Fabrication and characterization of pulsed laser deposited high-tunability, low-loss Ba0.6Sr0.4TiO3 thin films

YU Chenxi; JIANG Haolin; XIAO Zhifeng; BAO Xiaoqing; WANG Dan; DENG Gongxun; WANG Aiji

doi:10.7498/aps.74.20250938

Abstract

Microwave tunable devices are critical components in phased array antennas and RF front-ends, and essential for the precise controling of frequency, phase and amplitude. Although bulk dielectric ceramic materials are widely used in these devices, they pose challenges for integration. In contrast, dielectric thin films offer significant advantages, including easy integration, low cost, high tuning speed, low power consumption, compact size, and continuous tunability, making them more compatible with modern integrated circuit fabrication processes. Currently, a key prerequisite for designing devices based on dielectric thin films is the use of low-permittivity, low-loss substrates to mitigate their influence on the overall dielectric performance, while enhancing the crystalline quality of the films themselves. However, suitable substrates for epitaxial growth, such as MgO and Si, exhibit a significant lattice mismatch (>5%) with dielectric thin films. This poses a substantial challenge to achieving high-quality epitaxial growth, making it difficult to obtain dielectric thin films with both high tunability and low loss.To address this challenge, pulsed laser deposition (PLD) is used to provide high-energy, non-equilibrium growth conditions. By precisely controlling parameters such as substrate temperature and growth oxygen pressure, a suitable growth window that induce domain matching epitaxy (DME) mechanism can be determined, effectively adapting to mismatched strain, and thus successfully preparing high-performance Ba_0.6Sr_0.4TiO₃ (BSTO) epitaxial thin films on MgO(001) substrates.To investigate the effect of substrate temperature on the properties of the BSTO thin films, a series of films is prepared on MgO(001) substrates at temperatures of 680 ℃, 700 ℃, 730 ℃, 760 ℃ and 780 ℃, while other growth conditions are kept constant. The study reveals that as the substrate temperature increases, the crystallinity, tunability, and figure of merit (FOM) of the films are significantly improved. The film grown at 780 ℃ shows a high tunability value of 67.2%, a quality (Q) factor of 49, and an FOM of 32.93. Compared with previously reported films, the Ba_0.6Sr_0.4TiO₃ thin films prepared in this work demonstrate superior dielectric tunability and lower dielectric loss.To explore the thermal stability of the Ba_0.6Sr_0.4TiO₃ thin film, its performance is characterized using Raman spectroscopy and Capacitance-Voltage measurements in a temperature range from 25 ℃ to 225 ℃. Raman spectra indicate that the lattice vibrational modes of the Ba_0.6Sr_0.4TiO₃ film change with the increase of temperature. When temperature is in a range between 175 ℃ and 225 ℃, the film will completely transform from the tetragonal phase to the Raman-inactive cubic phase. At the same time, the nonlinear “butterfly” characteristic of the C-V curves vanishes due to the disappearance of ferroelectric domains. The dielectric constant and tunability reach their maximum values at approximately 60 ℃, then decrease, whereas the Q-factor reaches its peak at around 205 ℃. The motion of domain walls in films is constrained not only by internal stress fields and defects but also by strong pinning effects at the film-substrate interface and the free surface of the film.This research systematically analyzes the influences of surface morphology, crystal structure, and temperature on the dielectric properties of Ba_0.6Sr_0.4TiO₃ epitaxial thin films. It lays a foundation for elucidating the broadband structure-property relationships of Ba_1–xSr_xTiO₃ thin films and highlights their significant potential applications in tunable microwave devices.

Keywords:

Authors and contacts

1.
School of Physics and Astronomy, Beijing Normal University, Beijing 100875, China
2.
Key Laboratory of Multiscale Spin Physics (Ministry of Education), Beijing Normal University, Beijing 100875, China

Corresponding author: WANG Aiji, aijiwang@bnu.edu.cn

Funds: Project supported by the National Key R&D Program of China (Grant No. 2021YFA0718700), the National Natural Science Foundation of China (Grant No. 12304117), and the Natural Science Foundation of Beijing, China (Grant No. Z240008).

