Thermal resistance and heat capacity in hafnium zirconium oxide (Hf1–xZrxO2) dielectrics and ferroelectric thin films

Scott, Ethan A.; Smith, Sean W.; Henry, M. David; Rost, Christina M.; Giri, Ashutosh; Gaskins, John T.; Fields, Shelby S.; Jaszewski, Samantha T.; Ihlefeld, Jon F.; Hopkins, Patrick E.

doi:10.1063/1.5052244

Title: Thermal resistance and heat capacity in hafnium zirconium oxide (Hf_1–xZr_xO₂) dielectrics and ferroelectric thin films

Abstract

We report on the thermal resistances of thin films (20 nm) of hafnium zirconium oxide (Hf_1–xZr_xO₂) with compositions ranging from 0 ≤ x ≤ 1. Measurements were made via time-domain thermoreflectance and analyzed to determine the effective thermal resistance of the films in addition to their associated thermal boundary resistances. We find effective thermal resistances ranging from 28.79 to 24.72 m² K GW^-1 for amorphous films, which decreased to 15.81 m² K GW^-1 upon crystallization. Furthermore, we analyze the heat capacity for two compositions, x = 0.5 and x = 0.7, of Hf_1–xZr_xO₂ and find them to be 2.18 ± 0.56 and 2.64 ± 0.53 MJ m^-3 K^-1, respectively.

Authors:

^[1]; Smith, Sean W. ^[2]; Henry, M. David ^[2];

^[1]; Giri, Ashutosh ^[1];

^[1]; Fields, Shelby S. ^[3]; Jaszewski, Samantha T. ^[3];

^[4]; Hopkins, Patrick E. ^[5]

Univ. of Virginia, Charlottesville, VA (United States). Dept. of Mechanical and Aerospace Engineering
Sandia National Lab. (SNL-NM), Albuquerque, NM (United States)
Univ. of Virginia, Charlottesville, VA (United States). Dept. of Materials Science and Engineering
Univ. of Virginia, Charlottesville, VA (United States). Dept. of Materials Science and Engineering, Dept. of Electrical and Computer Engineering
Univ. of Virginia, Charlottesville, VA (United States). Dept. of Mechanical and Aerospace Engineering, Dept. of Materials Science and Engineering, Dept. of Physics

Publication Date:: Mon Nov 05 00:00:00 EST 2018

Research Org.:: Sandia National Lab. (SNL-NM), Albuquerque, NM (United States)

Sponsoring Org.:: USDOE National Nuclear Security Administration (NNSA)

OSTI Identifier:: 1483978

Report Number(s):: SAND-2018-12885J
Journal ID: ISSN 0003-6951; 669810

Grant/Contract Number:: AC04-94AL85000

Resource Type:: Accepted Manuscript

Journal Name:: Applied Physics Letters

Additional Journal Information:: Journal Volume: 113; Journal Issue: 19; Journal ID: ISSN 0003-6951

Publisher:: American Institute of Physics (AIP)

Country of Publication:: United States

Language:: English

Subject:: 36 MATERIALS SCIENCE

Citation Formats


                    Scott, Ethan A., Smith, Sean W., Henry, M. David, Rost, Christina M., Giri, Ashutosh, Gaskins, John T., Fields, Shelby S., Jaszewski, Samantha T., Ihlefeld, Jon F., and Hopkins, Patrick E. Thermal resistance and heat capacity in hafnium zirconium oxide (Hf1–xZrxO2) dielectrics and ferroelectric thin films.  United States: N. p., 2018. 
Web.  doi:10.1063/1.5052244.

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                    Scott, Ethan A., Smith, Sean W., Henry, M. David, Rost, Christina M., Giri, Ashutosh, Gaskins, John T., Fields, Shelby S., Jaszewski, Samantha T., Ihlefeld, Jon F., & Hopkins, Patrick E. Thermal resistance and heat capacity in hafnium zirconium oxide (Hf1–xZrxO2) dielectrics and ferroelectric thin films.  United States.  https://doi.org/10.1063/1.5052244

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                    Scott, Ethan A., Smith, Sean W., Henry, M. David, Rost, Christina M., Giri, Ashutosh, Gaskins, John T., Fields, Shelby S., Jaszewski, Samantha T., Ihlefeld, Jon F., and Hopkins, Patrick E. Mon .  
"Thermal resistance and heat capacity in hafnium zirconium oxide (Hf1–xZrxO2) dielectrics and ferroelectric thin films".  United States.  https://doi.org/10.1063/1.5052244.  https://www.osti.gov/servlets/purl/1483978.

