硅片上集成高介电调谐率的柱状纳米晶BaTiO3铁电薄膜

doi:10.15541/jim20210437

无机材料学报 ›› 2022, Vol. 37 ›› Issue (6): 596-602.DOI: 10.15541/jim20210437 CSTR: 32189.14.10.15541/jim20210437

所属专题：【信息功能】介电、铁电、压电材料（202409）

硅片上集成高介电调谐率的柱状纳米晶BaTiO₃铁电薄膜

赵玉垚¹(), 欧阳俊¹^,²()

1.山东大学材料科学与工程学院, 材料液固结构演变与加工教育部重点实验室, 济南 250061
2.齐鲁工业大学(山东省科学院) 化学与化工学院, 济南 250353

收稿日期:2021-07-13 修回日期:2021-08-25 出版日期:2022-06-20 网络出版日期:2021-08-20
通讯作者: 欧阳俊, 男, 教授. E-mail: ouyangjun@qlu.edu.cn
作者简介:赵玉垚(1994-), 男, 博士研究生. E-mail: zhaoyuyao920606@163.com
基金资助:
国家自然科学基金(51772175);国家自然科学基金(11672036);济南市“新高校20条”项目(2021GXRC055);济南市“新高校20条”项目(济南市科技局)

Columnar Nanograined BaTiO₃ Ferroelectric Thin Films Integrated on Si with a Sizable Dielectric Tunability

ZHAO Yuyao¹(), OUYANG Jun¹^,²()

1. Key Laboratory for Liquid-Solid Structure Evolution and Processing of Materials, School of Materials Science and Engineering, Shandong University, Jinan 250061, China
2. School of Chemistry and Chemical Engineering, Qilu University of Technology (Shandong Academy of Sciences), Jinan 250353, China

Received:2021-07-13 Revised:2021-08-25 Published:2022-06-20 Online:2021-08-20
Contact: OUYANG Jun, male, professor. E-mail: ouyangjun@qlu.edu.cn
About author:ZHAO Yuyao (1994–), male, PhD candidate. E-mail: zhaoyuyao920606@163.com
Supported by:
National Natural Science Foundation of China(51772175);National Natural Science Foundation of China(11672036);Jinan “New Universities” 20 Project(2021GXRC055);Jinan “New Universities” 20 Project(Science and Technology Bureau of Jinan)

摘要/Abstract

摘要：

钛酸钡(BaTiO₃)具有优异的介电、铁电、压电和热释电等性能, 在微电子机械系统和集成电路领域具有广泛的应用。降低BaTiO₃薄膜的制备温度使其与现有的CMOS-Si工艺兼容, 已成为应用研究和技术开发中亟需解决的问题。本研究引入与BaTiO₃晶格常数相匹配的LaNiO₃作为缓冲层, 以调控其薄膜结晶取向, 在单晶Si(100)基底上450 ℃溅射制备了结构致密的柱状纳米晶BaTiO₃薄膜。研究表明：450 ℃溅射温度在保持连续柱状晶结构和(001)择优取向的前提下, 能获得相对较大的柱状晶粒(平均晶粒直径27 nm), 一定残余应变也有助于其获得了较好的铁电和介电性能。剩余极化强度和最大极化强度分别达到了7和43 μC·cm^-2。该薄膜具有良好的绝缘性, 在 0.8 MV·cm^-1电场下, 漏电流密度仅为10^-5 A·cm^-2。其相对介电常数ε_r展现了优异的频率稳定性：在1 kHz时ε_r为155, 当测试频率升至1 MHz, ε_r仅轻微降低至145。薄膜的介电损耗较小, 约为0.01~0.03 (1 kHz ~ 1 MHz)。通过电容-电压测试, 该薄膜材料展示出高达51%的介电调谐率, 品质因子亦达到17(@1 MHz)。本研究所获得的BaTiO₃薄膜在介电调谐器件中有着良好的应用前景。

关键词: 硅, BaTiO₃, 铁电薄膜, 柱状纳米晶, 介电调谐率, 品质因子

Abstract:

