硅酸盐学报

高外延应变下铁酸铋薄膜的生长模式与畴结构

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杨华宇 ¹ , 郭常青 ¹ , 王静 ¹^,² , 黄厚兵 ¹^,²

硅酸盐学报 | 面向新一代信息技术应用的铁电薄膜与器件专题—研究论文 2025,53(9): 2452-2460

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硅酸盐学报 |面向新一代信息技术应用的铁电薄膜与器件专题—研究论文 2025 , 53 (9) : 2452 -2460

高外延应变下铁酸铋薄膜的生长模式与畴结构

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杨华宇¹, 郭常青¹, 王静¹^,², 黄厚兵¹^,²

作者信息

^1．北京理工大学前沿交叉科学院，北京理工大学材料学院，北京 100081

^2．北京理工大学（珠海）空天信息学域，广东珠海 519088

通讯作者:

王静（1988—），女，博士，副教授；

黄厚兵（1986—），男，博士，教授。

作者简介:

杨华宇（1998—），男，博士研究生。

Growth Mode and Domain Structure of Bismuth Ferrite Thin Films at High-Substrate Strain

Huayu YANG¹, Changqing GUO¹, Jing WANG¹^,², Houbing HUANG¹^,²

Affiliations

^1.School of Interdisciplinary Science, and School of Materials Science and Engineering, Beijing Institute of Technology, Beijing 100081, China

^2.Division of Atmosphere and Aerospace Information Technology, Beijing Institute of Technology, Zhuhai, Zhuhai 519088, Guangdong, China

Corresponding Author:

WANG Jing (1988-), female, Ph.D., Associate Professor. E-mail: jwang@bit.edu.cn;

HUANG Houbing (1986-), male, Ph.D., Professor. hbhuang@bit.edu.cn

YANG Huayu (1998-), male, Doctoral Candidate. E-mail: 1226245225@gq.com

出版时间: 2025-09-20 doi: 10.14062/j.issn.0454-5648.20250256

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摘要

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铁酸铋薄膜因其卓越的压电和铁电性能，在传感及信息存储领域备受关注。在薄膜体系中，外延应变与结构限域等因素可诱导出丰富的铁电畴结构，从而改变其宏观铁电、压电性能。因此，利用脉冲激光沉积技术精准调控铁酸铋薄膜的畴结构具有重要意义。本工作研究了铁酸铋薄膜的外延应变与生长模式对其畴结构的影响。通过调整沉积次数以增加薄膜厚度，实现了薄膜从T相到R/T混合相再到R’相的转变，并通过调整激光能量实现了薄膜从层状生长到层-岛混合生长的转变。此外，借助有限元模拟分析了外延应变的弛豫规律，并结合靶材蒸发的物质量探讨了沉积速率对薄膜生长模式的影响，从而深入理解了应变及空间结构限域对铁电相结构及畴结构的作用规律，为后续压电性能优化及高密度铁电纳米岛存储等领域的研究奠定了基础。

关键词

铁酸铋 / 脉冲激光沉积 / 外延应变 / 晶体结构 / 畴结构

Abstract

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Introduction

Bismuth ferrite (BiFeO₃, BFO) is a well-known ferroelectric material with excellent piezoelectric and ferroelectric properties at room and high temperatures, attributed to its high Curie temperature (1103 K). Its rich topological domain structures, such as vortex domains and skyrmions, show potential for high-density data storage due to their small size and stability. Recent studies show that ferroelectric materials near the morphotropic phase boundary (MPB) exhibit enhanced piezoelectric properties. Methods like applying strain, changing substrate orientation, and doping can create MPB structures in BFO films, improving their performance. Ferroelectric topological domains can be induced by engineering film boundaries, offering new opportunities for high-density information storage and logic devices. Pulsed Laser Deposition (PLD) was used to fabricate BFO films. By adjusting parameters, T-phase, R/T mixed-phase, and R-phase films were prepared. The effects of thickness and laser energy on crystal structure, growth mode, and domain structure were investigated. Finite element simulation and thermodynamic analysis revealed the influence of strain relaxation and deposition rate on film properties.

Methods

BFO films were fabricated on (001)-oriented LaAlO₃ (LAO) substrates using PLD with a KrF excimer laser (248 nm wavelength, 3 Hz frequency). By adjusting the number of pulses (2700, 3600, 5400) and laser energy density (0.90-1.50 J/cm²), various BFO films (T-phase, R/T mixed-phase, R-phase) were prepared. A Bi-rich B_1.1FeO₃ target was used to compensate for Bi evaporation. Growth conditions were 700 ℃ substrate temperature and 13 Pa oxygen pressure, followed by annealing at 650 ℃ in 20000 Pa oxygen for 30 min and cooling to room temperature at 5 ℃/min. The epitaxial strain on BFO from LAO was -4.5%. Characterization was performed using X-ray Diffraction (XRD) with a Rigaku Ultima IV, Atomic Force Microscopy (AFM) with a Bruker Dimension XR, and Piezoresponse Force Microscopy (PFM) with a Pt/Ir-coated Si cantilever. Finite element simulation was conducted to study strain distribution in BFO films on LAO, assuming a -4.5% strain boundary condition. The simulation, performed at 300 K with a 1 nm grid size, provided theoretical support for the experimental results.

