生长条件对BiFeO3纳米岛内自组装铁电拓扑畴形成的影响

doi:10.15541/jim20240543

无机材料学报 ›› 2025, Vol. 40 ›› Issue (6): 667-674.DOI: 10.15541/jim20240543

生长条件对BiFeO₃纳米岛内自组装铁电拓扑畴形成的影响

周厚霖(), 宋志庆, 田国(), 高兴森()

华南师范大学华南先进光电子研究院, 先进材料研究所, 广州 510006

收稿日期:2024-12-28 修回日期:2025-02-28 出版日期:2025-06-20 网络出版日期:2025-03-06
通讯作者: 田国, 副研究员. E-mail: guotian@m.scnu.edu.cn;
高兴森, 研究员. E-mail: xingsengao@scnu.edu.cn
作者简介:周厚霖(2000-), 男, 硕士研究生. E-mail: zhouhoulin2000@163.com
基金资助:
国家重点研发计划(2022YFB3807603);国家自然科学基金重大研究计划重点项目(92163210);广东省自然科学基金(2024A1515011608)

Effects of Growth Conditions on the Formation of Self-assembly Grown Topological Domain in BiFeO₃ Nanoislands

ZHOU Houlin(), SONG Zhiqing, TIAN Guo(), GAO Xingsen()

Institute for Advanced Materials, South China Academy of Advanced Optoelectronics, South China Normal University, Guangzhou 510006, China

Received:2024-12-28 Revised:2025-02-28 Published:2025-06-20 Online:2025-03-06
Contact: TIAN Guo, associate professor. E-mail: guotian@m.scnu.edu.cn;
GAO Xingsen, professor. E-mail: xingsengao@scnu.edu.cn
About author:ZHOU Houlin (2000-), male, Master candidate. E-mail: zhouhoulin2000@163.com
Supported by:
National Key R&D Program of China(2022YFB3807603);Major Research Plan of the National Natural Science Foundation of China(92163210);Guangdong Basic and Applied Basic Research Foundation(2024A1515011608)

摘要/Abstract

摘要：

铁电材料中的极化拓扑畴结构具有丰富的物理特性, 在新型微纳电子器件领域展示出广泛的应用前景。设计与调控铁电拓扑畴的形态是实现其器件化应用的基础。本工作系统地研究了生长条件对铁酸铋(BiFeO₃, BFO)薄膜弯曲隆起形成的纳米岛内中心型极化拓扑畴形态的影响机制。实验结果表明, 中心型拓扑畴的形成与底层钌酸锶(SrRuO₃, SRO)电极纳米岛、纳米岛尺寸、BFO外延生长的温度与沉积厚度紧密相关。当电极纳米岛横向尺寸介于300~500 nm时, 后续BFO薄膜生长隆起并诱导形成纳米岛, 同时也诱导形成四象限中心型拓扑畴构型。随着电极纳米岛高度逐渐增加, 铁电纳米岛的畴结构从薄膜的条带畴转变为中心型拓扑畴; 当电极直径大于500 nm时, 中心畴会转变为之字形畴壁的构型, 表明形貌隆起带来的挠曲电效应对拓扑畴形成具有重要作用。在特定参数范围内(生长温度690~730 ℃, BFO厚度30~60 nm), 提高生长温度有利于形成完整四象限中心型拓扑畴, 也进一步说明薄膜缺陷、畴壁能与挠曲等多种因素协同作用机制。同时, 这种中心型拓扑畴可以通过外场调控翻转, 并诱导高/低导电态切换, 为开发基于极化拓扑电子器件奠定基础。

关键词: 铁酸铋, 自组装, 纳米岛阵列, 中心型拓扑畴, 挠曲电效应

Abstract:

Ferroelectric topological domain structures exhibit rich physical properties, displaying a wide range of application potential for next-generation nanoelectronic devices. The fundamental issue for the applications of topological devices lies in the precise design and control of ferroelectric topological domain states. Here, the effects of growth conditions on center-type quadrant topological domain configurations in BiFeO₃ (BFO) nanoislands formed through bending-induced bulges were investigated, which were generated by underlying electrode SrRuO₃ (SRO) nanoislands. The experimental results indicate that the formation of central-type topological domains is closely related to the growing conductions of SRO electrode nanoislands, nanoislands dimensions, temperature of BFO epitaxial growth, and BFO deposition thickness. When the lateral size of the electrode nanoislands ranges from 300 to 400 nm, the subsequently grown BFO thin film with nanoislands, and central-type four-quadrant topological domains can be induced by the underlying electrode protrusions. As the height of the electrode nanoislands gradually increases, the domain structure of the ferroelectric nanoislands changes from stripe domains of the thin film to central-type topological domains. However, at the diameter of electrode nanoisland exceeding 500 nm, the central domain transforms into a zigzag domain-wall configuration, demonstrating the important role of flexoelectric effects induced by morphological protrusions in the formation of topological domains. Within certain growth parameters (growth temperature in the range of 690-730 ℃ and BFO thickness in the range of 30-60 nm), increasing the growth temperature facilitates formation of complete four-quadrant central-type topological domains, revealing synergistic interactions among defects, domain wall energy, and flexoelectric effects on the formation of central domain states. This central-type topological domain can also be switched by external field, and simultaneously induce switching between high/low conductive states, laying a foundation for the further construction of polarization topological electronic devices.