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@article{osti_1483978,

  title        = {Thermal resistance and heat capacity in hafnium zirconium oxide (Hf1–xZrxO2) dielectrics and ferroelectric thin films},

  author       = {Scott, Ethan A. and Smith, Sean W. and Henry, M. David and Rost, Christina M. and Giri, Ashutosh and Gaskins, John T. and Fields, Shelby S. and Jaszewski, Samantha T. and Ihlefeld, Jon F. and Hopkins, Patrick E.},

  abstractNote = {We report on the thermal resistances of thin films (20 nm) of hafnium zirconium oxide (Hf1–xZrxO2) with compositions ranging from 0 ≤ x ≤ 1. Measurements were made via time-domain thermoreflectance and analyzed to determine the effective thermal resistance of the films in addition to their associated thermal boundary resistances. We find effective thermal resistances ranging from 28.79 to 24.72 m2 K GW-1 for amorphous films, which decreased to 15.81 m2 K GW-1 upon crystallization. Furthermore, we analyze the heat capacity for two compositions, x = 0.5 and x = 0.7, of Hf1–xZrxO2 and find them to be 2.18 ± 0.56 and 2.64 ± 0.53 MJ m-3 K-1, respectively.},

  doi          = {10.1063/1.5052244},

  journal      = {Applied Physics Letters},

  number       = 19,

  volume       = 113,

  place        = {United States},

  year         = {Mon Nov 05 00:00:00 EST 2018},

  month        = {Mon Nov 05 00:00:00 EST 2018}

}

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Title: Thermal resistance and heat capacity in hafnium zirconium oxide (Hf1–xZrxO2) dielectrics and ferroelectric thin films

Abstract

Citation Formats

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Simultaneous measurement of thermal conductivity and heat capacity of bulk and thin film materials using frequency-dependent transient thermoreflectance method journal, March 2013

Comparison of the 3ω method and time-domain thermoreflectance for measurements of the cross-plane thermal conductivity of epitaxial semiconductors journal, March 2009

Evolution of phases and ferroelectric properties of thin Hf 0.5 Zr 0.5 O 2 films according to the thickness and annealing temperature journal, June 2013

High temperature thermal properties of thin tantalum nitride films journal, December 2011

Thermal conductivity and thermal boundary resistance of atomic layer deposited high- k dielectric aluminum oxide, hafnium oxide, and titanium oxide thin films on silicon journal, May 2018

Mechanism of the monoclinic-to-tetragonal phase transition induced in zirconia and hafnia by swift heavy ions journal, September 2005

The heat capacity of pure silicon and germanium and properties of their vibrational frequency spectra journal, March 1959

Direct Visualization of Thermal Conductivity Suppression Due to Enhanced Phonon Scattering Near Individual Grain Boundaries journal, April 2018

On the structural origins of ferroelectricity in HfO 2 thin films journal, April 2015

Heat capacity and thermodynamic functions of zirconia and yttria-stabilized zirconia journal, July 1999

Diameter dependence of SiGe nanowire thermal conductivity journal, September 2010

Low-Voltage Steep Turn-On pMOSFET Using Ferroelectric High-$\kappa$ Gate Dielectric journal, February 2014

Reduction in thermal conductivity and tunable heat capacity of inorganic/organic hybrid superlattices journal, January 2016

Hafnium nitride films for thermoreflectance transducers at high temperatures: Potential based on heating from laser absorption journal, October 2017

A frequency-domain thermoreflectance method for the characterization of thermal properties journal, September 2009

Experimental Investigation of Size Effects on the Thermal Conductivity of Silicon-Germanium Alloy Thin Films journal, November 2012

Probing anisotropic heat transport using time-domain thermoreflectance with offset laser spots journal, October 2012

Fundamentals of picosecond laser ultrasonics journal, February 2015

Pyroelectric response in crystalline hafnium zirconium oxide (Hf 1- x Zr x O 2 ) thin films journal, February 2017

