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Title: Phonon scattering mechanisms dictating the thermal conductivity of lead zirconate titanate (PbZr 1- xTi xO 3) thin films across the compositional phase diagram

Abstract

This paper represents a thorough investigation of the thermal conductivity (κ) in both thin film and bulk PbZr 1–xTi xO 3 (PZT) across the compositional phase diagram. Given the technological importance of PZT as a superb piezoelectric and ferroelectric material in devices and systems impacting a wide array of industries, this research serves to fill the gap in knowledge regarding the thermal properties. The thermal conductivities of both thin film and bulk PZT are found to vary by a considerable margin as a function of composition x. Additionally, we observe a discontinuity in κ in the vicinity of the morphotropic phase boundary (MPB, x = 0.48) where there is a 20%–25% decrease in κ in our thin film data, similar to that found in literature data for bulk PZT. The comparison between bulk and thin film materials highlights the sensitivity of κ to size effects such as film thickness and grain size even in disordered alloy/solid-solution materials. A model for the thermal conductivity of PZT as a function of composition (κ(x)) is presented, which enables the application of the virtual crystal approximation for alloy-type material systems with very different crystals structures, resulting in differing temperature trends for κ. We showmore » that in the case of crystalline solid-solutions where the thermal conductivity of one of the parent materials exhibits glass-like temperature trends the compositional dependence of thermal conductivity is relatively constant for most values of x. Finally, this is in stark contrast with the typical trends of thermal conductivity with x in alloys, where the thermal conductivity increases dramatically as the composition of the alloy or solid-solution approaches that of a pure parent materials (i.e., as x = 0 or 1).« less

Authors:
 [1];  [2];  [2];  [2];  [2]; ORCiD logo [3];  [1];  [2];  [1]
  1. Univ. of Virginia, Charlottesville, VA (United States). Dept. of Mechanical and Aerospace Engineering
  2. Sandia National Lab. (SNL-NM), Albuquerque, NM (United States)
  3. Colorado School of Mines, Golden, CO (United States). Dept. of Metallurgical and Materials Engineering
Publication Date:
Research Org.:
Sandia National Lab. (SNL-NM), Albuquerque, NM (United States); Univ. of Virginia, Charlottesville, VA (United States)
Sponsoring Org.:
USDOE Laboratory Directed Research and Development (LDRD) Program; USDOE National Nuclear Security Administration (NNSA); US Air Force Office of Scientific Research (AFOSR)
Contributing Org.:
Colorado School of Mines, Golden, CO (United States)
OSTI Identifier:
1372309
Report Number(s):
SAND2017-7366J
Journal ID: ISSN 0021-8979; 655303
Grant/Contract Number:
AC04-94AL85000; FA9550-14-1-0067
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Journal of Applied Physics
Additional Journal Information:
Journal Volume: 121; Journal Issue: 20; Journal ID: ISSN 0021-8979
Publisher:
American Institute of Physics (AIP)
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; Thermal conductivity; Lead zirconate titanate; Phonons; Computer modeling; Piezoelectric transducers

Citation Formats

Foley, Brian M., Paisley, Elizabeth A., DiAntonio, Christopher, Chavez, Tom, Blea-Kirby, Mia, Brennecka, Geoff, Gaskins, John T., Ihlefeld, Jon F., and Hopkins, Patrick E. Phonon scattering mechanisms dictating the thermal conductivity of lead zirconate titanate (PbZr1-xTixO3) thin films across the compositional phase diagram. United States: N. p., 2017. Web. doi:10.1063/1.4983356.
Foley, Brian M., Paisley, Elizabeth A., DiAntonio, Christopher, Chavez, Tom, Blea-Kirby, Mia, Brennecka, Geoff, Gaskins, John T., Ihlefeld, Jon F., & Hopkins, Patrick E. Phonon scattering mechanisms dictating the thermal conductivity of lead zirconate titanate (PbZr1-xTixO3) thin films across the compositional phase diagram. United States. doi:10.1063/1.4983356.
Foley, Brian M., Paisley, Elizabeth A., DiAntonio, Christopher, Chavez, Tom, Blea-Kirby, Mia, Brennecka, Geoff, Gaskins, John T., Ihlefeld, Jon F., and Hopkins, Patrick E. Tue . "Phonon scattering mechanisms dictating the thermal conductivity of lead zirconate titanate (PbZr1-xTixO3) thin films across the compositional phase diagram". United States. doi:10.1063/1.4983356.
@article{osti_1372309,
title = {Phonon scattering mechanisms dictating the thermal conductivity of lead zirconate titanate (PbZr1-xTixO3) thin films across the compositional phase diagram},
author = {Foley, Brian M. and Paisley, Elizabeth A. and DiAntonio, Christopher and Chavez, Tom and Blea-Kirby, Mia and Brennecka, Geoff and Gaskins, John T. and Ihlefeld, Jon F. and Hopkins, Patrick E.},
abstractNote = {This paper represents a thorough investigation of the thermal conductivity (κ) in both thin film and bulk PbZr1–xTixO3 (PZT) across the compositional phase diagram. Given the technological importance of PZT as a superb piezoelectric and ferroelectric material in devices and systems impacting a wide array of industries, this research serves to fill the gap in knowledge regarding the thermal properties. The thermal conductivities of both thin film and bulk PZT are found to vary by a considerable margin as a function of composition x. Additionally, we observe a discontinuity in κ in the vicinity of the morphotropic phase boundary (MPB, x = 0.48) where there is a 20%–25% decrease in κ in our thin film data, similar to that found in literature data for bulk PZT. The comparison between bulk and thin film materials highlights the sensitivity of κ to size effects such as film thickness and grain size even in disordered alloy/solid-solution materials. A model for the thermal conductivity of PZT as a function of composition (κ(x)) is presented, which enables the application of the virtual crystal approximation for alloy-type material systems with very different crystals structures, resulting in differing temperature trends for κ. We show that in the case of crystalline solid-solutions where the thermal conductivity of one of the parent materials exhibits glass-like temperature trends the compositional dependence of thermal conductivity is relatively constant for most values of x. Finally, this is in stark contrast with the typical trends of thermal conductivity with x in alloys, where the thermal conductivity increases dramatically as the composition of the alloy or solid-solution approaches that of a pure parent materials (i.e., as x = 0 or 1).},
doi = {10.1063/1.4983356},
journal = {Journal of Applied Physics},
number = 20,
volume = 121,
place = {United States},
year = {Tue May 23 00:00:00 EDT 2017},
month = {Tue May 23 00:00:00 EDT 2017}
}

