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13 May 2002

Volume 80, Issue 19, pp. 3467-3650

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High-piezoelectric behavior of c-axis-oriented lead zirconate titanate thin films with composition near the morphotropic phase boundary

Desheng Fu, Hisao Suzuki, Takeshi Ogawa, and Kenji Ishikawa

Appl. Phys. Lett. 80, 3572 (2002); http://dx.doi.org/10.1063/1.1477619 (3 pages) | Cited 19 times

Online Publication Date: 7 May 2002

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The piezoelectric responses of c-axis-oriented Pb(Zr0.53Ti0.47)O3 (PZT) thin films have been studied by measuring the stress-induced charge with an accurate charge integrator. These measurements reveal that the c-axis-oriented PZT films have high values of d33, which are several times those of ceramic materials. The intrinsic d33 values of poled films are about 680 and 800 pC/N for the c-axis-oriented films on Si and MgO single-crystal substrates, respectively. It shows that the thin-film deposition technique opens an approach for exploring the potential superior properties of PZT near the morphotropic phase boundary. © 2002 American Institute of Physics.
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77.65.Bn Piezoelectric and electrostrictive constants
77.55.-g Dielectric thin films
77.84.Ek Niobates and tantalates
77.84.Cg PZT ceramics and other titanates
81.15.Lm Liquid phase epitaxy; deposition from liquid phases (melts, solutions, and surface layers on liquids)
77.80.B- Phase transitions and Curie point
68.55.-a Thin film structure and morphology
77.22.Ej Polarization and depolarization

Water absorption and interface reactivity of yttrium oxide gate dielectrics on silicon

D. Niu, R. W. Ashcraft, and G. N. Parsons

Appl. Phys. Lett. 80, 3575 (2002); http://dx.doi.org/10.1063/1.1477268 (3 pages) | Cited 28 times

Online Publication Date: 7 May 2002

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High dielectric constant insulators deposited at low temperatures rapidly absorb water during exposure to the atmosphere, and the resulting OH leads to detrimental interface reactions. We report the effect of atmospheric exposure on ultrathin yttrium oxide, and details of silicon substrate reactions during postdeposition anneals. Infrared absorption analysis indicates significant absorption of water vapor during atmospheric exposure, even for very short times (<15 min). X-ray photoelectron spectroscopy demonstrates that after OH absorption, a thermally activated interface reaction proceeds with an activation energy of 0.33 eV, consistent with substrate reaction with OH present in the film. The OH absorption rate is reduced for annealed films or when capping layers are deposited in situ. Similar oxidation processes are expected to occur in other high-k materials of interest, where the rate of OH absorption will depend on the deposition process and material thermal history. © 2002 American Institute of Physics.
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82.65.+r Surface and interface chemistry; heterogeneous catalysis at surfaces
77.84.Bw Elements, oxides, nitrides, borides, carbides, chalcogenides, etc.
81.65.Mq Oxidation
77.55.-g Dielectric thin films
78.30.Hv Other nonmetallic inorganics
79.60.Dp Adsorbed layers and thin films
79.60.Jv Interfaces; heterostructures; nanostructures
68.35.-p Solid surfaces and solid-solid interfaces: structure and energetics

Enhanced dielectric properties of low-temperature sintered SrBi2Nb2O9/Ag composites

Can Wang, Q. F. Fang, and Z. G. Zhu

Appl. Phys. Lett. 80, 3578 (2002); http://dx.doi.org/10.1063/1.1477616 (3 pages) | Cited 13 times