Upper limit to the thermal penetration depth during modulated heating of multilayer thin films with pulsed and continuous wave lasers: A numerical study journal, May 2017

Thermal Conductivity and Thermoelectric Power of Germanium‐Silicon Alloys journal, November 1958

Thermal conductivity and sound velocity measurements of plasma enhanced chemical vapor deposited a-SiC:H thin films journal, September 2011

Thermometry and Thermal Transport in Micro/Nanoscale Solid-State Devices and Structures journal, December 2001

Impact of mechanical stress on ferroelectricity in (Hf 0.5 Zr 0.5 )O 2 thin films journal, June 2016

Antiferroelectricity in thin-film ZrO 2 from first principles journal, October 2014

Ferroelectricity in hafnium oxide thin films journal, September 2011

Toward a multifunctional monolithic device based on pyroelectricity and the electrocaloric effect of thin antiferroelectric Hf x Zr 1−x O 2 films journal, March 2015

Heat capacity of hafnia at low temperature journal, June 2011

On the Steady-State Temperature Rise During Laser Heating of Multilayer Thin Films in Optical Pump–Probe Techniques journal, February 2018

Frequency dependence of the thermal conductivity of semiconductor alloys journal, August 2007

Micromachined infrared detectors based on pyroelectric thin films journal, September 2001

"The Zirconia?Hafnia System: DTA Measurements and Thermodynamic Calculations" journal, June 2007

Diameter dependence of SiGe nanowire thermal conductivity text, January 2011

Direct Visualization of Thermal Conductivity Suppression Due to Enhanced Phonon Scattering Near Individual Grain Boundaries text, January 2018

Design strategies for improvement in nonvolatile memory characteristics of metal-ferroelectric-metal-insulator-semiconductor capacitors using ferroelectric Hf 0.5 Zr 0.5 O 2 thin films journal, January 2020

Title: Thermal resistance and heat capacity in hafnium zirconium oxide (Hf_1–xZr_xO₂) dielectrics and ferroelectric thin films

Characterization of Mechanical and Thermal Properties Using Ultrafast Optical Metrology
journal, August 2006

LIPRAS: Line-Profile Analysis Software
text, January 2017

Characterization of Ta and TaN diffusion barriers beneath Cu layers using picosecond ultrasonics
journal, December 2006

Solid state epitaxy of (Hf,Zr)O<sub>2</sub> thin films with orthorhombic phase
journal, January 2016

Lattice Thermal Conductivity of Disordered Semiconductor Alloys at High Temperatures
journal, September 1963

Thermal Properties of Ultrathin Hafnium Oxide Gate Dielectric Films
journal, December 2009

Doped Hf _0.5 Zr _0.5 O ₂ for high efficiency integrated supercapacitors
journal, June 2017

Review—Investigation and Review of the Thermal, Mechanical, Electrical, Optical, and Structural Properties of Atomic Layer Deposited High- k Dielectrics: Beryllium Oxide, Aluminum Oxide, Hafnium Oxide, and Aluminum Nitride
journal, January 2017

Heat Capacities at Low Temperatures and Entropies at 298.16°K. of Hafnium Dioxide and Hafnium Tetrachloride
journal, June 1953

Analysis of heat flow in layered structures for time-domain thermoreflectance
journal, December 2004

Specific heat of aluminum from zero to its melting temperature and beyond. Equation for representation of the specific heat of solids
journal, October 1970

The Zirconia?Hafnia System: DTA Measurements and Thermodynamic Calculations
journal, December 2006

Ultralow thermal conductivity of fullerene derivatives
journal, August 2013

Thermal conductivity and refractive index of hafnia-alumina nanolaminates
journal, August 2011

Pyroelectric devices and materials
journal, December 1986

Ten-Nanometer Ferroelectric $\hbox{Si:HfO}_{2}$ Films for Next-Generation FRAM Capacitors
journal, September 2012

Criteria for Cross-Plane Dominated Thermal Transport in Multilayer Thin Film Systems During Modulated Laser Heating
journal, May 2010

Surface generation and detection of phonons by picosecond light pulses
journal, September 1986

Modeling ballistic effects in frequency-dependent transient thermal transport using diffusion equations
journal, March 2016