BaTiO₃ has a wide range of applications in microelectromechanical systems and integrated circuits due to its excellent dielectric, ferroelectric, piezoelectric, and pyroelectric properties. For the applied research and device applications of BaTiO₃ films, reducing its deposition temperature to be compatible with the CMOS-Si technology is an important Challenge. Here, with the help of a LaNiO₃ buffer layer which has a closely-matched lattice with BaTiO₃, (001)-textured BaTiO₃ films were sputter-deposited at 450 ℃ on single crystalline Si(100) substrates, which consisting of well-cryotallized, evenly-distributed columnar nanograins with an average grain size of 27 nm. Our result showed that this deposition temperature can maintain the columnar nanograin structure with a relatively large grain size, leading to a good ferroelectric performance. In addition, a small residual strain on Si was also helpful to improve its ferroelectric and dielectric properties. The remnant polarization and saturated polarization of these BaTiO₃ films reached 7 and 43 μC·cm^-2, respectively, while leakage current densities were as low as 10^-5 A·cm^-2 at an applied electric field of 0.8 MV·cm^-1. These BaTiO₃ films also displayed excellent frequency stability with a low dielectric loss in which relative dielectric constant measured to be ~155 at 1 kHz, slightly being reduced to ~145 after increasing the frequency to 1 MHz. Meanwhile, the dielectric loss slightly increased from 0.01 at 1 kHz to 0.03 at 1 MHz. Lastly, through capacitance-voltage (C-V) tests, these films exhibited a large dielectric tunability of~51% and a figure of merit (FOM) of ~17 (@1 MHz). These films have a good potential for applications in tunable dielectrics.

Key words: silicon, BaTiO₃, ferroelectric film, columnar nanograins, dielectric tunability, figure of merit

中图分类号:

TQ174

赵玉垚, 欧阳俊. 硅片上集成高介电调谐率的柱状纳米晶BaTiO₃铁电薄膜[J]. 无机材料学报, 2022, 37(6): 596-602.

ZHAO Yuyao, OUYANG Jun. Columnar Nanograined BaTiO₃ Ferroelectric Thin Films Integrated on Si with a Sizable Dielectric Tunability[J]. Journal of Inorganic Materials, 2022, 37(6): 596-602.

图/表 4

图1 BaTiO3薄膜的物相结构分析

Fig. 1 Phase structure analyses of BaTiO3 films (a) XRD patterns of BaTiO3 films deposited at different temperatures; (b) Magnified area near BaTiO3(002)/LaNiO3(200) peaks from (a) with inset showing XRD patterns over 20°-50° at a low scanning rate (1 (°)/min)

图2 (a-c) 450 ℃和(d-f) 500 ℃沉积BaTiO3薄膜的纳米结构

Fig. 2 Nanostructures of BaTiO3 films deposited at (a-c) 450 ℃ and (d-f) 500 ℃ (a-c) 450 ℃-deposited BaTiO3 film: (a) Low magnification cross-sectional TEM image; (b) Low-resolution TEM image of the interface between LaNiO3 and BaTiO3; (c) High-resolution TEM image of the interface between LaNiO3 and BaTiO3 with the yellow dashed line showing the interface of LaNiO3/BaTiO3, while the white dashed lines showing a conformally grown BaTiO3 nanograin from its interface with LaNiO3 (d-f) 500 ℃-deposited BaTiO3 film: (d) Low magnification cross-sectional TEM image; (e) Low-resolution TEM image of the interface between LaNiO3 and BaTiO3; (f) High-resolution TEM image of the interface between LaNiO3 and BaTiO3 with the yellow dashed line showing the interface of LaNiO3/BaTiO3

图3 BaTiO3薄膜的电学性能

Fig. 3 Electrical performance of BaTiO3 films (a) Standard P-E hysteresis loops; (b) The maximum polarization (Pm) and self-polarization (PS), as well as Pm-Ps of the BaTiO3 films as functions of the applied electric field; (c) Small-field (Vp-p=1 V) dielectric constant and loss tangent as functions of the measuring frequency (εr-f and tanδ-f); (d) Leakage current density vs the applied DC electric field

图4 BaTiO3薄膜的介电调谐性能

Fig. 4 Dielectric tunability performance of the BaTiO3 films Dielectric constant (εr) as a function of E from (a) P-E and (b) C-V test results with loss tangent as a function of E; (c) Dielectric tunability and figure of merit as functions of E with data points were taken from (b); (d) Comparison with other leading ferroelectric films in dielectric tunability and deposition temperature

