Skip to main content
U.S. Department of Energy
Office of Scientific and Technical Information

Phase-Exchange-Driven Wake-Up and Fatigue in Ferroelectric Hafnium Zirconium Oxide Films

Journal Article · · ACS Applied Materials and Interfaces
 [1];  [2];  [3];  [1];  [1];  [1];  [2];  [2];  [2];  [2];  [1]
  1. Univ. of Virginia, Charlottesville, VA (United States)
  2. Sandia National Lab. (SNL-NM), Albuquerque, NM (United States)
  3. Argonne National Lab. (ANL), Lemont, IL (United States). Advanced Photon Source (APS)

Ferroelectric hafnium zirconium oxide holds great promise for a broad spectrum of complementary metal–oxide–semiconductor (CMOS) compatible and scaled microelectronic applications, including memory, low-voltage transistors, and infrared sensors, among others. An outstanding challenge hindering the implementation of this material is polarization instability during field cycling. Herein, the nanoscale phenomena contributing to both polarization fatigue and wake-up are reported. Using synchrotron X-ray diffraction, the conversion of non-polar tetragonal and polar orthorhombic phases to a non-polar monoclinic phase while field cycling devices comprising noble metal contacts is observed. This phase exchange accompanies a diminishing ferroelectric remanent polarization and provides device-scale crystallographic evidence of phase exchange leading to ferroelectric fatigue in these structures. A reduction in the full width at half-maximum of the superimposed tetragonal (101) and orthorhombic (111) diffraction reflections is observed to accompany wake-up in structures comprising tantalum nitride and tungsten electrodes. Combined with polarization and relative permittivity measurements, the observed peak narrowing and a shift in position to lower angles is attributed, in part, to a phase exchange of the non-polar tetragonal to the polar orthorhombic phase during wake-up. These results provide insight into the role of electrodes in the performance of hafnium oxide-based ferroelectrics and mechanisms driving wake-up and fatigue, and demonstrate a non-destructive means to characterize the phase changes accompanying polarization instabilities.

Research Organization:
Sandia National Laboratories (SNL-NM), Albuquerque, NM (United States); Argonne National Laboratory (ANL), Argonne, IL (United States). Advanced Photon Source (APS)
Sponsoring Organization:
USDOE National Nuclear Security Administration (NNSA); USDOE Laboratory Directed Research and Development (LDRD) Program; Semiconductor Research Corporation (SRC)
Grant/Contract Number:
AC04-94AL85000; NA0003525; AC02-06CH11357
OSTI ID:
1639052
Alternate ID(s):
OSTI ID: 1798708
Report Number(s):
SAND--2020-6195J; 686741
Journal Information:
ACS Applied Materials and Interfaces, Journal Name: ACS Applied Materials and Interfaces Journal Issue: 23 Vol. 12; ISSN 1944-8244; ISSN 1944-8252
Publisher:
American Chemical Society (ACS)Copyright Statement
Country of Publication:
United States
Language:
English

References (46)