Online Publication Date: 7 May 2002

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Strontium bismuth niobate (SBN) matrix composites containing Ag particles were prepared by the conventional solid-state reaction method. With the addition of Ag particles to the SBN matrix, the single-phase layered perovskite structure of the matrix was preserved and the sintering temperature of the system was lowered about 200 °C compared with monolithic SBN. The SBN/Ag composites showed a significant increase of the dielectric constant and the loss tangent of SBN/Ag composites decreased in certain Ag content. With increasing Ag content, a gradual increase of the dielectric constant was observed in the temperature range from room temperature to 600 °C. The Curie temperature was found to decrease from 439 °C for the monolithic SBN to 435 °C for the composite with 3.5 vol % Ag, and then with increasing Ag content, the Curie temperature gradually increased to 445 °C for the composite with 14 vol % Ag. The results show that the SBN/Ag composites have enhanced dielectric properties and an improved processing condition, which could be further exploited in capacitor applications. © 2002 American Institute of Physics.
Show PACS
77.84.Ek Niobates and tantalates
77.84.Cg PZT ceramics and other titanates
77.22.Ch Permittivity (dielectric function)
77.22.Gm Dielectric loss and relaxation
77.80.B- Phase transitions and Curie point
81.05.Je Ceramics and refractories (including borides, carbides, hydrides, nitrides, oxides, and silicides)

Large nonlinear dielectric properties of artificial BaTiO3/SrTiO3 superlattices

Juho Kim, Youngnam Kim, Young Sung Kim, Jaichan Lee, Leejun Kim, and Donggeun Jung

Appl. Phys. Lett. 80, 3581 (2002); http://dx.doi.org/10.1063/1.1477934 (3 pages) | Cited 75 times

Online Publication Date: 7 May 2002

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BaTiO3(BTO)/SrTiO3(STO) artificial superlattices have been made on MgO (100) substrates. The periodicity of the BTO/STO layers in the superlattice was varied from one-unit cell to 125-unit cell thickness. The dielectric constant and its nonlinearity (or voltage tunability) showed similar behavior as the periodicity was varied. The voltage tunability of the superlattice increased with decreasing stacking periodicity of the BTO/STO within the critical thickness. Similarly, the lattice distortion, i.e., the ratio of the lattice parameter along surface normal to parallel, of the BTO and STO layers increased with decreasing the periodicity. Remarkable enhancement of the voltage tunability has been achieved. The superlattice exhibited large voltage tunability (94%, the highest value to date) at the periodicity of BTO2-unit cell/STO2-unit cell at which the maximum lattice distortion of each layer was obtained. This suggests that the nonlinear dielectric property of the superlattice is closely related with the lattice distortion of the individual layers. © 2002 American Institute of Physics.
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77.55.-g Dielectric thin films
68.65.Cd Superlattices
77.84.Ek Niobates and tantalates
77.84.Cg PZT ceramics and other titanates
77.80.-e Ferroelectricity and antiferroelectricity
77.22.Ch Permittivity (dielectric function)
77.22.Ej Polarization and depolarization

Evolution of Rayleigh constant in fatigued lead zirconate titanate capacitors

J. L. Sun, J. Chen, X. J. Meng, J. Yu, L. X. Bo, S. L. Guo, and J. H. Chu

Appl. Phys. Lett. 80, 3584 (2002); http://dx.doi.org/10.1063/1.1478781 (3 pages) | Cited 7 times

Online Publication Date: 7 May 2002

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The capacitance of Pt/PbZr0.5Ti0.5O3/Pt capacitors versus the strength of applied ac electric field E has been measured for samples that fatigued at different square pulse switching cycles. Based on the in-series capacitor model, the variation of interface capacitance and bulk ferroelectric capacitance at different stages of fatigue were treated separately. A simplified method was derived to calculate the initial dielectric constant and Rayleigh constant for the bulk ferroelectric film from the ac electric field dependence of the sample capacitance. It was found that the initial dielectric constant and Rayleigh constant for the bulk ferroelectric film changed a little when the number of cycles is less than 3×106, whereas it decreased remarkably when the number of cycles is greater than 3×106. The suppression of polarization was attributed to pinning of the domain walls at the electrode/ferroelectric interface. © 2002 American Institute of Physics.
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77.22.Ch Permittivity (dielectric function)
84.32.Tt Capacitors
77.84.Ek Niobates and tantalates
77.84.Cg PZT ceramics and other titanates
81.05.Je Ceramics and refractories (including borides, carbides, hydrides, nitrides, oxides, and silicides)
77.80.Dj Domain structure; hysteresis
85.50.-n Dielectric, ferroelectric, and piezoelectric devices
77.55.-g Dielectric thin films

