Mechanism of Antiferroelectricity in Polycrystalline ZrO2

Ganser, Richard; Lomenzo, Patrick D.; Collins, Liam; Xu, Bohan; Antunes, Luis Azevedo; Mikolajick, Thomas; Schroeder, Uwe; Kersch, Alfred

doi:10.1002/adfm.202405513

Mechanism of Antiferroelectricity in Polycrystalline ZrO₂

Journal Article · Fri Jun 28 00:00:00 EDT 2024 · Advanced Functional Materials

DOI:https://doi.org/10.1002/adfm.202405513· OSTI ID:2538418

^[1]; Lomenzo, Patrick D. ^[2]; ^[3]; Xu, Bohan ^[2]; Antunes, Luis Azevedo ^[1]; Mikolajick, Thomas ^[4]; Schroeder, Uwe ^[2]; ^[1]

Munich Univ. of Applied Sciences (Germany)
NaMLab, Dresden (Germany)
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Sciences (CNMS)
NaMLab, Dresden (Germany); Technische Universität Dresden (Germany)

The size and electric field dependent induction of polarization in antiferroelectric ZrO₂ is the key to several technological applications that are unimaginable a decade ago. However, the lack of a deeper understanding of the mechanism hinders progress. Molecular dynamics simulations of polycrystalline ZrO₂, based on machine-learned interatomic forces with near ab initio quality, shed light on the fundamental mechanism of the size effect on the transition fields. Stress in the oxygen sublattice is the most important factor. The so constructed interatomic forces allow the calculation of the transition fields as a function of the ZrO₂ film thickness and predict the ferroelectricity at large thickness. The simulation results are validated with electrical and piezo response force microscopy measurements. The results allow a clear interpretation of the properties of the double-hysteresis loops as well as the construction of the free energy landscape of ZrO₂ grains.

View Accepted Manuscript (DOE)

Research Organization:: Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: AC05-00OR22725

OSTI ID:: 2538418

Journal Information:: Advanced Functional Materials, Journal Name: Advanced Functional Materials Journal Issue: 40 Vol. 34; ISSN 1616-301X

Publisher:: WileyCopyright Statement

Country of Publication:: United States

Language:: English

References (47)

