Metal Nitride Electrode Stress and Chemistry Effects on Phase and Polarization Response in Ferroelectric Hf0.5Zr0.5O2 Thin Films

Shelby S. Fields; Sean W. Smith; Chris M. Fancher; Michael David Henry; Steve L. Wolfley; Maria G. Sales; Samantha T. Jaszewski; Mark A. Rodriguez; Giovanni Esteves; Paul S. Davids; Stephen J. McDonnell; Jon F. Ihlefeld

doi:10.1002/admi.202100018

Metal Nitride Electrode Stress and Chemistry Effects on Phase and Polarization Response in Ferroelectric Hf_0.5Zr_0.5O₂ Thin Films

Shelby S. Fields, Sean W. Smith, Chris M. Fancher, Michael David Henry, Steve L. Wolfley, Maria G. Sales, Samantha T. Jaszewski, Mark A. Rodriguez, Giovanni Esteves, Paul S. Davids, Stephen J. McDonnell, Jon F. Ihlefeld

Materials for Advanced Manufacturing

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

25 Scopus citations

Abstract

Ferroelectric phase stability in hafnium oxide is reported to be influenced by factors that include composition, biaxial stress, crystallite size, and oxygen vacancies. In the present work, the ferroelectric performance of atomic layer deposited Hf_0.5Zr_0.5O₂ (HZO) prepared between TaN electrodes that are processed under conditions to induce variable biaxial stresses is evaluated. The post-processing stress states of the HZO films reveal no dependence on the as-deposited stress of the adjacent TaN electrodes. All HZO films maintain tensile biaxial stress following processing, the magnitude of which is not observed to strongly influence the polarization response. Subsequent composition measurements of stress-varied TaN electrodes reveal changes in stoichiometry related to the different preparation conditions. HZO films in contact with Ta-rich TaN electrodes exhibit higher remanent polarizations and increased ferroelectric phase fractions compared to those in contact with N-rich TaN electrodes. HZO films in contact with Ta-rich TaN electrodes also have higher oxygen vacancy concentrations, indicating that a chemical interaction between the TaN and HZO layers ultimately impacts the ferroelectric orthorhombic phase stability and polarization performance. The results of this work demonstrate a necessity to carefully consider the role of electrode processing and chemistry on performance of ferroelectric hafnia films.

Original language	English
Article number	2100018
Journal	Advanced Materials Interfaces
Volume	8
Issue number	10
DOIs	https://doi.org/10.1002/admi.202100018
State	Published - May 21 2021

Funding

This work was supported, in part, by the Laboratory Directed Research and Development program at Sandia National Laboratories. Sandia is a multimission laboratory managed and operated by National Technology & Engineering Solutions of Sandia, LLC, a wholly owned subsidiary of Honeywell International, Inc., for the U.S. DOE's National Nuclear Security Administration under Contract No. DE-NA-0003525. The views expressed in the article do not necessarily represent the views of the U.S. DOE or the United States Government. This work was also supported, in part, by the Semiconductor Research Corporation's (SRC) Global Research Collaboration in the NanoMaterials and Processing program. This research was supported, in part, by the National Science Foundation through a major instrumentation grant (DMR-1626201). S.T.J. acknowledges support from the National Science Foundation Graduate Research Fellowship Program under Award No. DGE-1842490. A portion of this research used resources at the Spallation Neutron Source, a DOE Office of Science User Facility operated by the Oak Ridge National Laboratory. This manuscript was coauthored by UT-Battelle, LLC, under Contract No. DE-AC05-00OR22725 with the U.S. Department of Energy. The United States Government retains and the publisher, by accepting the article for publication, acknowledges that the United States Government retains a nonexclusive, paid-up, irrevocable, world-wide license to publish or reproduce the published form of this manuscript, or allow others to do so, for United States Government purposes. This work was supported, in part, by the Laboratory Directed Research and Development program at Sandia National Laboratories. Sandia is a multimission laboratory managed and operated by National Technology & Engineering Solutions of Sandia, LLC, a wholly owned subsidiary of Honeywell International, Inc., for the U.S. DOE's National Nuclear Security Administration under Contract No. DE‐NA‐0003525. The views expressed in the article do not necessarily represent the views of the U.S. DOE or the United States Government. This work was also supported, in part, by the Semiconductor Research Corporation's (SRC) Global Research Collaboration in the NanoMaterials and Processing program. This research was supported, in part, by the National Science Foundation through a major instrumentation grant (DMR‐1626201). S.T.J. acknowledges support from the National Science Foundation Graduate Research Fellowship Program under Award No. DGE‐1842490. A portion of this research used resources at the Spallation Neutron Source, a DOE Office of Science User Facility operated by the Oak Ridge National Laboratory. This manuscript was coauthored by UT‐Battelle, LLC, under Contract No. DE‐AC05‐00OR22725 with the U.S. Department of Energy. The United States Government retains and the publisher, by accepting the article for publication, acknowledges that the United States Government retains a nonexclusive, paid‐up, irrevocable, world‐wide license to publish or reproduce the published form of this manuscript, or allow others to do so, for United States Government purposes.

