面向宽温域功能器件的连续组分外延铁电薄膜

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

doi:10.7498/aps.72.20230154

摘要

Ba_xSr_1–xTiO₃ (BST)铁电薄膜因为拥有高介电常数、强电场调谐性和较低的微波频段介电损耗可应用于微波可调谐器件. 然而铁电材料中普遍存在的介电常数-温度依赖性使得常规单组分铁电薄膜的高可调率温区受制于相变温度, 难以满足宽温域适用性的需求. 为研究可用于宽温域功能器件的铁电薄膜, 采用脉冲激光沉积(PLD)技术制备了单组分Ba_0.5Sr_0.5TiO₃薄膜、Ba_0.2Sr_0.8TiO₃薄膜以及Ba_0.2Sr_0.8TiO₃/Ba_0.5Sr_0.5TiO₃异质结构薄膜. 通过对比其介电性能, 发现垂直方向上Ba/Sr组分分布可有效改善BST薄膜的温度依赖性, 然而异质结构的构建可能带来界面问题, 同时也使其品质因子难以提升. 本文提出采用独特的水平方向连续组分薄膜制备技术制备BST组合薄膜, 有望在拓宽BST薄膜相变温区的同时避免界面控制的难题.

关键词:

Abstract

Ba_xSr_1–xTiO₃ (BST) ferroelectric thin films are widely used in microwave tunable devices due to their high dielectric constants, strong electric field tunabilities and low microwave losses. However, because of the temperature dependence of dielectric constant in ferroelectric material, the high-tunability for conventional single component ferroelectric thin film can only be achieved in the vicinity of Curie Temperature (T_C) which leads the ferroelectric thin films to be difficult to operate in a wide temperature range. To obtain ferroelectric thin films for temperature stable functional devices, single composition Ba_0.2Sr_0.8TiO₃ thin films, Ba_0.5Sr_0.5TiO₃ thin films, and Ba_0.2Sr_0.8TiO₃/Ba_0.5Sr_0.5TiO₃ heterostructure thin films are deposited by pulsed laser deposition (PLD). By comparing their dielectric properties in a wide temperature range, it is found that the temperature sensitivity of BST film can be effectively reduced by introducing a composition gradient along the epitaxial direction. However, the heterostructure engineering may bring extra troubles caused by interfaces, which may limit the quality factor Q. In this paper, we extend our combinatorial film deposition technique to ferroelectric materials, and we successfully fabricate in-plane composition-spread Ba_1–xSr_xTiO₃ thin films, which are expected to broaden the phase transition temperature ranges of BST films while avoiding the problem of interface control.

Keywords:

作者及机构信息

1.
武汉大学物理科学与技术学院, 武汉　430072

2.
中国科学院物理研究所, 北京凝聚态物理国家研究中心, 北京　100190

通信作者: 王旭, risingsunwx@iphy.ac.cn ; 石兢, jshi@whu.edu.cn ;

基金项目: 国家重点研发计划(批准号: 2021YFA0718700)资助的课题

Authors and contacts

1.
School of Physics and Technology, Wuhan University, Wuhan 430072, China

2.
Beijing National Laboratory for Condensed Matter Physics, Institute of Physics, Chinese Academy of Sciences, Beijing 100190, China

Corresponding author: Wang Xu, risingsunwx@iphy.ac.cn ; Shi Jing, jshi@whu.edu.cn ;

Funds: Project supported by the National Key R&D Program of China (Grant No. 2021YFA0718700).

