DOE PAGES title logo U.S. Department of Energy
Office of Scientific and Technical Information

Title: Unraveling Ferroelectric Polarization and Ionic Contributions to Electroresistance in Epitaxial Hf0.5Zr0.5O2 Tunnel Junctions

Abstract

Tunnel devices based on ferroelectric Hf0.5Zr0.5O2 (HZO) barriers hold great promises for emerging data storage and computing technologies. The resistance state of the device can be changed through use of a suitable writing voltage. However, the microscopic mechanisms leading to the resistance change are an intricate interplay between ferroelectric polarization controlled barrier properties and defect-related transport mechanisms. Herein, the fundamental role of the microstructure of HZO films determining the balance between those contributions is demonstrated. The HZO film presents coherent or incoherent grain boundaries, associated to the coexistance of monoclinic and orthorhombic phases, which are dictated by the mismatch with the substrates for epitaxial growth. These grain boundaries are the toggle that allows to obtain either large (up to ≈450%) and fully reversible genuine polarization controlled electroresistance when only the orthorhombic phase is present or an irreversible and extremely large (≈103–105%) electroresistance when both phases coexist.

Authors:
 [1];  [1];  [1];  [1];  [1];  [1]; ORCiD logo [2]; ORCiD logo [1]; ORCiD logo [1];  [1]
  1. Univ. Autònoma de Barcelona (Spain). Inst. de Ciència de Materials de Barcelona (ICMAB-CSIC)
  2. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Science (CNMS)
Publication Date:
Research Org.:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Sponsoring Org.:
Spanish Ministry of Economy, Competitiveness and Universities; Generalitat de Catalunya; “la Caixa Foundation”; Ramón y Cajal; China Scholarship Council (CSC); USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Materials Sciences & Engineering Division
OSTI Identifier:
1606631
Grant/Contract Number:  
AC05-00OR22725; RYC-2017-22531; RYC- 2012-11709; SEV-2015-0496-16-3); 2017 SGR 1377; 100010434; LCF/BQ/IN17/11620051; SEV‐2015‐0496; MAT2017‐85232‐R; RYC‐2017‐22531; RYC‐2012‐11709; SEV‐2015‐0496‐16‐3; MAT2015‐73839‐JIN; 201506080019; 201806100207
Resource Type:
Accepted Manuscript
Journal Name:
Advanced Electronic Materials
Additional Journal Information:
Journal Volume: 6; Journal Issue: 1; Journal ID: ISSN 2199-160X
Publisher:
Wiley
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; ferroelectric tunnel junctions; hafnium oxides; Hf0.5Zr0.5O2; resistive switching; tunnel electroresistance

Citation Formats

Sulzbach, Milena Cervo, Estandía, Saúl, Long, Xiao, Lyu, Jike, Dix, Nico, Gàzquez, Jaume, Chisholm, Matthew F., Sánchez, Florencio, Fina, Ignasi, and Fontcuberta, Josep. Unraveling Ferroelectric Polarization and Ionic Contributions to Electroresistance in Epitaxial Hf0.5Zr0.5O2 Tunnel Junctions. United States: N. p., 2019. Web. doi:10.1002/aelm.201900852.
Sulzbach, Milena Cervo, Estandía, Saúl, Long, Xiao, Lyu, Jike, Dix, Nico, Gàzquez, Jaume, Chisholm, Matthew F., Sánchez, Florencio, Fina, Ignasi, & Fontcuberta, Josep. Unraveling Ferroelectric Polarization and Ionic Contributions to Electroresistance in Epitaxial Hf0.5Zr0.5O2 Tunnel Junctions. United States. https://doi.org/10.1002/aelm.201900852
Sulzbach, Milena Cervo, Estandía, Saúl, Long, Xiao, Lyu, Jike, Dix, Nico, Gàzquez, Jaume, Chisholm, Matthew F., Sánchez, Florencio, Fina, Ignasi, and Fontcuberta, Josep. Thu . "Unraveling Ferroelectric Polarization and Ionic Contributions to Electroresistance in Epitaxial Hf0.5Zr0.5O2 Tunnel Junctions". United States. https://doi.org/10.1002/aelm.201900852. https://www.osti.gov/servlets/purl/1606631.
@article{osti_1606631,
title = {Unraveling Ferroelectric Polarization and Ionic Contributions to Electroresistance in Epitaxial Hf0.5Zr0.5O2 Tunnel Junctions},
author = {Sulzbach, Milena Cervo and Estandía, Saúl and Long, Xiao and Lyu, Jike and Dix, Nico and Gàzquez, Jaume and Chisholm, Matthew F. and Sánchez, Florencio and Fina, Ignasi and Fontcuberta, Josep},
abstractNote = {Tunnel devices based on ferroelectric Hf0.5Zr0.5O2 (HZO) barriers hold great promises for emerging data storage and computing technologies. The resistance state of the device can be changed through use of a suitable writing voltage. However, the microscopic mechanisms leading to the resistance change are an intricate interplay between ferroelectric polarization controlled barrier properties and defect-related transport mechanisms. Herein, the fundamental role of the microstructure of HZO films determining the balance between those contributions is demonstrated. The HZO film presents coherent or incoherent grain boundaries, associated to the coexistance of monoclinic and orthorhombic phases, which are dictated by the mismatch with the substrates for epitaxial growth. These grain boundaries are the toggle that allows to obtain either large (up to ≈450%) and fully reversible genuine polarization controlled electroresistance when only the orthorhombic phase is present or an irreversible and extremely large (≈103–105%) electroresistance when both phases coexist.},
doi = {10.1002/aelm.201900852},
journal = {Advanced Electronic Materials},
number = 1,
volume = 6,
place = {United States},
year = {Thu Nov 14 00:00:00 EST 2019},
month = {Thu Nov 14 00:00:00 EST 2019}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record

