第三代半导体互连材料与低温烧结纳米铜材的研究进展

doi:10.15541/jim20230345

无机材料学报 ›› 2024, Vol. 39 ›› Issue (1): 17-31.DOI: 10.15541/jim20230345

第三代半导体互连材料与低温烧结纳米铜材的研究进展

柯鑫¹^,²(), 谢炳卿¹^,², 王忠¹^,³(), 张敬国¹^,³^,⁴, 王建伟¹^,³, 李占荣¹^,³^,⁴, 贺会军¹^,³, 汪礼敏¹^,³

1.中国有研科技集团有限公司金属粉体材料产业技术研究院, 北京 101407
2.北京有色金属研究总院, 北京 100088
3.有研粉末新材料股份有限公司, 北京 101407
4.重庆有研重冶新材料有限公司, 重庆 401431

收稿日期:2023-08-01 修回日期:2023-10-12 出版日期:2024-01-20 网络出版日期:2023-11-22
通讯作者: 王忠, 教授级高工. E-mail: wzwz99@126.com
作者简介:柯鑫(1997-), 男, 博士研究生. E-mail: kexin0308@qq.com
基金资助:
科技部国家重点研发计划(2018YFE0204600);重庆市技术创新与应用发展专项重点项目(CSTB2022TIAD-KPX0027)

Progress of Interconnect Materials in the Third-generation Semiconductor and Their Low-temperature Sintering of Copper Nanoparticles

KE Xin¹^,²(), XIE Bingqing¹^,², WANG Zhong¹^,³(), ZHANG Jingguo¹^,³^,⁴, WANG Jianwei¹^,³, LI Zhanrong¹^,³^,⁴, HE Huijun¹^,³, WANG Limin¹^,³

1. Metal Powder Materials Industrial Technology Research Institute of CHINA GRINM, Beijing 101407, China
2. General Research Institute for Nonferrous Metals, Beijing 100088, China
3. GRIPM Advanced Materials Co. Ltd., Beijing 101407, China
4. Gricy Advanced Materials Co., Ltd., Chongqing 401431, China

Received:2023-08-01 Revised:2023-10-12 Published:2024-01-20 Online:2023-11-22
Contact: WANG Zhong, professor. E-mail: wzwz99@126.com
About author:KE Xin (1997-), male, PhD candidate. E-mail: kexin0308@qq.com
Supported by:
National Key R&D Program of the Ministry of Science and Technology(2018YFE0204600);Special Key Project for Technological Innovation and Application Development in Chongqing(CSTB2022TIAD-KPX0027)

摘要/Abstract

摘要：

半导体材料是现代科技发展和产业革新的核心, 随着高频、高压、高温、高功率等工况的日趋严峻及“双碳”目标的需要, 以新型碳化硅(SiC)和氮化镓(GaN)等为代表的第三代半导体材料逐步进入工业应用。半导体产业的贯通以及市场规模的快速扩大, 导致摩尔定律正逐渐达到极限, 先进封装互连将成为半导体行业关注的焦点。第三代半导体封装互连材料有高温焊料、瞬态液相键合材料、导电胶、低温烧结纳米Ag/Cu等几个发展方向, 其中纳米Cu因其优异的导电导热性、低温烧结特性和良好的可加工性成为一种封装互连的新型方案, 具有低成本、高可靠性和可扩展性, 近年来从材料研究向产业链终端应用贯通的趋势非常明显。本文首先介绍了半导体材料的发展概况并总结了第三代半导体封装互连材料类别; 然后结合近期研究成果进一步围绕纳米Cu低温烧结在封装互连等电子领域中的应用进行重点阐述, 主要包括纳米铜粉的粒度、形貌、表面处理和烧结工艺对纳米铜烧结体导电性能和剪切性能的影响; 最后总结了目前纳米铜在应用转化中面临的困境和亟待解决的难点, 并展望了未来的发展方向, 以期为低温烧结纳米铜领域的研究提供参考。

关键词: 半导体, 封装互连, 低温烧结, 纳米铜, 综述

Abstract:

Semiconductor materials are the core of modern technology development and industrial innovation, with high frequency, high pressure, high temperature, high power, and other high properties under severe conditions or super properties needed by the “double carbon” goal, the new silicon carbide (SiC) and gallium nitride (GaN) as representative of the third generation of semiconductor materials gradually into industrial applications. For the third-generation semiconductor, there are several development directions in its packaging interconnection materials, including high-temperature solder, transient liquid phase bonding materials, conductive adhesives, and low-temperature sintered nano-Ag/Cu, of which nano-Cu, due to its excellent thermal conductivity, low-temperature sintering characteristics, and good processability, has become a new scheme for packaging interconnection, with low cost, high reliability, and scalability. Recently, the trend from material research to industrial chain end-use is pronounced. This review firstly introduces the development overview of semiconductor materials and summarizes the categories of third-generation semiconductor packaging interconnect materials. Then, combined with recent research results, it further focuses on the application of nano-Cu low-temperature sintering in electronic fields such as packaging and interconnection, mainly including the impact of particle size and morphology, surface treatment, and sintering process on the impact of nano-Cu sintered body conductivity and shear properties. Finally, it summarizes the current dilemmas and the difficulties, looking forward to the future development. This review provides a reference for the research on low-temperature sintered copper nanoparticles in the field of interconnect materials for the third-generation semiconductor.