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参考文献

[1]	Valasek J 1921 Phys. Rev. 17 475 Google Scholar
[2]	Busch G 1987 Ferroelectrics 74 267 Google Scholar
[3]	Fousek J 1994 Proceedings of 1994 IEEE International Symposium on Applications of Ferroelectrics PA, USA, Augest 7–10, 1994 pp1–5
[4]	Xu Y 1991 Ferroelectric Materials and their Applications (Amsterdam: Elsevier) pp1–36
[5]	Mikami N 1997 Thin Film Ferroelectric Materials and Devices (Boston, MA: Springer US) pp43–70
[6]	Acosta M, Novak N, Rojas V, Patel S, Vaish R, Koruza J, Rossetti Jr G A, Rödel J 2017 Appl. Phys. Rev. 4 041305 Google Scholar
[7]	Tagantsev A K, Sherman V O, Astafiev K F, Venkatesh J, Setter N 2003 J. Electroceramics 11 5 Google Scholar
[8]	Lancaster M J, Powell J, Porch A 1998 Supercond. Sci. and Technol. 11 1323 Google Scholar
[9]	Vendik O G, Hollmann E K, Kozyrev A B, Prudan A M 1999 J. Supercond. 12 325 Google Scholar
[10]	Xi X X, Li H, Si W, Sirenko A A, Akimov I A, Fox J R, Clark A M, Hao J 2000 J. Electroceram. 4 393 Google Scholar
[11]	Baik S, Setter N, Auciello O 2006 J. Appl. Phys. 100 051501 Google Scholar
[12]	Korn D S, Wu H D 1999 Integr. Ferroelectr. 24 215 Google Scholar
[13]	Setter N, Damjanovic D, Eng L, Fox G, Gevorgian S, Hong S, Kingon A, Kohlstedt H, Park N Y, Stephenson G B, Stolitchnov I, Taganstev A K, Taylor D V, Yamada T, Streiffer S 2006 J. Appl. Phys. 100 051606 Google Scholar
[14]	Scott J F 2000 Ferroelectric Memories (Berlin, Heidelberg: Springer) pp1–22
[15]	Scheele P, Goelden F, Giere A, Mueller S, Jakoby R 2005 IEEE MTT-S International Microwave Symposium Digest Long Beach, CA, USA, June 17, 2005 pp603–606
[16]	Deleniv A, Abadei S, Gevorgian S 2003 IEEE MTT-S International Microwave Symposium Digest (Vol. 2), Philadelphia, PA, USA, June 8–13, 2003 p1267
[17]	Kuylenstierna D, Vorobiev A, Linner P, Gevorgian S 2006 IEEE Microw. Wirel. Compon. Lett. 16 167 Google Scholar
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[20]	Cole M W, Ngo E, Hirsch S, Demaree J D, Zhong S, Alpay S P 2007 J. Appl. Phys. 102 034104 Google Scholar
[21]	Li F, Zhang S, Damjanovic D, Chen L-Q, Shrout T R 2018 Adv. Funct. Mater. 28 1801504 Google Scholar
[22]	Setter N, Cross L E 1980 J. Appl. Phys. 51 4356 Google Scholar
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[24]	Yao G, Wang X, Wu Y, Li L 2012 J. Am. Ceram. Soc. 95 614 Google Scholar
[25]	Wang S F, Li J H, Hsu Y F, Wu Y C, Lai Y C, Chen M H 2013 J. Eur. Ceram. Soc. 33 1793 Google Scholar
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[27]	Zhu X H, Meng Q D, Yong L P, He Y S, Cheng B L, Zheng D N 2006 J. Phys. D: Appl. Phys. 39 2282 Google Scholar
[28]	Kim W J, Chang W, Qadri S B, Pond J M, Kirchoefer S W, Chrisey D B, Horwitz J S 2000 Appl. Phys. Lett. 76 1185 Google Scholar
[29]	金魁, 吴颉 2021 物理学报 70 017403 Google Scholar Jin K, Wu J 2021 Acta Phys. Sin. 70 017403 Google Scholar
[30]	Chang W, Horwitz J S, Carter A C, Pond J M, Kirchoefer S W, Gilmore C M, Chrisey D B 1999 Appl. Phys. Lett. 74 1033 Google Scholar
[31]	Chang W, Kirchoefer S W, Pond J M, Horwitz J S, Sengupta L 2002 J. Appl. Phys. 92 1528 Google Scholar
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[33]	Wang H Z, Dong Y X, Zhu R J, Wang Z M, Guo X L, Zhang T, Yuan G L, Kimura H 2019 Ceram. Int. 45 8300 Google Scholar
[34]	Kim W J, Wu H D, Chang W, Qadri S B, Pond J M, Kirchoefer S W, Chrisey D B, Horwitz J S 2000 J. Appl. Phys. 88 5448 Google Scholar
[35]	Ding Y P, Wu J S, Meng Z Y, Chan H L, Choy Z L 2002 Mater. Chem. Phys. 75 220 Google Scholar
[36]	Schimizu T 1997 Solid State Commun. 102 523 Google Scholar
[37]	Gevorgian S, Petrov P K, Ivanov Z, Wikborg E 2001 Appl. Phys. Lett. 79 1861 Google Scholar
[38]	Dong H T, Lu G P, Jin D P, Chen J G, Cheng J R 2016 J. Mater. Sci. 51 8414 Google Scholar
[39]	Zhu R J, Wang Z M, Cheng Z X, Guo X L, Zhang T, Cai Z L, Kimura H, Matsumoto T, Shibata N, Ikuhara Y 2020 Ceram. Int. 46 20284 Google Scholar
[40]	Cole M W, Ngo E, Hirsch S, Okatan M B, Alpay S P 2008 Appl. Phys. Lett. 92 072906 Google Scholar
[41]	Marksz E J, Hagerstrom A M, Zhang X, Al Hasan N, Pearson J, Drisko J A, Booth J C, Long C J, Takeuchi I, Orloff N D 2021 Phys. Rev. Appl. 15 064061 Google Scholar