参考文献 30

[1]	TAGANTSEV A K, SHERMAN V O, ASTAFIEV K F, et al. Ferroelectric materials for microwave tunable applications. Journal of Electroceramics, 2003, 11(1/2): 5-66. DOI URL
[2]	MIN H K, KIM T Y, SEUNG E M, et al. Microwave properties of Mn doped (Ba_1-_x, Sr_x)TiO₃thin films for tunable phase shifter. Integrated FerroeLectrics, 2004, 66(1): 283-289. DOI URL
[3]	HARIBABU P, MAHESH P, HWANG G T, et al. High-performance dielectric ceramic films for energy storage capacitors: progress and outlook. Advanced Functional Materials, 2018, 28(42): 1803665.
[4]	NIU G, YIN S, SAINT-GIRONS G, et al. Epitaxy of BaTiO₃ thin film on Si (001) using a SrTiO₃ buffer layer for non-volatile memory application. Microelectronic Engineering, 2011, 88(7): 1232-1235. DOI URL
[5]	GAO T, LIAO J J, WANG J S, et al. Highly oriented BaTiO₃ film self-assembled using an interfacial strategy and its application as a flexible piezoelectric generator for wind energy harvesting. Journal of Materials Chemistry A, 2015, 3(18): 9965-9971. DOI URL
[6]	ZHANG W, CHENG H B, YANG Q, et al. Crystallographic orientation dependent dielectric properties of epitaxial BaTiO₃ thin films. Ceramics International, 2016, 42(3): 4400-4405. DOI URL
[7]	ZHAO J Y, CHEN H W, WEI M, et al. Effects of Bi₂O₃, Sm₂O₃ content on the structure, dielectric properties and dielectric tunability of BaTiO₃ ceramics. Journal of Materials Science, 2019, 30(21): 19279-19288.
[8]	ZHU C Q, WANG X H, ZHAO Q C, et al. Effects of grain size and temperature on the energy storage and dielectric tunability of non-reducible BaTiO₃-based ceramics. Journal of the European Ceramic Society, 2019, 39(4): 1142-1148. DOI URL
[9]	GAO L N, ZHAO J W, YAO X. Low dielectric loss and enhanced tunability of Ba(Zr_0.3Ti_0.7)O₃-based thin film by Sol-Gel method. Ceramics International, 2008, 34(4): 1023-1026. DOI URL
[10]	ZHANG H F, GIDDEN H, SAUNDERS T G, et al. High tunability and low loss in layered perovskite dielectrics through intrinsic elimination of oxygen vacancies. Chemistry of Materials, 2020, 32(23): 10120-10129. DOI URL
[11]	SREENIVAS P, PRADHAN D, PEREZ W, et al. Structure, dielectric tunability, thermal stability and diffuse phase transition behavior of lead free BZT-BCT ceramic capacitors. Journal of Physics and Chemistry of Solids, 2013, 74(3): 466-475. DOI URL
[12]	PENG B L, ZHANG Q, LI X, et al. High dielectric tunability, electrostriction strain and electrocaloric strength at a tricritical point of tetragonal, rhombohedral and pseudocubic phases. Journal of Alloys and Compounds, 2015, 646(15): 597-602. DOI URL
[13]	SANGLE A L, LEE O J, KURSUMOVIC A, et al. Very high commutation quality factor and dielectric tunability in nanocomposite SrTiO₃ thin films with Tc enhanced to >300 ℃. Nanoscale, 2018, 10(7): 2460-3468.
[14]	HAO L X, YANG Y L, HUAN Y, et al. Achieving a high dielectric tunability in strain-engineered tetragonal K_0.5Na_0.5NbO₃ films. npj Computational Materials, 2021, 7(1): 62. DOI URL
