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Toward Nonvolatile Spin–Orbit Devices: Deposition of Ferroelectric Hafnia on Monolayer Graphene/Co/HM Stacks

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    Functional Nanostructured Materials (including low-D carbon)

    Toward Nonvolatile Spin–Orbit Devices: Deposition of Ferroelectric Hafnia on Monolayer Graphene/Co/HM Stacks
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    • Suzanne Lancaster*
      Suzanne Lancaster
      NaMLab gGmbH, Nöthnitzer Strasse 64a, Dresden 01187, Germany
      *Email: [email protected]
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      Orcidhttps://orcid.org/0000-0002-5689-2795
    • Iciar Arnay
      Iciar Arnay
      IMDEA Nanociencia, c/Faraday 9, Madrid 28049, Spain
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    • Ruben Guerrero
      Ruben Guerrero
      IMDEA Nanociencia, c/Faraday 9, Madrid 28049, Spain
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    • Adrian Gudín
      Adrian Gudín
      IMDEA Nanociencia, c/Faraday 9, Madrid 28049, Spain
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    • Alejandra Guedeja-Marrón
      Alejandra Guedeja-Marrón
      Departamento de Física de Materiales and Instituto Pluridisciplinar, Universidad Complutense de Madrid, Ciudad Universitaria, Madrid 28040, Spain
      More by Alejandra Guedeja-Marrón
    • Jose Manuel Diez
      Jose Manuel Diez
      Departamento de Física de la Materia Condensada & Departamento de Física Aplicada & Instituto Nicolás Cabrera, Universidad Autónoma de Madrid, Madrid 28049, Spain
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    • Jan Gärtner
      Jan Gärtner
      NaMLab gGmbH, Nöthnitzer Strasse 64a, Dresden 01187, Germany
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    • Alberto Anadón
      Alberto Anadón
      IMDEA Nanociencia, c/Faraday 9, Madrid 28049, Spain
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      Orcidhttps://orcid.org/0000-0001-5939-6415
    • Maria Varela
      Maria Varela
      Departamento de Física de Materiales and Instituto Pluridisciplinar, Universidad Complutense de Madrid, Ciudad Universitaria, Madrid 28040, Spain
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    • Julio Camarero
      Julio Camarero
      Departamento de Física de la Materia Condensada & Departamento de Física Aplicada & Instituto Nicolás Cabrera, Universidad Autónoma de Madrid, Madrid 28049, Spain
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      Orcidhttps://orcid.org/0000-0003-0078-7280
    • Thomas Mikolajick
      Thomas Mikolajick
      NaMLab gGmbH, Nöthnitzer Strasse 64a, Dresden 01187, Germany
      Institute of Semiconductors and Microsystems, Technische Universität Dresden, Nöthnitzer Strasse 64, Dresden 01187, Germany
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      Orcidhttps://orcid.org/0000-0003-3814-0378
    • Paolo Perna
      Paolo Perna
      IMDEA Nanociencia, c/Faraday 9, Madrid 28049, Spain
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      Orcidhttps://orcid.org/0000-0001-8537-4834
    • Stefan Slesazeck
      Stefan Slesazeck
      NaMLab gGmbH, Nöthnitzer Strasse 64a, Dresden 01187, Germany
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    ACS Applied Materials & Interfaces

    Cite this: ACS Appl. Mater. Interfaces 2023, 15, 13, 16963–16974
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    https://doi.org/10.1021/acsami.2c22205
    Published March 23, 2023
    Copyright © 2023 American Chemical Society
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    Abstract

