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Applied Physics Reviews / Volume 2012 / APPLIED PHYSICS REVIEWS

J. Appl. Phys. 111, 031301 (2012); http://dx.doi.org/10.1063/1.3679521 (50 pages)

High performance ferroelectric relaxor-PbTiO3 single crystals: Status and perspective

Shujun Zhang1 and Fei Li1,2

1Materials Research Institute, Pennsylvania State University, University Park, Pennsylvania 16802, USA
2Electronic Materials Research Laboratory and International Center for Dielectric Research, Xi’an Jiaotong University, Xi’an 710049, China

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(Received 7 October 2011; accepted 4 January 2012; published online 7 February 2012)

Ferroelectrics are essential components in a wide range of applications, including ultrasonic transducers, sensors, and actuators. In the single crystal form, relaxor-PbTiO3 (PT) piezoelectric materials have been extensively studied due to their ultrahigh piezoelectric and electromechanical properties. In this article, a perspective and future development of relaxor-PT crystals are given. Initially, various techniques for the growth of relaxor-PT crystals are reviewed, with crystals up to 100 mm in diameter and 200 mm in length being readily achievable using the Bridgman technique. Second, the characterizations of dielectric and electromechanical properties are surveyed. Boundary conditions, including temperature, electric field, and stress, are discussed in relation to device limitations. Third, the physical origins of the high piezoelectric properties and unique loss characteristics in relaxor-PT crystals are discussed with respect to their crystal structure, phase, engineered domain configuration, macrosymmetry, and domain size. Finally, relaxor-PT single crystals are reviewed with respect to specific applications and contrasted to conventional piezoelectric ceramics.

© 2012 American Institute of Physics

Article Outline

  1. INTRODUCTION AND BACKGROUND
    1. Introduction
    2. Background on piezoelectricity and ferroelectricity
      1. Piezoelectricity and related parameters
        1. Dielectric permittivity
        2. Piezoelectric coefficients
        3. Frequency constant and elastic constant
        4. Acoustic impedance
        5. Electromechanical coupling
        6. Mechanical quality factor
      2. Ferroelectricity and related phenomena
        1. Ferroelectric domains and domain walls
        2. Ferroelectric hysteresis loop
        3. Polymorphotropic phase transitions and morphotropic phase boundary (MPB)
        4. Domain engineering
        5. Aging behavior and piezoelectric nonlinearity
    3. Background on pervoskite ferroelectric materials
      1. History of pervoskite ferroelectric ceramics
      2. Relaxor-PT single crystals
  2. SINGLE CRYSTAL GROWTH: ISSUES AND FUTURE DIRECTION
    1. High temperature solution growth
      1. Conventional flux method
      2. Flux Bridgman
    2. Modified Bridgman
    3. Solid state conversion
  3. STRUCTURE AND PROPERTY CHARACTERIZATIONS
    1. Crystal phase determination
      1. Microscopic characterization
      2. Macroscopic characterization
        1. [111] poled relaxor-PT crystals
        2. [011] poled relaxor-PT crystals
        3. [001] poled relaxor-PT crystals
    2. Dielectric and piezoelectric measurements
    3. Loss determination
      1. Hysteresis loop measurements
      2. Impedance spectrum measurements
    4. Determination of full matrix material constants
    5. Piezoelectric properties as function of orientation and composition
      1. Orientation dependent properties
      2. Composition dependent properties
    6. Pyroelectric and electro-optic properties
  4. ORIGIN OF PIEZOELECTRIC RESPONSE AND LOSSES
    1. Piezoelectric properties
      1. Electric field induced phase transitions
      2. Polarization rotation mechanism
        1. “Polarization rotation” vs “domain wall motion”
      3. High shear piezoelectric response and MPB
      4. The role of a monoclinic phase
      5. The role of relaxor end member
      6. Critical factors for high piezoelectricity
    2. Loss in relaxor-PT crystals
      1. Internal bias and domain wall motion
      2. Polarization rotation
      3. Polarization rotation angle
      4. Morphotropic phase boundary
      5. Losses under high ac drive field
  5. PROPERTIES UNDER EXTERNAL BOUNDARY CONDITIONS
    1. Temperature dependence
    2. Uniaxial stress and dc bias field effects
      1. Stress/electric field induced phase transitions
      2. Piezoelectric properties as a function of dc bias and uniaxial stress
        1. dc bias field
        2. Uniaxial stress
        3. Temperature usage range under dc bias
    3. Hydrostatic pressure
    4. Relaxor-PT crystals under high drive field
      1. Dielectric and piezoelectric properties under high drive field
      2. Field stability of the shear properties
      3. Fatigue behavior
  6. APPLICATIONS
    1. Ultrasound transducers
      1. Medical ultrasonic transducers
      2. Underwater acoustic transducers
    2. Sensors
      1. Hydrophones
      2. Accelerometers
    3. Actuators
      1. Stack/in-plane actuators
      2. Flextensional actuators
      3. Ultrasonic motors (Resonant actuators)
  7. SUMMARY AND FUTURE PERSPECTIVE
    1. Summary
    2. Future perspectives

