米铜粒子、除铜粒子以外的其他金属粒子等。
(亚微米铜粒子)
作为亚微米铜粒子，可举出含有粒径为0.12μm以上且0.8μm以下的铜粒子者，例如可以使用体积平均粒径为0.12μm以上且0.8μm以下的铜粒子。亚微米铜粒子的体积平均粒径若为0.12μm以上，则易于获得抑制亚微米铜粒子的合成成本、良好的分散性、抑制表面处理剂的使用量的效果。亚微米铜粒子的体积平均粒径为0.8μm以下时，易于获得亚微米铜粒子的烧结性优异的效果。从进一步发挥上述效果的观点出发，亚微米铜粒子的体积平均粒径可以是0.15μm以上且0.8μm以下、还可以是0.15μm以上且0.6μm以下、还可以是0.2μm以上且0.5μm以下、还可以是0.3μm以上且0.45μm以下。
此外，本申请说明书中，体积平均粒径是指50％体积平均粒径。求算铜粒子的体积平均粒径时，可以通过利用光散射法粒度分布测定装置(例如岛津纳米粒径分布测定装置(SALD-7500nano，株式会社岛津制作所制))对使用分散剂使成为原料的铜粒子、或者从接合用铜糊料中除去了挥发成分的干燥铜粒子分散在分散介质而成的物质进行测定的方法等来求得。使用光散射法粒度分布测定装置时，作为分散介质可以使用己烷、甲苯、α-萜品醇等。
亚微米铜粒子可以含有10质量％以上的粒径为0.12μm以上且0.8μm以下的铜粒子。从接合用铜糊料的烧结性的观点出发，亚微米铜粒子可以含有20质量％以上、可以含有30质量％以上、可以含有100质量％的粒径为0.12μm以上且0.8μm以下的铜粒子。亚微米铜粒子中的粒径为0.12μm以上且0.8μm以下的铜粒子的含有比例为20质量％以上时，铜粒子的分散性进一步提高，可以进一步抑制粘度的上升、糊料浓度的下降。
铜粒子的粒径可以通过下述方法求算。铜粒子的粒径例如可以由SEM图像求出。利用刮铲将铜粒子的粉末放在SEM用的碳带上，制成SEM用样品。利用SEM装置以5000倍对该SEM用样品进行观察。利用图像处理软件对外切于该SEM图像的铜粒子的四边形进行作图，将其一边作为该粒子的粒径。
亚微米铜粒子的含量以金属粒子的总质量为基准计，可以是20质量％以上且90质量％以下，还可以是30质量％以上且90质量％以下，还可以是35质量％以上且85质量％以下，还可以是40质量％以上且80质量％以下。亚微米铜粒子的含量为上述范围内时，易于确保通过烧结接合用铜糊料而制造的接合体的接合强度。将接合用铜糊料用于半导体元件的接合时，亚微米铜粒子的含量若为上述范围内，则半导体装置具有显示良好的芯片剪切强度及连接可靠性的倾向。
亚微米铜粒子的含量以亚微米铜粒子的质量及微米铜粒子的质量之和为基准计，优选为20质量％以上且90质量％以下。亚微米铜粒子的上述含量为20质量％以上时，则可以将微米铜粒子之间充分地填充，易于确保通过烧结接合用铜糊料而制造的接合体的接合强度，将接合用铜糊料用于半导体元件的接合时,半导体装置具有显示良好的芯片剪切强度及连接可靠性的倾向。亚微米铜粒子的含量为90质量％以下时，由于可以充分地抑制烧结接合用铜糊料时的体积收缩，因此易于确保通过烧结接合用铜糊料而制造的接合体的接合强度。将接合用铜糊料用于半导体元件的接合时，亚微米铜粒子的含量为90质量％以下时，半导体装置具有显示良好的芯片剪切强度及连接可靠性的倾向。从进一步发挥上述效果的观点出发，亚微米铜粒子的含量以亚微米铜粒子的质量及微米铜粒子的质量之和为基准计，可以是30质量％以上且85质量％以下、还可以是35质量％以上且85质量％以下、还可以是40质量％以上且80质量％以下。
亚微米铜粒子的形状并无特别限定。作为亚微米铜粒子的形状，例如可举出球状、块状、针状、薄片状、略球状及它们的凝聚体。从分散性及填充性的观点出发，亚微米铜粒子的形状可以是球状、略球状、薄片状，从燃烧性、分散性、与薄片状微米粒子的混合性等观点出发，可以是球状或略球状。本说明书中“薄片状”包含板状、鳞片状等平板状的形状。
亚微米铜粒子从分散性、填充性及与薄片状微米粒子的混合性的观点出发，长宽比可以为5以下、也可以为3以下。本说明书中“长宽比”表示粒子的长边/厚度。粒子的长边及厚度的测定例如可以由粒子的SEM图像求算。
亚微米铜粒子可以用特定的表面处理剂进行处理。作为特定的表面处理剂，例如可举出碳数为8～16的有机酸。作为碳数为8～16的有机酸，例如可举出辛酸、甲基庚酸、乙基己酸、丙基戊酸、壬酸、甲基辛酸、乙基庚酸、丙基己酸、癸酸、甲基壬酸、乙基辛酸、丙基庚酸、丁基己酸、十一烷酸、甲基癸酸、乙基壬酸、丙基辛酸、丁基庚酸、月桂酸、甲基十一烷酸、乙基癸酸、丙基壬酸、丁基辛酸、戊基庚酸、十三烷酸、甲基十二烷酸、乙基十一烷酸、丙基癸酸、丁基壬酸、戊基辛酸、肉豆蔻酸、甲基十三烷酸、乙基十二烷酸、丙基十一烷酸、丁基癸酸、戊基壬酸、己基辛酸、十五烷酸、甲基十四烷酸、乙基十三烷酸、丙基十二烷酸、丁基十一烷酸、戊基癸酸、己基壬酸、棕榈酸、甲基十五烷酸、乙基十四烷酸、丙基十三烷酸、丁基十二烷酸、戊基十一烷酸、己基癸酸、庚基壬酸、甲基环己酸、乙基环己酸、丙基环己酸、丁基环己酸、戊基环己酸、己基环己酸、庚基环己酸、辛基环己酸、壬基环己酸等饱和脂肪酸；辛烯酸、壬烯酸、甲基壬烯酸、癸烯酸、十一碳烯酸、十二碳烯酸、十三碳烯酸、十四碳烯酸、肉豆蔻脑酸、十五碳烯酸、十六碳烯酸、棕榈油酸、6(Z)-十六碳烯酸(sapienic acid)等不饱和脂肪酸；对苯二甲酸、均苯四酸、邻苯氧基苯甲酸、甲基苯甲酸、乙基苯甲酸、丙基苯甲酸、丁基苯甲酸、戊基苯甲酸、己基苯甲酸、庚基苯甲酸、辛基苯甲酸、壬基苯甲酸等芳香族羧酸。有机酸可以单独使用1种，也可以组合使用2种以上。通过将这种有机酸和上述亚微米铜粒子组合，具有能够兼顾亚微米铜粒子的分散性与烧结时的有机酸的离去性的倾向。
表面处理剂的处理量可以是在亚微米铜粒子的表面附着一分子层～三分子层的量。该量可以由附着在亚微米铜粒子表面上的分子层数(n)、亚微米铜粒子的比表面积(Ap)(单位为m2/g)、表面处理剂的分子量(Ms)(单位为g/mol)、表面处理剂的最小被覆面积(SS)(单位为m2/个)、阿伏伽德罗常数(NA)(6.02×1023个)求出。具体地说，表面处理剂的处理量按照表面处理剂的处理量(质量％)＝{(n·Ap·Ms)/(SS·NA+n·Ap·Ms)}×100％的公式求出。
亚微米铜粒子的比表面积可以通过利用BET比表面积测定法测定经干燥的亚微米铜粒子来求出。表面处理剂的最小被覆面积在表面处理剂为直链饱和脂肪酸时，为2.05×10-19m2/1分子。为除此之外的表面处理剂时，例如可以通过由分子模型的求算或《化学と教育(化学和教育)》(上江田捷博、稻福纯夫、森严、40(2)，1992，p114-117)所记载的方法进行测定。示出表面处理剂的定量方法之一例。表面处理剂可以通过从接合用铜糊料除去了分散介质之后的干燥粉的热离去气体-气相色谱质谱分析计进行鉴定，由此可以确定表面处理剂的碳数及分子量。表面处理剂的碳部分比例可以利用碳部分分析进行分析。作为碳部分分析法，例如可举出高频感应加热炉燃烧/红外线吸收法。由经鉴定的表面处理剂的碳数、分子量及碳部分比例，利用上述公式，可以求出表面处理剂量。
表面处理剂的上述处理量可以是0.07质量％以上且2.1质量％以下、还可以是0.10质量％以上且1.6质量％以下、还可以是0.2质量％以上且1.1质量％以下。
上述亚微米铜粒子由于具有良好的烧结性，因此可以减少主要使用铜纳米粒子的接合材料中所见的高价合成成本、并不良好的分散性、烧结后的体积收缩降低等课题。