施引文献

图 1 Ba_0.5Sr_0.5TiO₃样品的(a)面外X射线θ-2θ扫描, (b) (031)峰倒易空间衍射(RSM), (c) X射线面内φ扫描, (d)室温下电容值与品质因子随外加电场的变化

Fig. 1. (a) Out of plane XRD spectra of θ-2θ scanning for Ba_0.5Sr_0.5TiO₃ film; (b) RSM of (301) diffraction peak for Ba_0.5Sr_0.5TiO₃ film; (c) XRD spectra of φ scanning for Ba_0.5Sr_0.5TiO₃ film; (d) dependence of capacitance and Q with electric field at room temperature.

下载: 全尺寸图片幻灯片

图 2 不同生长氧压的Ba_0.5Sr_0.5TiO₃薄膜的(a) C₀和(b)品质因子随温度变化; 不同生长氧压的Ba_0.2Sr_0.8TiO₃薄膜的(c) C₀和(d)品质因子随温度变化

Fig. 2. Temperature dependence of C₀ (a) and Q (b) for Ba_0.5Sr_0.5TiO₃ films deposited at different oxygen pressures; the temperature dependence of C₀ (c) and Q (d) for Ba_0.2Sr_0.8TiO₃ films deposited at different oxygen pressures.

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图 3 Ba_0.5Sr_0.5TiO₃和Ba_0.2Sr_0.8TiO₃薄膜的(a) T_M和(b) n_rMAX随生长氧压的变化

Fig. 3. Relationship between T_M (a) and n_rMAX (b) for the Ba_0.5Sr_0.5TiO₃ and Ba_0.2Sr_0.8TiO₃ films and their growth oxygen pressure.

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图 4 (a) Ba_0.5Sr_0.5TiO₃组分样品的面内(a)、面外晶格常数(c)及四方畸变比(a/c)随生长氧压的变化; (b) Ba_0.5Sr_0.5TiO₃组分样品的可调率随四方畸变比a/c的变化

Fig. 4. (a) Relationship between the in-plane lattice constant (a), out-of-plane lattice constant (c), the ratio of in-plane lattice constant/ out-of-plane lattice constant (a/c) of Ba_0.5Sr_0.5TiO₃ films and their growth oxygen pressure; (b) the relationship between the n_rMAX and a/c of Ba_0.5Sr_0.5TiO₃ films.

