Freestanding epitaxial SrTiO3 nanomembranes via remote epitaxy using hybrid molecular beam epitaxy

Hyojin Yoon; Tristan K. Truttmann; Fengdeng Liu; Bethany E. Matthews; Sooho Choo; Qun Su; Vivek Saraswat; Sebastian Manzo; Michael S. Arnold; Mark E. Bowden; Jason K. Kawasaki; Steven J. Koester; Steven R. Spurgeon; Scott A. Chambers; Bharat Jalan

doi:10.1126/sciadv.add5328

Freestanding epitaxial SrTiO₃ nanomembranes via remote epitaxy using hybrid molecular beam epitaxy

Hyojin Yoon, Tristan K. Truttmann, Fengdeng Liu, Bethany E. Matthews, Sooho Choo, Qun Su, Vivek Saraswat, Sebastian Manzo, Michael S. Arnold, Mark E. Bowden, Jason K. Kawasaki, Steven J. Koester, Steven R. Spurgeon, Scott A. Chambers, Bharat Jalan

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Abstract

The epitaxial growth of functional oxides using a substrate with a graphene layer is a highly desirable method for improving structural quality and obtaining freestanding epitaxial nanomembranes for scientific study, applications, and economical reuse of substrates. However, the aggressive oxidizing conditions typically used in growing epitaxial oxides can damage graphene. Here, we demonstrate the successful use of hybrid molecular beam epitaxy for SrTiO₃ growth that does not require an independent oxygen source, thus avoiding graphene damage. This approach produces epitaxial films with self-regulating cation stoichiometry. Furthermore, the film (46-nm-thick SrTiO₃) can be exfoliated and transferred to foreign substrates. These results open the door to future studies of previously unattainable freestanding oxide nanomembranes grown in an adsorption-controlled manner by hybrid molecular beam epitaxy. This approach has potentially important implications for the commercial application of perovskite oxides in flexible electronics and as a dielectric in van der Waals thin-film electronics.

Original language	English (US)
Article number	eadd5328
Journal	Science Advances
Volume	8
Issue number	51
DOIs	https://doi.org/10.1126/sciadv.add5328
State	Published - Dec 2022

Bibliographical note

Funding Information:
We thank J. Kim for discussion. Funding: Hybrid MBE growth and characterization of SrTiO3 films were supported by the U.S. Department of Energy (DOE) through grant DE-SC0020211. Graphene growth and integration with the oxide substrate was supported by the Air Force Office of Scientific Research through grants FA9550-21-0460 and FA9550-21-1-0025. Film growth was performed using instrumentation funded by DURIP award FA9550-18-1-0294. Preliminary graphene growth and sample preparation at the University of Wisconsin was supported by the DOE, Office of Science, Basic Energy Sciences, under award no. DE-SC0016007, and the NSF through grant DMR-1752797. Parts of this work were carried out at the Characterization Facility, University of Minnesota, which receives partial support from the NSF through the MRSEC program under award DMR-2011401. Substrate preparation was carried out at the Minnesota Nano Center, which is supported by the NSF through the National Nano Coordinated Infrastructure under award ECCS-2025124. STEM and XPS were supported by the DOE, Office of Science, Office of Basic Energy Sciences, Division of Materials Sciences and Engineering under award no. 10122. Pacific Northwest National Laboratory (PNNL) is a multiprogram national laboratory operated by Battelle for the DOE under contract DE-AC05-79RL01830. We acknowledge facility support from the Environmental Molecular Sciences Laboratory, a DOE Office of Science User Facility sponsored by the Biological and Environmental Research program and located at PNNL. A portion of the microscopy work was performed in the Radiological Microscopy Suite (RMS), located in the Radiochemical Processing Laboratory (RPL) at PNNL.

