Electrical Behavior of Combinatorial Thin-Film ZrxTa1−xOy

Matthew Flynn-Hepford; Reece Emery; Steven J. Randolph; Scott T. Retterer; Gyula Eres; Bobby Sumpter; Anton V. Ievlev; Olga S. Ovchinnikova; Philip D. Rack

doi:10.3390/nano15100732

Electrical Behavior of Combinatorial Thin-Film Zr_xTa_1−xO_y

Matthew Flynn-Hepford, Reece Emery, Steven J. Randolph, Scott T. Retterer, Gyula Eres, Bobby Sumpter, Anton V. Ievlev, Olga S. Ovchinnikova, Philip D. Rack

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

Abstract

Combinatorial magnetron sputtering and electrical characterization were used to systematically study the impact of compositional changes in the resistive switching of transition metal oxides, specifically the Zr_xTa_1−xO_y system. Current-voltage behavior across a range of temperatures provided insights into the mechanisms that contribute to differences in the electrical conductivity of the pristine Ta₂O₅ and ZrO₂, and mixed Zr_xTa_1−xO_y devices. The underlying conductive mechanism was found to be a mixture of charge trapping and ionic motion, where charge trapping/emission dictated the short-term cycling behavior while ion motion contributed to changes in the conduction with increased cycling number. ToF-SIMS was used to identify the origin of the “wake-up” behavior of the devices, revealing an ionic motion contribution. This understanding of how cation concentration affects conduction in mixed valence systems helps provide a foundation for a new approach toward manipulating resistive switching in these active layer materials.

Original language	English
Article number	732
Journal	Nanomaterials
Volume	15
Issue number	10
DOIs	https://doi.org/10.3390/nano15100732
State	Published - May 2025

Funding

This research was funded by the DOE Office of Science Research Program for Microelectronics Codesign (sponsored by ASCR, BES, HEP, NP, and FES) through the Abisko Project with program managers Robinson Pino (ASCR). Hal Finkel (ASCR), and Andrew Schwartz (BES). Electrical measurements, ToF-SIMS, and DFT calculations were conducted at the Center for Nanophase Materials Sciences (CNMS), which was a US Department of Energy, Office of Science User Facility at Oak Ridge National Laboratory (ORNL). This manuscript has been authored by UT-Battelle, LLC, under contract DE-AC05-00OR22725 with the US Department of Energy (DOE). The US government retains and the publisher, by accepting this article for publication, acknowledges that the US government retains a nonexclusive, paid-up, irrevocable, worldwide license to publish or reproduce the published form of this manuscript, or allow others to do so, for US government purposes. DOE will provide public access to these results of federally sponsored research in accordance with the DOE Public Access Plan (https://www.energy.gov/doe-public-access-plan) (accessed on 13 March 2025). The contribution by G.E. was supported by U.S. DOE, Office of Science, Basic Energy Sciences, Materials Science and Engineering Division.

Keywords

combinatorial sputtering
resistive switching
tantalum oxide
thin films
zirconium oxide

Access to Document

10.3390/nano15100732

Cite this

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title = "Electrical Behavior of Combinatorial Thin-Film ZrxTa1−xOy",

abstract = "Combinatorial magnetron sputtering and electrical characterization were used to systematically study the impact of compositional changes in the resistive switching of transition metal oxides, specifically the ZrxTa1−xOy system. Current-voltage behavior across a range of temperatures provided insights into the mechanisms that contribute to differences in the electrical conductivity of the pristine Ta2O5 and ZrO2, and mixed ZrxTa1−xOy devices. The underlying conductive mechanism was found to be a mixture of charge trapping and ionic motion, where charge trapping/emission dictated the short-term cycling behavior while ion motion contributed to changes in the conduction with increased cycling number. ToF-SIMS was used to identify the origin of the “wake-up” behavior of the devices, revealing an ionic motion contribution. This understanding of how cation concentration affects conduction in mixed valence systems helps provide a foundation for a new approach toward manipulating resistive switching in these active layer materials.",

keywords = "combinatorial sputtering, resistive switching, tantalum oxide, thin films, zirconium oxide",

author = "Matthew Flynn-Hepford and Reece Emery and Randolph, \{Steven J.\} and Retterer, \{Scott T.\} and Gyula Eres and Bobby Sumpter and Ievlev, \{Anton V.\} and Ovchinnikova, \{Olga S.\} and Rack, \{Philip D.\}",

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AU - Emery, Reece

AU - Randolph, Steven J.

AU - Retterer, Scott T.

AU - Eres, Gyula

AU - Sumpter, Bobby

AU - Ievlev, Anton V.

AU - Ovchinnikova, Olga S.

AU - Rack, Philip D.

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N2 - Combinatorial magnetron sputtering and electrical characterization were used to systematically study the impact of compositional changes in the resistive switching of transition metal oxides, specifically the ZrxTa1−xOy system. Current-voltage behavior across a range of temperatures provided insights into the mechanisms that contribute to differences in the electrical conductivity of the pristine Ta2O5 and ZrO2, and mixed ZrxTa1−xOy devices. The underlying conductive mechanism was found to be a mixture of charge trapping and ionic motion, where charge trapping/emission dictated the short-term cycling behavior while ion motion contributed to changes in the conduction with increased cycling number. ToF-SIMS was used to identify the origin of the “wake-up” behavior of the devices, revealing an ionic motion contribution. This understanding of how cation concentration affects conduction in mixed valence systems helps provide a foundation for a new approach toward manipulating resistive switching in these active layer materials.

AB - Combinatorial magnetron sputtering and electrical characterization were used to systematically study the impact of compositional changes in the resistive switching of transition metal oxides, specifically the ZrxTa1−xOy system. Current-voltage behavior across a range of temperatures provided insights into the mechanisms that contribute to differences in the electrical conductivity of the pristine Ta2O5 and ZrO2, and mixed ZrxTa1−xOy devices. The underlying conductive mechanism was found to be a mixture of charge trapping and ionic motion, where charge trapping/emission dictated the short-term cycling behavior while ion motion contributed to changes in the conduction with increased cycling number. ToF-SIMS was used to identify the origin of the “wake-up” behavior of the devices, revealing an ionic motion contribution. This understanding of how cation concentration affects conduction in mixed valence systems helps provide a foundation for a new approach toward manipulating resistive switching in these active layer materials.

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