PMN-PT单晶与Ag电极共烧界面结构及扩散行为研究

摘要/Abstract

摘要： 采用丝网印刷工艺在PMN-PT弛豫铁电单晶晶片表面涂覆了中温及高温两种银浆,通过快速烧结工艺分别在650和850 ℃条件下制备了银电极。采用扫描电子显微镜观察银电极表面及金属-晶体界面的微观结构,采用能谱分析了界面的元素分布情况。银电极厚度为几十微米,呈多孔结构,与晶体结合良好。经过烧结后,晶体中的Pb、Nb、Ti等原子向银电极发生了迁移,而高温银浆烧结后在界面形成几微米厚的过渡层,晶体中原子向电极中的迁移大幅度减少。不同晶向的PMN-PT晶片在高温下向银电极扩散过程中具有很强的晶面效应,[110]方向晶体中Pb、Nb、Ti原子向电极中的扩散程度小于[100]方向晶体。

关键词: PMN-PT, 弛豫铁电单晶, Ag电极, 金属-晶体界面, 原子扩散

Abstract: The surface of PMN-PT relaxor ferroelectric single crystal was coated with medium and high temperature Ag paste by screen printing process. Ag electrodes were prepared by rapid sintering process at 650 and 850 ℃, respectively. The microstructure of Ag electrode surface and metal-crystal interface was observed by scanning electron microscope. The distribution of elements at the interface was analyzed by energy spectrum. The Ag electrode has a thickness of tens of microns, a porous structure, and a good combination with crystals. After sintering, atoms such as Pb, Nb and Ti in the crystal migrate to the Ag electrode, and a transition layer of several microns thickness is formed at the interface after sintering of the high temperature Ag paste, which greatly reduces the migration of atoms in the crystal to the electrode. PMN-PT wafers with different crystal orientation have a strong crystal face effect during the diffusion process to the Ag electrode at high temperature, and the diffusion degree of Pb, Nb and Ti atoms in the [110] direction crystal is smaller than that in the [100] direction crystal.

Key words: PMN-PT, relaxor ferroelectric single crystal, Ag electrode, metal-crystal interface, atomic diffusion

中图分类号:

O782
TB34

郑彧, 童亚琦, 李辉, 张微, 张璇, 王震. PMN-PT单晶与Ag电极共烧界面结构及扩散行为研究[J]. 人工晶体学报, 2023, 52(12): 2167-2173.

ZHENG Yu, TONG Yaqi, LI Hui, ZHANG Wei, ZHANG Xuan, WANG Zhen. Interfacial Structure and Diffusion Behavior of Co-Fired PMN-PT Single Crystal and Ag Electrode[J]. JOURNAL OF SYNTHETIC CRYSTALS, 2023, 52(12): 2167-2173.