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Yoon, H., Truttmann, T. K., Liu, F., Matthews, B. E., Choo, S., Su, Q., Saraswat, V., Manzo, S., Arnold, M. S., Bowden, M. E., Kawasaki, J. K., Koester, S. J., Spurgeon, S. R., Chambers, S. A., & Jalan, B. (2022). Freestanding epitaxial SrTiO₃ nanomembranes via remote epitaxy using hybrid molecular beam epitaxy. Science Advances, 8(51), Article eadd5328. https://doi.org/10.1126/sciadv.add5328

@article{6dd656a341bd40f68883b24433de55e7,

title = "Freestanding epitaxial SrTiO3 nanomembranes via remote epitaxy using hybrid molecular beam epitaxy",

abstract = "The epitaxial growth of functional oxides using a substrate with a graphene layer is a highly desirable method for improving structural quality and obtaining freestanding epitaxial nanomembranes for scientific study, applications, and economical reuse of substrates. However, the aggressive oxidizing conditions typically used in growing epitaxial oxides can damage graphene. Here, we demonstrate the successful use of hybrid molecular beam epitaxy for SrTiO3 growth that does not require an independent oxygen source, thus avoiding graphene damage. This approach produces epitaxial films with self-regulating cation stoichiometry. Furthermore, the film (46-nm-thick SrTiO3) can be exfoliated and transferred to foreign substrates. These results open the door to future studies of previously unattainable freestanding oxide nanomembranes grown in an adsorption-controlled manner by hybrid molecular beam epitaxy. This approach has potentially important implications for the commercial application of perovskite oxides in flexible electronics and as a dielectric in van der Waals thin-film electronics.",

author = "Hyojin Yoon and Truttmann, {Tristan K.} and Fengdeng Liu and Matthews, {Bethany E.} and Sooho Choo and Qun Su and Vivek Saraswat and Sebastian Manzo and Arnold, {Michael S.} and Bowden, {Mark E.} and Kawasaki, {Jason K.} and Koester, {Steven J.} and Spurgeon, {Steven R.} and Chambers, {Scott A.} and Bharat Jalan",

note = "Funding Information: We thank J. Kim for discussion. Funding: Hybrid MBE growth and characterization of SrTiO3 films were supported by the U.S. Department of Energy (DOE) through grant DE-SC0020211. Graphene growth and integration with the oxide substrate was supported by the Air Force Office of Scientific Research through grants FA9550-21-0460 and FA9550-21-1-0025. Film growth was performed using instrumentation funded by DURIP award FA9550-18-1-0294. Preliminary graphene growth and sample preparation at the University of Wisconsin was supported by the DOE, Office of Science, Basic Energy Sciences, under award no. DE-SC0016007, and the NSF through grant DMR-1752797. Parts of this work were carried out at the Characterization Facility, University of Minnesota, which receives partial support from the NSF through the MRSEC program under award DMR-2011401. Substrate preparation was carried out at the Minnesota Nano Center, which is supported by the NSF through the National Nano Coordinated Infrastructure under award ECCS-2025124. STEM and XPS were supported by the DOE, Office of Science, Office of Basic Energy Sciences, Division of Materials Sciences and Engineering under award no. 10122. Pacific Northwest National Laboratory (PNNL) is a multiprogram national laboratory operated by Battelle for the DOE under contract DE-AC05-79RL01830. We acknowledge facility support from the Environmental Molecular Sciences Laboratory, a DOE Office of Science User Facility sponsored by the Biological and Environmental Research program and located at PNNL. A portion of the microscopy work was performed in the Radiological Microscopy Suite (RMS), located in the Radiochemical Processing Laboratory (RPL) at PNNL. Publisher Copyright: Copyright {\textcopyright} 2022 The Authors, some rights reserved.",

year = "2022",

month = dec,

doi = "10.1126/sciadv.add5328",

language = "English (US)",

volume = "8",

journal = "Science Advances",

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T1 - Freestanding epitaxial SrTiO3 nanomembranes via remote epitaxy using hybrid molecular beam epitaxy

AU - Yoon, Hyojin

AU - Truttmann, Tristan K.

AU - Liu, Fengdeng

AU - Matthews, Bethany E.

AU - Choo, Sooho

AU - Su, Qun

AU - Saraswat, Vivek

AU - Manzo, Sebastian

AU - Arnold, Michael S.

AU - Bowden, Mark E.

AU - Kawasaki, Jason K.

AU - Koester, Steven J.

AU - Spurgeon, Steven R.

AU - Chambers, Scott A.