作为本实施方式的亚微米铜粒子，可以使用市售品。作为市售的亚微米粒子，例如可举出CH-0200(三井金属矿业株式会社制、体积平均粒径为0.36μm)、HT-14(三井金属矿业株式会社制、体积平均粒径为0.41μm)、CT-500(三井金属矿业株式会社制、体积平均粒径为0.72μm)、Tn-Cu100(太阳日酸株式会社制、体积平均粒径为0.12μm)。
(微米铜粒子)
作为微米铜粒子，可举出含有粒径为2μm以上且50μm以下的铜粒子的粒子，例如可以使用体积平均粒径为2μm以上且50μm以下的铜粒子。微米铜粒子的体积平均粒径若为上述范围内，则可以充分地减少烧结接合用铜糊料时的体积收缩，易于确保通过烧结接合用铜糊料而制造的接合体的接合强度。将接合用铜糊料用于半导体元件的接合时，若微米铜粒子的体积平均粒径为上述范围内，则半导体装置具有显示良好的芯片剪切强度及连接可靠性的倾向。从进一步发挥上述效果的观点出发，微米铜粒子的体积平均粒径可以是3μm以上且20μm以下、还可以是3μm以上且10μm以下。
微米铜粒子可以含有50质量％的粒径为2μm以上且50μm以下的铜粒子。从接合体内的取向、增强效果、接合糊料的填充性的观点出发，微米铜粒子可以含有70质量％以上、可以含有80质量％以上、可以含有100质量％的粒径为2μm以上且50μm以下的铜粒子。从抑制接合故障的观点出发，微米铜粒子例如优选不含最大径超过20μm的粒子等超过接合厚度的尺寸的粒子。
微米铜粒子的含量以金属粒子的总质量为基准计，可以是10质量％以上且90质量％以下、还可以是15质量％以上且65质量％以下、还可以是20质量％以上且60质量％以下。微米铜粒子的含量为上述范围内时，易于确保通过烧结接合用铜糊料而制造的接合体的接合强度。将接合用铜糊料用于半导体元件的接合时，若微米铜粒子的含量为上述范围内，则半导体装置具有显示良好的芯片剪切强度及连接可靠性的倾向。
亚微米铜粒子的含量及微米铜粒子的含量之和以金属粒子的总质量为基准计，可以是80质量％以上。亚微米铜粒子的含量及微米铜粒子的含量之和若为上述范围内，则可以充分地减少烧结接合用铜糊料时的体积收缩，易于确保通过烧结接合用铜糊料而制造的接合体的接合强度。将接合用铜糊料用于半导体元件的接合时，半导体装置具有显示良好的芯片剪切强度及连接可靠性的倾向。从进一步发挥上述效果的观点出发，亚微米铜粒子的含量及微米铜粒子的含量之和以金属粒子的总质量为基准计，可以是90质量％以上、还可以是95质量％以上、还可以是100质量％。
微米铜粒子的形状并无特别限定。作为微米铜粒子的形状，例如可举出球状、块状、针状、薄片状、略球状及它们的凝聚体。微米铜粒子的形状中优选薄片状。通过使用薄片状的微米铜粒子，接合用铜糊料内的微米铜粒子通过相对于接合面大致平行地进行取向，可以抑制烧结接合用铜糊料时的体积收缩、易于确保通过烧结接合用铜糊料而制造的接合体的接合强度。将接合用铜糊料用于半导体元件的接合时，半导体装置具有显示良好的芯片剪切强度及连接可靠性的倾向。从进一步发挥上述效果的观点出发，作为薄片状的微米铜粒子，其中长宽比可以为4以上、也可以为6以上。
对于微米铜粒子，有无表面处理剂的处理并无特别限定。从分散稳定性及耐氧化性的观点出发，微米铜粒子可以经表面处理剂处理。表面处理剂可以在接合时被除去。作为这种表面处理剂，例如可举出棕榈酸、硬脂酸、花生酸、油酸等脂肪族羧酸；对苯二甲酸、均苯四酸、邻苯氧基苯甲酸等芳香族羧酸；鲸蜡醇、硬脂醇、异冰片基环己醇、四乙二醇等脂肪族醇；对苯基苯酚等芳香族醇；辛基胺、十二烷基胺、硬脂胺等烷基胺；硬脂腈、癸腈等脂肪族腈；烷基烷氧基硅烷等硅烷偶联剂；聚乙二醇、聚乙烯醇、聚乙烯基吡咯烷酮、有机硅低聚物等高分子处理剂等。表面处理剂可以单独使用1种，也可组合使用2种以上。
表面处理剂的处理量可以是粒子表面上一分子层以上的量。这种表面处理剂的处理量随微米铜粒子的比表面积、表面处理剂的分子量及表面处理剂的最小被覆面积而变化。表面处理剂的处理量通常为0.001质量％以上。对于微米铜粒子的比表面积、表面处理剂的分子量及表面处理剂的最小被覆面积而言，可以利用上述方法求出。
仅由上述亚微米铜粒子制备接合用铜糊料时，由于伴随分散介质的干燥的体积收缩及烧结收缩较大，因而接合用铜糊料在烧结时易于自被接合面剥离，在半导体元件等的接合中难以获得充分的芯片剪切强度及连接可靠性。通过并用亚微米铜粒子和微米铜粒子，可以抑制烧结接合用铜糊料时的体积收缩，接合体可以具有充分的接合强度。将接合用铜糊料用于半导体元件的接合时，可获得半导体装置显示良好的芯片剪切强度及连接可靠性的效果。
作为本实施方式的微米铜粒子，可以使用市售品。作为市售的微米粒子，例如可举出MA-C025(三井金属矿业株式会社制、体积平均粒径为7.5μm)、3L3(福田金属箔粉工业株式会社制、体积平均粒径为8.0μm)、1110F(三井金属矿业株式会社制、体积平均粒径为3.8μm)、Cu-HWQ3.0μm(福田金属箔粉工业株式会社制、体积平均粒径为3.0μm)。
(除铜粒子以外的其他金属粒子)
作为金属粒子，可以含有除亚微米铜粒子及微米铜粒子以外的其他金属粒子，例如可以含有镍、银、金、钯、铂等粒子。其他的金属粒子可以是体积平均粒径为0.01μm以上且10μm以下、也可以是0.01μm以上且5μm以下、也可以是0.05μm以上且3μm以下。含有其他金属粒子时，其含量从获得充分接合性的观点出发，以金属粒子的总质量为基准计，可以小于20质量％、还可以是10质量％以下。也可以不含其他的金属粒子。其他金属粒子的形状并无特别限定。
通过含有除铜粒子以外的金属粒子，由于可以获得多种金属经固溶或分散而成的烧结体，因而可改善烧结体的屈服应力、疲劳强度等机械特性，连接可靠性易于提高。另外，通过添加多种金属粒子，接合用铜糊料的烧结体相对于特定被接合体可以具有充分的接合强度。将接合用铜糊料用于半导体元件的接合时，半导体装置的芯片剪切强度及连接可靠性易于提高。
(分散介质)
分散介质并无特别限定，可以是挥发性的分散介质。作为挥发性的分散介质，例如可举出戊醇、己醇、庚醇、辛醇、癸醇、乙二醇、二乙二醇、丙二醇、丁二醇、α-萜品醇、异冰片基环己醇(MTPH)等一元及多元醇类；乙二醇丁基醚、乙二醇苯基醚、二乙二醇甲基醚、二乙二醇乙基醚、二乙二醇丁基醚、二乙二醇异丁基醚、二乙二醇己基醚、三乙二醇甲基醚、二乙二醇二甲基醚、二乙二醇二乙基醚、二乙二醇二丁基醚、二乙二醇丁基甲基醚、二乙二醇异丙基甲基醚、三乙二醇二甲基醚、三乙二醇丁基甲基醚、丙二醇丙基醚、二丙二醇甲基醚、二丙二醇乙基醚、二丙二醇丙基醚、二丙二醇丁基醚、二丙二醇二甲基醚、三丙二醇甲基醚、三丙二醇二甲基醚等醚类；乙二醇乙基醚乙酸酯、乙二醇丁基醚乙酸酯、二乙二醇乙基醚乙酸酯、二乙二醇丁基醚乙酸酯、二丙二醇甲基醚乙酸酯(DPMA)、乳酸乙酯、乳酸丁酯、γ-丁内酯、碳酸亚丙酯等酯类；N-甲基-2-吡咯烷酮、N,N-二甲基乙酰胺、N,N-二甲基甲酰胺等酸酰胺；环己酮、辛烷、壬烷、癸烷、十一烷等脂肪族烃；苯、甲苯、二甲苯等芳香族烃；具有碳数为1～18的烷基的硫醇类；具有碳数为5～7的环烷基的硫醇类。作为具有碳数为1～18的烷基的硫醇类，例如可举出乙基硫醇、正丙基硫醇、异丙基硫醇、正丁基硫醇、异丁基硫醇、叔丁基硫醇、戊基硫醇、己基硫醇及十二烷基硫醇。作为具有碳数为5～7的环烷基的硫醇类，例如可举出环戊基硫醇、环己基硫醇及环庚基硫醇。
