Investigating the Electromechanical Behavior of Unconventionally Ferroelectric Hf0.5Zr0.5O2-Based Capacitors Through Operando Nanobeam X-Ray Diffraction

Evgenios Stylianidis; Pranav Surabhi; Ruben Hamming-Green; Mart Salverda; Yingfen Wei; Arjan Burema; Sylvia Matzen; Tamalika Banerjee; Alexander Björling; Binayak Mukherjee; Sangita Dutta; Hugo Aramberri; Jorge Íñiguez; Beatriz Noheda; Dina Carbone; Pavan Nukala

doi:10.1002/aelm.202201298

Investigating the Electromechanical Behavior of Unconventionally Ferroelectric Hf_0.5Zr_0.5O₂-Based Capacitors Through Operando Nanobeam X-Ray Diffraction

Evgenios Stylianidis, Pranav Surabhi, Ruben Hamming-Green, Mart Salverda, Yingfen Wei, Arjan Burema, Sylvia Matzen, Tamalika Banerjee, Alexander Björling, Binayak Mukherjee, Sangita Dutta, Hugo Aramberri, Jorge Íñiguez, Beatriz Noheda, Dina Carbone^*, Pavan Nukala^*

^*Corresponding author for this work

Research output: Contribution to journal › Article › Academic › peer-review

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Abstract

Understanding various aspects of ferroelectricity in hafnia-based nanomaterials is of vital importance for the development of future nonvolatile memory and logic devices. Here, the unconventional and weak electromechanical response of epitaxial La_0.67Sr_0.33MnO₃/Hf_0.5Zr_0.5O₂/La_0.67Sr_0.33MnO₃ ferroelectric capacitors is investigated, via the sensitivity offered by nanobeam X-ray diffraction experiments during application of electrical bias. It is shown that the pristine rhombohedral phase exhibits a linear piezoelectric effect with piezoelectric coefficient (|d₃₃|) ≈ 0.5–0.8 pmV⁻¹. It is found that the piezoelectric response is suppressed above the coercive voltage. For higher voltages, and with the onset of DC conductivity throughout the capacitor, a second-order effect is observed. The work sheds light into the electromechanical response of rhombohedral Hf_0.5Zr_0.5O₂ and suggests its (un)correlation with ferroelectric switching.

Original language	English
Article number	2201298
Number of pages	7
Journal	Advanced electronic materials
Volume	9
Issue number	6
DOIs	https://doi.org/10.1002/aelm.202201298
Publication status	Published - Jun-2023

Keywords

electrochemical polarization
first-principles
nanobeam diffraction
rhombohedral Hf Zr O

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2201298 (1 of 7)© 2023 The Authors. Advanced Electronic Materials published by Wiley-VCH GmbHwww.advelectronicmat.deInvestigating the Electromechanical Behavior of Unconventionally Ferroelectric Hf0.5Zr0.5O2-Based Capacitors Through Operando Nanobeam X-Ray DiffractionFinal publisher's version, 2.32 MBLicence: CC BY

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Stylianidis, E., Surabhi, P., Hamming-Green, R., Salverda, M., Wei, Y., Burema, A., Matzen, S., Banerjee, T., Björling, A., Mukherjee, B., Dutta, S., Aramberri, H., Íñiguez, J., Noheda, B., Carbone, D., & Nukala, P. (2023). Investigating the Electromechanical Behavior of Unconventionally Ferroelectric Hf_0.5Zr_0.5O₂-Based Capacitors Through Operando Nanobeam X-Ray Diffraction. Advanced electronic materials, 9(6), Article 2201298. https://doi.org/10.1002/aelm.202201298

@article{1639b16eba9d4f67b98e17bdaeb23fd4,

title = "Investigating the Electromechanical Behavior of Unconventionally Ferroelectric Hf0.5Zr0.5O2-Based Capacitors Through Operando Nanobeam X-Ray Diffraction",

abstract = "Understanding various aspects of ferroelectricity in hafnia-based nanomaterials is of vital importance for the development of future nonvolatile memory and logic devices. Here, the unconventional and weak electromechanical response of epitaxial La0.67Sr0.33MnO3/Hf0.5Zr0.5O2/La0.67Sr0.33MnO3 ferroelectric capacitors is investigated, via the sensitivity offered by nanobeam X-ray diffraction experiments during application of electrical bias. It is shown that the pristine rhombohedral phase exhibits a linear piezoelectric effect with piezoelectric coefficient (|d33|) ≈ 0.5–0.8 pmV−1. It is found that the piezoelectric response is suppressed above the coercive voltage. For higher voltages, and with the onset of DC conductivity throughout the capacitor, a second-order effect is observed. The work sheds light into the electromechanical response of rhombohedral Hf0.5Zr0.5O2 and suggests its (un)correlation with ferroelectric switching.",