Key words: BiFeO₃, self-assembly, nanoisland array, central-type topological domain, flexoelectric effect

中图分类号:

O469

周厚霖, 宋志庆, 田国, 高兴森. 生长条件对BiFeO₃纳米岛内自组装铁电拓扑畴形成的影响[J]. 无机材料学报, 2025, 40(6): 667-674.

ZHOU Houlin, SONG Zhiqing, TIAN Guo, GAO Xingsen. Effects of Growth Conditions on the Formation of Self-assembly Grown Topological Domain in BiFeO₃ Nanoislands[J]. Journal of Inorganic Materials, 2025, 40(6): 667-674.

图/表 7

图1 (a)模板辅助生长法制备BFO纳米岛阵列流程示意图; (b~d)各阶段样品表面阵列形貌

Fig. 1 (a) Schematic diagram illustrating procedures of fabricating the BFO nanoisland arrays with templated growth strategy; (b-d) Images of sample surface at each fabrication stage

图2 BFO纳米岛阵列生长机理示意图

Fig. 2 Schematic illustration of the growth mechanism of BFO nanoislands (a) Preferential nucleation process of BFO during self-assembly; (b) Coexistence of two growth modes during the self-assembly process on the SRO nanoisland arrays; (c) Formation of self-assembled BFO nanoislands; (d) SEM image of growing ~30 nm of BFO nanoislands (corresponding to the growth stage in (b)); (e) SEM image of well-ordered BFO nanoisland arrays (corresponding to the growth stage in (c)). Colorful figures are available on website

图3 BFO纳米岛阵列的晶体结构及拓扑畴分析

Fig. 3 Crystal structure and topological domain analysis of BFO nanoisland arrays (a) XRD pattern of BFO nanoisland arrays, where ■ denotes the impurity peaks generated in the substrate; (b) Piezoresponse hysteresis loops acquired on a randomly selected nanoisland exhibiting amplitude butterfly loop (blue) and phase hysteresis loop (red); (c, d) Vertical PFM phase image (c) and lateral PFM phase image (d) of BFO nanoisland arrays; (e) Schematic of 3D domain structures. Sample preparation conditions: 710 ℃, BFO thickness of 50 nm, SRO nanoisland height of 30 nm, and lateral size of 300 nm. Colorful figures are available on website

图4 BFO纳米岛阵列导电性调控

Fig. 4 Tunable conductivity in BFO nanoisland arrays (a) Phase images of the domain structures in BFO nanoislands before and after resistive switching between high-low resistance states, in which a write voltage of -5.0 V was applied within the red dashed box; (b) CAFM images of the nanoislands before and after resistive switching between high-low resistance states, in which a -5.0 V voltage is written in the blue dashed box. Sample preparation conditions: 710 ℃, BFO thickness of 50 nm, SRO nanoisland height of 30 nm, and lateral size of 300 nm. Colorful figures are available on website

图5 SRO纳米岛高度对BFO纳米岛拓扑畴结构的影响

Fig. 5 Effect of SRO nanoisland height on the topological domain structure of BFO nanoislands (a-i) Morphologies (a-c), lat-phase (d-f) and lat-amplitude (g-i) PFM images of BFO nanoisland arrays analyzed as a function of SRO nanoisland height (0, 5 and 30 nm); (j-l) Schematic diagrams of different domain structures formed at heights of 0, 5 and 30 nm (from left to right), respectively. Colorful figures are available on website

图6 不同横向尺寸的SRO纳米岛对BFO纳米岛拓扑畴结构的影响

Fig. 6 Effect of lateral dimensions of SRO nanoislands on topological domain structure of BFO nanoislands (a-i) Morphologies (a-c), lat-phase (d-f) and ver-phase (g-i) PFM images of BFO nanoislands with varying lateral dimensions, including isolated BFO nanoislands with ~300 and ~500 nm diameters, as well as a wide BFO nanoisland chain of ~500 nm (from left to right); (j, k) Schematic diagrams of quad-domain texture and chain-shaped zigzag domain structure. Colorful figures are available on website