分散介质的含量以金属粒子的总质量为100质量份计，可以为5～50质量份。分散介质的含量若为上述范围内，则可以将接合用铜糊料调整至更为适当的粘度，而且不易阻碍铜粒子的烧结。
(添加剂)
接合用铜糊料中还可根据需要适当添加非离子系表面活性剂、氟系表面活性剂等润湿性提高剂；有机硅油等消泡剂；无机离子交换体等离子捕获剂等。
作为本实施方式的接合用铜糊料的一个方式，可以举出下述接合用铜糊料：上述金属粒子含有体积平均粒径为0.12μm以上且0.8μm以下、优选为0.15μm以上且0.8μm以下的亚微米铜粒子及体积平均粒径为2μm以上且50μm以下的微米铜粒子，亚微米铜粒子的含量及微米铜粒子的含量之和以金属粒子的总质量为基准计为80质量％以上，亚微米铜粒子的含量以亚微米铜粒子的质量及微米铜粒子的质量之和作为基准计为30质量％以上且90质量％以下。
作为上述接合用铜糊料，可举出下述接合用铜糊料：配合有体积平均粒径为0.12μm以上且0.8μm以下、优选为0.15μm以上且0.8μm以下的亚微米铜粒子；体积平均粒径为2μm以上且50μm以下的微米铜粒子；分散介质；以及根据需要的其他上述成分，亚微米铜粒子的配合量及微米铜粒子的配合量之和以金属粒子的总质量为基准计为80质量％以上，亚微米铜粒子的配合量以亚微米铜粒子的配合量及微米铜粒子的配合量之和为基准计为30质量％以上且90质量％以下。
另外，作为本实施方式的接合用铜糊料的另一方式，可举出下述接合用铜糊料：作为亚微米铜粒子，以金属粒子的总质量为基准计，含有24～80质量％的粒径为0.12μm以上且0.8μm以下、优选为0.15μm以上且0.8μm以下的铜粒子，作为微米铜粒子，以金属粒子的总质量为基准计，含有8～70质量％的粒径为2μm以上且50μm以下的微米铜粒子，亚微米铜粒子的含量以亚微米铜粒子的质量及微米铜粒子的质量之和为基准计为30质量％以上且90质量％以下。这里的粒径是指最大粒径，通过利用扫描型电子显微镜(SEM)对成为原料的铜粒子或从接合用铜糊料中除去了挥发成分的干燥铜粒子进行观察的方法来进行求算。
铜粒子并非球状时，其粒径可以是通过下述方法求得的最大粒径。对由SEM图像求出铜粒子的最大粒径的方法进行示例。利用刮铲将铜粒子的粉末放置在SEM用的碳带上，制成SEM用样品。利用SEM装置以5000倍对该SEM用样品进行观察。利用图像处理软件对外切于该SEM图像的铜粒子的长方形进行作图，将长方形的长边作为该粒子的长径。将该长径作为最大粒径。
(接合用铜糊料的制备)
接合用铜糊料可以将上述亚微米铜粒子、微米铜粒子、其他金属粒子及任意的添加剂混合在分散介质中进行制备。在各成分的混合之后，还可以进行搅拌处理。接合用铜糊料还可以利用分级操作调整分散液的最大粒径。此时，分散液的最大粒径可以为20μm以下、还可以为10μm以下。
接合用铜糊料还可以是预先将亚微米铜粒子、表面处理剂、分散介质混合，进行分散处理制备亚微米铜粒子的分散液，进而混合微米铜粒子、其他金属粒子及任意的添加剂来进行制备。通过采取这种顺序，亚微米铜粒子的分散性提高、与微米铜粒子的混合性变好、接合用铜糊料的性能进一步提高。还可以利用分级操作对亚微米铜粒子的分散液除去凝聚物。
搅拌处理可以使用搅拌机进行。作为搅拌机，例如可举出自转公转型搅拌装置、Raikai机、双螺杆混炼机、三辊磨机、行星式搅拌机、薄层剪切分散机。
分级操作例如可以使用过滤、自然沉降、离心分离进行。作为过滤用的过滤器，例如可举出金属筛、金属过滤器、尼龙筛。
作为分散处理，例如可举出薄层剪切分散机、珠磨机、超声波匀浆机、高剪切搅拌器、窄间隙三辊轧机、湿式超微粒化装置、超音速式喷磨机、超高压匀浆机。
接合用铜糊料在进行成型时，可以调整至适于各种印刷、涂布手法的粘度。作为接合用铜糊料的粘度，例如25℃下的Casson粘度可以为0.05Pa·s以上且2.0Pa·s以下、还可以为0.06Pa·s以上且1.0Pa·s以下。
根据本实施方式的接合用铜糊料，通过以固定比例并用上述亚微米铜粒子及微米铜粒子，可以获得良好的烧结性，进而可以抑制烧结时的体积收缩。因此，本实施方式的接合用铜糊料可以在不进行过度加压的情况下确保与构件的接合力，通过烧结接合用铜糊料而制造的接合体可以具有充分的接合强度。将接合用铜糊料用于半导体元件的接合时，半导体装置显示良好的芯片剪切强度及连接可靠性。即，本实施方式的接合用铜糊料可以作为无加压接合用的接合材料进行使用。另外，根据本实施方式的接合用铜糊料，通过使用较为廉价的铜粒子，可以抑制制造成本、可以大量生产。特别是，本实施方式的接合用铜糊料由于可以通过亚微米铜粒子及微米铜粒子获得上述效果，因此与以高价的铜纳米粒子为主成分的接合材料相比，具有能够更为廉价且稳定地供给的优点。由此，例如在制造半导体装置等接合体时，可以进一步提高生产稳定性。
＜接合体及半导体装置＞
以下一边参照附图一边详细地说明优选的实施方式。此外，附图中，相同或相当部分带有相同符号，重复的说明省略。另外，附图的尺寸比例并非限定于图示的比例。
图1是表示使用本实施方式的接合用铜糊料所制造的接合体之一例的示意截面图。本实施方式的接合体100具备第一构件2、第二构件3、以及将第一构件和第二构件接合的上述接合用铜糊料的烧结体1。
作为第一构件2及第二构件3，例如可举出IGBT、二极管、肖特基势垒二极管、MOS-FET、晶闸管、逻辑电路、传感器、模拟集成电路、LED、半导体激光器、信号发送器等半导体元件、引线框、贴有金属板的陶瓷基板(例如DBC)、LED封装等半导体元件搭载用基材、铜带及金属框等金属布线、金属块等块体、端子等给电用构件、放热板、水冷板等。
第一构件2及第二构件3可以在与接合用铜糊料的烧结体相接触的面4a及4b中含有金属。作为金属，例如可举出铜、镍、银、金、钯、铂、铅、锡、钴等。金属可以单独使用1种，也可组合使用2种以上。另外，与烧结体相接触的面可以是含上述金属的合金。作为合金中使用的金属，除了上述金属之外，还可举出锌、锰、铝、铍、钛、铬、铁、钼等。作为在与烧结体相接触的面中含有金属的构件，例如可举出具有各种金属镀覆的构件、电线、具有金属镀覆的芯片、散热片、贴有金属板的陶瓷基板、具有各种金属镀覆的引线框或由各种金属形成的引线框、铜板、铜箔。另外，当第二构件3为半导体元件时，第一构件2还可以是金属框等金属布线、金属块等具有导热性及导电性的块体等。
接合体的芯片剪切强度从将第一构件及第二构件充分地接合的观点出发，可以是10MPa以上、还可以是15MPa以上、还可以是20MPa以上、还可以是30MPa以上。芯片剪切强度可以使用万能型黏结强度试验机(4000系列、DAGE公司制)等进行测定。
接合用铜糊料的烧结体的导热率从散热性及高温化下的连接可靠性的观点出发，可以是100W/(m·K)以上、还可以是120W/(m·K)以上、还可以是150W/(m·K)以上。导热率可以由接合用铜糊料的烧结体的热扩散率、比热容量及密度求出。
以下，对使用了本实施方式的接合用铜糊料的接合体的制造方法进行说明。
使用了本实施方式的接合用铜糊料的接合体的制造方法具备以下工序：准备层叠有第一构件、在该第一构件的自重作用方向一侧上依次为上述接合用铜糊料及第二构件的层叠体，在第一构件的自重或者在受到第一构件的自重及0.01MPa以下的压力的状态下对接合用铜糊料进行烧结。第一构件的自重作用方向还可以称作重力作用方向。