Water-induced degradation in lead zirconate titanate piezoelectric ceramics

W. P. Chen, H. L. W. Chan, F. C. H. Yiu, K. M. W. Ng, and P. C. K. Liu

Appl. Phys. Lett. 80, 3587 (2002); http://dx.doi.org/10.1063/1.1479205 (3 pages) | Cited 17 times

Online Publication Date: 7 May 2002

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Water-induced degradation in lead zirconate titanate (PZT) piezoelectric ceramics was studied by a comparison experiment. In one treatment, PZT rings were immersed in a 0.01 M NaOH solution for long periods of time; in the other treatment, PZT rings were placed in a 0.01 M NaOH solution and hydrogen was evolved onto their silver electrodes by the electrolysis of water. No degradation occurred to samples immersed in the NaOH solution; but for the samples that were also treated by electrolysis of water, serious degradation occurred as their mechanical quality factor decreased dramatically and their dielectric loss increased considerably. I–V measurement showed that the resistance decreased greatly in the degraded samples, which could be explained by the formation of charge carriers due to the reduction reaction of atomic hydrogen from the electrolysis of water. It was proposed that the reduction reaction of atomic hydrogen at ambient temperature is an important origin for the degradation of piezoelectric ceramic devices. © 2002 American Institute of Physics.
Show PACS
77.84.Ek Niobates and tantalates
77.84.Cg PZT ceramics and other titanates
81.65.-b Surface treatments
81.05.Je Ceramics and refractories (including borides, carbides, hydrides, nitrides, oxides, and silicides)
77.65.-j Piezoelectricity and electromechanical effects
77.22.Gm Dielectric loss and relaxation
77.22.Ej Polarization and depolarization

Raman characterization of boron carbonitride nanotubes

C. Y. Zhi, X. D. Bai, and E. G. Wang

Appl. Phys. Lett. 80, 3590 (2002); http://dx.doi.org/10.1063/1.1479207 (3 pages) | Cited 27 times

Online Publication Date: 7 May 2002

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A systematic Raman study of boron carbonitride (BCN) nanotubes, synthesized by bias-assisted hot filament chemical vapor deposition, is reported. Raman spectra up to the fourth order are observed from the BCN nanotubes. Comparing with pure carbon nanotubes, the Raman bands in BCN nanotubes are broadened and the relative intensity of the D mode with respect to the G mode varies with increasing B and N atomic concentrations. The underlying mechanism has been studied on the basis of the microstructures obtained by high-resolution transmission electron microscopy. © 2002 American Institute of Physics.
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61.46.-w Structure of nanoscale materials
78.67.Ch Nanotubes
78.30.Na Fullerenes and related materials
81.15.Gh Chemical vapor deposition (including plasma-enhanced CVD, MOCVD, ALD, etc.)

Correlation between internal stress and ferroelectric fatigue in Bi4−xLaxTi3O12 thin films

Jung-Kun Lee, Chang-Hoon Kim, Hee-Sang Suh, and Kug-Sun Hong

Appl. Phys. Lett. 80, 3593 (2002); http://dx.doi.org/10.1063/1.1477272 (3 pages) | Cited 62 times