RELATED DATABASES

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KEYWORDS, PACS, and IPC

Keywords

crystal growth from melt, crystal structure, dielectric losses, electric domains, lead compounds, piezoelectric materials, relaxor ferroelectrics

PACS

  • 77.65.-j

    Piezoelectricity and electromechanical effects

  • 77.80.Dj

    Domain structure; hysteresis

  • 81.10.Fq

    Growth from melts; zone melting and refining

  • 77.80.Jk

    Relaxor ferroelectrics

  • 61.66.Fn

    Inorganic compounds

  • 77.22.Gm

    Dielectric loss and relaxation

International Patent Classification (IPC)

  • B01D9/00

    Crystallisation

  • C30B9/00

    Single-crystal growth from melt solutions using molten solvents

  • C30B11/00

    Single-crystal-growth by normal freezing or freezing under temperature gradient, e.g. bridgman- stockbarger method

  • C30B15/00

    Single-crystal growth by pulling from a melt, e.g. czochralski method

ARTICLE DATA

Digital Object Identifier
http://dx.doi.org/10.1063/1.3679521

PUBLICATION DATA

ISSN

1931-9401 (online)

Publisher

$abstract.society.value is a Member of CrossRef American Institute of Physics

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Figures (55) Tables (11)

Figures (click on thumbnails to view enlargements)

FIG.1
A typical polarization hysteresis loop in ferroelectrics.

FIG.1 Download High Resolution Image (.zip file) | Export Figure to PowerPoint

FIG.2
Piezoelectric d33 (a) and electromechanical k33 (b) of relaxor-PT crystals, compared to polycrystalline ceramics as function of Curie temperature (data are from Ref. 76).

FIG.2 Download High Resolution Image (.zip file) | Export Figure to PowerPoint

FIG.3
Schematic experimental set-up of the PZN-PT crystal growth from high temperature solution.

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FIG.4
(Color) Large PZN-PT single crystals grown from PbO flux (Courtesy of Dr. L. C. Lim from Microfine Materials Technologies).159

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FIG.5
(Color) PMN-PT and PIN-PMN-PT single crystals (100 mm diameter) grown by multi-crucible Bridgman method (courtesy of Dr. J. Luo from TRS Technologies).199

FIG.5 Download High Resolution Image (.zip file) | Export Figure to PowerPoint

FIG.6
Schematic experimental set-up of a Bridgman growth system.

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FIG.7
Ti concentration along the growth direction in PMN-PT crystal boules grown by Bridgman and Zone-melting methods (data from Ref. 186).

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FIG.8
(Color online) Schematic plot for D-E loop with certain dielectric loss tanδE.

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FIG.9
(Color online) Samples for the full matrix material constants determination, for crystals with 4 mm, mm2, and 3 m symmetries.