上述层叠体例如可以通过在第二构件的必要部分上设置本实施方式的接合用铜糊料，接着在接合用铜糊料上配置第一构件来准备。
作为将本实施方式的接合用铜糊料设置在第二构件的必要部分上的方法，使接合用铜糊料堆积的方法即可。作为这种方法，例如可以使用丝网印刷、转印印刷、胶版印刷、喷墨印刷法、分配器、喷射式分配器、针形分配器、逗号涂布机、狭缝式涂布机、模涂机、凹版涂布机、狭缝式涂布、凸版印刷、凹版印刷、照相凹版印刷、钢网印刷、软刻、棒涂、涂抹器、粒子堆积法、喷涂机、旋涂机、浸涂机、电沉积涂装等。接合用铜糊料的厚度可以是1μm以上且1000μm以下、还可以是10μm以上且500μm以下、还可以是50μm以上且200μm以下、还可以是10μm以上且3000μm以下、还可以是15μm以上且500μm以下、还可以是20μm以上且300μm以下、还可以是5μm以上且500μm以下、还可以是10μm以上且250μm以下、还可以是15μm以上且150μm以下。
设置于第二构件上的接合用铜糊料从抑制烧结时的流动及孔隙的发生的观点出发，还可以适当地干燥。干燥时的环境气体可以是大气中，也可以是氮气、稀有气体等无氧环境气体中，还可以是氢、甲酸等还原环境气体中。干燥方法可以是利用常温放置进行的干燥，也可以是加热干燥，也可以是减压干燥。加热干燥或减压干燥例如可以使用加热板、温风干燥机、温风加热炉、氮干燥机、红外线干燥机、红外线加热炉、远红外线加热炉、微波加热装置、激光加热装置、电磁加热装置、加热器加热装置、蒸汽加热炉、热板压制装置等。干燥的温度及时间可以根据所使用的分散介质的种类及量适当地调整。作为干燥的温度及时间，例如可以是在50℃以上且180℃以下、干燥1分钟以上且120分钟以下。
作为在接合用铜糊料上配置第一构件的方法，例如可举出贴片机、倒装片接合机、碳制或陶瓷制的定位夹具。
通过对层叠体进行加热处理，进行接合用铜糊料的烧结。加热处理例如可以使用加热板、温风干燥机、温风加热炉、氮干燥机、红外线干燥机、红外线加热炉、远红外线加热炉、微波加热装置、激光加热装置、电磁加热装置、加热器加热装置、蒸汽加热炉等。
烧结时的环境气体从烧结体、第一构件及第二构件的氧化抑制的观点出发，可以是无氧环境气体。烧结时的环境气体从将接合用铜糊料的铜粒子的表面氧化物除去的观点出发，还可以是还原环境气体。作为无氧环境气体，例如可举出氮气、稀有气体等无氧气体的导入或真空下。作为还原环境气体，例如可举出纯氢气中、代表组成气体的氢及氮的混合气体中、含甲酸气体的氮气中、氢及稀有气体的混合气体中、含甲酸气体的稀有气体中等。
加热处理时的到达最高温度从降低对第一构件及第二构件的热损害及提高合格率的观点出发，可以是250℃以上且450℃以下、还可以是250℃以上且400℃以下、还可以是250℃以上且350℃以下。到达最高温度为200℃以上时，到达最高温度保持时间为60分钟以下时，有烧结充分地进行的倾向。
到达最高温度保持时间从使分散介质全部挥发、而且提高合格率的观点出发，可以是1分钟以上且60分钟以下，还可以是1分钟以上且小于40分钟，还可以是1分钟以上且小于30分钟。
通过使用本实施方式的接合用铜糊料，在对层叠体进行烧结时，即便进行无加压下的接合时接合体也具有充分的接合强度。即，在仅由层叠于接合用铜糊料的第一构件所产生的自重、或者在除了受到第一构件的自重以外还受到0.01MPa以下、优选0.005MPa以下的压力的状态下，即可获得充分的接合强度。烧结时受到的压力为上述范围内时，由于不需要特别的加压接置，因此可以在不损害合格率的情况下减少孔隙、进一步提高芯片剪切强度及连接可靠性。作为接合用铜糊料受到0.01MPa以下的压力的方法，例如可举出在第一构件上放置重物的方法等。
上述接合体中，第一构件及第二构件中的至少一个可以是半导体元件。作为半导体元件，例如可举出二极管、整流器、晶闸管、MOS门驱动器、电源开关、功率MOSFET、IGBT、肖特基二极管、快恢复二极管等形成的功率模块、信号发送器、放大器、LED模块等。此时，上述接合体成为半导体装置。所得半导体装置可以具有充分的芯片剪切强度及连接可靠性。
图2是表示使用本实施方式的接合用铜糊料所制造的半导体装置之一例的示意截面图。图2所示的半导体装置110由介由本实施方式的接合用铜糊料的烧结体1连接在引线框5a上的半导体元件8和对它们进行注塑的注塑树脂7形成。半导体元件8介由电线6连接在引线框5b上。
作为使用本实施方式的接合用铜糊料所制造的半导体装置，例如可举出二极管、整流器、晶闸管、MOS门驱动器、电源开关、功率MOSFET、IGBT、肖特基二极管、快恢复二极管等形成的功率模块、信号发送器、放大器、高亮度LED模块、传感器等。
上述半导体装置可以与上述接合体的制造方法同样地制造。即，半导体装置的制造方法具备以下工序：第一构件及第二构件中的至少一个使用半导体元件，准备层叠有第一构件、在该第一构件的自重作用方向一侧上依次为上述接合用铜糊料及第二构件的层叠体，在第一构件的自重、或在受到第一构件的自重及0.01MPa以下的压力的状态下对接合用铜糊料进行烧结。例如，可以举出在引线框5a上设置接合用铜糊料、配置半导体元件8进行加热的工序。所得半导体装置即便是进行无加压下的接合时，也可具有充分的芯片剪切强度及连接可靠性。本实施方式的半导体装置通过具备具有充分的接合力、导热率及熔点高的铜的烧结体，在具有充分的芯片剪切强度、连接可靠性优异的同时，动力循环耐受性也可变得优异。
上述方法在第二构件为半导体元件时，可以减少将作为第一构件的金属布线或块体等接合在半导体元件上时的对半导体元件造成的损伤。以下说明在半导体元件上接合有金属布线或块体等构件的半导体装置。
作为这种半导体装置的一个实施方式，可举出下述半导体装置：具备第一电极、电连接于第一电极的半导体元件、以及介由金属布线与半导体元件电连接的第二电极，在半导体元件与金属布线之间及金属布线与第二电极之间具有上述接合用铜糊料的烧结体。
图3为表示上述半导体装置之一例的示意截面图。图3所示的半导体装置200具备：具有第一电极22及第二电极24的绝缘基板21、通过上述接合用铜糊料的烧结体1接合于第一电极22上的半导体元件23、以及将半导体元件23与第二电极24电连接的金属布线25。金属布线25与半导体元件23、及金属布线25与第二电极24分别通过接合用铜糊料的烧结体1而接合。另外，半导体元件23介由电线27连接于第三电极26。半导体装置200在绝缘基板21的与搭载有上述电极等的面成相反侧上具备铜板28。半导体装置200的上述结构体用绝缘体29密封。半导体装置200在第一电极22上具有1个半导体元件23，但也可以具有2个以上。此时，具有多个的半导体元件23可以分别通过接合用铜糊料的烧结体1与金属布线25相接合。
图4为表示半导体装置另一例的示意截面图。图4所示的半导体装置210在半导体元件23与金属布线25之间设有块体30，半导体元件23与块体30、及块体30与金属布线25分别通过接合用铜糊料的烧结体1相接合，除此之外具有与图3所示半导体装置200相同的构成。此外，块体30的位置可以适当变更，例如也可以设置在第一电极22与半导体元件23之间。
