Analysis of Performance Instabilities of Hafnia-Based Ferroelectrics Using Modulus Spectroscopy and Thermally Stimulated Depolarization Currents
Abstract
The discovery of the ferroelectric orthorhombic phase in doped hafnia films has sparked immense research efforts. Presently, a major obstacle for hafnia's use in high-endurance memory applications like nonvolatile random-access memories is its unstable ferroelectric response during field cycling. Different mechanisms are proposed to explain this instability including field-induced phase change, electron trapping, and oxygen vacancy diffusion. However, none of these is able to fully explain the complete behavior and interdependencies of these phenomena. Up to now, no complete root cause for fatigue, wake-up, and imprint effects is presented. In this study, the first evidence for the presence of singly and doubly positively charged oxygen vacancies in hafnia–zirconia films using thermally stimulated currents and impedance spectroscopy is presented. Moreover, it is shown that interaction of these defects with electrons at the interfaces to the electrodes may cause the observed instability of the ferroelectric performance.
- Authors:
-
[1];
[2];
[3];
[5];
[1]
- NaMLab gGmbH, Dresden (Germany)
- Lab. de Céramique, Lausanne (Switzerland)
- North Carolina State Univ., Raleigh, NC (United States)
- Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
- Dresden Univ. of Technology (Germany)
- Publication Date:
- Research Org.:
- Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
- Sponsoring Org.:
- USDOE
- OSTI Identifier:
- 1470841
- Grant/Contract Number:
- AC05-00OR22725
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Advanced Electronic Materials
- Additional Journal Information:
- Journal Volume: 4; Journal Issue: 3; Journal ID: ISSN 2199-160X
- Publisher:
- Wiley
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 36 MATERIALS SCIENCE
Citation Formats
Fengler, Franz P. G., Nigon, Robin, Muralt, Paul, Grimley, Everett D., Sang, Xiahan, Sessi, Violetta, Hentschel, Rico, LeBeau, James M., Mikolajick, Thomas, and Schroeder, Uwe. Analysis of Performance Instabilities of Hafnia-Based Ferroelectrics Using Modulus Spectroscopy and Thermally Stimulated Depolarization Currents. United States: N. p., 2018.
Web. doi:10.1002/aelm.201700547.
Fengler, Franz P. G., Nigon, Robin, Muralt, Paul, Grimley, Everett D., Sang, Xiahan, Sessi, Violetta, Hentschel, Rico, LeBeau, James M., Mikolajick, Thomas, & Schroeder, Uwe. Analysis of Performance Instabilities of Hafnia-Based Ferroelectrics Using Modulus Spectroscopy and Thermally Stimulated Depolarization Currents. United States. https://doi.org/10.1002/aelm.201700547
Fengler, Franz P. G., Nigon, Robin, Muralt, Paul, Grimley, Everett D., Sang, Xiahan, Sessi, Violetta, Hentschel, Rico, LeBeau, James M., Mikolajick, Thomas, and Schroeder, Uwe. Thu .
"Analysis of Performance Instabilities of Hafnia-Based Ferroelectrics Using Modulus Spectroscopy and Thermally Stimulated Depolarization Currents". United States. https://doi.org/10.1002/aelm.201700547. https://www.osti.gov/servlets/purl/1470841.
@article{osti_1470841,
title = {Analysis of Performance Instabilities of Hafnia-Based Ferroelectrics Using Modulus Spectroscopy and Thermally Stimulated Depolarization Currents},
author = {Fengler, Franz P. G. and Nigon, Robin and Muralt, Paul and Grimley, Everett D. and Sang, Xiahan and Sessi, Violetta and Hentschel, Rico and LeBeau, James M. and Mikolajick, Thomas and Schroeder, Uwe},
abstractNote = {The discovery of the ferroelectric orthorhombic phase in doped hafnia films has sparked immense research efforts. Presently, a major obstacle for hafnia's use in high-endurance memory applications like nonvolatile random-access memories is its unstable ferroelectric response during field cycling. Different mechanisms are proposed to explain this instability including field-induced phase change, electron trapping, and oxygen vacancy diffusion. However, none of these is able to fully explain the complete behavior and interdependencies of these phenomena. Up to now, no complete root cause for fatigue, wake-up, and imprint effects is presented. In this study, the first evidence for the presence of singly and doubly positively charged oxygen vacancies in hafnia–zirconia films using thermally stimulated currents and impedance spectroscopy is presented. Moreover, it is shown that interaction of these defects with electrons at the interfaces to the electrodes may cause the observed instability of the ferroelectric performance.},
doi = {10.1002/aelm.201700547},
journal = {Advanced Electronic Materials},
number = 3,
volume = 4,
place = {United States},
year = {2018},
month = {2}
}
Free Publicly Available Full Text
Publisher's Version of Record
Other availability
Search WorldCat to find libraries that may hold this journal
Cited by: 11 works
Citation information provided by
Web of Science
Web of Science
Save to My Library
You must Sign In or Create an Account in order to save documents to your library.