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FIG.10
(Color online) Domain structure (or possible domain vectors) of [001] poled rhombohedral and orthorhombic crystals.

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FIG.11
(Color online) Orientation dependence of piezoelectric coefficient d33* of (a) rhombohedral, (b) tetragonal, and (c) orthorhombic PIN-PMN-PT crystals. Li et al., Advanced Functional Materials 21, 2118, 2011. Copyright © 2011, Wiley.

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FIG.12
(Color online)Orientation dependence of shear piezoelectric coefficient for rhombohedral PMN-PT crystals, where input data are from Ref. 72.

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FIG.13
(Color online) Schematic of polarization rotation for [001] poled R crystals under [010] perpendicular electric field, related to d24 ( = d15).

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FIG.14
(Color online) Two independent shear piezoelectric response (15 - and 24-modes) and related polarization rotation paths in crystals with “2 R” engineered domain state, where the shear deformations were contributed by polarization rotation of domain I (DI) and domain II (DII). Reprinted with permission from Zhang et al., Applied Physics Letter 97, 132903, 2010. Copyright © 2010, the American Institute of Physics.

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FIG.15
(Color online) Composition dependence of piezoelectric response for (a) [001] poled PMN-xPT and (b) [001] and [011] poled PIN-PMN-PT crystals.116 , 225 , 259 , 260

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FIG.16
Variation of polarization for rhombohedral relaxor-PT crystals under [001] electric field.

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FIG.17
Polarization rotation path (a) and related free energy (b).Reprinted by permission form H. Fu and R. E. Cohen, Nature 403, 281 (2000). Copyright © 2000, Nature Publishing Group.

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FIG.18
(a) 90° domain wall motion upon electric field and (b) Schematic of free energy with respect to domain wall position.36

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FIG.19
(Color online) Shear piezoelectric deformation and polarization rotation.

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FIG.20
(Color online) Various monoclinic phases for relaxor-PT crystals.

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FIG.21
Compositional dependence of Rayleigh parameters for PMN-xPT crystals at 1 Hz: (a) reversible contribution dinit and (b) irreversible contribution. Reprinted with permission from F. Li et al., Journal of Applied Physics 108, 034106 (2010). Copyright © 2010, the American Institute of Physics.

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FIG.22
(Color online) Transition electric fields and the electric field induced strain levels at 70 kV/cm for PMN-xPT crystals.

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FIG.23
Relaxor factor γ for [001] oriented PMN-xPT crystals, small inset is the dielectric constant vs. temperature for PMN-0.30PT.

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FIG.24
(Color online) Schematic for polarization rotation and extension. The polarization rotation can be found in soft materials (soft PZT and domain engineered crystals); In hard ceramics and single domain crystals, polarization rotation is minimized, due to the internal bias field (hard ceramics) and external field being along polar direction (single domain crystals).

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FIG.25
Mechanical quality factor Qm vs. composition for PMN-xPT crystals.

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FIG.26
(Color online) (a) Piezoelectric loss (determined by S-E loops) and (b) mechanical loss as function of drive field (data are from Refs.137 , 295).

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FIG.27
Temperature dependence of (a) piezoelectric coefficients and (b) relative dielectric permittivities for [001] poled R, T, and M/O crystals.

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FIG.28
(Color online) Temperature dependence of single domain shear piezoelectric responses for (a) PIN-PMN-PT crystals with R and T phases and (b) PIN-PMN-PT crystals with O phase. Reprinted with permission from F. Li et al., Applied Physics Letters 97, 252903 (2010). Copyright © 2010, the American Institute of Physics.

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FIG.29
(Color online) Schematic phase diagram and the polarization rotations for relaxor-PT based crystals.