图5为表示半导体装置另一例的示意截面图。图5所示的半导体装置220在第一电极22上进一步设置有半导体元件23及块体30以及将它们接合的接合用铜糊料的烧结体1，除此之外具有与图4所示半导体装置210相同的构成。半导体装置220在第一电极22上具有2个半导体元件，也可以具有3个以上。此时，具有3个以上的半导体元件23也可以分别介由块体30、通过接合用铜糊料的烧结体1与金属布线25相接合。此外，块体30的位置可以适当变更，例如也可以设置在第一电极22与半导体元件23之间。
作为绝缘基板21，例如可举出氧化铝、氮化铝、氮化硅等陶瓷、高导热粒子/树脂复合物、聚酰亚胺树脂、聚马来酰亚胺树脂等。
作为构成第一电极22、第二电极24及第三电极26的金属，例如可举出铜、镍、银、金、钯、铂、铅、锡、钴等。这些金属可以单独使用1种，也可组合使用2种以上。另外，电极还可在与接合用铜糊料与烧结体1相接触的面中具有含有上述金属的合金。作为合金中使用的金属，除了上述金属之外，还可举出锌、锰、铝、铍、钛、铬、铁、钼等。
作为金属布线，可举出具有带状、板状、立方体状、圆筒状、L字状、コ字状、へ字状等形状的金属框等。作为金属布线的材质，例如可举出银、铜、铁、铝、钼、钨、钽、铌、或它们的合金。另外，金属布线可以是宽度为1μm～30μm、厚度为20μm～5mm。
作为块体，优选导热性及导电性优异者，例如可以使用银、铜、铁、铝、钼、钨、钽、铌、或它们的合金。通过在半导体元件上设置块体，散热性进一步提高。块体的数量可以适当变更。
作为绝缘体29，例如可举出硅胶、聚马来酰亚胺树脂、聚酰亚胺树脂、聚酰胺酰亚胺树脂等。
图3～5所示的半导体装置可以用于大容量、要求高可靠性的功率模块。
图3～5所示的半导体装置例如可通过具备以下工序的方法进行制造：准备具备第一电极及第二电极的绝缘基板，在第一电极上从第一电极侧开始按顺序设置接合用铜糊料、半导体元件、根据需要的接合用铜糊料、块体、接合用铜糊料，在第二电极上设置接合用铜糊料，在半导体元件或块体上的接合用铜糊料及第二电极上的接合用铜糊料上按照将这些接合用铜糊料交联的方式配置金属布线的工序；和在各构件的自重或者在受到各构件的自重及0.01MPa以下的压力的状态下对接合用铜糊料进行烧结的工序。
根据这种制造方法，可以在无加压下制造半导体装置，因此可以在不使具有电桥部的金属布线变形的情况下进行接合，而且即便是在半导体元件上接合面积小于半导体元件的构件时，也可以进一步减轻对半导体元件的损害。
图6为表示半导体装置又一例的示意截面图。图6所示的半导体装置300具备第一电极22、通过接合用铜糊料的烧结体1接合在第一电极22上的半导体元件23、以及将半导体元件23与第二电极24电连接的金属布线25。金属布线25与半导体元件23、及金属布线25与第二电极24分别通过接合用铜糊料的烧结体1相接合。另外，半导体元件23介由电线27连接于第三电极26。半导体装置300的上述结构体用密封材料31密封。半导体装置300在第一电极22上具有1个半导体元件23，也可以具有2个以上。此时，具有多个的半导体元件23可以分别通过接合用铜糊料的烧结体1与金属布线25相接合。
图7为表示半导体装置又一例的示意截面图。图7所示的半导体装置310在半导体元件23与金属布线25之间设有块体30，半导体元件23与块体30、及块体30与金属布线25分别通过接合用铜糊料的烧结体1相接合，除此之外具有与图6所示半导体装置300相同的构成。此外，块体30的位置可以适当变更，例如也可以设置在第一电极22与半导体元件23之间。
图8为表示半导体装置又一例的示意截面图。图8所示的半导体装置320在第一电极22上进一步设有半导体元件23及块体30以及将它们接合的接合用铜糊料的烧结体1，除此之外具有与图7所示半导体装置310相同的构成。半导体装置320在第一电极22上具有2个半导体元件，也可具有3个以上。此时，有3个以上的半导体元件23可以分别介由块体30、通过接合用铜糊料的烧结体1与金属布线25相接合。此外，块体30的位置可以适当变更，例如也可以设置在第一电极22与半导体元件23之间。
图6～8所示的第一电极22及第二电极24还可以是引线框、铜板、铜/钼烧结体等。
作为密封材料31，例如可举出耐热性固形密封材料、高导热复合物等。
接合用铜糊料的烧结体1可以与半导体装置200～220中说明过的相同。
图6～8所示实施方式的半导体装置通过作为第一电极及第二电极采用引线框等，从而可以用于经小型化的功率模块。这种半导体装置可以与上述半导体装置的制造方法同样地进行制造。
进而，对具有在半导体元件上接合有块体的结构的半导体装置的其他实施方式进行说明。
作为上述半导体装置，可举出下述半导体装置：具备第一导热构件、第二导热构件、以及配置在第一导热构件及第二导热构件之间的半导体元件，在第一导热构件与半导体元件之间、及半导体元件与第二导热构件之间的至少1个之间具有上述接合用铜糊料的烧结体。
图9为表示本实施方式之一例的示意截面图。图9所示的半导体装置400具备第一导热构件32、通过接合用铜糊料的烧结体1接合在第一导热构件32上的半导体元件23、通过接合用铜糊料的烧结体1接合在半导体元件23上的块体30、以及通过接合用铜糊料的烧结体1接合在块体30上的第二导热构件33。半导体元件23介由电线35连接在电极34上。半导体装置400的第一导热构件32与第二导热构件之间用密封材料31密封。半导体装置400具有2个半导体元件，也可具有1个或3个以上，块体的数量也可适当地变更。此外，块体30的位置可以适当变更，例如也可以设置在第一电极22与半导体元件23之间。
导热构件兼具将自半导体元件23产生的热量释放到外部的功能、及作为用于将半导体元件电连接于外部的电极的功能。这种导热构件例如使用铜、铝、或它们的合金。
图9所示的半导体装置通过在半导体元件的两个面侧具备导热构件，可以具有散热性优异的两面冷却结构。这种半导体装置可以通过具备以下工序的方法进行制造：准备在第一导热构件上从第一导热构件侧开始按顺序层叠有接合用铜糊料、半导体元件、接合用铜糊料、块体、接合用铜糊料、第二导热构件的层叠体，在各构件的自重或者在受到各构件的自重及0.01MPa以下的压力的状态下对接合用铜糊料进行烧结。此外，上述层叠体还可以是按照与上述相反的顺序进行层叠而成的。
实施例
以下通过实施例更为具体地说明本发明。但本发明并非限定于以下的实施例。
(制备例1)
利用玛瑙研钵对作为分散介质的α-萜品醇(和光纯药工业株式会社制)0.35g及异冰片基环己醇(MTPH、日本Terpene化学株式会社制)0.85g、作为亚微米铜粒子的CH-0200(表面处理剂：月桂酸、三井金属矿业株式会社制)3.52g、作为微米铜粒子的MA-C025(三井金属矿业株式会社制)5.28g进行混炼，至干燥粉消失，将混合液移至塑料瓶。使用自转公转型搅拌装置(Planetary Vacuum Mixer ARV-310、株式会社Shinkey制)以2000min-1(2000转/分钟)对盖严了的塑料瓶搅拌2分钟。之后，利用超声波匀浆机(US-600、日本精机株式会社制)对混合液进行19.6kHz、600W、1分钟的处理。接着，利用自转公转型搅拌装置(Planetary Vacuum Mixer ARV-310、株式会社Shinkey制)以2000min-1(2000转/分钟)对盖严了的塑料瓶搅拌2分钟。将该混合液作为接合用铜糊料1。
(制备例2)