AU - Jalan, Bharat

N1 - Funding Information: We thank J. Kim for discussion. Funding: Hybrid MBE growth and characterization of SrTiO3 films were supported by the U.S. Department of Energy (DOE) through grant DE-SC0020211. Graphene growth and integration with the oxide substrate was supported by the Air Force Office of Scientific Research through grants FA9550-21-0460 and FA9550-21-1-0025. Film growth was performed using instrumentation funded by DURIP award FA9550-18-1-0294. Preliminary graphene growth and sample preparation at the University of Wisconsin was supported by the DOE, Office of Science, Basic Energy Sciences, under award no. DE-SC0016007, and the NSF through grant DMR-1752797. Parts of this work were carried out at the Characterization Facility, University of Minnesota, which receives partial support from the NSF through the MRSEC program under award DMR-2011401. Substrate preparation was carried out at the Minnesota Nano Center, which is supported by the NSF through the National Nano Coordinated Infrastructure under award ECCS-2025124. STEM and XPS were supported by the DOE, Office of Science, Office of Basic Energy Sciences, Division of Materials Sciences and Engineering under award no. 10122. Pacific Northwest National Laboratory (PNNL) is a multiprogram national laboratory operated by Battelle for the DOE under contract DE-AC05-79RL01830. We acknowledge facility support from the Environmental Molecular Sciences Laboratory, a DOE Office of Science User Facility sponsored by the Biological and Environmental Research program and located at PNNL. A portion of the microscopy work was performed in the Radiological Microscopy Suite (RMS), located in the Radiochemical Processing Laboratory (RPL) at PNNL. Publisher Copyright: Copyright © 2022 The Authors, some rights reserved.

PY - 2022/12

Y1 - 2022/12

N2 - The epitaxial growth of functional oxides using a substrate with a graphene layer is a highly desirable method for improving structural quality and obtaining freestanding epitaxial nanomembranes for scientific study, applications, and economical reuse of substrates. However, the aggressive oxidizing conditions typically used in growing epitaxial oxides can damage graphene. Here, we demonstrate the successful use of hybrid molecular beam epitaxy for SrTiO3 growth that does not require an independent oxygen source, thus avoiding graphene damage. This approach produces epitaxial films with self-regulating cation stoichiometry. Furthermore, the film (46-nm-thick SrTiO3) can be exfoliated and transferred to foreign substrates. These results open the door to future studies of previously unattainable freestanding oxide nanomembranes grown in an adsorption-controlled manner by hybrid molecular beam epitaxy. This approach has potentially important implications for the commercial application of perovskite oxides in flexible electronics and as a dielectric in van der Waals thin-film electronics.

AB - The epitaxial growth of functional oxides using a substrate with a graphene layer is a highly desirable method for improving structural quality and obtaining freestanding epitaxial nanomembranes for scientific study, applications, and economical reuse of substrates. However, the aggressive oxidizing conditions typically used in growing epitaxial oxides can damage graphene. Here, we demonstrate the successful use of hybrid molecular beam epitaxy for SrTiO3 growth that does not require an independent oxygen source, thus avoiding graphene damage. This approach produces epitaxial films with self-regulating cation stoichiometry. Furthermore, the film (46-nm-thick SrTiO3) can be exfoliated and transferred to foreign substrates. These results open the door to future studies of previously unattainable freestanding oxide nanomembranes grown in an adsorption-controlled manner by hybrid molecular beam epitaxy. This approach has potentially important implications for the commercial application of perovskite oxides in flexible electronics and as a dielectric in van der Waals thin-film electronics.

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Freestanding epitaxial SrTiO₃ nanomembranes via remote epitaxy using hybrid molecular beam epitaxy

Abstract

Bibliographical note

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IRG-1: Ionic Control of Materials

University of Minnesota Materials Research Science and Engineering Center (DMR-2011401)

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Freestanding epitaxial SrTiO3 nanomembranes via remote epitaxy using hybrid molecular beam epitaxy

Abstract

Bibliographical note

MRSEC Support

PubMed: MeSH publication types

Publisher link

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Projects

IRG-1: Ionic Control of Materials

University of Minnesota Materials Research Science and Engineering Center (DMR-2011401)

Cite this

Freestanding epitaxial SrTiO₃ nanomembranes via remote epitaxy using hybrid molecular beam epitaxy