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References

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Cited By

图 1 不同衬底温度下生长的Ba_0.6Sr_0.4TiO₃薄膜的表面形貌及其表面粗糙度　(a) 680 ℃; (b) 700 ℃; (c) 730 ℃; (d) 760 ℃; (e) 780 ℃; (f) 薄膜的均方根表面粗糙度

Figure 1. Surface morphology and surface roughness of Ba_0.6Sr_0.4TiO₃ films grown on wafers of different temperatures: (a) 680 ℃; (b) 700 ℃; (c) 730 ℃; (d) 760 ℃; (e) 780 ℃; (f) RMS of films.

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图 2 不同衬底温度下生长的薄膜晶格结构表征　(a) XRD谱图; (b) (002)取向衍射峰的半高宽; (c) 晶格常数

Figure 2. Characterization of the lattice structure of thin films grown at different wafers’ temperatures: (a) XRD patterns; (b) the FWHM of (002) diffraction peak; (c) lattice constant.

DownLoad: Full-Size Img PowerPoint

图 3 薄膜电容器　(a) 叉指电极示意图; (b) 本研究制备的叉指电极

Figure 3. Thin film capacitor: (a) Interdigital electrodes; (b) photograph of the planar interdigitated capacitor structure.

DownLoad: Full-Size Img PowerPoint

图 4 不同衬底温度下生长的Ba_0.6Sr_0.4TiO₃薄膜的介电性能　(a) C-V曲线; (b) 在零场下的相对介电常数; (c) 可调率与Q; (d) 优值因子

Figure 4. Dielectric properties of Ba_0.6Sr_0.4TiO₃ films grown at different wafers’ temperatures: (a) C-V curves; (b) dielectric constant (at 0 kV/cm); (c) tunability and Q factor; (d) figures of merit.

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图 5 Ba_0.6Sr_0.4TiO₃薄膜介电性能对比图

Figure 5. Comparison figure of dielectric properties of Ba_0.6Sr_0.4TiO₃ films.

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图 6 (a) Ba_0.6Sr_0.4TiO₃的(113)峰倒易空间衍射; (b) Ba_0.6Sr_0.4TiO₃/MgO(001)的HAADF图像

Figure 6. (a) Reciprocal space mapping of (113) diffraction peak for Ba_0.6Sr_0.4TiO₃; (b) HAADF imaging of Ba_0.6Sr_0.4TiO₃/MgO(001).

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图 7 Ba_0.6Sr_0.4TiO₃薄膜在不同温度下的Raman散射光谱与C-V曲线

Figure 7. Raman scattering spectra and C-V curves of Ba_0.6Sr_0.4TiO₃ thin films at different temperatures.

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图 8 Ba_0.6Sr_0.4TiO₃薄膜在不同测试温度下的介电性能　(a) 零场下的介电常数; (b) $ 1/\varepsilon{\text{-}}T $曲线与居里-外斯定律理论曲线; (c) 可调率; (d) Q值

Figure 8. Temperature-dependent dielectric properties of Ba_0.6Sr_0.4TiO₃ thin films: (a) Dielectric constant (at 0 kV/cm); (b) $ 1/\varepsilon{\text{-}}T $ and Curie-Weiss law curves; (c) tunability; (d) Q factor.