Ferroelectricity in Simple Binary ZrO ₂ and HfO ₂
journal, July 2012

Simultaneous measurement of thermal conductivity and heat capacity of bulk and thin film materials using frequency-dependent transient thermoreflectance method
journal, March 2013

Comparison of the 3ω method and time-domain thermoreflectance for measurements of the cross-plane thermal conductivity of epitaxial semiconductors
journal, March 2009

Evolution of phases and ferroelectric properties of thin Hf _0.5 Zr _0.5 O ₂ films according to the thickness and annealing temperature
journal, June 2013

High temperature thermal properties of thin tantalum nitride films
journal, December 2011

Thermal conductivity and thermal boundary resistance of atomic layer deposited high- k dielectric aluminum oxide, hafnium oxide, and titanium oxide thin films on silicon
journal, May 2018

Mechanism of the monoclinic-to-tetragonal phase transition induced in zirconia and hafnia by swift heavy ions
journal, September 2005

The heat capacity of pure silicon and germanium and properties of their vibrational frequency spectra
journal, March 1959

Direct Visualization of Thermal Conductivity Suppression Due to Enhanced Phonon Scattering Near Individual Grain Boundaries
journal, April 2018

On the structural origins of ferroelectricity in HfO ₂ thin films
journal, April 2015

Heat capacity and thermodynamic functions of zirconia and yttria-stabilized zirconia
journal, July 1999

Diameter dependence of SiGe nanowire thermal conductivity
journal, September 2010

Low-Voltage Steep Turn-On pMOSFET Using Ferroelectric High-$\kappa$ Gate Dielectric
journal, February 2014

Reduction in thermal conductivity and tunable heat capacity of inorganic/organic hybrid superlattices
journal, January 2016

Hafnium nitride films for thermoreflectance transducers at high temperatures: Potential based on heating from laser absorption
journal, October 2017

A frequency-domain thermoreflectance method for the characterization of thermal properties
journal, September 2009

Experimental Investigation of Size Effects on the Thermal Conductivity of Silicon-Germanium Alloy Thin Films
journal, November 2012

Probing anisotropic heat transport using time-domain thermoreflectance with offset laser spots
journal, October 2012

Fundamentals of picosecond laser ultrasonics
journal, February 2015

Pyroelectric response in crystalline hafnium zirconium oxide (Hf _1- _x Zr _x O ₂ ) thin films
journal, February 2017

Upper limit to the thermal penetration depth during modulated heating of multilayer thin films with pulsed and continuous wave lasers: A numerical study
journal, May 2017

Thermal Conductivity and Thermoelectric Power of Germanium‐Silicon Alloys
journal, November 1958

Thermal conductivity and sound velocity measurements of plasma enhanced chemical vapor deposited a-SiC:H thin films
journal, September 2011

Thermometry and Thermal Transport in Micro/Nanoscale Solid-State Devices and Structures
journal, December 2001

Impact of mechanical stress on ferroelectricity in (Hf _0.5 Zr _0.5 )O ₂ thin films
journal, June 2016

Antiferroelectricity in thin-film ${ZrO}_{2}$ from first principles
journal, October 2014

Ferroelectricity in hafnium oxide thin films
journal, September 2011

Toward a multifunctional monolithic device based on pyroelectricity and the electrocaloric effect of thin antiferroelectric Hf x Zr 1−x O 2 films
journal, March 2015

Heat capacity of hafnia at low temperature
journal, June 2011

On the Steady-State Temperature Rise During Laser Heating of Multilayer Thin Films in Optical Pump–Probe Techniques
journal, February 2018

Frequency dependence of the thermal conductivity of semiconductor alloys
journal, August 2007

Micromachined infrared detectors based on pyroelectric thin films
journal, September 2001

"The Zirconia?Hafnia System: DTA Measurements and Thermodynamic Calculations"
journal, June 2007

Diameter dependence of SiGe nanowire thermal conductivity
text, January 2011

Direct Visualization of Thermal Conductivity Suppression Due to Enhanced Phonon Scattering Near Individual Grain Boundaries
text, January 2018

Design strategies for improvement in nonvolatile memory characteristics of metal-ferroelectric-metal-insulator-semiconductor capacitors using ferroelectric Hf _0.5 Zr _0.5 O ₂ thin films
journal, January 2020