Discovery of Nanoscale Electric Field‐Induced Phase Transitions in ZrO₂ Lomenzo, Patrick D.; Collins, Liam; Ganser, Richard Advanced Functional Materials, Vol. 33, Issue 41 https://doi.org/10.1002/adfm.202303636	journal	June 2023
Insights Into Curie‐Temperature and Phase Formation of Ferroelectric Hf_1−xZr_xO₂with Oxygen Defects from a Leveled Energy Landscape Azevedo Antunes, Luis; Ganser, Richard; Schroeder, Uwe Advanced Materials Interfaces, Vol. 11, Issue 2 https://doi.org/10.1002/admi.202300710	journal	November 2023
Structural Changes Underlying Field-Cycling Phenomena in Ferroelectric HfO ₂ Thin Films Grimley, Everett D.; Schenk, Tony; Sang, Xiahan Advanced Electronic Materials, Vol. 2, Issue 9 https://doi.org/10.1002/aelm.201600173	journal	July 2016
Nucleation-Limited Ferroelectric Orthorhombic Phase Formation in Hf _0.5 Zr _0.5 O ₂ Thin Films Lee, Young Hwan; Hyun, Seung Dam; Kim, Hae Jin Advanced Electronic Materials, Vol. 5, Issue 2 https://doi.org/10.1002/aelm.201800436	journal	December 2018
Thermodynamic and Kinetic Origins of Ferroelectricity in Fluorite Structure Oxides Park, Min Hyuk; Lee, Young Hwan; Mikolajick, Thomas Advanced Electronic Materials, Vol. 5, Issue 3 https://doi.org/10.1002/aelm.201800522	journal	December 2018
Harnessing Phase Transitions in Antiferroelectric ZrO ₂ Using the Size Effect Lomenzo, Patrick D.; Materano, Monica; Mittmann, Terence Advanced Electronic Materials, Vol. 8, Issue 1 https://doi.org/10.1002/aelm.202100556	journal	October 2021
LAMMPS - a flexible simulation tool for particle-based materials modeling at the atomic, meso, and continuum scales Thompson, Aidan P.; Aktulga, H. Metin; Berger, Richard Computer Physics Communications, Vol. 271 https://doi.org/10.1016/j.cpc.2021.108171	journal	February 2022
A deep-neural network potential to study transformation-induced plasticity in zirconia Zhang, Jin-Yu; Huynh, Gaël; Dai, Fu-Zhi Journal of the European Ceramic Society, Vol. 44, Issue 6 https://doi.org/10.1016/j.jeurceramsoc.2024.01.007	journal	June 2024
Phase transitions in ferroelectric ZrO2 thin films Pereira, Rui M. P.; Istrate, Marian C.; Figueiras, Fábio G. Materials Science in Semiconductor Processing, Vol. 172 https://doi.org/10.1016/j.mssp.2023.108102	journal	March 2024
Toward a multifunctional monolithic device based on pyroelectricity and the electrocaloric effect of thin antiferroelectric Hf x Zr 1−x O 2 films Park, Min Hyuk; Kim, Han Joon; Kim, Yu Jin Nano Energy, Vol. 12 https://doi.org/10.1016/j.nanoen.2014.09.025	journal	March 2015
Ferroelectric phase transitions in nanoscale HfO 2 films enable giant pyroelectric energy conversion and highly efficient supercapacitors Hoffmann, Michael; Schroeder, Uwe; Künneth, Christopher Nano Energy, Vol. 18 https://doi.org/10.1016/j.nanoen.2015.10.005	journal	November 2015
Influence of Si-Doping on 45 nm Thick Ferroelectric ZrO₂ Films Xu, Bohan; Lomenzo, Patrick D.; Kersch, Alfred ACS Applied Electronic Materials, Vol. 4, Issue 7 https://doi.org/10.1021/acsaelm.2c00608	journal	July 2022
Emerging Fluorite-Structured Antiferroelectrics and Their Semiconductor Applications Park, Geun Hyeong; Lee, Dong Hyun; Choi, Hyojun ACS Applied Electronic Materials, Vol. 5, Issue 2 https://doi.org/10.1021/acsaelm.2c01615	journal	February 2023
Local Epitaxial Templating Effects in Ferroelectric and Antiferroelectric ZrO₂ Chae, Kisung; Lombardo, Sarah F.; Tasneem, Nujhat ACS Applied Materials & Interfaces, Vol. 14, Issue 32 https://doi.org/10.1021/acsami.2c03151	journal	August 2022
The Occurrence of Metastable Tetragonal Zirconia as a Crystallite Size Effect Garvie, Ronald C. The Journal of Physical Chemistry, Vol. 69, Issue 4 https://doi.org/10.1021/j100888a024	journal	April 1965