参考文献

[1] LUO H S, XU G S, XU H Q, et al. Compositional homogeneity and electrical properties of lead magnesium niobate titanate single crystals grown by a modified Bridgman technique[J]. Japanese Journal of Applied Physics, 2000, 39(9B): 5581-5585.
[2] 郭益平, 罗豪甦, 徐海清, 等. 铅基弛豫型铁电单晶研究进展及其应用[J]. 人工晶体学报, 2001, 30(4): 330-336.
GUO Y P, LUO H S, XU H Q, et al. Progresses in relaxor ferroelectric single crystals and their potential application[J]. Journal of Synthetic Crystals, 2001, 30(4): 330-336 (in Chinese).
[3] PARK S E, SHROUT T R. Ultrahigh strain and piezoelectric behavior in relaxor based ferroelectric single crystals[J]. Journal of Applied Physics, 1997, 82(4): 1804-1811.
[4] LI F, CABRAL M J, XU B, et al. Giant piezoelectricity of Sm-doped Pb(Mg_1/3Nb_2/3)O₃-PbTiO₃ single crystals[J]. Science, 2019, 364(6437): 264-268.
[5] 张绍锋, 李强, 杨子. 准同型相界组分PMNT弛豫铁电单晶的畴结构与极化特性[J]. 人工晶体学报, 2009, 38(2): 411-415.
ZHANG S F, LI Q, YANG Z. Study on domain morphology and polarizing characteristics of PMNT relaxor ferroelectric single crystal[J]. Journal of Synthetic Crystals, 2009, 38(2): 411-415 (in Chinese).
[6] 罗豪甦, 焦杰, 陈瑞, 等. 弛豫铁电单晶的多功能特性及其器件应用[J]. 人工晶体学报, 2021, 50(5): 783-802.
LUO H S, JIAO J, CHEN R, et al. Multifunctional properties and device applications of the relaxor ferroelectric single crystals[J]. Journal of Synthetic Crystals, 2021, 50(5): 783-802 (in Chinese).
[7] 徐嘉林. 弛豫铁电单晶高压电响应及其在医用超声换能器中的应用研究[D]. 上海: 中国科学院上海硅酸盐研究所, 2021.
XU J L. Study on high voltage electrical response of relaxor ferroelectric single crystal and its application in medical ultrasonic transducer[D].Shanghai: Shanghai Institute of Ceramics, Chinese Academy of Sciences, 2021 (in Chinese).
[8] JIANG Z B, HOU C X, FEI C L, et al. Effects of composition segregation in PMN-PT crystals on ultrasound transducer performance[J]. IEEE Transactions on Ultrasonics, Ferroelectrics, and Frequency Control, 2022, 69(2): 795-802.
[9] LV J B, XIE X, ZHU X L, et al. Cold ablated high frequency PMN-PT/epoxy 1-3 composite transducer[J]. Applied Acoustics, 2022, 188: 108540.
[10] 徐晶晶. 不同电极特性对0.3Pb(Mg_0.33Nb_0.67)O₃-0.7PbTiO₃光伏性质影响的研究[D]. 哈尔滨: 哈尔滨工业大学, 2019.
XU J J. Effects of different electrode characteristics on photovoltaic properties of 0.3Pb(Mg_0.33Nb_0.67)O₃-0.7PbTiO₃[D]. Harbin: Harbin Institute of Technology, 2019 (in Chinese).
[11] 汤森进, 彭帅, 邹文. 溶剂对晶硅太阳能电池背银电极用银浆的性能影响[J]. 功能材料, 2016, 47(11): 11072-11075.
TANG S J, PENG S, ZOU W. Effects of solvents on properties of silver paste for back electrode of silicon solar cells[J]. Journal of Functional Materials, 2016, 47(11): 11072-11075 (in Chinese).
[12] GAO Y J, FENG J J, LIU F, et al. Effects of organic vehicle on the rheological and screen-printing characteristics of silver paste for LTCC thick film electrodes[J]. Materials, 2022, 15(5): 1953.
[13] 谭浩巍, 谭富彬, 梁琦, 等. 晶体硅太阳能电池正面银浆的作用机制[J]. 贵金属, 2022, 43(1): 91-95.
TAN H W, TAN F B, LIANG Q, et al. The action mechanism of front silver paste upon crystal silicon solar cells[J]. Precious Metals, 2022, 43(1): 91-95 (in Chinese).
[14] 王靖, 李宏杰, 冀亮君. 氮化铝陶瓷用银浆的研制[J]. 陶瓷, 2023(9): 29-32+61.
WANG J, LI H J, JI L J. Development of silver paste for aluminum nitride ceramics[J]. Ceramics, 2023(9): 29-32+61 (in Chinese).
[15] SUN Y H, XUE H B, YANG C Q, et al. Improvement of wettability of Te-modified lead-free glass frit and its effect to front side silver paste in crystalline silicon solar cells[J]. Solar Energy Materials and Solar Cells, 2023, 253: 112214.
[16] 赵玲, 黄富春, 邬云川. PZT压电陶瓷谐振器用银电极浆料[J]. 贵金属, 2002, 23(2): 26-29.
ZHAO L, HUANG F C, WU Y C. The silver paste applied to PZT piezoelectric ceramic resonator[J]. Precious Metals, 2002, 23(2): 26-29 (in Chinese).
[17] 韦群燕. 高导电率精密印刷银浆制备技术研究[D]. 昆明: 昆明理工大学, 2007.
WEI Q Y. Study on preparation technology of high conductivity precision printing silver paste[D]. Kunming: Kunming University of Science and Technology, 2007 (in Chinese).
[18] ZHANG Z, NAKAMURA T, HANADA T. Research of silver sintering process and reliability for high temperature operation of SiC power devices[J]. Materials Science Forum, 2014, 778/779/780: 1114-1117.
[19] SCOLA J, TASSART X, VILAR C, et al. Microstructure and electrical resistance evolution during sintering of a Ag nanoparticle paste[J]. Journal of Physics D: Applied Physics, 2015, 48(14): 145302.
[20] CHIANG H W, CHUNG C L, CHEN L C, et al. Processing and shape effects on silver paste electrically conductive adhesives (ECAs)[J]. Journal of adhesion science and technology, 2005, 19: 565-578.
[21] 张宇涛. 丝网印刷法制备稀土改性CuFe₂O₄尖晶石涂层研究[D]. 西安: 长安大学, 2022.
ZHANG Y T. Study on preparation of rare earth modified CuFe₂O₄ spinel coating by screen printing method[D]. Xi’an: Chang’an University, 2022 (in Chinese).
[22] DONG M, YE Z G. High-temperature solution growth and characterization of the piezo-/ferroelectric (1-x)Pb(Mg_1/3Nb_2/3)O_3-xPbTiO₃ [PMNT] single crystals[J]. Journal of Crystal Growth, 2000, 209: 81-90.
[23] ZHANG Y C, YANG Z Z, YE W N, et al.Effect of excess Pb on microstructures and electrical properties of 0.67Pb(Mg_1/3Nb_2/3)O₃-0.33PbTiO₃ ceramics[J].Journal of Materials Science Materials in Electronics, 2010, 22: 309-314.
[24] LEE H J, KIM S W, RYU S S. Sintering behavior of aluminum nitride ceramics with MgO-CaO-Al₂O₃-SiO₂ glass additive[J]. International Journal of Refractory Metals and Hard Materials, 2015, 53: 46-50.
[25] KUMAZAWA T, SUZUKI H. Transient liquid phase sintering of high-purity mullite for high-temperature structural ceramics[J]. Ceramics International, 2021, 47(9): 12381-12388.