利用玛瑙研钵对作为分散介质的α-萜品醇(和光纯药工业株式会社制)0.44g及异冰片基环己醇(MTPH、日本Terpene化学株式会社制)0.76g、作为亚微米铜粒子的CH-0200(表面处理剂：月桂酸、三井金属矿业株式会社制)4.40g、作为微米铜粒子的MA-C025(三井金属矿业株式会社制)4.40g进行混炼，至干燥粉消失，将混合液移至塑料瓶。进行除了使用该混合液之外、与制备例1相同的方法，制备接合用铜糊料2。
(制备例3)
利用玛瑙研钵对作为分散介质的α-萜品醇(和光纯药工业株式会社制)0.52g及异冰片基环己醇(MTPH、日本Terpene化学株式会社制)0.68g、作为亚微米铜粒子的CH-0200(表面处理剂：月桂酸、三井金属矿业株式会社制)5.28g、作为微米铜粒子的MA-C025(三井金属矿业株式会社制)3.52g进行混炼，至干燥粉消失，将混合液移至塑料瓶。进行除了使用该混合液之外、与制备例1相同的方法，制备接合用铜糊料3。
(制备例4)
利用玛瑙研钵对作为分散介质的α-萜品醇(和光纯药工业株式会社制)0.61g及异冰片基环己醇(MTPH、日本Terpene化学株式会社制)0.59g、作为亚微米铜粒子的CH-0200(表面处理剂：月桂酸、三井金属矿业株式会社制)6.16g、作为微米铜粒子的MA-C025(三井金属矿业株式会社制)2.64g进行混炼，至干燥粉消失，将混合液移至塑料瓶。进行除了使用该混合液之外、与制备例1相同的方法，制备接合用铜糊料4。
(制备例5)
利用玛瑙研钵对作为分散介质的α-萜品醇(和光纯药工业株式会社制)0.78g及异冰片基环己醇(MTPH、日本Terpene化学株式会社制)0.42g、作为亚微米铜粒子的CH-0200(表面处理剂：月桂酸、三井金属矿业株式会社制)7.91g、作为微米铜粒子的MA-C025(三井金属矿业株式会社制)0.88g进行混炼，至干燥粉消失，将混合液移至塑料瓶。进行除了使用该混合液之外、与制备例1相同的方法，制备接合用铜糊料5。
(制备例6)
利用玛瑙研钵对作为分散介质的α-萜品醇(和光纯药工业株式会社制)0.90g、作为亚微米铜粒子的CH-0200(表面处理剂：月桂酸、三井金属矿业株式会社制)6.40g、作为微米铜粒子的3L3(福田金属箔粉工业株式会社制)2.75g进行混炼，至干燥粉消失，将混合液移至塑料瓶。进行除了使用该混合液之外、与制备例1相同的方法，制备接合用铜糊料6。
(制备例7)
利用玛瑙研钵对作为分散介质的α-萜品醇(和光纯药工业株式会社制)0.90g、作为亚微米铜粒子的CH-0200(表面处理剂：月桂酸、三井金属矿业株式会社制)4.58g、作为微米铜粒子的1110F(三井金属矿业株式会社制)4.58g进行混炼，至干燥粉消失，将混合液移至塑料瓶。进行除了使用该混合液之外、与制备例1相同的方法，制备接合用铜糊料7。
(制备例8)
利用玛瑙研钵对作为分散介质的α-萜品醇(和光纯药工业株式会社制)0.61g及异冰片基环己醇(MTPH、日本Terpene化学株式会社制)0.59g、作为亚微米铜粒子的CH-0200(表面处理剂：月桂酸、三井金属矿业株式会社制)6.16g、作为微米铜粒子的Cu-HWQ3.0μm(福田金属箔粉工业株式会社制)2.64g进行混炼，至干燥粉消失，将混合液移至塑料瓶。进行除了使用该混合液之外、与制备例1相同的方法，制备接合用铜糊料8。
(制备例9)
将作为分散介质的α-萜品醇6.1g及异冰片基环己醇(MTPH、日本Terpene化学株式会社制)0.59g、作为亚微米铜粒子的HT-14(不含表面处理剂，三井金属矿业株式会社制)6.16g、作为表面处理剂的月桂酸(和光纯药工业株式会社制)0.58g混合，利用自动研钵混合10分钟，制备混合液。之后，利用超声波匀浆机(US-600、日本精机株式会社制)对混合液进行19.6kHz、600W、2分钟的处理，将所得糊料状组合物通入尼龙筛(筛布(ボルティングクロス)355T、AS ONE株式会社制)中，获得HT-14糊料状组合物。利用玛瑙研钵对HT-14糊料状组合物7.36g、作为微米铜粒子的MA-C025(三井金属矿业株式会社制)2.64g进行混炼，至干燥粉消失，将混合液移至塑料瓶。进行除了使用该混合液之外、与制备例1相同的方法，制备接合用铜糊料9。
(制备例10)
利用玛瑙研钵对作为分散介质的α-萜品醇(和光纯药工业株式会社制)0.94g及异冰片基环己醇(MTPH、日本Terpene化学株式会社制)0.26g、作为亚微米铜粒子的CH-0200(表面处理剂：月桂酸、三井金属矿业株式会社制)2.64g、作为微米铜粒子的MA-C025(三井金属矿业株式会社制)6.16g进行混炼，至干燥粉消失，将混合液移至塑料瓶。进行除了使用该混合液之外、与制备例1相同的方法，制备接合用铜糊料10。
(制备例11)
利用玛瑙研钵对作为分散介质的α-萜品醇(和光纯药工业株式会社制)0.78g及异冰片基环己醇(MTPH、日本Terpene化学株式会社制)0.42g、作为亚微米铜粒子的CH-0200(表面处理剂：月桂酸、三井金属矿业株式会社制)7.92g、作为微米铜粒子的MA-C025(三井金属矿业株式会社制)0.88g进行混炼，至干燥粉消失，将混合液移至塑料瓶。进行除了使用该混合液之外、与制备例1相同的方法，制备接合用铜糊料11。
(制备例12)
利用玛瑙研钵对作为分散介质的α-萜品醇(和光纯药工业株式会社制)1.20g、作为亚微米铜粒子的CT-500(表面处理剂：不明、三井金属矿业株式会社制)7.00g、作为微米铜粒子的MA-C025(三井金属矿业株式会社制)3.00g进行混炼，至干燥粉消失，将混合液移至塑料瓶。进行除了使用该混合液之外、与制备例1相同的方法，制备接合用铜糊料12。
(制备例13)
利用玛瑙研钵对作为分散介质的α-萜品醇(和光纯药工业株式会社制)1.20g、作为微米铜粒子的MA-C025(三井金属矿业株式会社制)8.80g进行混炼，至干燥粉消失，将混合液移至塑料瓶。进行除了使用该混合液之外、与制备例1相同的方法，制备接合用铜糊料13。
(制备例14)
利用玛瑙研钵对作为分散介质的α-萜品醇(和光纯药工业株式会社制)0.22g及异冰片基环己醇(MTPH、日本Terpene化学株式会社制)1.12g、作为亚微米铜粒子的CH-0200(表面处理剂：月桂酸、三井金属矿业株式会社制)0.88g、作为微米铜粒子的MA-C025(三井金属矿业株式会社制)7.92g进行混炼，至干燥粉消失，将混合液移至塑料瓶。进行除了使用该混合液之外、与制备例1相同的方法，制备接合用铜糊料14。
(制备例15)
利用玛瑙研钵对作为分散介质的α-萜品醇(和光纯药工业株式会社制)1.20g、作为亚微米铜粒子的CH-0200(表面处理剂：月桂酸、三井金属矿业株式会社制)8.80g进行混炼，至干燥粉消失，将混合液移至塑料瓶。进行除了使用该混合液之外、与制备例1相同的方法，制备接合用铜糊料15。
(制备例16)
利用玛瑙研钵对作为分散介质的α-萜品醇(和光纯药工业株式会社制)1.50g、作为铜粒子的CS-10(表面处理剂：不明、三井金属矿业株式会社制、50％体积平均粒径：1.1μm、粒径为0.12～0.8μm的粒子的比例(质量％)：18％)5.95g、作为微米铜粒子的MA-C025(三井金属矿业株式会社制)2.55g进行混炼，至干燥粉消失，将混合液移至塑料瓶。进行除了使用该混合液之外、与制备例1相同的方法，制备接合用铜糊料16。
(制备例17)
