journal article·2021-05-06Open access

Achieving a high dielectric tunability in strain-engineered tetragonal K0.5Na0.5NbO3 films

Lanxia Hao, Yali Yang, Yu Huan, Hongbo Cheng, Yu-Yao Zhao, Yingying Wang, Jing Yan, Wei Ren, Jun Ouyang

npj Computational Materials· Volume 7· Issue 1

Abstract

Abstract Using a modified Landau-Devonshire type thermodynamic potential, we show that dielectric tunability η of a tetragonal ferroelectric film can be analytically solved. At a given electric field E, η is a function of the remnant polarization ($$P_0^f$$) and the small-field relative dielectric permittivity ($$\chi _0^f$$), which are commonly measured material properties. After a survey of materials, a large η~80% is predicted to be achievable in a (001)-oriented tetragonal (K0.5,Na0.5)NbO3 film. This strain-stabilized tetragonal phase is verified by density functional theory (DFT) calculations. (K0.5,Na0.5)NbO3 films based on this design were successfully prepared via a sputtering deposition process on SrRuO3-buffered (100)SrTiO3 substrates. The resulted epitaxial films showed a sizable $$P_0^f$$ (~0.21C m−2) and a large $$\chi _0^f$$ (~830–860), as well as a large η close to the theoretical value. The measured dielectric tunabilities as functions of E are well described by the theoretical η(E) curves, validating our integrated approach rooted in a theoretical understanding.
Source: crossref · Quality: candidate unverified · Source record ↗

Research context

OpenAlex topics: Ferroelectric and Piezoelectric Materials · Multiferroics and related materials · Dielectric properties of ceramics

SciVX discovery tags are terminology-based. OpenAlex topics are source-provided classifications.

References (64)