Works referenced in this record:
Impact of interface variations on J–V and C–V polarity asymmetry of MIM capacitors with amorphous and crystalline Zr(1−x)AlxO2 films
journal, July 2009
- Weinreich, W.; Reiche, R.; Lemberger, M.
- Microelectronic Engineering, Vol. 86, Issue 7-9
Optimizing process conditions for improved Hf1−xZrxO2 ferroelectric capacitor performance
journal, June 2017
- Mittmann, Terence; Fengler, Franz P. G.; Richter, Claudia
- Microelectronic Engineering, Vol. 178
Ferroelectric hafnium oxide: A CMOS-compatible and highly scalable approach to future ferroelectric memories
conference, December 2013
- Muller, J.; Boscke, T. S.; Muller, S.
- 2013 IEEE International Electron Devices Meeting (IEDM)
Vacancy and interstitial defects in hafnia
journal, May 2002
- Foster, A. S.; Lopez Gejo, F.; Shluger, A. L.
- Physical Review B, Vol. 65, Issue 17
Ultrathin Hf 0.5 Zr 0.5 O 2 Ferroelectric Films on Si
journal, March 2016
- Chernikova, Anna; Kozodaev, Maksim; Markeev, Andrei
- ACS Applied Materials & Interfaces, Vol. 8, Issue 11
On the structural origins of ferroelectricity in HfO 2 thin films
journal, April 2015
- Sang, Xiahan; Grimley, Everett D.; Schenk, Tony
- Applied Physics Letters, Vol. 106, Issue 16
Electric Field Cycling Behavior of Ferroelectric Hafnium Oxide
journal, October 2014
- Schenk, Tony; Schroeder, Uwe; Pešić, Milan
- ACS Applied Materials & Interfaces, Vol. 6, Issue 22
Defect ordering and defect–domain-wall interactions in PbTiO : A first-principles study
journal, December 2013
- Chandrasekaran, Anand; Damjanovic, Dragan; Setter, Nava
- Physical Review B, Vol. 88, Issue 21
Overview of emerging semiconductor non-volatile memories
journal, January 2012
- Fujisaki, Yoshihisa
- IEICE Electronics Express, Vol. 9, Issue 10
Impact of charge trapping on the ferroelectric switching behavior of doped HfO 2 : Trapping influence on the ferroelectric switching
journal, October 2015
- Pešić, Milan; Slesazeck, Stefan; Schenk, Tony
- physica status solidi (a), Vol. 213, Issue 2
Atomic Layer Deposition of Gd-Doped HfO[sub 2] Thin Films
journal, January 2010
- Adelmann, C.; Tielens, H.; Dewulf, D.
- Journal of The Electrochemical Society, Vol. 157, Issue 4
Pulse wake-up and breakdown investigation of ferroelectric yttrium doped HfO 2
journal, April 2017
- Starschich, S.; Menzel, S.; Böttger, U.
- Journal of Applied Physics, Vol. 121, Issue 15
Dielectric relaxation, resonance and scaling behaviors in Sr3Co2Fe24O41 hexaferrite
journal, August 2015
- Tang, Rujun; Jiang, Chen; Qian, Wenhu
- Scientific Reports, Vol. 5, Issue 1
Migration of oxygen vacancy in HfO2 and across the HfO2∕SiO2 interface: A first-principles investigation
journal, November 2007
- Capron, Nathalie; Broqvist, Peter; Pasquarello, Alfredo
- Applied Physics Letters, Vol. 91, Issue 19
Low leakage ZrO 2 based capacitors for sub 20 nm dynamic random access memory technology nodes
journal, February 2016
- Pešić, Milan; Knebel, Steve; Geyer, Maximilian
- Journal of Applied Physics, Vol. 119, Issue 6
On the origin of capacitance dispersion of rough electrodes
journal, November 2000
- Kerner, Zsolt; Pajkossy, Tamás
- Electrochimica Acta, Vol. 46, Issue 2-3
Effect of Zr Content on the Wake-Up Effect in Hf 1– x Zr x O 2 Films
journal, June 2016
- Park, Min Hyuk; Kim, Han Joon; Kim, Yu Jin
- ACS Applied Materials & Interfaces, Vol. 8, Issue 24
Atom Column Indexing: Atomic Resolution Image Analysis Through a Matrix Representation
journal, November 2014
- Sang, Xiahan; Oni, Adedapo A.; LeBeau, James M.
