Controlled sign reversal of electroresistance in oxide tunnel junctions by electrochemical-ferroelectric coupling

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Hernández Martín, David
Gallego Toledo, Fernando
Beltrán Finez, Juan Ignacio
Munuera, C.
Sánchez Manzano, David
Cuéllar Jiménez, Fabián Andrés
Arias Serna, Diego
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American Physical Society
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The persistence of ferroelectricity in ultrathin layers relies critically on screening or compensation of polarization charges which otherwise destabilize the ferroelectric state. At surfaces, charged defects play a crucial role in the screening mechanism triggering novel mixed electrochemical-ferroelectric states. At interfaces, however, the coupling between ferroelectric and electrochemical states has remained unexplored. Here, we make use of the dynamic formation of the oxygen vacancy profile in the nanometerthick barrier of a ferroelectric tunnel junction to demonstrate the interplay between electrochemical and ferroelectric degrees of freedom at an oxide interface. We fabricate ferroelectric tunnel junctions with a La_0.7Sr_0.3MnO_3 bottom electrode and BaTiO_3 ferroelectric barrier. We use poling strategies to promote the generation and transport of oxygen vacancies at the metallic top electrode. Generated oxygen vacancies control the stability of the ferroelectric polarization and modify its coercive fields. The ferroelectric polarization, in turn, controls the ionization of oxygen vacancies well above the limits of thermodynamic equilibrium, triggering the build up of a Schottky barrier at the interface which can be turned on and off with ferroelectric switching. This interplay between electronic and electrochemical degrees of freedom yields very large values of the electroresistance (more than 10^6% at low temperatures) and enables a controlled switching between clockwise and counterclockwise switching modes in the same junction (and consequently, a change of the sign of the electroresistance). The strong coupling found between electrochemical and electronic degrees of freedom sheds light on the growing debate between resistive and ferroelectric switching in ferroelectric tunnel junctions, and moreover, can be the source of novel concepts in memory devices and neuromorphie computing.
©2020 American Physical Society The authors acknowledge received funding from the project Quantox of QuantERA ERA-NET Cofund in Quantum Technologies (Grant Agreement No. 731473) implemented within the European Union's Horizon 2020 Programme. Work supported by Spanish MINECO through Grants No. MAT2014-52405-C02, No. MAT2017-87134-C02, No. MAT2015-066888-C3-1-3-R, and No. RTI2018-097895-B-C41 (-C43), Grant No. Santander-UCM PR87/19-22603, and computational support from Grant No. FI-2019-1-0012. J. S. thanks for the scholarship program Alembert funded by the IDEX Paris-Saclay, Grant No. ANR-11-IDEX-0003-02.