Show source-provided references
1. Cole, M. W., Nothwang, W. D., Hubbard, C., Ngo, E. & Ervin, M. Low dielectric loss and enhanced tunability of Ba0.6Sr0.4TiO3 based thin films via material compositional design and optimized film processing methods. J. Appl. Phys. 93, 9218–9225 (2003).10.1063/1.1569392 ↗
2. Tagantsev, A. K., Sherman, V. O., Astafiev, K. F., Venkatesh, J. & Setter, N. Ferroelectric materials for microwave tunable applications. J. Electroceram. 11, 5–66 (2003).10.1023/B:JECR.0000015661.81386.e6 ↗
3. Bao, P., Jackson, T. J., Wang, X. & Lancaster, M. J. Barium strontium titanate thin film varactors for room-temperature microwave device applications. J. Phys. D: Appl. Phys. 41, 63001 (2008).10.1088/0022-3727/41/6/063001 ↗
4. Zhao, J. et al. Effects of Bi2O3, Sm2O3 content on the structure, dielectric properties and dielectric tunability of BaTiO3 ceramics. J. Mater. Sci: Mater. Electron. 30, 19279–19288 (2019).
5. Everhardt, A. S. et al. Temperature-independent giant dielectric response in transitional BaTiO3 thin films. Appl. Phys. Rev. 7, 011402 (2020).10.1063/1.5122954 ↗
6. Zhang, W., Hu, F., Zhang, H. & Ouyang, J. Investigation of the electrical properties of RF sputtered BaTiO3 films grown on various substrates. Mater. Res. Bull. 95, 23–29 (2017).10.1016/j.materresbull.2017.07.012 ↗
7. Aymen, S., Mascot, M., Jomni, F. & Carru, J. High tunability in lead-free Ba0.85Sr0.15TiO3 thick films for microwave tunable applications. Ceram. Int. 45, 23084–23088 (2019).10.1016/j.ceramint.2019.07.357 ↗
8. Wang, F. & Ma, W. Phase stability and dielectric properties of (011) epitaxial (Ba0.6Sr0.4)TiO3 films. J. Appl. Phys. 125, 082528 (2019).10.1063/1.5054139 ↗
9. Yuan, Z. et al. Large dielectric tunability and microwave properties of Mn-doped (Ba,Sr)TiO3 thin films. Appl. Phys. Lett. 87, 152901 (2005).10.1063/1.2089181 ↗
10. Wu, M., Li, X., Yu, S., Sun, Y. & Dong, H. Dielectric properties of the bulk and interfacial layers in ferroelectric BaZr0.2Ti0.8O3 thin films. Ceram. Int. 45, 10917–10923 (2019).10.1016/j.ceramint.2019.02.171 ↗
11. Zhong, S. et al. Highly tunable and temperature insensitive multilayer barium strontium titanate films. Appl. Phys. Lett. 90, 092901 (2007).10.1063/1.2710005 ↗
12. Cole, M. W., Ngo, E., Hirsch, S., Okatan, M. B. & Alpay, S. P. Dielectric properties of MgO-doped compositionally graded multilayer barium strontium titanate films. Appl. Phys. Lett. 92, 072906 (2008).10.1063/1.2870079 ↗
13. Garten, L. M. & Trolier-McKinstry, S. The field induced e31,f piezoelectric and Rayleigh response in barium strontium titanate thin films. Appl. Phys. Lett. 105, 132905 (2014).10.1063/1.4897299 ↗
14. Tang, X. G., Chew, K. H. & Chan, H. L. W. Diffuse phase transition and dielectric tunability of Ba(ZryTi1−y)O3 relaxor ferroelectric ceramics. Acta Mater. 52, 5177–5183 (2004).10.1016/j.actamat.2004.07.028 ↗
15. Mahmoud, A. E., Afify, A. S. & Parashar, S. K. S. Dielectric, tunability, leakage current, and ferroelectric properties of (K0.45Na0.55)0.95Li0.05NbO3 lead free piezoelectric. J. Mater. Sci: Mater. Electron. 30, 2659–2668 (2019).
16. Yu, Z., Ang, C., Guo, R. & Bhalla, A. S. Dielectric properties and high tunability of Ba(Ti0.7Zr0.3)O3 ceramics under dc electric field. Appl. Phys. Lett. 81, 1285–1287 (2002).10.1063/1.1498496 ↗
17. Blomqvist, M., Koh, J., Khartsev, S., Grishin, A. & Andréasson, J. High-performance epitaxial Na0.5K0.5NbO3 thin films by magnetron sputtering. Appl. Phys. Lett. 81, 337–339 (2002).10.1063/1.1492854 ↗
18. Li, T., Wang, G., Li, K., Du, G. & Chen, Y. Electrical properties of lead-free KNN films on SRO/STO by RF magnetron sputtering. Ceram. Int. 40, 1195–1198 (2014).10.1016/j.ceramint.2013.07.005 ↗
19. Li, T., Wang, G., Remiens, D. & Dong, X. Characteristics of highly (001) oriented (K,Na)NbO3 films grown on LaNiO3 bottom electrodes by RF magnetron sputtering. Ceram. Int. 39, 1359–1363 (2013).10.1016/j.ceramint.2012.07.074 ↗
20. Ren, P. et al. Large nonlinear dielectric behavior in BaTi1−xSnxO3. Sci. Rep. 7, 6693 (2017).10.1038/s41598-017-07192-x ↗
21. Peng, B., Fan, H., Li, Q. & Zhang, Q. Dielectric tunability properties of the Pb[(Mg1/3Nb2/3)1−xZrx]O3 ceramics. J. Alloy. Compd. 549, 283–287 (2013).10.1016/j.jallcom.2012.09.001 ↗