keywords = "electrochemical polarization, first-principles, nanobeam diffraction, rhombohedral Hf Zr O",

author = "Evgenios Stylianidis and Pranav Surabhi and Ruben Hamming-Green and Mart Salverda and Yingfen Wei and Arjan Burema and Sylvia Matzen and Tamalika Banerjee and Alexander Bj{\"o}rling and Binayak Mukherjee and Sangita Dutta and Hugo Aramberri and Jorge {\'I}{\~n}iguez and Beatriz Noheda and Dina Carbone and Pavan Nukala",

note = "Funding Information: The authors acknowledge MAX IV Laboratory for time on Beamline NanoMAX under Proposal 20190954. Research conducted at MAX IV, a Swedish national user facility, was supported by the Swedish Research Council (under contract grant No. 2018—07152), the Swedish Governmental Agency for Innovation Systems (under contract grant No. 2018–04969), and Formas (under contract grant No. 2019–02496). Work at LIST was supported by the Luxembourg National Research Fund though (grant Nos. INTER/NOW/20/15079143/TRICOLOR (to B.M., H.A., J.I.) and PRIDE/15/10935404/MASSENA (to S.D.). P.N. acknowledges national nanofabrication and micro-nano characterization facilities at the center for nanoscience and engineering, IISc. P.N. also acknowledges SERB grant (SRG/000285) and Infosys Young Scientist Award. B.N. and T.B. acknowledge the financial support of the CogniGron research center and the Ubbo Emmius Funds (University of Groningen). Device fabrication were realized using NanoLab NL facilities. S.M. acknowledges the support from the French RENATECH network for the research at the Center for Nanoscience and Nanotechnology. Funding Information: The authors acknowledge MAX IV Laboratory for time on Beamline NanoMAX under Proposal 20190954. Research conducted at MAX IV, a Swedish national user facility, was supported by the Swedish Research Council (under contract grant No. 2018—07152), the Swedish Governmental Agency for Innovation Systems (under contract grant No. 2018–04969), and Formas (under contract grant No. 2019–02496). Work at LIST was supported by the Luxembourg National Research Fund though (grant Nos. INTER/NOW/20/15079143/TRICOLOR (to B.M., H.A., J.I.) and PRIDE/15/10935404/MASSENA (to S.D.). P.N. acknowledges national nanofabrication and micro‐nano characterization facilities at the center for nanoscience and engineering, IISc. P.N. also acknowledges SERB grant (SRG/000285) and Infosys Young Scientist Award. B.N. and T.B. acknowledge the financial support of the CogniGron research center and the Ubbo Emmius Funds (University of Groningen). Device fabrication were realized using NanoLab NL facilities. S.M. acknowledges the support from the French RENATECH network for the research at the Center for Nanoscience and Nanotechnology. Publisher Copyright: {\textcopyright} 2023 The Authors. Advanced Electronic Materials published by Wiley-VCH GmbH.",

year = "2023",

month = jun,

doi = "10.1002/aelm.202201298",

language = "English",

volume = "9",

journal = "Advanced electronic materials",

issn = "2199-160X",

publisher = "Wiley",

number = "6",

}

Stylianidis, E, Surabhi, P, Hamming-Green, R, Salverda, M, Wei, Y, Burema, A, Matzen, S, Banerjee, T, Björling, A, Mukherjee, B, Dutta, S, Aramberri, H, Íñiguez, J, Noheda, B, Carbone, D & Nukala, P 2023, 'Investigating the Electromechanical Behavior of Unconventionally Ferroelectric Hf_0.5Zr_0.5O₂-Based Capacitors Through Operando Nanobeam X-Ray Diffraction', Advanced electronic materials, vol. 9, no. 6, 2201298. https://doi.org/10.1002/aelm.202201298

Investigating the Electromechanical Behavior of Unconventionally Ferroelectric Hf_0.5Zr_0.5O₂-Based Capacitors Through Operando Nanobeam X-Ray Diffraction. / Stylianidis, Evgenios; Surabhi, Pranav; Hamming-Green, Ruben et al.
In: Advanced electronic materials, Vol. 9, No. 6, 2201298, 06.2023.