- Microscopy and Microanalysis, Vol. 20, Issue 6
On the theory of the universal dielectric relaxation
journal, April 2014
- Fu, John Y.
- Philosophical Magazine, Vol. 94, Issue 16
Investigation of the amorphous to crystalline phase transition of chemical solution deposited Pb(Zr0.3Ti0.7)O3 thin films by soft X-ray absorption and soft X-ray emission spectroscopy
journal, September 2008
- Schneller, T.; Kohlstedt, H.; Petraru, A.
- Journal of Sol-Gel Science and Technology, Vol. 48, Issue 1-2
Modelling of thermally stimulated depolarization current peaks obtained by global and thermal cleaning experiments
journal, October 1998
- Mano, João F.
- Journal of Physics D: Applied Physics, Vol. 31, Issue 20
An asymmetric double-well potential model for structural relaxation processes in amorphous materials
journal, May 1981
- Gilroy, K. S.; Phillips, W. A.
- Philosophical Magazine B, Vol. 43, Issue 5
Complex Internal Bias Fields in Ferroelectric Hafnium Oxide
journal, August 2015
- Schenk, Tony; Hoffmann, Michael; Ocker, Johannes
- ACS Applied Materials & Interfaces, Vol. 7, Issue 36
Physical Mechanisms behind the Field-Cycling Behavior of HfO 2 -Based Ferroelectric Capacitors
journal, May 2016
- Pešić, Milan; Fengler, Franz Paul Gustav; Larcher, Luca
- Advanced Functional Materials, Vol. 26, Issue 25
Si Doped Hafnium Oxide-A “Fragile” Ferroelectric System
journal, August 2017
- Richter, Claudia; Schenk, Tony; Park, Min Hyuk
- Advanced Electronic Materials, Vol. 3, Issue 10
Defect energy levels in HfO2 high-dielectric-constant gate oxide
journal, October 2005
- Xiong, K.; Robertson, J.; Gibson, M. C.
- Applied Physics Letters, Vol. 87, Issue 18
The DC resistivity of modified PZT ceramics
journal, May 1983
- Wu, Long; Wu, Tien-Shou; Wei, Chung-Chuang
- Journal of Physics C: Solid State Physics, Vol. 16, Issue 14
Ferroelectricity in Gd-Doped HfO 2 Thin Films
journal, January 2012
- Mueller, S.; Adelmann, C.; Singh, A.
- ECS Journal of Solid State Science and Technology, Vol. 1, Issue 6
Incipient Ferroelectricity in Al-Doped HfO2 Thin Films
journal, March 2012
- Mueller, Stefan; Mueller, Johannes; Singh, Aarti
- Advanced Functional Materials, Vol. 22, Issue 11
Structural Changes Underlying Field-Cycling Phenomena in Ferroelectric HfO 2 Thin Films
journal, July 2016
- Grimley, Everett D.; Schenk, Tony; Sang, Xiahan
- Advanced Electronic Materials, Vol. 2, Issue 9
Dynamic observation of oxygen vacancies in hafnia layer by in situ transmission electron microscopy
journal, September 2015
- Li, Chao; Yao, Yuan; Shen, Xi
- Nano Research, Vol. 8, Issue 11
Structural and dynamic properties of oxygen vacancies in perovskite oxides—analysis of defect chemistry by modern multi-frequency and pulsed EPR techniques
journal, January 2011
- Eichel, Rüdiger-A.
- Phys. Chem. Chem. Phys., Vol. 13, Issue 2
Stabilizing the ferroelectric phase in doped hafnium oxide
journal, August 2015
- Hoffmann, M.; Schroeder, U.; Schenk, T.
- Journal of Applied Physics, Vol. 118, Issue 7
Overview of emerging nonvolatile memory technologies
journal, January 2014
- Meena, Jagan; Sze, Simon; Chand, Umesh
- Nanoscale Research Letters, Vol. 9, Issue 1
Oxygen migration during resistance switching and failure of hafnium oxide memristors
journal, March 2017
- Kumar, Suhas; Wang, Ziwen; Huang, Xiaopeng
- Applied Physics Letters, Vol. 110, Issue 10
Ferroelectricity in hafnium oxide thin films
journal, September 2011
- Böscke, T. S.; Müller, J.; Bräuhaus, D.