图7 厚度及生长温度对BFO纳米岛中心型畴结构的影响

Fig. 7 Effects of thickness and growth temperature on the central-type domain structure of BFO nanoislands PFM phase images of BFO nanoislands grown at 690, 710, and 730 ℃, with corresponding thickness gradients of 30, 40, 50, and 60 nm, respectively. Colorful figures are available on website

参考文献 30

[1]	SEIDEL J, VASUDEVAN R K, VALANOOR N. Topological structures in multiferroics-domain walls, skyrmions and vortices. Advanced Electronic Materials, 2016, 2(1): 1500292.
[2]	SEIDEL J. Nanoelectronics based on topological structures. Nature Materials, 2019, 18: 188.
[3]	DAS S, HONG Z, MCCARTER M, et al. A new era in ferroelectrics. APL Materials, 2020, 8(12): 120902.
[4]	TANG Y L, ZHU Y L, MA X L. Topological polar structures in ferroelectric oxide films. Journal of Applied Physics, 2021, 129(20): 200904.
[5]	TANG Y L, ZHU Y L, MA X L, et al. Observation of a periodic array of flux-closure quadrants in strained ferroelectric PbTiO₃ films. Science, 2015, 348(6234): 547.
[6]	YADAV A K, NELSON C T, HSU S L, et al. Observation of polar vortices in oxide superlattices. Nature, 2016, 530: 198.
[7]	DAS S, TANG Y L, HONG Z, et al. Observation of room- temperature polar skyrmions. Nature, 2019, 568: 368.
[8]	RODRIGUEZ B J, GAO X S, LIU L F, et al. Vortex polarization states in nanoscale ferroelectric arrays. Nano Letters, 2009, 9(3): 1127.
[9]	SCOTT J F. Applications of modern ferroelectrics. Science, 2007, 315(5814): 954.
[10]	OWCZAREK M, HUJSAK K A, FERRIS D P, et al. Flexible ferroelectric organic crystals. Nature Communications, 2016, 7: 13108.
[11]	MARTIN L W, RAPPE A M. Thin-film ferroelectric materials and their applications. Nature Reviews Materials, 2017, 2: 16087.
[12]	HAN S T, ZHOU Y, ROY V A L. Towards the development of flexible non-volatile memories. Advanced Materials, 2013, 25(38): 5424.
[13]	LI Z W, WANG Y J, TIAN G, et al. High-density array of ferroelectric nanodots with robust and reversibly switchable topological domain states. Science Advances, 2017, 3(8): e1700919.
[14]	KIM K E, JEONG S, CHU K, et al. Configurable topological textures in strain graded ferroelectric nanoplates. Nature Communications, 2018, 9: 403.
[15]	MA J, MA J, ZHANG Q H, et al. Controllable conductive readout in self-assembled, topologically confined ferroelectric domain walls. Nature Nanotechnology, 2018, 13: 947.
[16]	KIM K E, KIM Y J, ZHANG Y, et al. Ferroelastically protected polarization switching pathways to control electrical conductivity in strain-graded ferroelectric nanoplates. Physical Review Materials, 2018, 2: 084412.
[17]	HAN M J, WANG Y J, TANG Y L, et al. Shape and surface charge modulation of topological domains in oxide multiferroics. The Journal of Physical Chemistry C, 2019, 123(4): 2557.
[18]	DING L L, JI Y, ZHANG X Y, et al. Exotic quad-domain textures and transport characteristics of self-assembled BiFeO₃ nanoislands on Nb-doped SrTiO₃. ACS Applied Materials & Interfaces, 2021, 13(10): 12331.
[19]	ZHOU X, SUN H Y, LUO Z, et al. Ferroelectric diode characteristic and tri-state memory in self-assembled BiFeO₃ nanoislands with cross-shaped domain structure. Applied Physics Letters, 2022, 121(4): 042903.
[20]	WANG Y, CHEN M F, MA J, et al. A self-assembly growth strategy for a highly ordered ferroelectric nanoisland array. Nanoscale, 2022, 14(38): 14046.
[21]	TIAN G, CHEN D Y, FAN H, et al. Observation of exotic domain structures in ferroelectric nanodot arrays fabricated via a universal nanopatterning approach. ACS Applied Materials & Interfaces, 2017, 9(42): 37219.
[22]	TIAN G, YI X, SONG Z Q, et al. Templated growth strategy for highly ordered topological ferroelectric quad-domain textures. Applied Physics Reviews, 2023, 10(2): 021413.
[23]	TIAN G, YANG W D, SONG X, et al. Manipulation of conductive domain walls in confined ferroelectric nanoislands. Advanced Functional Materials, 2019, 29(32): 1807276.
[24]	ZHENG H M, ZHAN Q, ZAVALICHE F, et al. Controlling self-assembled perovskite-spinel nanostructures. Nano Letters, 2006, 6(7): 1401.
[25]	LI X L, WANG C X, YANG G W. Thermodynamic theory of growth of nanostructures. Progress in Materials Science, 2014, 64: 121.
[26]	PRESTIPINO S, LAIO A, TOSATTI E. Systematic improvement of classical nucleation theory. Physical Review Letters, 2012, 108(22): 225701.
[27]	LEE J K, CHOY J H, CHOI Y. Equilibrium shape and heterogeneous nucleation barrier at spherical interfaces. Surface Science, 1991, 256: 147.
[28]	GOMEZ L R, GARCIA N A, VITELLI V, et al. Phase nucleation in curved space. Nature Communications, 2015, 6: 6856.
[29]	MA J, WANG J, ZHOU H, et al. Self-assembly growth of a multiferroic topological nanoisland array. Nanoscale, 2019, 11(43): 20514.
[30]	WANG Z L. Steps and facets on annealed LaAlO₃{100} and {110} surfaces. Surface Science, 1996, 360: 180.