DownLoad: Full-Size Img PowerPoint

[1]	Emadi F, Nemati A, Hinterstein M, Adabiroozjaei E 2019 Ceram. Int. 45 5503 Google Scholar
[2]	Borderon C, Ginestar S, Gundel H W, Haskou A, Nadaud K, Renoud R, Sharaiha A 2020 IEEE Trans. Ultrason. Ferroelectr. Freq. Control. 67 1733 Google Scholar
[3]	马华, 娄菁, 王军, 董博文, 冯明德, 李智强, 屈绍波 2019 空军工程大学学报 20 53 Google Scholar Ma H, Lou J, Wang J, Dong B W, Feng M D, Li Z Q, Qu S B 2019 J. Air Force Eng. Univ. 20 53 Google Scholar
[4]	Johnson K M 1962 J. Appl. Phys. 33 2826 Google Scholar
[5]	Dong H T, Jian J, Li H F, Jin D R, Chen J G, Cheng J R 2017 J. Alloys Compd. 725 54 Google Scholar
[6]	Bayrak T, Ozgit-Akgun C, Goldenberg E 2017 J. Non-Cryst. Solids 475 76 Google Scholar
[7]	Subramanyam G, Cole M W, Sun N X, Kalkur T S, Sbrockey N M, Tompa G S, Guo X M, Chen C L, Alpay S P, Rossetti G A Jr, Dayal K, Chen L Q, Schlom D G 2013 J. Appl. Phys. 114 191301 Google Scholar
[8]	Liu H G, Avrutin V, Zhu C Y, Özgür Ü, Yang J, Lu C Z, Morkoç H 2013 J. Appl. Phys. 113 044108 Google Scholar
[9]	Luo W, Chen X Y, Fan J W, Hu Y X, Zheng Z P, Fu Q W 2016 Ceram. Int. 42 17229 Google Scholar
[10]	Jiao T J, You C, Tian N, Ma L, Duan Z F, Yan F X, Ren P R, Zhao G Y 2022 Appl. Surf. Sci. 590 153112 Google Scholar
[11]	Wang J, Zhang T J, Xia H Y, Xiang J H, Li W K, Duo S W 2008 J. Sol-Gel Sci. Technol. 47 102 Google Scholar
[12]	Wander A, Bush I J, Harrison N M 2003 Phys. Rev. B 68 233405 Google Scholar
[13]	Misirlioglu I B, Alpay S P, He F, Wells B O 2006 J. Appl. Phys. 99 104103 Google Scholar
[14]	Peng L S J, Xi X X, Moeckly B H, Alpay S P 2003 Appl. Phys. Lett. 83 4592 Google Scholar
[15]	Tagantsev A K, Sherman V O, Astafev K F, Venkatesh J, Setter N 2003 J. Electroceram. 11 5 Google Scholar
[16]	Acikel B 2002 Ph. D. Dissertation (Santa Barbara: University of California
[17]	Su H T, Lancaster M J, Huang F, Wellhofer F 2000 Microwave Opt. Technol. Lett. 24 155 Google Scholar
[18]	Gao L B, Guan Z P, Huang S X, Liang K X, Chen H W, Zhang J H 2019 J. Mater. Sci. : Mater. Electron. 30 12821 Google Scholar
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[21]	熊沛雨, 倪壮, 林泽丰, 柏欣博, 刘天想, 张翔宇, 袁洁, 王旭, 石兢, 金魁 2023 物理学报 72 097701 Google Scholar Xiong P Y, Ni Z, Lin Z F, Bai X B, Liu T X, Zhang X Y, Yuan J, Wang X, Shi J, Jin K 2023 Acta Phys. Sin. 72 097701 Google Scholar
[22]	沈德坤, 杨淄涵, 郭沛源, 赵梦玲, 葛健, 邓功勋, 王爱记 2024 硅酸盐学报 52 229 Google Scholar Shen D K, Yang Z H, Guo P Y, Zhao M L, Ge J, Deng G X, Wang A J 2024 J. Chin. Ceram. Soc. 52 229 Google Scholar
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[25]	Chung U, Elissalde C, Maglione M, Estournès C, Pate M, Ganne J P 2008 Appl. Phys. Lett. 92 042902 Google Scholar