- Applied Physics Letters, Vol. 99, Issue 10
Charge migration in Pb(Zr,Ti)O3 ceramics and its relation to ageing, hardening, and softening
journal, February 2010
- Morozov, M. I.; Damjanovic, D.
- Journal of Applied Physics, Vol. 107, Issue 3
Ferroelectricity in yttrium-doped hafnium oxide
journal, December 2011
- Müller, J.; Schröder, U.; Böscke, T. S.
- Journal of Applied Physics, Vol. 110, Issue 11
Thermally Stimulated Characteristics in Solid Dielectrics
journal, June 1980
- Hino, Taro
- IEEE Transactions on Electrical Insulation, Vol. EI-15, Issue 3
Oxygen vacancy in monoclinic HfO2: A consistent interpretation of trap assisted conduction, direct electron injection, and optical absorption experiments
journal, December 2006
- Broqvist, Peter; Pasquarello, Alfredo
- Applied Physics Letters, Vol. 89, Issue 26
Thermally Stimulated Relaxation in Fe-Doped SrTiO 3 Systems:I. Single Crystals
journal, October 2008
- Liu, Wayne; Randall, Clive A.
- Journal of the American Ceramic Society, Vol. 91, Issue 10
Strontium doped hafnium oxide thin films: Wide process window for ferroelectric memories
conference, September 2013
- Schenk, T.; Mueller, S.; Schroeder, U.
- 2013 43rd European Solid-State Device Research Conference (ESSDERC), 2013 Proceedings of the European Solid-State Device Research Conference (ESSDERC)
Domain Pinning: Comparison of Hafnia and PZT Based Ferroelectrics
journal, March 2017
- Fengler, Franz P. G.; Pešić, Milan; Starschich, Sergej
- Advanced Electronic Materials, Vol. 3, Issue 4
Ferroelectricity in Simple Binary ZrO 2 and HfO 2
journal, July 2012
- Müller, Johannes; Böscke, Tim S.; Schröder, Uwe
- Nano Letters, Vol. 12, Issue 8
Dielectric and electric modulus properties of vacuum evaporated Cd0.8Zn0.2Te thin films
journal, April 2003
- Prabakar, K.; Narayandass, Sa. K.; Mangalaraj, D.
- Materials Science and Engineering: B, Vol. 98, Issue 3
Oxygen migration during resistance switching and failure of hafnium oxide memristors
text, January 2017
- Kumar, Suhas; Wang, Ziwen; Huang, Xiaopeng
- arXiv
Works referencing / citing this record:
Origin of Ferroelectric Phase in Undoped HfO 2 Films Deposited by Sputtering
journal, April 2019
- Mittmann, Terence; Materano, Monica; Lomenzo, Patrick D.
- Advanced Materials Interfaces
Investigating structural features of Ba and Zr co-substituted strontium bismuth tantalate thin films
journal, February 2019
- Bozgeyik, Mehmet S.
- Bulletin of Materials Science, Vol. 42, Issue 2
Polarization-dependent electric potential distribution across nanoscale ferroelectric Hf 0.5 Zr 0.5 O 2 in functional memory capacitors
journal, January 2019
- Matveyev, Yury; Mikheev, Vitalii; Negrov, Dmitry
- Nanoscale, Vol. 11, Issue 42
Pyroelectricity of silicon-doped hafnium oxide thin films
journal, April 2018
- Jachalke, Sven; Schenk, Tony; Park, Min Hyuk
- Applied Physics Letters, Vol. 112, Issue 14
On the relationship between field cycling and imprint in ferroelectric Hf 0.5 Zr 0.5 O 2
journal, May 2018
- Fengler, F. P. G.; Hoffmann, M.; Slesazeck, S.
- Journal of Applied Physics, Vol. 123, Issue 20
Model of dielectric breakdown in hafnia-based ferroelectric capacitors
journal, July 2018
- Xue, Kan-Hao; Su, Hai-Lei; Li, Yi
- Journal of Applied Physics, Vol. 124, Issue 2
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
Review and perspective on ferroelectric HfO2-based thin films for memory applications
journal, August 2018
- Park, Min Hyuk; Lee, Young Hwan; Mikolajick, Thomas
- MRS Communications, Vol. 8, Issue 03
Origin of Ferroelectric Phase in Undoped HfO 2 Films Deposited by Sputtering
journal, August 2019
- Mittmann, Terence; Materano, Monica; Lomenzo, Patrick D.
- Advanced Materials Interfaces, Vol. 6, Issue 20