利用玛瑙研钵对作为分散介质的α-萜品醇(和光纯药工业株式会社制)1.06g、作为铜粒子的Cu-HWQ1.5μm(表面处理剂：无、福田金属箔粉工业株式会社制、50％体积平均粒径：1.7μm、粒径为0.12～0.8μm的粒子的比例(质量％)：11％)6.37g、作为微米铜粒子的MA-C025(三井金属矿业株式会社制)2.73g进行混炼，至干燥粉消失，将混合液移至塑料瓶。进行除了使用该混合液之外、与制备例1相同的方法，制备接合用铜糊料17。
(制备例18)
利用玛瑙研钵对作为分散介质的α-萜品醇(和光纯药工业株式会社制)0.67g及异冰片基环己醇(MTPH、日本Terpene化学株式会社制)0.60g、作为微米铜粒子的Cu-HWQ3.0μm(表面处理剂：无、福田金属箔粉工业株式会社制、50％体积平均粒径：3μm、粒径为0.12～0.8μm的粒子的比例(质量％)：0.3％)6.17g和MA-C025(三井金属矿业株式会社制)2.64g进行混炼，至干燥粉消失，将混合液移至塑料瓶。进行除了使用该混合液之外、与制备例1相同的方法，制备接合用铜糊料18。
＜接合体的制造＞
(实施例1～11、16)
使用接合用铜糊料1～12，按照以下的方法制造接合体。接合体的芯片剪切强度利用后述的方法进行测定。
在19mm×25mm的铜板(厚度：3mm)上放置具有3行3列的3mm×3mm正方形开口的不锈钢制金属掩模(厚度：100μm)，利用使用了金属刮刀的钢网印刷涂布接合用铜糊料。在经涂布的接合用铜糊料上放置2mm×2mm的被接合面经镀镍的铜块(厚度：250μm)，利用小镊子轻轻按压。将其安装在管式炉(株式会社AVC制)中，以3L/min流入氩气，将空气置换成氩气。之后，以300ml/min流入氢气，同时升温10分钟。升温后，在最高到达温度为350℃、最高到达温度保持时间为10分钟的条件下进行烧结处理，获得接合有铜板和经镀镍的铜块的接合体。烧结后，将氩气换为0.3L/min进行冷却，在50℃以下将接合体取出至空气中。
(实施例12)
使用接合用铜糊料4，按照以下的方法制造接合体。接合体的芯片剪切强度利用后述的方法进行测定。
在19mm×25mm的铜板(厚度：3mm)上放置具有3行3列的3mm×3mm正方形开口的不锈钢制金属掩模(厚度：100μm)，利用使用了金属刮刀的钢网印刷涂布接合用铜糊料。在经涂布的接合用铜糊料上放置2mm×2mm的被接合面经镀金的铜块(厚度：250μm)，利用小镊子轻轻按压。将其安装在管式炉(株式会社AVC制)中，以3L/min流入氩气，将空气置换成氩气。之后，以300ml/min流入氢气，同时升温10分钟。升温后，在最高到达温度为350℃、最高到达温度保持时间为10分钟的条件下进行烧结处理，获得接合有铜板和经镀金的铜块的接合体。烧结后，将氩气换为0.3L/min进行冷却，在50℃以下将接合体取出至空气中。
(实施例13)
使用接合用铜糊料4，按照以下的方法制造接合体。接合体的芯片剪切强度利用后述的方法进行测定。
在19mm×25mm的铜板(厚度：3mm)上放置具有3行3列的3mm×3mm正方形开口的不锈钢制金属掩模(厚度：100μm)，利用使用了金属刮刀的钢网印刷涂布接合用铜糊料。在经涂布的接合用铜糊料上放置2mm×2mm的被接合面经镀镍的铜块(厚度：250μm)，利用小镊子轻轻按压。在其上按照重叠于9张2mm×2mm的被接合面经镀镍的铜块(厚度：250μm)的方式、静置15mm×15mm的SUS块(重量：15g)，将其安装在管式炉(株式会社AVC制)中，以3L/min流入氩气，将空气置换成氩气。之后，以300ml/min流入氢气，同时升温10分钟。升温后，在最高到达温度为350℃、最高到达温度保持时间为10分钟的条件下进行烧结处理，获得接合有铜板和经镀镍的铜块的接合体。烧结后，将氩气换为0.3L/min进行冷却，在50℃以下将接合体取出至空气中。
(实施例14)
使用接合用铜糊料4，按照以下的方法制造接合体。接合体的芯片剪切强度利用后述的方法进行测定。
在19mm×25mm的铜板(厚度：3mm)上放置具有3行3列的3mm×3mm正方形开口的不锈钢制金属掩模(厚度：100μm)，利用使用了金属刮刀的钢网印刷涂布接合用铜糊料。在经涂布的接合用铜糊料上放置2mm×2mm的被接合面经镀镍的铜块(厚度：250μm)，将其安装在管式炉(株式会社AVC制)中，以3L/min流入氩气，将空气置换成氩气。之后，以300ml/min流入氢气，同时升温10分钟。升温后，在最高到达温度为250℃、最高到达温度保持时间为60分钟的条件下进行烧结处理，获得接合有铜板和经镀镍的铜块的接合体。烧结后，将氩气换为0.3L/min进行冷却，在50℃以下将接合体取出至空气中。
(实施例15)
使用接合用铜糊料4，按照以下的方法制造接合体。接合体的芯片剪切强度利用后述的方法进行测定。
在19mm×25mm的铜板(厚度：3mm)上放置具有3行3列的3mm×3mm正方形开口的不锈钢制金属掩模(厚度：100μm)，利用使用了金属刮刀的钢网印刷涂布接合用铜糊料。在经涂布的接合用铜糊料上放置2mm×2mm的被接合面经镀镍的铜块(厚度：250μm)，将其安装在管式炉(株式会社AVC制)中，以3L/min流入氩气，将空气置换成氩气。之后，以300ml/min流入氢气，同时升温20分钟。升温后，在最高到达温度为450℃、最高到达温度保持时间为10分钟的条件下进行烧结处理，获得接合有铜板和经镀镍的铜块的接合体。烧结后，将氩气换为0.3L/min进行冷却，在50℃以下将接合体取出至空气中。
(比较例1～6)
除了使用接合用铜糊料13～18之外，利用与实施例1相同的方法制造接合体。接合体的芯片剪切强度利用后述的方法进行测定。
＜测定方法＞
(芯片剪切强度)
接合体的接合强度利用芯片剪切强度进行评价。使用安装有DS-100测力传感器的万能型黏结强度试验机(4000系列、DAGE公司制)，以测定速度为5mm/min、测定高度为50μm将铜块在水平方向上按压，测定接合体的芯片剪切强度。将测定了8个接合体的值的平均值作为芯片剪切强度。
(50％体积平均粒径)
使用岛津纳米粒径分布测定装置(SALD-7500nano、株式会社岛津制作所制)和附带的软件(WingSALDII-7500-for Japanese V3.、株式会社岛津制作所制)，按照以下的(1)～(5)测定50％体积平均粒径。
(1)软件的设定
利用测定装置附带的计算机启动WingSALDII-7500-for Japanese V3.1，按下手控，进行装置的初始化。初始化结束后，指定保存文件名，点击“下一步”，如下设定测定条件及粒径分布计算条件，点击“下一步”。
(测定条件)
·衍射/散射光的检测
平均次数(测定次数：1)：128、测定次数：1、测定间隔(秒)：2
·测定吸光范围
最大值：0.2、最小值：0
·空白区域/测定区域
空白测定允许变动最大值：150、测定最佳范围(MAX)：45000、测定最佳范围(MIN)：15000
(粒径分布计算条件)
折射率的选择：参照试样/纯金属/半导体等(固体值)
样品的物质：4Copper(铜)
折射率的选择：1.18-2.21、核选“对侧方/后方传感器进行评价”
(2)空白测定
将岛津纳米粒径分布测定装置SALD-7500nano用分批池(SALD-BC75、株式会社岛津制作所制)安装在SALD-7500nano中进行测定。在SALD-BC75附带的带漏斗的分批池(构件编号为S347-61030-41、株式会社岛津制作所制、以下称作“分批池”)内用玻璃吸管滴加α-萜品醇(和光纯药工业株式会社制)，使得达到分批池的2个标线之间。自WingSALDII-7500-for Japanese V3.的画面上选择“诊断”、“调整”，确认位置传感器功率在装置允许范围内。点击“取消”回到原来的画面，选择空白测定进行测定。