Citation Metrics:
Cited by: 32 works
Citation information provided by
Web of Science

Save / Share:

Works referenced in this record:

A ferroelectric memristor
journal, September 2012

  • Chanthbouala, André; Garcia, Vincent; Cherifi, Ryan O.
  • Nature Materials, Vol. 11, Issue 10
  • DOI: 10.1038/nmat3415

A Resistive Memory in Semiconducting BiFeO3 Thin-Film Capacitors
journal, January 2011


Enhanced ferroelectricity in epitaxial Hf 0.5 Zr 0.5 O 2 thin films integrated with Si(001) using SrTiO 3 templates
journal, June 2019

  • Lyu, J.; Fina, I.; Bachelet, R.
  • Applied Physics Letters, Vol. 114, Issue 22
  • DOI: 10.1063/1.5096002

Incoherent imaging using dynamically scattered coherent electrons
journal, June 1999


APPLIED PHYSICS: Tunneling Across a Ferroelectric
journal, July 2006


Metal oxide resistive memory switching mechanism based on conductive filament properties
journal, December 2011

  • Bersuker, G.; Gilmer, D. C.; Veksler, D.
  • Journal of Applied Physics, Vol. 110, Issue 12
  • DOI: 10.1063/1.3671565

Determination of electron effective mass and electron affinity in HfO2 using MOS and MOSFET structures
journal, April 2009


Large Room-Temperature Electroresistance in Dual-Modulated Ferroelectric Tunnel Barriers
journal, March 2015

  • Radaelli, Greta; Gutiérrez, Diego; Sánchez, Florencio
  • Advanced Materials, Vol. 27, Issue 16
  • DOI: 10.1002/adma.201405117

Growth Window of Ferroelectric Epitaxial Hf 0.5 Zr 0.5 O 2 Thin Films
journal, January 2019

  • Lyu, Jike; Fina, Ignasi; Solanas, Raul
  • ACS Applied Electronic Materials, Vol. 1, Issue 2
  • DOI: 10.1021/acsaelm.8b00065

Four-state ferroelectric spin-valve
journal, May 2015

  • Quindeau, Andy; Fina, Ignasi; Marti, Xavi
  • Scientific Reports, Vol. 5, Issue 1
  • DOI: 10.1038/srep09749

Ferroelectric Tunnel Memristor
journal, October 2012


Electrode dependence of filament formation in HfO 2 resistive-switching memory
journal, April 2011

  • Lin, Kuan-Liang; Hou, Tuo-Hung; Shieh, Jiann
  • Journal of Applied Physics, Vol. 109, Issue 8
  • DOI: 10.1063/1.3567915

Nonferroelectric contributions to the hysteresis cycles in manganite thin films: A comparative study of measurement techniques
journal, April 2011

  • Fina, I.; Fàbrega, L.; Langenberg, E.
  • Journal of Applied Physics, Vol. 109, Issue 7
  • DOI: 10.1063/1.3555098

Crossing an Interface: Ferroelectric Control of Tunnel Currents in Magnetic Complex Oxide Heterostructures
journal, June 2010

  • Hambe, Michael; Petraru, Adrian; Pertsev, Nikolay A.
  • Advanced Functional Materials, Vol. 20, Issue 15
  • DOI: 10.1002/adfm.201000265