[26]	Zhu X H, Zheng D N, Peng W, Li J, Chen Y F 2006 Mater. Lett. 60 1224 Google Scholar
[27]	Gou X L, Gervais M, Gervais F, Catherinot A, Champeaux C, Sabary F 2002 Mater. Sci. Semicond. Process. 5 189 Google Scholar
[28]	Wang S X, Hao J H, Wu Z P, Wang D Y, Zhuo Y, Zhao X Z 2007 Appl. Phys. Lett. 91 252908 Google Scholar
[29]	Zhi Y N, Liu D A, Qu W J, Luan Z, Liu L R 2007 Appl. Phys. Lett. 90 042904 Google Scholar
[30]	Feng Z Y, Chen W, Tan O K 2009 Mater. Res. Bull. 44 1709 Google Scholar
[31]	Qin W F, Zhu J, Xiong J, Tang J L, Feng X 2007 J. Electron. Sci. Technol. China 5 303
[32]	秦杨晓, 李卓, 梁文学, 刘娜, 赵鹏 2018 压电与声光 40 95 Google Scholar Qin Y X, Li Z, Liang W X, Liu N, Zhao P 2018 Piezoelectr. Acoustoopt. 40 95 Google Scholar
[33]	Xu Q, Zhang X F, Huang Y H, Chen W, Liu H X, Chen M, Kim B H 2009 J. Alloys Compd. 488 448 Google Scholar
[34]	戚炜恒, 王震, 李翔飞, 禹日成, 王焕华 2022 物理学报 71 178103 Google Scholar Qi W H, Wang Z, Li X F, Yu R C, Wang H H 2022 Acta Phys. Sin. 71 178103 Google Scholar
[35]	张奇伟, 翟继卫, 岳振星 2013 物理学报 62 237702 Google Scholar Zhang Q W, Zhai J W, Yue Z X 2013 Acta Phys. Sin. 62 237702 Google Scholar
[36]	Zhang Q W, Zhai J W, Kong L B, Yao X 2012 J. Appl. Phys. 112 124112 Google Scholar
[37]	Verma A, Raghavan S, Stemmer S, Jena D 2015 Appl. Phys. Lett. 107 192908 Google Scholar
[38]	陈渝, 周华将, 谢少雄, 徐倩, 朱建国, 王清远 2021 力学进展 51 755 Google Scholar Chen Y, Zhou H J, Xie S X, Xu Q, Zhu J G, Wang Q Y 2021 Adv. Mech. 51 755 Google Scholar
[39]	Chen J H, Su X, Yuan T, Tang W B, Ding S C, Shi Y, Li F M, Chen K, Yu Y, Zhang H C, Zhu S Y, Yuan G L, Lu J 2025 Adv. Mater. Interfaces 12 2400949 Google Scholar
[40]	唐秋文, 沈明荣, 方亮 2006 物理学报 55 1346 Google Scholar Tang Q W, Shen M R, Fang L 2006 Acta Phys. Sin. 55 1346 Google Scholar
[41]	Zhu X H, Chong N, Chan H L, Choy C, Wong K, Liu Z G, Ming N B 2002 Appl. Phys. Lett. 80 3376 Google Scholar
[42]	吕笑梅, 黄凤珍, 朱劲松 2020 物理学报 69 127704 Google Scholar Lü X M, Huang F Z, Zhu J S 2020 Acta Phys. Sin. 69 127704 Google Scholar
[43]	Alema F, Pokhodnya K 2015 J. Adv. Dielectr. 5 1550030 Google Scholar
[44]	Sahoo S K, Misra D, Sahoo M, MacDonald C A, Bakhru H, Agrawal D C, Mohapatra Y N, Majumder S B, Katiyar R S 2011 J. Appl. Phys. 109 064108 Google Scholar
[45]	Zhang J R, Chen C, Xiang S Q, Zhang J C, Qi Q, Huang R, Yu Y, Chen K, Han Z D, Yuan G L, Liu J M, Zhu J S 2022 Mater. Res. Express 9 106303 Google Scholar

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Vol. 74, Issue 19 - 2025-10-05

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Fabrication and characterization of pulsed laser deposited high-tunability, low-loss Ba_0.6Sr_0.4TiO₃ thin films