[15]	CHEN H W, YANG C R, FU C L, et al. The size effect of Ba_0.6Sr_0.4TiO₃ thin films on the ferroelectric properties. Applied Surface Science, 2006, 252(12): 4171-4177. DOI URL
[16]	GAO Y Q, YUAN M L, SUN X, et al. In situ preparation of high quality BaTiO₃ dielectric films on Si at 350-500 ℃. Journal of Materials Science: Materials in Electronics, 2016, 28(1): 337-343. DOI URL
[17]	ZHAO Y Y, OUYANG J, WANG K, et al. Achieving an ultra-high capacitive energy density in ferroelectric films consisting of superfine columnar nanograins. Energy Storage Materials, 2021, 39: 81-88. DOI URL
[18]	RAYMOND M V, SMYTH D M. Defects and charge transport in perovskite ferroelectrics. Journal of Physics and Chemistry of Solids, 1996, 57(10): 1507-1511. DOI URL
[19]	CHOI K J, BIEGALSKI M, LI Y L, et al. Enhancement of ferroelectricity in strained BaTiO₃ thin films. Science, 2004, 306(5698): 1005-1009. DOI URL
[20]	WANG K, ZHANG Y, WANG S X, et al. High energy performance ferroelectric (Ba,Sr)(Zr,Ti)O₃ film capacitors integrated on Si at 400 ℃. ACS Applied Materials& Interface, 2021, 13: 22717-22727.
[21]	MILTON O. Materials Science of Thin Films. Academic Press, 2002.
[22]	CAI Z M, WANG X H, HONG W, et al. Grain-size- dependent dielectric properties in nanograin ferroelectrics. Journal of the American Ceramic Society, 2018, 101(12): 5487-5496. DOI URL
[23]	CHENG J G, MENG X J, TANG J, et al. Effects of individual layer thickness on the structure and electrical properties of Sol-Gel- derived Ba_0.8Sr_0.2TiO₃ thin films. Journal of the Ceramic Society, 2000, 83(10): 2616-2618.
[24]	LIU S W, WEAVER J, YUAN Z, et al. Ferroelectric (Pb,Sr)TiO₃ epitaxial thin films on (001)MgO for room temperature high- frequency tunable microwave elements. Applied Physics Letters, 2005, 87(14): 142905. DOI URL
[25]	WU Z, ZHOU J, CHEN W, et al. Improvement in temperature dependence and dielectric tenability properties of PbZr_0.52Ti_0.48O₃ thin films using Ba(Mg_1/3Ta_2/3)O₃ buffer layer. Applied Surface Science, 2016, 388: 579-583. DOI URL
[26]	DONG H T, JIAN J, LI H F, et al. Improved dielectric tunability of PZT/BST multilayer thin films on Ti substrates. Journal of Alloys and Compounds, 2017, 725: 54-59. DOI URL
[27]	ZHENG Z, YAO Y Y, WENG W J, et al. High dielectric tunability of (100) oriented Pb_xSr_1-_xTiO₃ thin film coordinately controlled by dipole activation and phase anisotropy. Journal of Applied Physics, 2011, 110(12): 124107. DOI URL
[28]	TAKEDA K, MURAISHI T, HOSHINA T, et al. Dielectric tunability and electro-optic effect of Ba_0.5Sr_0.5TiO₃ thin films. Journal of Applied Physics, 2010, 107(7): 074105. DOI URL
[29]	GAO L B, JIANG S W, LI R G. Effect of sputtering pressure on structure and dielectric properties of bismuth magnesium niobate thin films prepared by RF magnetron sputtering. Thin Solid Films, 2016, 603: 391-394. DOI URL
[30]	ZHAI J W, YAO X, ZHANG L Y, et al. Dielectric nonlinear characteristics of BaZr_0.35T_i0.65O₃ thin films grown by a Sol-Gel process. Applied Physics Letters, 2004, 84(16): 3136-3138. DOI URL