Results and Discussion

In thin film systems, strain relaxation occurs as film thickness increases. Changing deposition cycles to increase thickness significantly impacts the crystal and domain structures of epitaxial films. With 2700 deposition cycles, the film exhibits a layer-by-layer step-flow growth mode with distinct in-plane polarization components in the T-phase BFO, forming regular stripe-like domains. Increasing cycles to 3600 results in an interwoven R/T mixed-phase stripe pattern and crescent-shaped domains, indicating a transition from T-phase to R/T mixed-phase structure. Further increasing cycles to 5400 leads to significant surface roughness, transitioning the film to R-phase BFO as the epitaxial relationship is disrupted. This suggests that excessive thickness causes strain relaxation, enhancing in-plane polarization signals in PFM images and increasing domain size.

Laser energy is another crucial factor affecting film growth. Higher laser energy increases the amount of evaporated target material and the plume size. At low energy (0.90 J/cm²), the film maintains layer-by-layer growth with impurity particles, showing in-plane polarizations in different orientations. Increasing energy to 1.35 J/cm² induces a transition to layer-island mixed growth, forming interconnected nanodots with ferroelectric characteristics. Further increasing energy to 1.50 J/cm² results in higher-density, smaller nanodots in an island growth mode, with fragmented domain structures.

Finite element simulation was used to analyze the effect of film thickness on strain relaxation in BFO/LAO films. Films with thicknesses of 10 nm and 50 nm showed minimal strain relaxation, maintaining -4.5% strain (T-phase). However, at 80 nm, strain relaxation began (-4.41%), and at 130 nm, it became more pronounced (-3.87%). This indicates that thicker films experience more significant strain relaxation, consistent with experimental observations. The concept of "evaporation depth" helps explain the impact of laser energy on growth modes. At low laser energy, fewer BFO cells are evaporated, allowing them to diffuse and form layer-by-layer structures. Conversely, high laser energy increases the number of evaporated cells and nucleation sites, promoting island growth. This study provides valuable insights into the effects of deposition cycles and laser energy on BFO film growth, offering guidance for optimizing film properties.

Conclusions

This study explores how epitaxial strain and growth mode affect the crystal structure and ferroelectric domains in BFO films. As film thickness increases, epitaxial strain relaxes, causing significant changes in high-strain BFO films. Films transition from T-phase to R/T mixed-phase and then R-phase BFO with increasing deposition cycles (2700 to 5400), highlighting thickness's role in strain relaxation and structure. Adjusting laser energy density (0.90 J/cm² to 1.50 J/cm²) shifts growth modes from T-phase to nanodot films, altering microstructure and domain distribution. Finite element simulations show that strain relaxation accelerates when film thickness exceeds 80 nm, with surface strain relaxing from -4.5% to -4.41%. Calculations of evaporated material per pulse reveal that low laser energy promotes layer-by-layer growth, while high energy induces island growth. These findings provide crucial insights into laser energy's role in controlling film growth and offer valuable guidance for developing high-performance piezoelectric materials and information storage devices.

Key words

bismuth ferrate / pulsed laser deposition / epitaxial strain / crystal structure / domain structure

引用本文

杨华宇, 郭常青, 王静, 黄厚兵. 高外延应变下铁酸铋薄膜的生长模式与畴结构. 硅酸盐学报, 2025 , 53 (9) : 2452 -2460 . DOI: 10.14062/j.issn.0454-5648.20250256

Huayu YANG, Changqing GUO, Jing WANG, Houbing HUANG. Growth Mode and Domain Structure of Bismuth Ferrite Thin Films at High-Substrate Strain[J]. Journal of the Chinese Ceramic Society, 2025 , 53 (9) : 2452 -2460 . DOI: 10.14062/j.issn.0454-5648.20250256

基金

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国家自然科学基金重大研究计划(92463306)
国家自然科学基金面上项目(52472119; 52372100)
北京市自然科学基金面上项目(2242057)

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2025年第53卷第9期

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文章信息

doi: 10.14062/j.issn.0454-5648.20250256

接收时间：2025-04-08
首发时间：2026-10-21
出版时间：2025-09-20

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出版历史

收稿日期：2025-04-08
修回日期：2025-04-25

基金

国家自然科学基金重大研究计划(92463306)

国家自然科学基金面上项目(52472119; 52372100)

北京市自然科学基金面上项目(2242057)

作者信息

^1．北京理工大学前沿交叉科学院，北京理工大学材料学院，北京 100081

^2．北京理工大学（珠海）空天信息学域，广东珠海 519088

通讯作者:

王静（1988—），女，博士，副教授；

黄厚兵（1986—），男，博士，教授。

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https://castjournals.cast.org.cn/joweb/gsyxb/CN/10.14062/j.issn.0454-5648.20250256

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2种不同金属材料的力学参数

科 Family	属数 Number of genus	种数 Number of species	占总种数比例 Percentage of total species (%)	属 Genus	种数 Number of species	占总种数比例 Percentage of total species (%)
鹅膏菌科Amanitaceae	2	11	5.26	鹅膏菌属 Amanita	10	4.78
小菇科 Mycenaceae	2	12	5.74	丝盖伞属 Inocybe	5	2.39
多孔菌科 Polyporaceae	8	14	6.70	蜡蘑属 Laccaria	5	2.39
红菇科 Russulaceae	3	23	11.00	小皮伞属 Marasmius	6	2.87
				小菇属 Mycena	11	5.26
				光柄菇属 Pluteus	5	2.39
				红菇属 Russula	17	8.13
				栓菌属 Trametes	5	2.39

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