Sn-modified BaTiO3thin film with enhanced polarization

William T Nunn; Abinash Kumar; Rui Zu; Bailey Nebgen; Shukai Yu; Anusha Kamath Manjeshwar; Venkatraman Gopalan; James M. Lebeau; Richard D. James; Bharat Jalan

doi:10.1116/6.0002208

Sn-modified BaTiO₃thin film with enhanced polarization

William T Nunn, Abinash Kumar, Rui Zu, Bailey Nebgen, Shukai Yu, Anusha Kamath Manjeshwar, Venkatraman Gopalan, James M. Lebeau, Richard D. James, Bharat Jalan

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Abstract

Hybrid molecular beam epitaxy (MBE) growth of Sn-modified BaTiO3 films was realized with varying domain structures and crystal symmetries across the entire composition space. Macroscopic and microscopic structures and the crystal symmetry of these thin films were determined using a combination of optical second harmonic generation (SHG) polarimetry and scanning transmission electron microscopy (STEM). SHG polarimetry revealed a variation in the global crystal symmetry of the films from tetragonal (P4mm) to cubic (P m 3 ¯ m) across the composition range, x = 0 to 1 in BaTi1-xSnxO3 (BTSO). STEM imaging shows that the long-range polar order observed when the Sn content is low (x = 0.09) transformed to a short-range polar order as the Sn content increased (x = 0.48). Consistent with atomic displacement measurements from STEM, the largest polarization was obtained at the lowest Sn content of x = 0.09 in Sn-modified BaTiO3 as determined by SHG. These results agree with recent bulk ceramic reports and further identify this material system as a potential replacement for Pb-containing relaxor-based thin film devices.

Original language	English (US)
Article number	022701
Journal	Journal of Vacuum Science and Technology A: Vacuum, Surfaces and Films
Volume	41
Issue number	2
DOIs	https://doi.org/10.1116/6.0002208
State	Published - Mar 1 2023

Bibliographical note

Funding Information:
Hybrid MBE growth and characterization of BaTiSnO films were supported primarily by the U.S. Department of Energy (DOE) through Grant No. DE-SC0020211. Part of the work was supported as part of the Center for Programmable Energy Catalysis, an Energy Frontier Research Center funded by the U.S. Department of Energy, Office of Science, Basic Energy Sciences at the University of Minnesota, under Award No. DE-SC0023464. 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 No. DMR-2011401. This work also benefitted from the Vannevar Bush Faculty Fellowship. Part of this work was carried out at the Minnesota Nano Center, which is supported by the NSF through the National Nano Coordinated Infrastructure under Award No. ECCS-2025124. A.K. and J.M.L. were supported by the Army Research Laboratory via the Collaborative for Hierarchical Agile and Responsive Materials (CHARM) under Cooperative Agreement No. W911NF-19-2-0119. R.Z. and V.G. were supported by the Department of Energy (DOE), Office of Science, Basic Energy Sciences, under Award No. DE-SC002111. B.N. was supported by NSF Research Experiences for Undergraduates (REU) (No. DMR 185-1987). S.Y. and V.G. were supported under Award No. DE-SC0012375. 1− x x 3

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title = "Sn-modified BaTiO3thin film with enhanced polarization",

abstract = "Hybrid molecular beam epitaxy (MBE) growth of Sn-modified BaTiO3 films was realized with varying domain structures and crystal symmetries across the entire composition space. Macroscopic and microscopic structures and the crystal symmetry of these thin films were determined using a combination of optical second harmonic generation (SHG) polarimetry and scanning transmission electron microscopy (STEM). SHG polarimetry revealed a variation in the global crystal symmetry of the films from tetragonal (P4mm) to cubic (P m 3 ¯ m) across the composition range, x = 0 to 1 in BaTi1-xSnxO3 (BTSO). STEM imaging shows that the long-range polar order observed when the Sn content is low (x = 0.09) transformed to a short-range polar order as the Sn content increased (x = 0.48). Consistent with atomic displacement measurements from STEM, the largest polarization was obtained at the lowest Sn content of x = 0.09 in Sn-modified BaTiO3 as determined by SHG. These results agree with recent bulk ceramic reports and further identify this material system as a potential replacement for Pb-containing relaxor-based thin film devices.",

author = "Nunn, {William T} and Abinash Kumar and Rui Zu and Bailey Nebgen and Shukai Yu and {Kamath Manjeshwar}, Anusha and Venkatraman Gopalan and Lebeau, {James M.} and James, {Richard D.} and Bharat Jalan",