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FIG.30
Temperature dependence of electromechanical coupling factors for relaxor-PT crystals (a) longitudinal mode and (b) shear mode.F. Li et al., Advanced Functional Materials 21, 2118 (2011). (Copyright © 2011, Wiley)

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FIG.31
(Color online) Temperature dependence of longitudinal piezoelectric coefficients and electromechanical coupling factors for (a) [011] poled tetragonal crystals and (b) [111] poled orthorhombic crystals.

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FIG.32
(Color online) Temperature dependence of mechanical quality factors for PIN-PMN-PT crystals.

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FIG.33
(Color online) Uniaxial compressive strain-stress response of [001] poled PIN-PMN-PT single crystal at various temperatures and zero dc bias. Reprinted with permission from P. Finkel et al., Applied Physics Letters 97, 122903 (2010). Copyright © 2010, the American Institute of Physics.

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FIG.34
Polarization rotation and phase transition of [001] poled rhombohedral crystals under uniaxial stress.

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FIG.35
(Color online) Strain-stress behaviors for relaxor-PT based crystals under various dc bias fields. Reprinted with permission from P. Finkel et al., Applied Physics Letters 97, 122903 (2010). Copyright © 2010, the American Institute of Physics.

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FIG.36
(Color online) Electric field induced strain for PMN-xPT crystals. (data from Ref. 116).

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FIG.37
(Color online) dc bias field dependence of piezoelectric response for PIN-PMN-PT crystals with various phases.

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FIG.38
Uniaxial stress dependence of piezoelectric response for PMN-PT crystals. Reprinted with permission from D. Viehland et al., Journal of Applied Physics 90, 2479 (2001). Copyright © 2001, the American Institute of Physics.

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FIG.39
Schematic for stress induced phase boundary motion for PZN-PT crystals. Reprinted with permission from A. Amin et al., IEEE Transactions on Ultrasonics Ferroelectrectrics Frequency Control 54, 1090 (2007). Copyright © 2007, IEEE.

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FIG.40
(Color online) Strain-electric field behaviors for PMN-PT crystals under various prestress. Reprinted with permission from D. Viehland et al., J. Appl. Phys. 90, 2479 (2001). Copyright 2001, the American Institute of Physics.

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FIG.41
Phase diagram for PMN-PT single crystals under different dc bias fields. Reprinted with permission from S. J. Zhang et al., in 15th IEEE International Symposium Appl. Ferroeletr. (2006), pp. 261–264. Copyright © 2006, IEEE.

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FIG.42
(Color online) (a) The ac electric field dependent dielectric behavior for PZN-PT crystals, (b) piezoelectric coefficients for PMN-PT crystals as function of dynamic stress, and (c) piezoelectric coefficients for PIN-PMN-PT crystals as a function of electric field, α values are calculated from the slope of d33 vs E curves. Reprinted with permissions from A. Bernal et al., Applied Physics Letters 95, 142911 (2009); M. Davis et al., Journal of Applied Physics 95, 5679 (2004); F. Li et al., Journal of Applied Physics 109, 014108 (2011). Copyright © 2004, 2009, 2011, the American Institute of Physics.

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FIG.43
(Color online) Fatigue behavior for relaxor-PT crystals (a) PZN-0.05PT. Reprinted with permission from J. K. Lee et al., Journal of Applied Physics 96, 7471 (2004). Copyright © 2004, the American Institute of Physics) (b) PMN-0.30PT. Reprinted with permission from Y. Zhang et al., Journal of European Ceramic Society 24, 2983 (2004). Copyright © 2004, Elsevier, and (c) PIN-PMN-PT crystals (data from Ref. 332).

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FIG.44
Properties of 1-3 and 2-2 composites, compared to monolithic plate.

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FIG.45
Composite transducers dice-and-fill process. P. W. Rehrig et al., “Micromachined imaging transducer,” U.S. patent US7622853 (24 November 2009); X. N. Jiang et al., Proceedings on SPIE 6531, 65310 F (2007); X. N. Jiang et al., Proceedings on SPIE 6934, 69340D (2008). Copyright © 2008, SPIE.