A Complementary Metal Oxide Semiconductor Process-Compatible Ferroelectric Tunnel Junction
journal, April 2017

  • Ambriz-Vargas, Fabian; Kolhatkar, Gitanjali; Broyer, Maxime
  • ACS Applied Materials & Interfaces, Vol. 9, Issue 15
  • DOI: 10.1021/acsami.6b16173

Robust ferroelectricity in epitaxial Hf 1/2 Zr 1/2 O 2 thin films
journal, August 2018

  • Lyu, J.; Fina, I.; Solanas, R.
  • Applied Physics Letters, Vol. 113, Issue 8
  • DOI: 10.1063/1.5041715

Tunneling Electroresistance Effect in Ferroelectric Tunnel Junctions at the Nanoscale
journal, October 2009

  • Gruverman, A.; Wu, D.; Lu, H.
  • Nano Letters, Vol. 9, Issue 10
  • DOI: 10.1021/nl901754t

Direct Reversible Magnetoelectric Coupling in a Ferroelectric/Ferromagnetic Structure Controlled by Series Resistance Engineering
journal, August 2019

  • González-Casal, Sergio; Fina, Ignasi; Sánchez, Florencio
  • ACS Applied Electronic Materials, Vol. 1, Issue 9
  • DOI: 10.1021/acsaelm.9b00427

Magnetic Tunnel Junctions Based on Ferroelectric Hf 0.5 Zr 0.5 O 2 Tunnel Barriers
journal, September 2019


Epitaxial Integration on Si(001) of Ferroelectric Hf 0.5 Zr 0.5 O 2 Capacitors with High Retention and Endurance
journal, January 2019

  • Lyu, Jike; Fina, Ignasi; Fontcuberta, Josep
  • ACS Applied Materials & Interfaces, Vol. 11, Issue 6
  • DOI: 10.1021/acsami.8b18762

On the Gradual Unipolar and Bipolar Resistive Switching of TiN\HfO[sub 2]\Pt Memory Systems
journal, January 2010

  • Goux, L.; Chen, Y. -Y; Pantisano, L.
  • Electrochemical and Solid-State Letters, Vol. 13, Issue 6
  • DOI: 10.1149/1.3373529

Band offsets and Schottky barrier heights of high dielectric constant oxides
journal, October 2002

  • Peacock, P. W.; Robertson, J.
  • Journal of Applied Physics, Vol. 92, Issue 8
  • DOI: 10.1063/1.1506388

Synergetic Electronic and Ionic Contributions to Electroresistance in Ferroelectric Capacitors
journal, February 2019

  • Qian, Mengdi; Fina, Ignasi; Sulzbach, Milena Cervo
  • Advanced Electronic Materials, Vol. 5, Issue 3
  • DOI: 10.1002/aelm.201800646

Giant tunnel electroresistance for non-destructive readout of ferroelectric states
journal, May 2009

  • Garcia, V.; Fusil, S.; Bouzehouane, K.
  • Nature, Vol. 460, Issue 7251, p. 81-84
  • DOI: 10.1038/nature08128

Towards Oxide Electronics: a Roadmap
journal, July 2019


Asymmetric Resistive Switching Dynamics in BaTiO 3 Tunnel Junctions
journal, November 2018

  • Qian, Mengdi; Fina, Ignasi; Sánchez, Florencio
  • Advanced Electronic Materials, Vol. 5, Issue 1
  • DOI: 10.1002/aelm.201800407

A rhombohedral ferroelectric phase in epitaxially strained Hf0.5Zr0.5O2 thin films
journal, October 2018


Epitaxial Ferroelectric Hf 0.5 Zr 0.5 O 2 Thin Films and Their Implementations in Memristors for Brain‐Inspired Computing
journal, October 2018

  • Yoong, Herng Yau; Wu, Haijun; Zhao, Jianhui
  • Advanced Functional Materials, Vol. 28, Issue 50
  • DOI: 10.1002/adfm.201806037

Impact of Bi Deficiencies on Ferroelectric Resistive Switching Characteristics Observed at p-Type Schottky-Like Pt/Bi1-δFeO3 Interfaces
journal, January 2012

  • Tsurumaki, Atsushi; Yamada, Hiroyuki; Sawa, Akihito
  • Advanced Functional Materials, Vol. 22, Issue 5
  • DOI: 10.1002/adfm.201102883

Giant Electroresistance in Ferroelectric Tunnel Junctions
journal, June 2005


Giant Electroresistance of Super-tetragonal BiFeO 3 -Based Ferroelectric Tunnel Junctions
journal, May 2013