生长条件对BiFeO₃纳米岛内自组装铁电拓扑畴形成的影响

Effects of Growth Conditions on the Formation of Self-assembly Grown Topological Domain in BiFeO₃ Nanoislands

RichHTML

PDF (PC)

可视化

摘要/Abstract

引用本文

使用本文

图/表 7

参考文献 30

相关文章 15

编辑推荐

Metrics

本文评价

[1]	戴乐, 刘洋, 高轩, 王书豪, 宋雅婷, 唐明猛, 刘丽莎, 汪尧进. 浓度梯度掺杂实现BiFeO₃薄膜自极化[J]. 无机材料学报, 2024, 39(1): 99-106.
[2]	张祥松, 刘业通, 王永瑛, 武子瑞, 刘振中, 李毅, 杨娟. 自组装制备PtIr合金气凝胶及其高效电催化氨氧化性能[J]. 无机材料学报, 2023, 38(5): 511-520.
[3]	李华鑫, 陈俊勇, 肖洲, 乐弦, 余显波, 向军辉. 纳米材料形貌和性能调控的仿生自组装研究进展[J]. 无机材料学报, 2021, 36(7): 695-710.
[4]	李铁, 李玥, 王颖异, 张珽. 石墨烯-铁酸铋纳米晶复合材料的制备及其催化性能研究[J]. 无机材料学报, 2021, 36(7): 725-732.
[5]	彭新村, 王智栋, 曾梦丝, 刘云, 邹继军, 朱志甫, 邓文娟. SiO₂纳米球的粒径均一性研究及其在硅光学共振纳米柱阵列中的应用[J]. 无机材料学报, 2019, 34(7): 734-740.
[6]	程国峰, 阮音捷, 孙玥, 尹晗迪. 纯相BiFeO₃的热稳定和热膨胀性质研究[J]. 无机材料学报, 2019, 34(10): 1128-1133.
[7]	程国峰, 阮音捷, 孙玥, 尹晗迪, 解其云. 元素配比对BiFeO₃反应烧结相变影响的高温X射线衍射研究[J]. 无机材料学报, 2019, 34(10): 1035-1040.
[8]	宋建民, 代秀红, 梁杰通, 赵磊, 周阳, 葛大勇, 孟旭东, 刘保亭. 偏轴磁控溅射法外延BiFeO₃薄膜的介电性能与阻变效应[J]. 无机材料学报, 2018, 33(9): 1017-1021.
[9]	王景平, 成方媛, 杜显锋, 徐友龙. 表面自组装法制备高比容Al₂O₃/TiO₂复合膜[J]. 无机材料学报, 2018, 33(6): 617-622.
[10]	范闻, 武利民. 硅油两步脱水法可控制备纳米二氧化钛透镜[J]. 无机材料学报, 2018, 33(12): 1337-1342.
[11]	罗维, 魏晶, 邓勇辉, 李宇慧, 王连军, 赵涛, 江莞. 新型两亲性嵌段共聚物导向合成有序大孔径介孔材料的研究进展[J]. 无机材料学报, 2017, 32(1): 1-10.
[12]	武萱蓉, 杨巧珍, 赵永祥, 路艳罗. ZnS微球的水热/溶剂热法合成及其光催化性能研究[J]. 无机材料学报, 2016, 31(5): 473-478.
[13]	张文强, 张锌. 厘米级盘形硅藻微粒单层密排研究[J]. 无机材料学报, 2015, 30(11): 1208-1212.
[14]	孙志娟, 陈雪莲, 蒋春跃. 自组装法制备中空二氧化硅纳米粒子减反射薄膜[J]. 无机材料学报, 2014, 29(9): 947-955.
[15]	陈峰, 孙团伟, 漆超, 吴进, 崔大祥, 朱英杰. 微波辅助溶剂热法制备磷酸钙微球和多面体[J]. 无机材料学报, 2014, 29(7): 776-780.