Electrically induced cancellation and inversion of piezoelectricity in ferroelectric Hf0.5Zr0.5O2
Abstract HfO2-based thin films hold huge promise for integrated devices as they show full compatibility with semiconductor technologies and robust ferroelectric properties at nanometer scale. While their polarization switching behavior has been widely investigated, their electromechanical response r...
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Nature Portfolio
2024-01-01
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Online Access: | https://doi.org/10.1038/s41467-024-44690-9 |
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author | Haidong Lu Dong-Jik Kim Hugo Aramberri Marco Holzer Pratyush Buragohain Sangita Dutta Uwe Schroeder Veeresh Deshpande Jorge Íñiguez Alexei Gruverman Catherine Dubourdieu |
author_facet | Haidong Lu Dong-Jik Kim Hugo Aramberri Marco Holzer Pratyush Buragohain Sangita Dutta Uwe Schroeder Veeresh Deshpande Jorge Íñiguez Alexei Gruverman Catherine Dubourdieu |
author_sort | Haidong Lu |
collection | DOAJ |
description | Abstract HfO2-based thin films hold huge promise for integrated devices as they show full compatibility with semiconductor technologies and robust ferroelectric properties at nanometer scale. While their polarization switching behavior has been widely investigated, their electromechanical response received much less attention so far. Here, we demonstrate that piezoelectricity in Hf0.5Zr0.5O2 ferroelectric capacitors is not an invariable property but, in fact, can be intrinsically changed by electrical field cycling. Hf0.5Zr0.5O2 capacitors subjected to ac cycling undergo a continuous transition from a positive effective piezoelectric coefficient d 33 in the pristine state to a fully inverted negative d 33 state, while, in parallel, the polarization monotonically increases. Not only can the sign of d 33 be uniformly inverted in the whole capacitor volume, but also, with proper ac training, the net effective piezoresponse can be nullified while the polarization is kept fully switchable. Moreover, the local piezoresponse force microscopy signal also gradually goes through the zero value upon ac cycling. Density functional theory calculations suggest that the observed behavior is a result of a structural transformation from a weakly-developed polar orthorhombic phase towards a well-developed polar orthorhombic phase. The calculations also suggest the possible occurrence of a non-piezoelectric ferroelectric Hf0.5Zr0.5O2. Our experimental findings create an unprecedented potential for tuning the electromechanical functionality of ferroelectric HfO2-based devices. |
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spelling | doaj.art-4f5ee4837dbb4177a3443d1b75c527662024-03-05T19:31:18ZengNature PortfolioNature Communications2041-17232024-01-011511910.1038/s41467-024-44690-9Electrically induced cancellation and inversion of piezoelectricity in ferroelectric Hf0.5Zr0.5O2Haidong Lu0Dong-Jik Kim1Hugo Aramberri2Marco Holzer3Pratyush Buragohain4Sangita Dutta5Uwe Schroeder6Veeresh Deshpande7Jorge Íñiguez8Alexei Gruverman9Catherine Dubourdieu10Department of Physics and Astronomy, University of Nebraska-LincolnHelmholtz-Zentrum Berlin für Materialien und Energie, Insitute Functional Oxides for Energy-Efficient Information TechnologyMaterials Research and Technology Department, Luxembourg Institute of Science and Technology (LIST)Helmholtz-Zentrum Berlin für Materialien und Energie, Insitute Functional Oxides for Energy-Efficient Information TechnologyDepartment of Physics and Astronomy, University of Nebraska-LincolnMaterials Research and Technology Department, Luxembourg Institute of Science and Technology (LIST)NaMLab gGmbHHelmholtz-Zentrum Berlin für Materialien und Energie, Insitute Functional Oxides for Energy-Efficient Information TechnologyMaterials Research and Technology Department, Luxembourg Institute of Science and Technology (LIST)Department of Physics and Astronomy, University of Nebraska-LincolnHelmholtz-Zentrum Berlin für Materialien und Energie, Insitute Functional Oxides for Energy-Efficient Information TechnologyAbstract HfO2-based thin films hold huge promise for integrated devices as they show full compatibility with semiconductor technologies and robust ferroelectric properties at nanometer scale. While their polarization switching behavior has been widely investigated, their electromechanical response received much less attention so far. Here, we demonstrate that piezoelectricity in Hf0.5Zr0.5O2 ferroelectric capacitors is not an invariable property but, in fact, can be intrinsically changed by electrical field cycling. Hf0.5Zr0.5O2 capacitors subjected to ac cycling undergo a continuous transition from a positive effective piezoelectric coefficient d 33 in the pristine state to a fully inverted negative d 33 state, while, in parallel, the polarization monotonically increases. Not only can the sign of d 33 be uniformly inverted in the whole capacitor volume, but also, with proper ac training, the net effective piezoresponse can be nullified while the polarization is kept fully switchable. Moreover, the local piezoresponse force microscopy signal also gradually goes through the zero value upon ac cycling. Density functional theory calculations suggest that the observed behavior is a result of a structural transformation from a weakly-developed polar orthorhombic phase towards a well-developed polar orthorhombic phase. The calculations also suggest the possible occurrence of a non-piezoelectric ferroelectric Hf0.5Zr0.5O2. Our experimental findings create an unprecedented potential for tuning the electromechanical functionality of ferroelectric HfO2-based devices.https://doi.org/10.1038/s41467-024-44690-9 |
spellingShingle | Haidong Lu Dong-Jik Kim Hugo Aramberri Marco Holzer Pratyush Buragohain Sangita Dutta Uwe Schroeder Veeresh Deshpande Jorge Íñiguez Alexei Gruverman Catherine Dubourdieu Electrically induced cancellation and inversion of piezoelectricity in ferroelectric Hf0.5Zr0.5O2 Nature Communications |
title | Electrically induced cancellation and inversion of piezoelectricity in ferroelectric Hf0.5Zr0.5O2 |
title_full | Electrically induced cancellation and inversion of piezoelectricity in ferroelectric Hf0.5Zr0.5O2 |
title_fullStr | Electrically induced cancellation and inversion of piezoelectricity in ferroelectric Hf0.5Zr0.5O2 |
title_full_unstemmed | Electrically induced cancellation and inversion of piezoelectricity in ferroelectric Hf0.5Zr0.5O2 |
title_short | Electrically induced cancellation and inversion of piezoelectricity in ferroelectric Hf0.5Zr0.5O2 |
title_sort | electrically induced cancellation and inversion of piezoelectricity in ferroelectric hf0 5zr0 5o2 |
url | https://doi.org/10.1038/s41467-024-44690-9 |
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