Ferroelectricity in Simple Binary ZrO ₂ and HfO ₂ Müller, Johannes; Böscke, Tim S.; Schröder, Uwe Nano Letters, Vol. 12, Issue 8 https://doi.org/10.1021/nl302049k	journal	July 2012
Antiferroelectric negative capacitance from a structural phase transition in zirconia Hoffmann, Michael; Wang, Zheng; Tasneem, Nujhat Nature Communications, Vol. 13, Issue 1 https://doi.org/10.1038/s41467-022-28860-1	journal	March 2022
First demonstration of in-memory computing crossbar using multi-level Cell FeFET Soliman, Taha; Chatterjee, Swetaki; Laleni, Nellie Nature Communications, Vol. 14, Issue 1 https://doi.org/10.1038/s41467-023-42110-y	journal	October 2023
Thermal transport and phase transitions of zirconia by on-the-fly machine-learned interatomic potentials Verdi, Carla; Karsai, Ferenc; Liu, Peitao npj Computational Materials, Vol. 7, Issue 1 https://doi.org/10.1038/s41524-021-00630-5	journal	September 2021
Kinetically stabilized ferroelectricity in bulk single-crystalline HfO2:Y Xu, Xianghan; Huang, Fei-Ting; Qi, Yubo Nature Materials, Vol. 20, Issue 6 https://doi.org/10.1038/s41563-020-00897-x	journal	January 2021
The fundamentals and applications of ferroelectric HfO2 Schroeder, Uwe; Park, Min Hyuk; Mikolajick, Thomas Nature Reviews Materials, Vol. 7, Issue 8 https://doi.org/10.1038/s41578-022-00431-2	journal	March 2022
Surface and grain boundary energy as the key enabler of ferroelectricity in nanoscale hafnia-zirconia: a comparison of model and experiment Park, Min Hyuk; Lee, Young Hwan; Kim, Han Joon Nanoscale, Vol. 9, Issue 28 https://doi.org/10.1039/C7NR02121F	journal	January 2017
Ferroelectricity in hafnium oxide thin films Böscke, T. S.; Müller, J.; Bräuhaus, D. Applied Physics Letters, Vol. 99, Issue 10 https://doi.org/10.1063/1.3634052	journal	September 2011
The origin of ferroelectricity in Hf _1−x Zr _x O ₂ : A computational investigation and a surface energy model Materlik, R.; Künneth, C.; Kersch, A. Journal of Applied Physics, Vol. 117, Issue 13 https://doi.org/10.1063/1.4916707	journal	April 2015
Growth of epitaxial orthorhombic YO _1.5 -substituted HfO ₂ thin film Shimizu, Takao; Katayama, Kiliha; Kiguchi, Takanori Applied Physics Letters, Vol. 107, Issue 3 https://doi.org/10.1063/1.4927450	journal	July 2015
Stability of ferroelectric and antiferroelectric hafnium–zirconium oxide thin films Chae, Kisung; Hwang, Jeongwoon; Chagarov, Evgueni Journal of Applied Physics, Vol. 128, Issue 5 https://doi.org/10.1063/5.0011547	journal	August 2020
A Gibbs energy view of double hysteresis in ZrO ₂ and Si-doped HfO ₂ Lomenzo, Patrick D.; Materano, Monica; Richter, Claudia Applied Physics Letters, Vol. 117, Issue 14 https://doi.org/10.1063/5.0018199	journal	October 2020
Ab initio interphase characteristics in HfO₂ and ZrO₂ and nucleation of the polar phase Falkowski, Max; Kersch, Alfred Applied Physics Letters, Vol. 118, Issue 3 https://doi.org/10.1063/5.0029610	journal	January 2021
Progress and future prospects of negative capacitance electronics: A materials perspective Hoffmann, Michael; Slesazeck, Stefan; Mikolajick, Thomas APL Materials, Vol. 9, Issue 2 https://doi.org/10.1063/5.0032954	journal	February 2021
Polarization switching in thin doped HfO₂ ferroelectric layers Materano, Monica; Lomenzo, Patrick D.; Mulaosmanovic, Halid Applied Physics Letters, Vol. 117, Issue 26 https://doi.org/10.1063/5.0035100	journal	December 2020
Antiferroelectric properties of ZrO₂ ultra-thin films prepared by atomic layer deposition Luo, Xuan; Toprasertpong, Kasidit; Takenaka, Mitsuru Applied Physics Letters, Vol. 118, Issue 23 https://doi.org/10.1063/5.0051068	journal	June 2021