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图 5 (a) Ba_0.2Sr_0.8TiO₃/Ba_0.5Sr_0.5TiO₃异质结构样品介电可调率的温度依赖性与单组分样品对比; (b) 异质结构样品的介电可调率与品质因子随温度的变化

Fig. 5. (a) Temperature dependence of n_r of the BST heterostructure film compared with BST single component films; (b) temperature dependence of n_r and Q of the BST heterostructure film.

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图 6 连续组分Ba_xSr_1–xTiO₃薄膜的(a)微区XRD θ-2θ扫描, (b) c轴晶格常数随Ba掺杂量x的演化

Fig. 6. (a) Micro-region θ-2θ X-ray patterns of composition-spread Ba_xSr_1–xTiO₃ thin film; (b) Ba content x dependence of the c-axis lattice constants for a composition-spread Ba_xSr_1–xTiO₃ thin film.

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图 7 连续组分Ba_xSr_1–xTiO₃薄膜叉指电容示意图

Fig. 7. Schematic diagram of composition-spread Ba_xSr_1–xTiO₃ thin film interdigital capacitor.

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[1]	Valasek J 1921 Phys. Rev. 17 475 Google Scholar
[2]	Busch G 1987 Ferroelectrics 74 267 Google Scholar
[3]	Fousek J 1994 Proceedings of 1994 IEEE International Symposium on Applications of Ferroelectrics PA, USA, Augest 7–10, 1994 pp1–5
[4]	Xu Y 1991 Ferroelectric Materials and their Applications (Amsterdam: Elsevier) pp1–36
[5]	Mikami N 1997 Thin Film Ferroelectric Materials and Devices (Boston, MA: Springer US) pp43–70
[6]	Acosta M, Novak N, Rojas V, Patel S, Vaish R, Koruza J, Rossetti Jr G A, Rödel J 2017 Appl. Phys. Rev. 4 041305 Google Scholar
[7]	Tagantsev A K, Sherman V O, Astafiev K F, Venkatesh J, Setter N 2003 J. Electroceramics 11 5 Google Scholar
[8]	Lancaster M J, Powell J, Porch A 1998 Supercond. Sci. and Technol. 11 1323 Google Scholar
[9]	Vendik O G, Hollmann E K, Kozyrev A B, Prudan A M 1999 J. Supercond. 12 325 Google Scholar
[10]	Xi X X, Li H, Si W, Sirenko A A, Akimov I A, Fox J R, Clark A M, Hao J 2000 J. Electroceram. 4 393 Google Scholar
[11]	Baik S, Setter N, Auciello O 2006 J. Appl. Phys. 100 051501 Google Scholar
[12]	Korn D S, Wu H D 1999 Integr. Ferroelectr. 24 215 Google Scholar
[13]	Setter N, Damjanovic D, Eng L, Fox G, Gevorgian S, Hong S, Kingon A, Kohlstedt H, Park N Y, Stephenson G B, Stolitchnov I, Taganstev A K, Taylor D V, Yamada T, Streiffer S 2006 J. Appl. Phys. 100 051606 Google Scholar
[14]	Scott J F 2000 Ferroelectric Memories (Berlin, Heidelberg: Springer) pp1–22
[15]	Scheele P, Goelden F, Giere A, Mueller S, Jakoby R 2005 IEEE MTT-S International Microwave Symposium Digest Long Beach, CA, USA, June 17, 2005 pp603–606
[16]	Deleniv A, Abadei S, Gevorgian S 2003 IEEE MTT-S International Microwave Symposium Digest (Vol. 2), Philadelphia, PA, USA, June 8–13, 2003 p1267
[17]	Kuylenstierna D, Vorobiev A, Linner P, Gevorgian S 2006 IEEE Microw. Wirel. Compon. Lett. 16 167 Google Scholar