Key words: semiconductor, packaging interconnections, low-temperature sintering, nano-Cu, review

中图分类号:

TM23

柯鑫, 谢炳卿, 王忠, 张敬国, 王建伟, 李占荣, 贺会军, 汪礼敏. 第三代半导体互连材料与低温烧结纳米铜材的研究进展[J]. 无机材料学报, 2024, 39(1): 17-31.

KE Xin, XIE Bingqing, WANG Zhong, ZHANG Jingguo, WANG Jianwei, LI Zhanrong, HE Huijun, WANG Limin. Progress of Interconnect Materials in the Third-generation Semiconductor and Their Low-temperature Sintering of Copper Nanoparticles[J]. Journal of Inorganic Materials, 2024, 39(1): 17-31.

图/表 18

图1 2014-2020年全球GDP总额和半导体市场规模[7]

Fig. 1 Global GDP and semiconductor market size in 2014-2020[7]

表1 主要半导体材料性能参数对比[10]

Table 1 Comparison on performance parameters of the main semiconductor material [10]

Parameter	Si	GaAs	SiC	GaN	Diamond
Band gap/eV	1.12	1.43	3.26	3.45	5.45
Dielectric constant	11.9	13.1	10.1	9	5.5
Breakdown field/ (kV·cm^-1)	300	400	2200	2000	10000
Electron mobility/(cm²·V^-1·s^-1)	1500	8500	1000	1250	2200
Hole mobility/ (cm²·V^-1·s^-1）	600	400	115	850	850
Thermal conductivity/ (W·cm^-1·K^-1)	1.5	0.46	4.9	1.3	22
Electron saturation drift velocity/(×10⁷, cm·s^-1)	1	1	2	2.2	2.7

图2 第三代半导体应用领域

Fig. 2 Third-generation semiconductor applications

图3 典型功率半导体模块封装互连结构[14]

Fig. 3 Package interconnection structure of typical power semiconductor module[14]

图4 不同封装互连材料的使用温度范围和应用可能性[22]

Fig. 4 Applied temperature range and application possibilities of different package interconnect materials[22]

图5 TLP键合时的虚拟平衡相图[32]

Fig. 5 Virtual equilibrium phase diagram for TLP bonding[32]

图6 TLP键合原理示意图[33]

Fig. 6 Schematic diagram of TLP bonding principle[33]

表2 各种TLP键合材料及其性能[60]

Table 2 Various TLP bonding materials and their properties[60]

Material	Temperature/℃		Relative market price*	Relative performance
Material	Bonding	IMC	Relative market price*	Thermal conductivity	Electrical conductivity
Cu-Sn	280	415(Cu₆Sn₅)	Cu: 0.5	Cu: 4.4	Cu: 4.1
Cu-Sn	280	676(Cu₃Sn)	Sn: 0.8	Cu: 4.4	Cu: 4.1
Ni-Sn	300	800(Ni₃Sn₃)	Ni: 1	Ni: 1	Ni: 1
Ni-Sn	300	800(Ni₃Sn₃)	Sn: 0.8	Ni: 1	Ni: 1
Au-Sn	250	419(AuSn)	Au: 2600	Au: 3.5	Au: 3.1
Au-Sn	250	419(AuSn)	Sn: 0.8	Au: 3.5	Au: 3.1
Ag-Sn	250	480(Ag₃Sn)	Ag: 63	Ag: 4.7	Ag: 4.4
Ag-Sn	250	480(Ag₃Sn)	Sn: 0.8	Ag: 4.7	Ag: 4.4
Ag-In	200	495	Ag: 63	Ag: 4.7	Ag: 4.7
Ag-In	200	495	In: 37.5	Ag: 4.7	Ag: 4.7
Au-In	175	880	Au: 2600	Au: 3.1	Au: 3.1
Au-In	175	880	In: 37.5	Au: 3.1	Au: 3.1

图7 Cu@Ag纳米颗粒及性能表征[85]

Fig. 7 Cu@Ag nanoparticles and performance characterization[85] (a, b) STEM images of Cu@Ag nanoparticles; (c) Schematic diagram of the filling effect of nanoparticles on silver conductive adhesive; (d) Influence of the conductive fillers’ percentages on the strength of the conductive adhesives; (e) Dependence of conductive fillers’ percentages on the strength and conductivity of conductive adhesive with 60%Cu@Ag/40% Ag plates