Pyroelectric dependence of atomic layer-deposited Hf_0.5Zr_0.5O₂ on film thickness and annealing temperature Lomenzo, Patrick D.; Alcala, Ruben; Richter, Claudia Applied Physics Letters, Vol. 119, Issue 11 https://doi.org/10.1063/5.0062789	journal	September 2021
The effect of stress on HfO2-based ferroelectric thin films: A review of recent advances Han, Runhao; Hong, Peizhen; Ning, Shuai Journal of Applied Physics, Vol. 133, Issue 24 https://doi.org/10.1063/5.0146998	journal	June 2023
Roadmap on ferroelectric hafnia- and zirconia-based materials and devices Silva, José P. B.; Alcala, Ruben; Avci, Uygar E. APL Materials, Vol. 11, Issue 8 https://doi.org/10.1063/5.0148068	journal	August 2023
Comprehensive interpretations of thermodynamic and kinetic effects on the phase fractions in Hf1-xZrxO2 by first principle calculations Ye, Kun Hee; Yeu, In Won; Han, Gyuseung Applied Physics Reviews, Vol. 10, Issue 3 https://doi.org/10.1063/5.0160719	journal	September 2023
Mechanisms of polarization switching in ferroelectric thin films Tagantsev, Alexander K. Ferroelectrics, Vol. 184, Issue 1 https://doi.org/10.1080/00150199608230247	journal	August 1996
Piezo- and Pyroelectricity in Zirconia: A Study with Machine-Learned Force Fields Ganser, Richard; Bongarz, Simon; von Mach, Alexander Physical Review Applied, Vol. 18, Issue 5 https://doi.org/10.1103/PhysRevApplied.18.054066	journal	November 2022
Modular development of deep potential for complex solid solutions Wu, Jing; Yang, Jiyuan; Ma, Liyang Physical Review B, Vol. 107, Issue 14 https://doi.org/10.1103/PhysRevB.107.144102	journal	April 2023
Ab initiomolecular dynamics for liquid metals Kresse, G.; Hafner, J. Physical Review B, Vol. 47, Issue 1, p. 558-561 https://doi.org/10.1103/PhysRevB.47.558	journal	January 1993
Antiferroelectricity in thin-film ZrO 2 from first principles Reyes-Lillo, Sebastian E.; Garrity, Kevin F.; Rabe, Karin M. Physical Review B, Vol. 90, Issue 14 https://doi.org/10.1103/PhysRevB.90.140103	journal	October 2014
Restoring the Density-Gradient Expansion for Exchange in Solids and Surfaces Perdew, John P.; Ruzsinszky, Adrienn; Csonka, Gábor I. Physical Review Letters, Vol. 100, Issue 13 https://doi.org/10.1103/PhysRevLett.100.136406	journal	April 2008
Quantum Thermal Bath for Molecular Dynamics Simulation Dammak, Hichem; Chalopin, Yann; Laroche, Marine Physical Review Letters, Vol. 103, Issue 19 https://doi.org/10.1103/PhysRevLett.103.190601	journal	November 2009
Deep Potential Molecular Dynamics: A Scalable Model with the Accuracy of Quantum Mechanics Zhang, Linfeng; Han, Jiequn; Wang, Han Physical Review Letters, Vol. 120, Issue 14 https://doi.org/10.1103/PhysRevLett.120.143001	journal	April 2018
Thickness dependence of phase stability in epitaxial (HfxZr1−x)O2 films Mimura, Takanori; Shimizu, Takao; Sakata, Osami Physical Review Materials, Vol. 5, Issue 11 https://doi.org/10.1103/PhysRevMaterials.5.114407	journal	November 2021
Stabilization of the epitaxial rhombohedral ferroelectric phase in ZrO2 by surface energy El Boutaybi, Ali; Maroutian, Thomas; Largeau, Ludovic Physical Review Materials, Vol. 6, Issue 7 https://doi.org/10.1103/PhysRevMaterials.6.074406	journal	July 2022
Scale-free ferroelectricity induced by flat phonon bands in HfO ₂ Lee, Hyun-Jae; Lee, Minseong; Lee, Kyoungjun Science, Vol. 369, Issue 6509 https://doi.org/10.1126/science.aba0067	journal	July 2020
First-principles Phonon Calculations with Phonopy and Phono3py Togo, Atsushi Journal of the Physical Society of Japan, Vol. 92, Issue 1 https://doi.org/10.7566/JPSJ.92.012001	journal	January 2023

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