[18]	Mahmud A, Kalkur T S, Jamil A, Cramer N 2006 IEEE Microw. Wirel. Compon. Lett. 16 261 Google Scholar
[19]	Bao P, Jackson T J, Wang X, Lancaster M J 2008 J. Phys. D Appl. Phys. 41 063001 Google Scholar
[20]	Cole M W, Ngo E, Hirsch S, Demaree J D, Zhong S, Alpay S P 2007 J. Appl. Phys. 102 034104 Google Scholar
[21]	Li F, Zhang S, Damjanovic D, Chen L-Q, Shrout T R 2018 Adv. Funct. Mater. 28 1801504 Google Scholar
[22]	Setter N, Cross L E 1980 J. Appl. Phys. 51 4356 Google Scholar
[23]	Jeong I K, Darling T W, Lee J K, Proffen T, Heffner R H, Park J S, Hong K S, Dmowski W, Egami T 2005 Phys. Rev. Lett. 94 147602 Google Scholar
[24]	Yao G, Wang X, Wu Y, Li L 2012 J. Am. Ceram. Soc. 95 614 Google Scholar
[25]	Wang S F, Li J H, Hsu Y F, Wu Y C, Lai Y C, Chen M H 2013 J. Eur. Ceram. Soc. 33 1793 Google Scholar
[26]	Vendik O G, Zubko S P 2000 J. Appl. Phys. 88 5343 Google Scholar
[27]	Zhu X H, Meng Q D, Yong L P, He Y S, Cheng B L, Zheng D N 2006 J. Phys. D: Appl. Phys. 39 2282 Google Scholar
[28]	Kim W J, Chang W, Qadri S B, Pond J M, Kirchoefer S W, Chrisey D B, Horwitz J S 2000 Appl. Phys. Lett. 76 1185 Google Scholar
[29]	金魁, 吴颉 2021 物理学报 70 017403 Google Scholar Jin K, Wu J 2021 Acta Phys. Sin. 70 017403 Google Scholar
[30]	Chang W, Horwitz J S, Carter A C, Pond J M, Kirchoefer S W, Gilmore C M, Chrisey D B 1999 Appl. Phys. Lett. 74 1033 Google Scholar
[31]	Chang W, Kirchoefer S W, Pond J M, Horwitz J S, Sengupta L 2002 J. Appl. Phys. 92 1528 Google Scholar
[32]	Boikov Y A, Claeson T 2001 Appl. Phys. Lett. 79 2052 Google Scholar
[33]	Wang H Z, Dong Y X, Zhu R J, Wang Z M, Guo X L, Zhang T, Yuan G L, Kimura H 2019 Ceram. Int. 45 8300 Google Scholar
[34]	Kim W J, Wu H D, Chang W, Qadri S B, Pond J M, Kirchoefer S W, Chrisey D B, Horwitz J S 2000 J. Appl. Phys. 88 5448 Google Scholar
[35]	Ding Y P, Wu J S, Meng Z Y, Chan H L, Choy Z L 2002 Mater. Chem. Phys. 75 220 Google Scholar
[36]	Schimizu T 1997 Solid State Commun. 102 523 Google Scholar
[37]	Gevorgian S, Petrov P K, Ivanov Z, Wikborg E 2001 Appl. Phys. Lett. 79 1861 Google Scholar
[38]	Dong H T, Lu G P, Jin D P, Chen J G, Cheng J R 2016 J. Mater. Sci. 51 8414 Google Scholar
[39]	Zhu R J, Wang Z M, Cheng Z X, Guo X L, Zhang T, Cai Z L, Kimura H, Matsumoto T, Shibata N, Ikuhara Y 2020 Ceram. Int. 46 20284 Google Scholar
[40]	Cole M W, Ngo E, Hirsch S, Okatan M B, Alpay S P 2008 Appl. Phys. Lett. 92 072906 Google Scholar
[41]	Marksz E J, Hagerstrom A M, Zhang X, Al Hasan N, Pearson J, Drisko J A, Booth J C, Long C J, Takeuchi I, Orloff N D 2021 Phys. Rev. Appl. 15 064061 Google Scholar

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面向宽温域功能器件的连续组分外延铁电薄膜