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

doi:10.15541/jim20210437

Abstract

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

CLC Number:

TQ174

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.

Figures/Tables 4

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)

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

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

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

References 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

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

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