Electrically induced cancellation and inversion of piezoelectricity in ferroelectric Hf0.5Zr0.5O2

Haidong Lu, Dong-Jik Kim, Hugo Aramberri, Marco Holzer, Pratyush Buragohain, Sangita Dutta, Uwe Schroeder, Veeresh Deshpande, Jorge Íñiguez (), Alexei Gruverman () and Catherine Dubourdieu ()
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Haidong Lu: University of Nebraska-Lincoln
Dong-Jik Kim: Insitute Functional Oxides for Energy-Efficient Information Technology
Hugo Aramberri: Luxembourg Institute of Science and Technology (LIST)
Marco Holzer: Insitute Functional Oxides for Energy-Efficient Information Technology
Pratyush Buragohain: University of Nebraska-Lincoln
Sangita Dutta: Luxembourg Institute of Science and Technology (LIST)
Uwe Schroeder: NaMLab gGmbH
Veeresh Deshpande: Insitute Functional Oxides for Energy-Efficient Information Technology
Jorge Íñiguez: Luxembourg Institute of Science and Technology (LIST)
Alexei Gruverman: University of Nebraska-Lincoln
Catherine Dubourdieu: Insitute Functional Oxides for Energy-Efficient Information Technology

Nature Communications, 2024, vol. 15, issue 1, 1-9

Abstract: 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 d33 in the pristine state to a fully inverted negative d33 state, while, in parallel, the polarization monotonically increases. Not only can the sign of d33 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.

Date: 2024
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DOI: 10.1038/s41467-024-44690-9

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