note = "Funding Information: Hybrid MBE growth and characterization of BaTiSnO films were supported primarily by the U.S. Department of Energy (DOE) through Grant No. DE-SC0020211. Part of the work was supported as part of the Center for Programmable Energy Catalysis, an Energy Frontier Research Center funded by the U.S. Department of Energy, Office of Science, Basic Energy Sciences at the University of Minnesota, under Award No. DE-SC0023464. 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 No. DMR-2011401. This work also benefitted from the Vannevar Bush Faculty Fellowship. Part of this work was carried out at the Minnesota Nano Center, which is supported by the NSF through the National Nano Coordinated Infrastructure under Award No. ECCS-2025124. A.K. and J.M.L. were supported by the Army Research Laboratory via the Collaborative for Hierarchical Agile and Responsive Materials (CHARM) under Cooperative Agreement No. W911NF-19-2-0119. R.Z. and V.G. were supported by the Department of Energy (DOE), Office of Science, Basic Energy Sciences, under Award No. DE-SC002111. B.N. was supported by NSF Research Experiences for Undergraduates (REU) (No. DMR 185-1987). S.Y. and V.G. were supported under Award No. DE-SC0012375. 1− x x 3 Publisher Copyright: {\textcopyright} 2023 Author(s).",

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AU - Kumar, Abinash

AU - Zu, Rui

AU - Nebgen, Bailey

AU - Yu, Shukai

AU - Kamath Manjeshwar, Anusha

AU - Gopalan, Venkatraman

AU - Lebeau, James M.

AU - James, Richard D.

AU - Jalan, Bharat

N1 - Funding Information: Hybrid MBE growth and characterization of BaTiSnO films were supported primarily by the U.S. Department of Energy (DOE) through Grant No. DE-SC0020211. Part of the work was supported as part of the Center for Programmable Energy Catalysis, an Energy Frontier Research Center funded by the U.S. Department of Energy, Office of Science, Basic Energy Sciences at the University of Minnesota, under Award No. DE-SC0023464. 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 No. DMR-2011401. This work also benefitted from the Vannevar Bush Faculty Fellowship. Part of this work was carried out at the Minnesota Nano Center, which is supported by the NSF through the National Nano Coordinated Infrastructure under Award No. ECCS-2025124. A.K. and J.M.L. were supported by the Army Research Laboratory via the Collaborative for Hierarchical Agile and Responsive Materials (CHARM) under Cooperative Agreement No. W911NF-19-2-0119. R.Z. and V.G. were supported by the Department of Energy (DOE), Office of Science, Basic Energy Sciences, under Award No. DE-SC002111. B.N. was supported by NSF Research Experiences for Undergraduates (REU) (No. DMR 185-1987). S.Y. and V.G. were supported under Award No. DE-SC0012375. 1− x x 3 Publisher Copyright: © 2023 Author(s).

PY - 2023/3/1

Y1 - 2023/3/1

N2 - Hybrid molecular beam epitaxy (MBE) growth of Sn-modified BaTiO3 films was realized with varying domain structures and crystal symmetries across the entire composition space. Macroscopic and microscopic structures and the crystal symmetry of these thin films were determined using a combination of optical second harmonic generation (SHG) polarimetry and scanning transmission electron microscopy (STEM). SHG polarimetry revealed a variation in the global crystal symmetry of the films from tetragonal (P4mm) to cubic (P m 3 ¯ m) across the composition range, x = 0 to 1 in BaTi1-xSnxO3 (BTSO). STEM imaging shows that the long-range polar order observed when the Sn content is low (x = 0.09) transformed to a short-range polar order as the Sn content increased (x = 0.48). Consistent with atomic displacement measurements from STEM, the largest polarization was obtained at the lowest Sn content of x = 0.09 in Sn-modified BaTiO3 as determined by SHG. These results agree with recent bulk ceramic reports and further identify this material system as a potential replacement for Pb-containing relaxor-based thin film devices.

AB - Hybrid molecular beam epitaxy (MBE) growth of Sn-modified BaTiO3 films was realized with varying domain structures and crystal symmetries across the entire composition space. Macroscopic and microscopic structures and the crystal symmetry of these thin films were determined using a combination of optical second harmonic generation (SHG) polarimetry and scanning transmission electron microscopy (STEM). SHG polarimetry revealed a variation in the global crystal symmetry of the films from tetragonal (P4mm) to cubic (P m 3 ¯ m) across the composition range, x = 0 to 1 in BaTi1-xSnxO3 (BTSO). STEM imaging shows that the long-range polar order observed when the Sn content is low (x = 0.09) transformed to a short-range polar order as the Sn content increased (x = 0.48). Consistent with atomic displacement measurements from STEM, the largest polarization was obtained at the lowest Sn content of x = 0.09 in Sn-modified BaTiO3 as determined by SHG. These results agree with recent bulk ceramic reports and further identify this material system as a potential replacement for Pb-containing relaxor-based thin film devices.

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Sn-modified BaTiO₃thin film with enhanced polarization

Abstract

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IRG-1: Ionic Control of Materials

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Sn-modified BaTiO3thin film with enhanced polarization

Abstract

Bibliographical note

MRSEC Support

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IRG-1: Ionic Control of Materials

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

Cite this

Sn-modified BaTiO₃thin film with enhanced polarization