(3)测定溶液的制备
在SALD-BC75附带的分批池支架(构件编号为S347-62301、株式会社岛津制作所制)的搅拌杆上放置欲进行测定的接合用铜糊料2mg，安装在带漏斗的分批池中。接着，从WingSALDII-7500-for Japanese V3.的画面上选择“搅拌”，进行15分钟的搅拌。
(4)测定
搅拌后，从WingSALDII-7500-for Japanese V3.的画面上选择“测定”，进行测定。反复(1)～(4)的操作4次，进行4次测定。
(5)统计
启动WingSALDII-7500-for Japanese V3.，点击“打开”，选择测定后的文件，在WingSALDII-7500-for Japanese V3.的画面上显示测定数据。点击“叠写”，在画面下段显示50.000％径，将4次的平均值作为50％体积平均粒径。
在表1～3中示出实施例及比较例的结果。
Figure GDA0001768813750000301
表2
Figure GDA0001768813750000311
表3
Figure GDA0001768813750000321
对实施例及比较例进行比较可知，亚微米铜粒子及微米铜粒子的质量比例对芯片剪切强度造成影响。认为其原因在于，当微米铜粒子过于增加时，则烧结铜层的填充率降低、烧结体易于产生大量空隙、芯片剪切强度降低。另一方面认为，当亚微米铜粒子过于增加时，因体积收缩在烧结体中易于产生大量空隙、芯片剪切强度降低。另外，由实施例的结果可知，若亚微米铜粒子与微米铜粒子的质量比例适当，则接合用铜糊料的烧结体牢固地接合于金、镍、铜中的任一者，显示良好的芯片剪切强度。另外，实施例13中，在对接合用铜糊料施加铜块自重的基础上还施加了0.0042MPa的压力的条件下制造接合体的结果是，接合时空隙被压坏、空隙减少、更为牢固地接合，因而芯片剪切强度增加。实施例15中，通过到达最高温度为450℃，与实施例4相比，接合用铜糊料的烧结进一步进行，因而芯片剪切强度变得更为良好。比较例4～6中，由于亚微米铜粒子的体积平均粒径过大，接合用铜糊料的烧结性降低，因此接合体的芯片剪切强度降低。
(截面形态学观察)
利用样品夹具(Samplklip I、Buehler公司制)将接合体固定在杯子内，向周围流入环氧注塑树脂(エポマウント、Refinetec株式会社制)至样品整体被包埋，在真空干燥器内进行静置，减压1分钟进行脱泡。之后，在室温(25℃)下放置10小时，将环氧注塑树脂固化。使用带有金刚石剪切轮(11-304、Refinetec株式会社制)的リファインソー·Lo(RCA-005、Refinetec株式会社制)，在注塑后的接合体的欲观察的截面附近进行剪切。利用带耐水研磨纸(Carbon Mac Paper、Refinetec株式会社制)的研磨装置(Refine Polisher Hv、Refinetec株式会社制)对截面进行刮削，使没有裂纹的截面露出至硅芯片，进而对多余的注塑树脂进行刮削，精加工成可置于CP(截面抛光机)加工机的尺寸。利用CP加工机(IM4000、株式会社日立High-Technologies制)在加速电压为6kV、氩气流量为0.07～0.1cm3/min、处理时间为2小时的条件下对经切削加工的样品进行截面抛光，进行截面加工。使用溅射装置((ION SPUTTER、株式会社日立High-Technologies制)对截面以10nm的厚度溅射铂，制成SEM观察用的样品。利用SEM装置(ESEM XL30、Philips公司制)以施加电压10kV对该SEM用样品的接合体的截面进行观察。
图10表示实施例1的接合体的截面的SEM图像。图11表示实施例12的接合体的截面的SEM图像。图12表示实施例13的截面的SEM图像。图13表示比较例2的接合体的截面的SEM图像。由图10～12可知，接合用铜糊料的烧结体可以通过微米铜粒子的烧结体10及亚微米铜粒子的烧结体11与铜板9、经镀金的铜块12及经镀镍的铜块13相接合。另外，由图10～12显示，当亚微米铜粒子与微米铜粒子的质量比例适当时，微米铜粒子相对于被接合面大致平行地取向，亚微米铜粒子将其间隙填埋。另一方面，由图13显示，当亚微米铜粒子相对于微米铜粒子过少时，无法充分地将微米铜粒子间的间隙填埋。认为由于这种结构的差异，比较例2的接合体未能获得充分的芯片剪切强度。
符号说明
1接合用铜糊料的烧结体、2第一构件、3第二构件、5a、5b引线框、6电线、7注塑树脂、8半导体元件、9铜板、10微米铜粒子的烧结体、11亚微米铜粒子的烧结体、12经镀金的铜块、13经镀镍的铜块、100接合体、110半导体装置、21绝缘基板、22第一电极、23半导体元件、24第二电极、25金属布线、26第三电极、27电线、28铜板、29绝缘体、30块体、31密封材料、32第一导热构件、33第二导热构件、34电极、35电线、200半导体装置、210半导体装置、220半导体装置、300半导体装置、310半导体装置、320半导体装置、400半导体装置。

Claims (8)

1.一种接合用铜糊料，其为含有金属粒子和分散介质的接合用铜糊料，其中，
所述金属粒子含有体积平均粒径为0.12μm以上且0.8μm以下的亚微米铜粒子和体积平均粒径为2μm以上且50μm以下的微米铜粒子，
所述亚微米铜粒子的含量及所述微米铜粒子的含量之和以所述金属粒子的总质量为基准计为80质量％以上，
所述亚微米铜粒子的含量以所述亚微米铜粒子的质量及所述微米铜粒子的质量之和为基准计为30质量％以上且90质量％以下。
2.根据权利要求1所述的接合用铜糊料，其中，所述微米铜粒子为薄片状。
3.根据权利要求1或2所述的接合用铜糊料，其为无加压接合用。
4.一种接合体的制造方法，其具备以下工序：
准备层叠有第一构件、以及在该第一构件的自重作用方向一侧上依次为权利要求1～3中任一项所述的接合用铜糊料及第二构件的层叠体，在所述第一构件的自重、或者在受到所述第一构件的自重及0.01MPa以下的压力的状态下对所述接合用铜糊料进行烧结。
5.一种半导体装置的制造方法，其具备以下工序：
准备层叠有第一构件、以及在该第一构件的自重作用方向一侧上依次为权利要求1～3中任一项所述的接合用铜糊料及第二构件的层叠体，在所述第一构件的自重、或者在受到所述第一构件的自重及0.01MPa以下的压力的状态下对所述接合用铜糊料进行烧结，
所述第一构件及所述第二构件中的至少一个为半导体元件。
6.一种接合体，其具备第一构件、第二构件、以及将所述第一构件与所述第二构件接合的权利要求1～3中任一项所述的接合用铜糊料的烧结体。
7.根据权利要求6所述的接合体，其中，所述第一构件及第二构件中的至少一个在与所述烧结体相接触的面中含有选自铜、镍、银、金及钯中的至少1种金属。
8.一种半导体装置，其具备第一构件、第二构件、以及将所述第一构件与所述第二构件接合的权利要求1～3中任一项所述的接合用铜糊料的烧结体，
所述第一构件及所述第二构件中的至少一个为半导体元件。
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