编辑推荐 0

Metrics

阅读次数

全文

897

HTML			PDF

最新录用	在线预览	正式出版	最新录用	在线预览	正式出版
0	0	33	92	0	772

来源	本网站	其他网站

次数	764	133
比例	85%	15%

摘要

587

最新录用	在线预览	正式出版

121	0	466

来源	本网站	其他网站

次数	467	120
比例	80%	20%

硅片上集成高介电调谐率的柱状纳米晶BaTiO₃铁电薄膜

Columnar Nanograined BaTiO₃ Ferroelectric Thin Films Integrated on Si with a Sizable Dielectric Tunability

RichHTML

PDF (PC)

可视化

摘要/Abstract

引用本文

使用本文

图/表 4

参考文献 30

相关文章 15

编辑推荐 0

Metrics

本文评价

[1]	王浩, 刘学超, 郑重, 潘秀红, 徐锦涛, 朱新锋, 陈锟, 邓伟杰, 汤美波, 郭辉, 高攀. 非本征背照触发平面型4H-SiC光导开关性能研究[J]. 无机材料学报, 2024, 39(9): 1070-1076.
[2]	刘鹏东, 王桢, 刘永锋, 温广武. 硅泥在锂离子电池中的应用研究进展[J]. 无机材料学报, 2024, 39(9): 992-1004.
[3]	王康龙, 殷杰, 陈晓, 王力, 刘学建, 黄政仁. 颗粒级配对选区激光烧结打印结合常压固相烧结制备碳化硅陶瓷性能的影响[J]. 无机材料学报, 2024, 39(7): 754-760.
[4]	李刘媛, 黄开明, 赵秀艺, 刘会超, 王超. RE-Si-Al-O玻璃相对高熵稀土双硅酸盐微结构及耐CMAS腐蚀性能的影响[J]. 无机材料学报, 2024, 39(7): 793-802.
[5]	曹青青, 陈翔宇, 吴健豪, 王筱卓, 王乙炫, 王禹涵, 李春颜, 茹菲, 李兰, 陈智. SiO₂增强自敏性氮化碳微球可见光降解盐酸四环素的研究[J]. 无机材料学报, 2024, 39(7): 787-792.
[6]	张育育, 吴轶城, 孙佳, 付前刚. 聚合物转化SiHfCN陶瓷的制备及其吸波性能[J]. 无机材料学报, 2024, 39(6): 681-690.
[7]	王伟明, 王为得, 粟毅, 马青松, 姚冬旭, 曾宇平. 以非氧化物为烧结助剂制备高导热氮化硅陶瓷的研究进展[J]. 无机材料学报, 2024, 39(6): 634-646.
[8]	郑雅雯, 张翠萍, 张瑞杰, 夏乾, 茹红强. 硼酸碳热还原-渗硅反应烧结制备碳化硼陶瓷复合材料[J]. 无机材料学报, 2024, 39(6): 707-714.
[9]	岳仔豪, 杨小兔, 张正亮, 邓瑞翔, 张涛, 宋力昕. Pb²⁺对掺杂硼硅酸盐玻璃中CsPbBr₃钙钛矿量子点发光性能的影响[J]. 无机材料学报, 2024, 39(4): 449-456.
[10]	孙川, 何鹏飞, 胡振峰, 王荣, 邢悦, 张志彬, 李竞龙, 万春磊, 梁秀兵. 含有石墨烯阵列的SiC基陶瓷材料的制备与力学性能[J]. 无机材料学报, 2024, 39(3): 267-273.
[11]	刘松, 张发强, 罗进, 刘志甫. 0.9BaTiO₃-0.1Bi(Mg_1/2Ti_1/2)O₃铁电薄膜制备及储能特性[J]. 无机材料学报, 2024, 39(3): 291-298.
[12]	陈梦杰, 王倩倩, 吴成铁, 黄健. 基于DFT的描述符预测生物陶瓷的降解性[J]. 无机材料学报, 2024, 39(10): 1175-1181.
[13]	赵雅文, 屈发进, 汪岩屹, 王智文, 陈初升. 基于硅酸铝纤维的柔性氧敏感元件的制备和性能[J]. 无机材料学报, 2024, 39(10): 1084-1090.
[14]	苏楠, 邱介山, 王治宇. 高容量氟掺杂碳包覆纳米硅负极材料: 气相氟化法制备及其储锂性能[J]. 无机材料学报, 2023, 38(8): 947-953.
[15]	倪晓诗, 林子扬, 秦沐严, 叶松, 王德平. 硅烷化介孔硼硅酸盐生物玻璃微球对PMMA骨水泥生物活性和力学性能的影响[J]. 无机材料学报, 2023, 38(8): 971-977.