图8 不同粒径混合的微纳米铜颗粒结构[90]

Fig. 8 Structures of micro-nano copper particles mixed with different particle sizes[90] (a) TEM image showing micron particles; (b) TEM image showing nanoparticles

图9 双峰铜浆在不同气氛下的烧结示意图[93]

Fig. 9 Schematic diagram of sintering of bimodal copper slurry under different atmospheres[93]

图10 铜纳米颗粒表层氧化对烧结性能的影响示意图[94]

Fig. 10 Schematic diagram of oxidation effect of surface layer of copper nanoparticles on the sintering performance[94] (a) With CuO outer layer; (b) No CuO outer layer

图11 抗坏血酸(AA)在铜浆中的促进作用机理[96]

Fig. 11 Mechanism of promotion in copper slurry by ascorbic acid (AA)[96]

图12 Cu NP膏体还原和烧结机理示意图[98]

Fig. 12 Schematic diagram of reduction and sintering mechanism of Cu NP paste[98]

图13 在不同温度下烧结试样的截面SEM照片[102]

Fig. 13 SEM images of cross sections of sintered specimens at different temperatures[102] (a, b) 200 ℃; (c, d) 225 ℃; (e, f) 250 ℃; (g, h) 275 ℃

图14 结合层在不同烧结温度下的电阻率[103]

Fig. 14 Resistivities of the bonding layer at different sintering temperatures[103]

图15 Cu-Cu连接接头的制备过程示意图[104]

Fig. 15 Schematic diagram of the preparation process of Cu-Cu connection joints[104]

表3 各种低温烧结工艺及性能对比

Table 3 Comparison of various low-temperature sintering processes and their performance

Particle size	Appearance	Sintering process	Electrical conductivity/ (μΩ·cm)	Shearing performance/ MPa	Ref.
10 and 1000 nm particle compound	Irregular	Ar, 250 ℃, 2 MPa, 15 min	5.44	45.6	[90]
200 nm, 1000 nm	Spherical	N₂, 350 ℃, 0.4 MPa	-	40	[91]
530 nm	Irregular	97% N₂-3% H₂, 300 ℃, 30 min	-	23	[92]
60-100 nm	Angular	N₂, 200 ℃, 60 min	18	-	[93]
Thick 200 nm, length 3-5 μm	Spherical	N₂, 275 ℃, 10 MPa, 30 min	-	50	[95]
30-400 nm	Angular	N₂, 300 ℃, 0.4 MPa, 30 min	-	24.8	[96]
6.5 nm	Spherical	Ar, 250 ℃, 5 MPa, 30 min	-	36.2	[97]
100 nm	Spherical	Air, 225 ℃, 8 MPa, 10 min	59±7	28.7±1.6	[98]
500 nm	Angular	HCOOH, 275 ℃, 5 MPa, 30 min	-	70	[102]
60.5 nm	Spherical	95% Ar-5% H₂, 300 ℃, 1.08 MPa, 60 min	11.2	31.88	[103]
30 nm	Spherical	95% N₂-5% H₂, 320 ℃, 10 MPa, 5 min	3.16	51.7	[104]
54-64 nm	Sphere-like	H₂, 400 ℃, 1.2 MPa, 5 min	-	37.7	[106]
5 nm	Sphere-like	95% Ar-5% H₂, 250 ℃, 1.08 MPa, 60 min	4.1	25.36	[107]
400-1200 nm	Sphere-like	Air, 200 ℃, 50 s	54±2	-	[108]
300-400 nm	Sphere-like	N₂, 200 ℃, 30 min	139±24	-	[109]
1-3 μm	Sphere-like	Air, 180 ℃, 5 min	30	-	[110]
200 nm	Spherical	Air, 300 ℃, 2 MPa, 1 min	-	21.8	[111]
50 nm	Spherical	Air, 220 ℃, 5 min	-	30	[112]
10 nm	Spherical	N₂, 200 ℃, 30 min	14.0±4.5	-	[113]
6.5 nm	Spherical	Air, 175 ℃, 2 MPa, 10 min	-	35.1	[114]
60 nm	Sphere-like	95% Ar-5% H₂, 250 ℃, 10 MPa, 60 min	-	32.4	[115]
4.4 nm	Angular	N₂, 150 ℃, 30 min	52	-	[116]
Tens to hundreds of nanometers	Irregular	Vacuum, 300 ℃, 0.4 MPa,30 min	-	20	[117]
<10 nm	Angular	Ar, 250 ℃, 3 MPa, 30 min	5.1	-	[118]

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第三代半导体互连材料与低温烧结纳米铜材的研究进展

Progress of Interconnect Materials in the Third-generation Semiconductor and Their Low-temperature Sintering of Copper Nanoparticles

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