Journal Article:
Free Publicly Available Full Text
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  • X-ray absorption fine structure (XAFS) experiments were carried out on a series of ferroelectric materials PbZr{sub 1-x}Ti{sub x}O{sub 3} (PZT) (x=0.40,0.47,0.49,0.55) to study the local structure around Ti and Zr atoms in each sample. Based on the fact that PZT has a single phase in the morphotropic phase boundary (MPB) from the x-ray diffraction measurements, both extended XAFS (EXAFS) and x-ray absorption near-edge structure results suggest that at 3 K the orientation of the Ti off-center displacement in these materials changes gradually from the [001] to [111] direction (in pseudocubic notation) as the Ti concentration x decreases from 0.55 tomore » 0.40. This is evidence for a continuous rotation of the local electrical polarization across the MPB region in PZT. The Zr K-edge EXAFS data suggest that at low temperature, the ZrO{sub 6} octahedra in PZT are less distorted than indicated from the average structure for all samples, though a small Zr displacement relative to the O atoms may exist. This possible small Zr displacement is also much less than that found in density functional theory calculations. The ZrO{sub 6} local structure hardly changes with Ti concentration across the MPB region. Finally, the XAFS data also show that the sizes of the ZrO{sub 6} octahedra are larger than that of the TiO{sub 6} octahedra which was also observed by experimental neutron pair distribution function analysis.« less
  • Thin films of highly (100) textured fine-grain (lateral grain size congruent with 0.1 to 0.15 {mu}m) PbZr{sub x}Ti{sub 1-x}O{sub 3} (PZT) (x=0 to 0.7) were grown on conductive perovskite LaNiO{sub 3}-buffered platinized Si substrates by metalorganic chemical vapor deposition. Domain configuration and crystalline orientation were studied using x-ray diffraction and transmission electron microscopy. The predominant domain boundaries of Ti-rich tetragonal-phase PZT and Zr-rich rhombohedral-phase PZT were found to be on the (110) planes and (100) planes, respectively. The equilibrium domain widths were observed and estimated numerically on the basis of transformation strain, grain size, and domain boundary energy. The peakmore » value of the dielectric constant was 790 near the morphotropic boundary. Hysteresis behavior of these PZT thin films was demonstrated. A decrease in coercive field with the increment of Zr content was found; this variation was attributed to domain density and the multiplicity of polarization axes. Furthermore, the low leakage current (J{<=}5x10{sup -7} A/cm{sup 2} at V=4 V) was observed for all samples, and the involvement of several possible conduction mechanisms was suggested. (c) 2000 Materials Research Society.« less
  • Interface-related degradation problems in PbZr[sub x]Ti[sub 1[minus]x]O[sub 3] (PZT) thin- film nonvolatile memories have led to the search for alternate electrode materials to replace the conventional metal electrodes. In this work, the suitability of ceramic electronic conductors [e.g., ruthenium oxide (RuO[sub 2]) and indium-tin-oxide (ITO)] as contact metallization for ferroelectric PbZr[sub x]Ti[sup 1[minus]x]O[sub 3] thin films has been investigated using techniques such as Rutherford backscattering spectrometry, X-ray diffraction, and electron spectroscopy for chemical analysis. Thin films of RuO[sub 2] and ITO were deposited onto Si Substrates by reactive sputtering. Sol-gel derived PZT thin films then were deposited onto the conductingmore » oxides and the samples were annealed at various temperatures between 400 and 700 C. Less intermixing was observed in Si/RuO[sub 2]/PZT films when compared to Si/ITO/PZT under similar processing conditions. The ferroelectric properties of PZT films (hysteresis, fatigue, and low voltage breakdown) on RuO[sub 2] electrodes were compared to those on PT electrodes. PZT films show improved fatigue properties on RuO[sub 2] electrodes. The films on RuO[sub 2] electrodes also showed better current-voltage characteristics (I-V) and time-dependent dielectric breakdown properties (TDDB).« less
  • For the first time, an unambiguous characterization of a sol-gel precursor solution for lead zirconate titanate (PZT) ceramics was carried out. A new lead-zirconium oxoacetatoalkoxide [PbZr[sub 2](O)(OAc)[sub 2](OEt)[sub 6]][sub 2] was crystallized from an ethanol solution of Pb(OAc)[sub 2], Zr(OEt)[sub 4], and Ti(OEt)[sub 4]. In this compound the Zr cations have a heptacoordination geometry instead of the hexacoordination as in the perovskite oxide phase. The chemical heterogeneity in solution may have an important effect on the evolution of phase development during the crystallization of sol-gel derived PZT. 24 refs., 2 figs.
  • No abstract prepared.