22. Fujii, I. et al. Fabrication of (K,Na)NbO3 films on SrRuO3/(001)SrTiO3 substrates by pulsed laser deposition. Jpn. J. Appl. Phys. 54, 10NA13 (2015).10.7567/JJAP.54.10NA13 ↗
23. Fujii, I., Yamauchi, T., Imai, T., Adachi, H. & Wada, T. Ferroelectric properties of (Li,K,Na)NbO3 epitaxial films fabricated by pulsed laser deposition. Jpn. J. Appl. Phys. 53, 09PA09 (2014).10.7567/JJAP.53.09PA09 ↗
24. Ito, Y. et al. Growth of epitaxial (K,Na)NbO3 films with various orientations by hydrothermal method and their properties. Jpn. J. Appl. Phys. 58, SLLB14 (2019).10.7567/1347-4065/ab3958 ↗
25. Khartsev, S., Grishin, A., Andrèasson, J., Koh, J. & Song, J. Comparative characteristics of Na0.5K0.5NbO3 films on Pt by pulsed laser deposition and magnetron sputtering. Integr. Ferroelectr. 55, 769–779 (2010).
26. Chen, L., Nagarajan, V., Ramesh, R. & Roytburd, A. L. Nonlinear electric field dependence of piezoresponse in epitaxial ferroelectric lead zirconate titanate thin films. J. Appl. Phys. 94, 5147–5152 (2003).10.1063/1.1610242 ↗
27. Li, T. et al. Influence of LNO top electrodes on electrical properties of KNN/LNO thin films prepared by RF magnetron sputtering. J. Am. Ceram. Soc. 96, 787–790 (2012).10.1111/jace.12047 ↗
28. Li, G. et al. Effects of excess amount of K and Na on properties of (K0.48Na0.52)NbO3 thin films. Ceram. Int. 38, S279–S281 (2012).10.1016/j.ceramint.2011.04.101 ↗
29. Bell, A. J. Phenomenologically derived electric field-temperature phase diagrams and piezoelectric coefficients for single crystal barium titanate under fields along different axes. J. Appl. Phys. 89, 3907–3914 (2001).10.1063/1.1352682 ↗
30. Huang, Y. H. et al. Thermodynamic and phase-field studies of phase transitions, domain structures, and switching for Ba(ZrxTi1−x)O3 solid solutions. Acta Mater. 186, 609–615 (2020).10.1016/j.actamat.2020.01.019 ↗
31. Jiang, Q. & Qiu, J. H. The thickness dependence of ferroelectric and magnetic properties in epitaxial BiFeO3 thin films. J. Appl. Phys. 99, 103901 (2006).10.1063/1.2196238 ↗
32. Winchester, B., Wu, P. & Chen, L. Q. Phase-field simulation of domain structures in epitaxial BiFeO3 films on vicinal substrates. Appl. Phys. Lett. 99, 052903 (2011).10.1063/1.3605674 ↗
33. Zhang, J. X. et al. Computer simulation of ferroelectric domain structures in epitaxial BiFeO3 thin films. J. Appl. Phys. 103, 094111 (2008).10.1063/1.2927385 ↗
34. Mtebwa, M., Tagantsev, A. K. & Setter, N. Effect of elastic compliances and higher order Landau coefficients on the phase diagram of single domain epitaxial Pb(Zr,Ti)O3 (PZT) thin films. Aip Adv. 4, 127150 (2014).10.1063/1.4905265 ↗
35. Zhou, M., Wang, J., Chen, L. & Nan, C. Strain, temperature, and electric-field effects on the phase transition and piezoelectric responses of K0.5Na0.5NbO3 thin films. J. Appl. Phys. 123, 154106 (2018).10.1063/1.5027505 ↗
36. Zhao, X., Wang, J. & Chen, L. A thermodynamic study of phase transitions and electrocaloric properties of K0.5Na0.5NbO3 single crystals. Appl. Phys. Lett. 116, 092902 (2020).10.1063/1.5144056 ↗
37. Liu, D., Bai, G. & Gao, C. Phase diagrams classification based on machine learning and phenomenological investigation of physical properties in K1− xNaxNbO3 thin films. J. Appl. Phys. 127, 154101 (2020).10.1063/5.0004167 ↗
38. Wang, J. J., Wu, P. P., Ma, X. Q. & Chen, L. Q. Temperature-pressure phase diagram and ferroelectric properties of BaTiO3 single crystal based on a modified Landau potential. J. Appl. Phys. 108, 114105 (2010).10.1063/1.3504194 ↗
39. Qiu, J. H., Zhao, T. X., Chen, Z. H., Yuan, N. Y. & Ding, J. N. Orientation dependence of phase diagrams and physical properties in epitaxial Ba0.6Sr0.4TiO3 films. Solid. State Commun. 272, 57–62 (2018).10.1016/j.ssc.2018.01.015 ↗
40. Peng, J. et al. A thermodynamic potential for barium zirconate titanate solid solutions. Npj. Comput. Mater. 4, 1–9 (2018).10.1038/s41524-018-0126-3 ↗
41. Li, H. et al. Dependence of dielectric properties on internal stresses in epitaxial barium strontium titanate thin films. Appl. Phys. Lett. 78, 2354–2356 (2001).10.1063/1.1359141 ↗
42. Kim, D. H., Lee, H. N., Biegalski, M. D. & Christen, H. M. Effect of epitaxial strain on ferroelectric polarization in multiferroic BiFeO3 films. Appl. Phys. Lett. 92, 012911 (2008).10.1063/1.2830799 ↗