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FIG.46
(Color online) High frequency composite transducers PC-MUT process. P. W. Rehrig et al., “Micromachined imaging transducer,” U.S. patent US7622853 (24 November 2009); X. N. Jiang et al., Proceedings on SPIE 6531, 65310 F (2007); X. N. Jiang et al., Proceedings on SPIE 6934, 69340D (2008). Copyright © 2008, SPIE.

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FIG.47
Electromechanical coupling k33 for monolithic and crystal/epoxy 1–3 composites, as a function of sample thickness and corresponding ultrasound frequency. Reprinted with permission from H. J. Lee et al., Journal of Applied Physics 107, 124107 (2010). Copyright © 2010, the American Institute of Physics.

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FIG.48
Cross-section of typical tonpilz transducer.186

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FIG.49
(Color online) Projector TP16 operating in transverse extensional mode, fabricated by MMT (Courtesy of Dr. L. C. Lim from Microfine Materials Technologies).159

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FIG.50
(Color online) PZN-PT crystal based high sensitivity seismic/infrasonic accelerometer fabricated by MMT (Courtesy of Dr. L. C. Lim from Microfine Materials Technologies).159

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FIG.51
(Color online) Schematic view of single crystal stack actuator assembly407 and crystal stack/actuator array fabricated by TRS Technologies199 (Courtesy of R. Sahul from TRS Technologies).

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FIG.52
(Color online) Flextensional actuators in “31” and “33” modes, fabricated by TRS Technologies.199 , 406 , 409

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FIG.53
(Color online) (a) Piezoelectric composite stator with two notches, (b) PMN-PT crystal ring, and (c) the assembled piezoelectric stator. Reprinted with permission from X. N. Jiang, in IEEE Ultrasonic Symposium (2004), pp. 1314–1317; S. X. Dong et al., Applied Physics Letters 86, 053501 (2005). Copyright © 2005, the American Institute of Physics.

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FIG.54
(Color online) (a) Piezoelectric coefficient as a function of TRT; (b) Electromechanical coupling as function of TC; and (c) Coercive field as function of TC; for various relaxor-PT crystal systems. The small inset shows polarization hysteresis of 1st, 2nd, and 3 rd generations crystals. Reprinted with permission from S. J. Zhang and T. R. Shrout, IEEE Transactions on Ultrasonics Ferroelectrectrics Frequency Control 57, 2138 (2010). Copyright © 2010, IEEE.

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FIG.55
The relationship between mechanical quality factor Qm and electromechanical coupling factor for different polycrystalline and single crystal systems. Reprinted with permission from S. J. Zhang and T. R. Shrout, IEEE Transactions on Ultrasonics Ferroelectrectrics Frequency Control 57, 2138 (2010). Copyright © 2010, IEEE.

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Tables

Table I. Domain engineered configuration in Relaxor-PT single crystal systems (Refs.33,40).

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Table II. The property comparison of various generation relaxor-PT single crystals.

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Table III. Relationship between the phase velocity and elastic constants for crystals with 4 mm, mm2, and 3 m symmetries in the pulse-echo ultrasonic measurements.

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Table IV. Piezoelectric, dielectric, and elastic constants for single domain PIN-PMN-PT crystals with various phases.t4n1

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Table V. Comparison of longitudinal and shear piezoelectricity for relaxor-PT crystals.19,31,71,110,114,115,245

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Table VI. Mechanical quality factor and dielectric loss of PMN-0.30PT crystals as a function of orientation.250

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Table VII. Pyroelectric properties and FOMs for relaxor-PT crystals.

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Table VIII. The loss/quality factors for relaxor-PT crystals as a function of polarization rotation angle.

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Table IX. Shear mode characteristics of relaxor-PT crystals with various domain configurations (PIN: PIN-PMN-PT).253,254,326

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Table X. Comparison of hydrostatic coefficients for various materials.186,398

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Table XI. Properties comparison for various materials relate to actuator applications.

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