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    While technologically challenging, the integration of ferroelectric thin films with graphene spintronics potentially allows the realization of highly efficient, electrically tunable, nonvolatile memories through control of the interfacial spin–orbit driven interaction occurring at graphene/Co interfaces deposited on heavy metal supports. Here, the integration of ferroelectric Hf0.5Zr0.5O2 on graphene/Co/heavy metal epitaxial stacks is investigated via the implementation of several nucleation methods in atomic layer deposition. By employing in situ Al2O3 as a nucleation layer sandwiched between Hf0.5Zr0.5O2 and graphene, the Hf0.5Zr0.5O2 demonstrates a remanent polarization (2Pr) of 19.2 μC/cm2. Using an ex situ, naturally oxidized sputtered Ta layer for nucleation, we could control 2Pr via the interlayer thickness, reaching maximum values of 28 μC/cm2 with low coercive fields. Magnetic hysteresis measurements taken before and after atomic layer deposition show strong perpendicular magnetic anisotropy, with minimal deviations in the magnetization reversal pathways due to the Hf0.5Zr0.5O2 deposition process, thus pointing to a good preservation of the magnetic stack including single-layer graphene. X-ray diffraction measurements further confirm that the high-quality interfaces demonstrated in the stack remain unperturbed by the ferroelectric deposition and anneal. The proposed graphene-based ferroelectric/magnetic structures offer the strong advantages of ferroelectricity and ferromagnetism at room temperature, enabling the development of novel magneto-electric and nonvolatile in-memory spin–orbit logic architectures with low power switching.

    Copyright © 2023 American Chemical Society

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    Supporting Information

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    The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acsami.2c22205.

    • Full methods for the fabrication and characterization of the stacks, as well as AFM and SEM analyses after the ALD process and on ferroelectric films; fitting of the GIXRD data presented in the Article; additional electrical data on ferroelectric films with the dielectric crystallization layer intact and on thinner ferroelectric films; HRTEM and EELs analysis of a full ferroelectric/graphene/Co/HM stack; and magnetic hysteresis measurements on a stack with Ir(111) as HM (PDF)

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    This article is cited by 5 publications.

    1. David Lehninger, Franz Müller, Yannick Raffel, Shouzhuo Yang, Markus Neuber, Sukhrob Abdulazhanov, Thomas Kämpfe, Konrad Seidel, Maximilian Lederer. Ferroelectric Hafnium Oxide: A Potential Game‐Changer for Nanoelectronic Devices and Systems. Advanced Electronic Materials 2025, 2 https://doi.org/10.1002/aelm.202400686
    2. Pablo Olleros‐Rodríguez, Adrián Gudín, Julio Camarero, Oksana Chubykalo‐Fesenko, Paolo Perna. Anatomy of the Dynamics of the Nucleation of Skyrmions in Nanodots via the Voltage‐Controlled Magnetic Anisotropy. Advanced Physics Research 2025, 4 (2) https://doi.org/10.1002/apxr.202400107
    3. Matteo Jugovac, Iulia Cojocariu, Vitaliy Feyer, Stefan Blügel, Gustav Bihlmayer, Paolo Perna. Spin-dependent electronic phenomena in heavily-doped monolayer graphene. Carbon 2024, 230 , 119666. https://doi.org/10.1016/j.carbon.2024.119666
    4. Tetiana Zakusylo, Alberto Quintana, Veniero Lenzi, José P. B. Silva, Luís Marques, José Luís Ortolá Yano, Jike Lyu, Jordi Sort, Florencio Sánchez, Ignasi Fina. Robust multiferroicity and magnetic modulation of the ferroelectric imprint field in heterostructures comprising epitaxial Hf 0.5 Zr 0.5 O 2 and Co. Materials Horizons 2024, 11 (10) , 2388-2396. https://doi.org/10.1039/D3MH01966G
    5. Suzanne Lancaster, Stefan Slesazeck, Thomas Mikolajick. On the Thickness Scaling of Ferroelectric Hafnia. IEEE Transactions on Materials for Electron Devices 2024, 1 , 36-48. https://doi.org/10.1109/TMAT.2024.3423665
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    ACS Applied Materials & Interfaces

    Cite this: ACS Appl. Mater. Interfaces 2023, 15, 13, 16963–16974
    Click to copy citationCitation copied!
    https://doi.org/10.1021/acsami.2c22205
    Published March 23, 2023
    Copyright © 2023 American Chemical Society
    Request reuse permissions

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