43. Luo, J. et al. Domain evolution and piezoelectric response across thermotropic phase boundary in (K,Na)NbO3-based epitaxial thin films. ACS Appl. Mater. Inter. 9, 13315–13322 (2017).10.1021/acsami.7b02263 ↗
44. Luo, J. et al. Monoclinic (K,Na)NbO3 ferroelectric phase in epitaxial films. Adv. Electron. Mater. 3, 1700226 (2017).10.1002/aelm.201700226 ↗
45. von Helden, L. et al. Huge impact of compressive strain on phase transition temperatures in epitaxial ferroelectric KxNa1−xNbO3 thin films. Appl. Phys. Lett. 114, 232905 (2019).10.1063/1.5094405 ↗
46. Shiraishi, T. et al. Structural and electrical characterization of hydrothermally deposited piezoelectric (K,Na)(Nb,Ta)O3 thick films. J. Mater. Sci. 55, 8829–8842 (2020).10.1007/s10853-020-04663-x ↗
47. Blochl, P. E. Projector augmented-wave method. Phys. Rev. B: Condens Matter 50, 17953–17979 (1994).10.1103/PhysRevB.50.17953 ↗
48. Kresse, G. & Joubert, D. From ultrasoft pseudopotentials to the projector augmented-wave method. Phys. Rev. B 59, 1758–1775 (1999).10.1103/PhysRevB.59.1758 ↗
49. Perdew, J. P., Burke, K. & Ernzerhof, M. Generalized gradient approximation made simple. Phys. Rev. Lett. 77, 3865–3868 (1996).10.1103/PhysRevLett.77.3865 ↗
50. Wang, K. & Li, J. F. Analysis of crystallographic evolution in (Na,K)NbO3-based lead-free piezoceramics by x-ray diffraction. Appl. Phys. Lett. 91, 262902 (2007).10.1063/1.2825280 ↗
51. Yu, Q., Zhu, F., Cheng, L., Wang, K. & Li, J. Determination of crystallographic orientation of lead-free piezoelectric (K,Na)NbO3 epitaxial thin films grown on SrTiO3(100) surfaces. Appl. Phys. Lett. 104, 102902 (2014).10.1063/1.4868431 ↗
52. Akmal, M. H. M., MWarikh, A. R. & Ralib, A. A. M. Vibrational piezoelectric energy harvester’s performance using PZT vs KNN. Mater. Res. Express 6, 115708 (2019).10.1088/2053-1591/ab492e ↗
53. Wang, L., Ren, W., Shi, P. & Wu, X. Cobalt doping effects on structures and electrical properties of lead-free ferroelectric K0.5Na0.5NbO3 films. J. Alloy. Compd. 608, 202–206 (2014).10.1016/j.jallcom.2014.04.118 ↗
54. Wang, L., Ren, W., Shi, P. & Wu, X. Structures, electrical properties, and leakage current behaviors of un-doped and Mn-doped lead-free ferroelectric K0.5Na0.5NbO3 films. J. Appl. Phys. 115, 034103 (2014).10.1063/1.4861415 ↗
55. Wang, L., Yao, K., Goh, P. C. & Ren, W. Volatilization of alkali ions and effects of molecular weight of polyvinylpyrrolidone introduced in solution-derived ferroelectric K0.5Na0.5NbO3 films. J. Mater. Res. 24, 3516–3522 (2009).10.1557/jmr.2009.0433 ↗
56. Wang, L. et al. Effect of pyrolysis temperature on K0.5Na0.5NbO3 thick films derived from polyvinylpyrrolidone-modified chemical solution. J. Am. Ceram. Soc. 93, 3686–3690 (2010).10.1111/j.1551-2916.2010.03965.x ↗
57. Xu, L. et al. Fabrication of the transparent ferroelectric heterostructures based on KNN-based lead-free films. J. Phys. D: Appl. Phys. 53, 415301 (2020).10.1088/1361-6463/ab9976 ↗
58. Zhang, Y. et al. Strain engineered CaBi2Nb2O9 thin films with enhanced electrical properties. Acs Appl. Mater. Inter. 8, 16744–16751 (2016).10.1021/acsami.6b00298 ↗
59. Niu, M. et al. Integration-friendly, chemically stoichiometric BiFeO3 films with a piezoelectric performance challenging that of PZT. Acs Appl. Mater. Inter. 12, 33899–33907 (2020).10.1021/acsami.0c07155 ↗
60. Kizaki, Y., Noguchi, Y. & Miyayama, M. Defect control for low leakage current in K0.5Na0.5NbO3 single crystals. Appl. Phys. Lett. 89, 142910 (2006).10.1063/1.2357859 ↗
61. Wang, L. et al. Enhanced ferroelectric properties in Mn-doped K0.5Na0.5NbO3 thin films derived from chemical solution deposition. Appl. Phys. Lett. 97, 072902 (2010).10.1063/1.3479530 ↗
62. Zhang, W. et al. Space-charge dominated epitaxial BaTiO3 heterostructures. Acta Mater. 85, 207–215 (2015).10.1016/j.actamat.2014.10.063 ↗
63. Wang, X. et al. Growth and field dependent dielectric properties of epitaxial Na0.5K0.5NbO3 thin films. Appl. Phys. Lett. 73, 927–929 (1998).10.1063/1.122040 ↗
64. Huan, Y., Wang, X. & Li, L. Displacement of Ta-O bonds near polymorphic phase transition in Li-, Ta-, and Sb-modified (K, Na)NbO3 ceramics. Appl. Phys. Lett. 104, 242905 (2014).10.1063/1.4884381 ↗