Online Publication Date: 7 May 2002

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La-substituted bismuth titanate [Bi4−xLaxTi3O12(BLT)] films were synthesized using pulsed-laser deposition and ferroelectric fatigue phenomenon was investigated. The internal strain present in the films, which was analyzed through the evaluation of the x-ray diffraction peak, was partially responsible for the fatigue in BLT films. When x ≥ 0.75, the change in the internal strain was saturated and there was no significant degradation of switching charge, at least up to 1010 cycles. It revealed that the internal strain, as well as chemical stability of oxygen ions, contributed to the ferroelectric fatigue of the BLT films. The origin of the internal strain is discussed in terms of the lattice mismatch between bulk materials and thin films. © 2002 American Institute of Physics.
Show PACS
77.55.-g Dielectric thin films
77.84.Ek Niobates and tantalates
77.84.Cg PZT ceramics and other titanates
68.60.Bs Mechanical and acoustical properties
77.22.Ej Polarization and depolarization
77.80.-e Ferroelectricity and antiferroelectricity

Sensitivity in extracting static dielectric constants from multiple film stacks

A. H. Mueller, N. A. Suvorova, and E. A. Irene

Appl. Phys. Lett. 80, 3596 (2002); http://dx.doi.org/10.1063/1.1478159 (3 pages) | Cited 1 time

Online Publication Date: 7 May 2002

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This study points out that there is a hyperbolic relationship between the static dielectric constants (Ks) in a dielectric film stack. It is shown using experimental data that this relationship renders K values that are extracted from capacitance–voltage measurements very sensitive to the other input values such as dielectric constants and film thicknesses. Errors as large as 100% and larger can be made in K from small changes in the input parameters. Thus there is a requirement for accurate film thicknesses and a specific knowledge of the nature of interface film(s) and dielectric properties are necessary for accurate K determinations. © 2002 American Institute of Physics.
Show PACS
77.55.-g Dielectric thin films
77.22.Ch Permittivity (dielectric function)
77.84.-s Dielectric, piezoelectric, ferroelectric, and antiferroelectric materials

Low-temperature integration of lead-based ferroelectric capacitors on Si with diffusion barrier layer

B. T. Liu, K. Maki, S. Aggarwal, B. Nagaraj, V. Nagarajan, L. Salamanca-Riba, R. Ramesh, A. M. Dhote, and O. Auciello

Appl. Phys. Lett. 80, 3599 (2002); http://dx.doi.org/10.1063/1.1477281 (3 pages) | Cited 20 times

Online Publication Date: 7 May 2002

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Ferroelectric lead zirconate titanate thin films have been integrated on silicon substrates using Ti–Al-based conducting diffusion barriers produced by sputter deposition. The microstructure of the Ti–Al barrier layer was systematically altered through changes in the sputtering conditions, specifically the power density and deposition pressure. We find that the crystallinity of the Ti–Al film strongly correlates with sputtering power density and ambient i.e., it is amorphous at low power density and/or high deposition pressure, and polycrystalline at high power density and/or low deposition pressure. Electron energy loss spectroscopy studies demonstrate that the amorphous Ti–Al (a-Ti–Al) films contain a higher concentration of dissolved oxygen than crystalline Ti–Al. A low temperature sol–gel process has been used to prepare Pb(Zr,Ti)O3 PZT films at 450 °C on conducting Si wafers with a-Ti–Al conducting barrier layer and La–Sr–Co–O top and bottom electrodes. The excellent ferroelectric properties obtained with the a-Ti–Al barrier provide a promising approach for integration of PZT-based capacitors with silicon transistor technology for the fabrication of nonvolatile ferroelectric memories. © 2002 American Institute of Physics.
Show PACS
77.84.Ek Niobates and tantalates
77.84.Cg PZT ceramics and other titanates
84.32.Tt Capacitors
85.50.Gk Non-volatile ferroelectric memories
77.55.-g Dielectric thin films
77.80.-e Ferroelectricity and antiferroelectricity
81.15.Cd Deposition by sputtering
85.40.-e Microelectronics: LSI, VLSI, ULSI; integrated circuit fabrication technology
81.10.Dn Growth from solutions
81.10.Fq Growth from melts; zone melting and refining
81.15.Lm Liquid phase epitaxy; deposition from liquid phases (melts, solutions, and surface layers on liquids)
79.20.Uv Electron energy loss spectroscopy
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