Research output: Contribution to journal › Article › Academic › peer-review

TY - JOUR

T1 - Investigating the Electromechanical Behavior of Unconventionally Ferroelectric Hf0.5Zr0.5O2-Based Capacitors Through Operando Nanobeam X-Ray Diffraction

AU - Stylianidis, Evgenios

AU - Surabhi, Pranav

AU - Hamming-Green, Ruben

AU - Salverda, Mart

AU - Wei, Yingfen

AU - Burema, Arjan

AU - Matzen, Sylvia

AU - Banerjee, Tamalika

AU - Björling, Alexander

AU - Mukherjee, Binayak

AU - Dutta, Sangita

AU - Aramberri, Hugo

AU - Íñiguez, Jorge

AU - Noheda, Beatriz

AU - Carbone, Dina

AU - Nukala, Pavan

N1 - Funding Information: The authors acknowledge MAX IV Laboratory for time on Beamline NanoMAX under Proposal 20190954. Research conducted at MAX IV, a Swedish national user facility, was supported by the Swedish Research Council (under contract grant No. 2018—07152), the Swedish Governmental Agency for Innovation Systems (under contract grant No. 2018–04969), and Formas (under contract grant No. 2019–02496). Work at LIST was supported by the Luxembourg National Research Fund though (grant Nos. INTER/NOW/20/15079143/TRICOLOR (to B.M., H.A., J.I.) and PRIDE/15/10935404/MASSENA (to S.D.). P.N. acknowledges national nanofabrication and micro-nano characterization facilities at the center for nanoscience and engineering, IISc. P.N. also acknowledges SERB grant (SRG/000285) and Infosys Young Scientist Award. B.N. and T.B. acknowledge the financial support of the CogniGron research center and the Ubbo Emmius Funds (University of Groningen). Device fabrication were realized using NanoLab NL facilities. S.M. acknowledges the support from the French RENATECH network for the research at the Center for Nanoscience and Nanotechnology. Funding Information: The authors acknowledge MAX IV Laboratory for time on Beamline NanoMAX under Proposal 20190954. Research conducted at MAX IV, a Swedish national user facility, was supported by the Swedish Research Council (under contract grant No. 2018—07152), the Swedish Governmental Agency for Innovation Systems (under contract grant No. 2018–04969), and Formas (under contract grant No. 2019–02496). Work at LIST was supported by the Luxembourg National Research Fund though (grant Nos. INTER/NOW/20/15079143/TRICOLOR (to B.M., H.A., J.I.) and PRIDE/15/10935404/MASSENA (to S.D.). P.N. acknowledges national nanofabrication and micro‐nano characterization facilities at the center for nanoscience and engineering, IISc. P.N. also acknowledges SERB grant (SRG/000285) and Infosys Young Scientist Award. B.N. and T.B. acknowledge the financial support of the CogniGron research center and the Ubbo Emmius Funds (University of Groningen). Device fabrication were realized using NanoLab NL facilities. S.M. acknowledges the support from the French RENATECH network for the research at the Center for Nanoscience and Nanotechnology. Publisher Copyright: © 2023 The Authors. Advanced Electronic Materials published by Wiley-VCH GmbH.

PY - 2023/6

Y1 - 2023/6

N2 - Understanding various aspects of ferroelectricity in hafnia-based nanomaterials is of vital importance for the development of future nonvolatile memory and logic devices. Here, the unconventional and weak electromechanical response of epitaxial La0.67Sr0.33MnO3/Hf0.5Zr0.5O2/La0.67Sr0.33MnO3 ferroelectric capacitors is investigated, via the sensitivity offered by nanobeam X-ray diffraction experiments during application of electrical bias. It is shown that the pristine rhombohedral phase exhibits a linear piezoelectric effect with piezoelectric coefficient (|d33|) ≈ 0.5–0.8 pmV−1. It is found that the piezoelectric response is suppressed above the coercive voltage. For higher voltages, and with the onset of DC conductivity throughout the capacitor, a second-order effect is observed. The work sheds light into the electromechanical response of rhombohedral Hf0.5Zr0.5O2 and suggests its (un)correlation with ferroelectric switching.

AB - Understanding various aspects of ferroelectricity in hafnia-based nanomaterials is of vital importance for the development of future nonvolatile memory and logic devices. Here, the unconventional and weak electromechanical response of epitaxial La0.67Sr0.33MnO3/Hf0.5Zr0.5O2/La0.67Sr0.33MnO3 ferroelectric capacitors is investigated, via the sensitivity offered by nanobeam X-ray diffraction experiments during application of electrical bias. It is shown that the pristine rhombohedral phase exhibits a linear piezoelectric effect with piezoelectric coefficient (|d33|) ≈ 0.5–0.8 pmV−1. It is found that the piezoelectric response is suppressed above the coercive voltage. For higher voltages, and with the onset of DC conductivity throughout the capacitor, a second-order effect is observed. The work sheds light into the electromechanical response of rhombohedral Hf0.5Zr0.5O2 and suggests its (un)correlation with ferroelectric switching.

KW - electrochemical polarization

KW - first-principles

KW - nanobeam diffraction

KW - rhombohedral Hf Zr O

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DO - 10.1002/aelm.202201298

M3 - Article

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JO - Advanced electronic materials

JF - Advanced electronic materials

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