Physical Mechanisms behind the Field-Cycling Behavior of HfO 2 -Based Ferroelectric Capacitors journal May 2016
Structural Changes Underlying Field-Cycling Phenomena in Ferroelectric HfO 2 Thin Films journal July 2016
Domain Pinning: Comparison of Hafnia and PZT Based Ferroelectrics journal March 2017
Effect of Annealing Ferroelectric HfO 2 Thin Films: In Situ, High Temperature X-Ray Diffraction journal May 2018
On the Origin of the Large Remanent Polarization in La:HfO 2 journal September 2019
Ferroelectric properties and switching endurance of Hf 0.5 Zr 0.5 O 2 films on TiN bottom and TiN or RuO 2 top electrodes : Ferroelectric properties and switching endurance of Hf journal February 2014
Surface electrical properties of tungsten oxides in equilibrium with the gas phase journal January 1979
The behaviour of oxygen at metal electrodes in HfO2 based resistive switching devices journal September 2013
Factors Favoring Ferroelectricity in Hafnia: A First-Principles Computational Study journal February 2017
Wake-Up in a Hf 0.5 Zr 0.5 O 2 Film: A Cycle-by-Cycle Emergence of the Remnant Polarization via the Domain Depinning and the Vanishing of the Anomalous Polarization Switching journal February 2019
Effect of Zr Content on the Wake-Up Effect in Hf 1– x Zr x O 2 Films journal June 2016
Electric Field Cycling Behavior of Ferroelectric Hafnium Oxide journal October 2014
Unveiling the double-well energy landscape in a ferroelectric layer journal January 2019
Enhanced ferroelectricity in ultrathin films grown directly on silicon journal April 2020
A study on the wake-up effect of ferroelectric Hf 0.5 Zr 0.5 O 2 films by pulse-switching measurement journal January 2016
Ferroelectric La‐Sr‐Co‐O/Pb‐Zr‐Ti‐O/La‐Sr‐Co‐O heterostructures on silicon via template growth journal December 1993
Polycrystalline La 0.5 Sr 0.5 CoO 3 /PbZr 0.53 Ti 0.47 O 3 / La 0.5 Sr 0.5 CoO 3 ferroelectric capacitors on platinized silicon with no polarization fatigue journal May 1994
Quantitative measurement of space‐charge effects in lead zirconate‐titanate memories journal July 1991
Identification of passive layer in ferroelectric thin films from their switching parameters journal August 1995
Ferroelectricity in hafnium oxide thin films journal September 2011
Ferroelectric Zr 0.5 Hf 0.5 O 2 thin films for nonvolatile memory applications journal September 2011
Evidence of domain wall contribution to the dielectric permittivity in PZT thin films at sub-switching fields journal August 1997
Wake-up effects in Si-doped hafnium oxide ferroelectric thin films journal November 2013
Chemical solution deposition of ferroelectric yttrium-doped hafnium oxide films on platinum electrodes journal May 2014
TaN interface properties and electric field cycling effects on ferroelectric Si-doped HfO 2 thin films journal April 2015
Stabilizing the ferroelectric phase in doped hafnium oxide journal August 2015
Evidence for oxygen vacancies movement during wake-up in ferroelectric hafnium oxide journal January 2016
Impact of mechanical stress on ferroelectricity in (Hf 0.5 Zr 0.5 )O 2 thin films journal June 2016
In-situ transmission electron microscopy study of oxygen vacancy ordering and dislocation annihilation in undoped and Sm-doped CeO 2 ceramics during redox processes journal December 2016
Pyroelectric response in crystalline hafnium zirconium oxide (Hf 1- x Zr x O 2 ) thin films journal February 2017
Tunneling electroresistance effect in a Pt/Hf 0.5 Zr 0.5 O 2 /Pt structure journal February 2017
Pulse wake-up and breakdown investigation of ferroelectric yttrium doped HfO 2 journal April 2017
Modeling ferroelectric film properties and size effects from tetragonal interlayer in Hf 1– x Zr x O 2 grains journal May 2017
Evolution of ferroelectric HfO2 in ultrathin region down to 3 nm journal March 2018
On the relationship between field cycling and imprint in ferroelectric Hf 0.5 Zr 0.5 O 2 journal May 2018
Nanoscopic studies of domain structure dynamics in ferroelectric La:HfO 2 capacitors journal May 2018
Thickness scaling of pyroelectric response in thin ferroelectric Hf 1− x Zr x O 2 films journal October 2018
Ferroelectricity mediated by ferroelastic domain switching in HfO 2 -based epitaxial thin films journal November 2018
Physical chemistry of the TiN/Hf 0.5 Zr 0.5 O 2 interface journal February 2020
The effect of the bottom electrode on ferroelectric tunnel junctions based on CMOS-compatible HfO 2 journal June 2018
Ten-Nanometer Ferroelectric $\hbox{Si:HfO}_{2}$ Films for Next-Generation FRAM Capacitors journal September 2012
Exploring New Metal Electrodes for Ferroelectric Aluminum-Doped Hafnium Oxide journal May 2019
Electronic and Ionic Trapping at Domain Walls in BaTiO3 journal October 1994
Scaling Effects in Perovskite Ferroelectrics: Fundamental Limits and Process-Structure-Property Relations journal July 2016
Realizing ferroelectric Hf 0.5 Zr 0.5 O 2 with elemental capping layers
  • Lin, Yuh-Chen; McGuire, Felicia; Franklin, Aaron D.
  • Journal of Vacuum Science & Technology B, Nanotechnology and Microelectronics: Materials, Processing, Measurement, and Phenomena, Vol. 36, Issue 1 https://doi.org/10.1116/1.5002558
journal January 2018
Contribution of electrodes and microstructures to the electrical properties of Pb(Zr 0.53 Ti 0.47 )O 3 thin film capacitors journal November 1994