  • Yamada, Hiroyuki; Garcia, Vincent; Fusil, Stéphane
  • ACS Nano, Vol. 7, Issue 6
  • DOI: 10.1021/nn401378t

Resistive Switching in All-Oxide Ferroelectric Tunnel Junctions with Ionic Interfaces
journal, June 2016

  • Qin, Qi Hang; Äkäslompolo, Laura; Tuomisto, Noora
  • Advanced Materials, Vol. 28, Issue 32
  • DOI: 10.1002/adma.201504519

Tunneling electroresistance effect in a Pt/Hf 0.5 Zr 0.5 O 2 /Pt structure
journal, February 2017

  • Ambriz-Vargas, F.; Kolhatkar, G.; Thomas, R.
  • Applied Physics Letters, Vol. 110, Issue 9
  • DOI: 10.1063/1.4977028

Grain boundaries as preferential sites for resistive switching in the HfO 2 resistive random access memory structures
journal, March 2012

  • Lanza, M.; Zhang, K.; Porti, M.
  • Applied Physics Letters, Vol. 100, Issue 12
  • DOI: 10.1063/1.3697648

Tunneling Conductance of Asymmetrical Barriers
journal, April 1970

  • Brinkman, W. F.; Dynes, R. C.; Rowell, J. M.
  • Journal of Applied Physics, Vol. 41, Issue 5
  • DOI: 10.1063/1.1659141

Ferroelectricity and Antiferroelectricity of Doped Thin HfO 2 -Based Films
journal, February 2015

  • Park, Min Hyuk; Lee, Young Hwan; Kim, Han Joon
  • Advanced Materials, Vol. 27, Issue 11
  • DOI: 10.1002/adma.201404531

Ferroelectric-field-effect-enhanced electroresistance in metal/ferroelectric/semiconductor tunnel junctions
journal, May 2013

  • Wen, Zheng; Li, Chen; Wu, Di
  • Nature Materials, Vol. 12, Issue 7
  • DOI: 10.1038/nmat3649

Ferroelectric hafnium oxide for ferroelectric random-access memories and ferroelectric field-effect transistors
journal, May 2018

  • Mikolajick, Thomas; Slesazeck, Stefan; Park, Min Hyuk
  • MRS Bulletin, Vol. 43, Issue 5
  • DOI: 10.1557/mrs.2018.92

Room-Temperature Ferroelectric Resistive Switching in Ultrathin Pb(Zr 0.2 Ti 0.8 )O 3 Films
journal, June 2011

  • Pantel, Daniel; Goetze, Silvana; Hesse, Dietrich
  • ACS Nano, Vol. 5, Issue 7
  • DOI: 10.1021/nn2018528

Ferroelectricity in hafnium oxide thin films
journal, September 2011

  • Böscke, T. S.; Müller, J.; Bräuhaus, D.
  • Applied Physics Letters, Vol. 99, Issue 10
  • DOI: 10.1063/1.3634052

In-memory computing with resistive switching devices
journal, June 2018


Overcoming the Fundamental Barrier Thickness Limits of Ferroelectric Tunnel Junctions through BaTiO 3 /SrTiO 3 Composite Barriers
journal, May 2016


Interplay between ferroelectric and resistive switching in doped crystalline HfO 2
journal, April 2018

  • Max, Benjamin; Pešić, Milan; Slesazeck, Stefan
  • Journal of Applied Physics, Vol. 123, Issue 13
  • DOI: 10.1063/1.5015985

Ferroelectric tunnel junctions for information storage and processing
journal, July 2014

  • Garcia, Vincent; Bibes, Manuel
  • Nature Communications, Vol. 5, Issue 1
  • DOI: 10.1038/ncomms5289

Engineering Ferroelectric Hf 0.5 Zr 0.5 O 2 Thin Films by Epitaxial Stress
journal, July 2019

  • Estandía, Saúl; Dix, Nico; Gazquez, Jaume
  • ACS Applied Electronic Materials, Vol. 1, Issue 8
  • DOI: 10.1021/acsaelm.9b00256

Investigation of switching uniformity in resistive memory via finite element simulation of conductive-filament formation
journal, January 2021


Towards Oxide Electronics : a Roadmap
text, January 2019


A ferroelectric memristor
text, January 2012


A rhombohedral ferroelectric phase in epitaxially-strained Hf0.5Zr0.5O2 thin films
text, January 2018


Engineering Ferroelectric Hf0.5Zr0.5O2 Thin Films by Epitaxial Stress
text, January 2019


Works referencing / citing this record:

Magneto-ionic control of spin polarization in multiferroic tunnel junctions
journal, December 2019