Keywords

ferroelectrics
hafnium zirconium oxide
metal nitride electrodes
oxygen vacancies
stress

Access to Document

10.1002/admi.202100018

Cite this

Fields, S. S., Smith, S. W., Fancher, C. M., Henry, M. D., Wolfley, S. L., Sales, M. G., Jaszewski, S. T., Rodriguez, M. A., Esteves, G., Davids, P. S., McDonnell, S. J., & Ihlefeld, J. F. (2021). Metal Nitride Electrode Stress and Chemistry Effects on Phase and Polarization Response in Ferroelectric Hf_0.5Zr_0.5O₂ Thin Films. Advanced Materials Interfaces, 8(10), Article 2100018. https://doi.org/10.1002/admi.202100018

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title = "Metal Nitride Electrode Stress and Chemistry Effects on Phase and Polarization Response in Ferroelectric Hf0.5Zr0.5O2 Thin Films",

abstract = "Ferroelectric phase stability in hafnium oxide is reported to be influenced by factors that include composition, biaxial stress, crystallite size, and oxygen vacancies. In the present work, the ferroelectric performance of atomic layer deposited Hf0.5Zr0.5O2 (HZO) prepared between TaN electrodes that are processed under conditions to induce variable biaxial stresses is evaluated. The post-processing stress states of the HZO films reveal no dependence on the as-deposited stress of the adjacent TaN electrodes. All HZO films maintain tensile biaxial stress following processing, the magnitude of which is not observed to strongly influence the polarization response. Subsequent composition measurements of stress-varied TaN electrodes reveal changes in stoichiometry related to the different preparation conditions. HZO films in contact with Ta-rich TaN electrodes exhibit higher remanent polarizations and increased ferroelectric phase fractions compared to those in contact with N-rich TaN electrodes. HZO films in contact with Ta-rich TaN electrodes also have higher oxygen vacancy concentrations, indicating that a chemical interaction between the TaN and HZO layers ultimately impacts the ferroelectric orthorhombic phase stability and polarization performance. The results of this work demonstrate a necessity to carefully consider the role of electrode processing and chemistry on performance of ferroelectric hafnia films.",

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Fields, SS, Smith, SW, Fancher, CM, Henry, MD, Wolfley, SL, Sales, MG, Jaszewski, ST, Rodriguez, MA, Esteves, G, Davids, PS, McDonnell, SJ & Ihlefeld, JF 2021, 'Metal Nitride Electrode Stress and Chemistry Effects on Phase and Polarization Response in Ferroelectric Hf_0.5Zr_0.5O₂ Thin Films', Advanced Materials Interfaces, vol. 8, no. 10, 2100018. https://doi.org/10.1002/admi.202100018

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AU - Henry, Michael David

AU - Wolfley, Steve L.

AU - Sales, Maria G.

AU - Jaszewski, Samantha T.

AU - Rodriguez, Mark A.

AU - Esteves, Giovanni

AU - Davids, Paul S.

AU - McDonnell, Stephen J.

AU - Ihlefeld, Jon F.

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AB - Ferroelectric phase stability in hafnium oxide is reported to be influenced by factors that include composition, biaxial stress, crystallite size, and oxygen vacancies. In the present work, the ferroelectric performance of atomic layer deposited Hf0.5Zr0.5O2 (HZO) prepared between TaN electrodes that are processed under conditions to induce variable biaxial stresses is evaluated. The post-processing stress states of the HZO films reveal no dependence on the as-deposited stress of the adjacent TaN electrodes. All HZO films maintain tensile biaxial stress following processing, the magnitude of which is not observed to strongly influence the polarization response. Subsequent composition measurements of stress-varied TaN electrodes reveal changes in stoichiometry related to the different preparation conditions. HZO films in contact with Ta-rich TaN electrodes exhibit higher remanent polarizations and increased ferroelectric phase fractions compared to those in contact with N-rich TaN electrodes. HZO films in contact with Ta-rich TaN electrodes also have higher oxygen vacancy concentrations, indicating that a chemical interaction between the TaN and HZO layers ultimately impacts the ferroelectric orthorhombic phase stability and polarization performance. The results of this work demonstrate a necessity to carefully consider the role of electrode processing and chemistry on performance of ferroelectric hafnia films.

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KW - hafnium zirconium oxide

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KW - oxygen vacancies

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