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Title: Strain-induced majority carrier inversion in ferromagnetic epitaxial LaCo O 3 - δ thin films

Abstract

Tensile-strained LaCoO3-δ thin films are ferromagnetic, in sharp contrast to the zero-spin bulk, although no clear consensus has emerged as to the origin of this phenomenon. While magnetism has been heavily studied, relatively little attention has been paid to electronic transport, due to the insulating nature of the strain-stabilized ferromagnetic state. Here, structure, magnetism, and transport are studied in epitaxial LaCoO3-δ films (10–22-nm thick) on various substrates (from 1.4% compressive to 2.5% tensile strain), using synchrotron x-ray diffraction, scanning probe and transmission electron microscopy, magnetometry, polarized neutron reflectometry, resistivity, and Hall effect. High quality, smooth films are obtained, exhibiting superstructures associated with both oxygen vacancy ordering and periodic in-plane ferroelastic domains. Consistent with prior work, ferromagnetism with an approximately 80–85 K Curie temperature is observed under tension; polarized neutron reflectometry confirms a relatively uniform magnetization depth profile, albeit with interfacial dead layer formation. Electrical transport is found to have similar semiconducting nature to bulk, but with reduced resistivity and activation energy. Hall effect measurements, however, reveal a striking inversion of the majority carrier type, from p-type in the bulk and under compression to n-type under tension. While thus far overlooked, ferromagnetism in epitaxial LaCoO3-δ films is thus directly correlated withmore » n-type behavior, providing important insight into the ferromagnetic state in this system. Here, aided by density functional theory calculations, these results are interpreted in terms of tensile-strain-induced orbital occupation and band structure changes, including a rapid decrease in effective mass at the eg-derived conduction band minimum, and corresponding increase at the valence band maximum.« less

Authors:
 [1];  [2];  [1]; ORCiD logo [3];  [3];  [1];  [4];  [4];  [1];  [1];  [1]; ORCiD logo [1]; ORCiD logo [1]
  1. Univ. of Minnesota, Minneapolis, MN (United States)
  2. Univ. of Minnesota, Minneapolis, MN (United States); Augsburg Univ., Minneapolis, MN (United States)
  3. National Inst. of Standards and Technology (NIST), Gaithersburg, MD (United States)
  4. Argonne National Lab. (ANL), Lemont, IL (United States)
Publication Date:
Research Org.:
Argonne National Laboratory (ANL), Argonne, IL (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES); National Science Foundation (NSF)
OSTI Identifier:
1614758
Alternate Identifier(s):
OSTI ID: 1603210
Grant/Contract Number:  
AC02-06CH11357; DMR-1420013; SC0016371
Resource Type:
Accepted Manuscript
Journal Name:
Physical Review Materials
Additional Journal Information:
Journal Volume: 4; Journal Issue: 3; Journal ID: ISSN 2475-9953
Publisher:
American Physical Society (APS)
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE

Citation Formats

Chaturvedi, Vipul, Walter, Jeff, Paul, Arpita, Grutter, Alexander, Kirby, Brian, Jeong, Jong Seok, Zhou, Hua, Zhang, Zhan, Yu, Biqiong, Greven, Martin, Mkhoyan, K. Andre, Birol, Turan, and Leighton, Chris. Strain-induced majority carrier inversion in ferromagnetic epitaxial LaCoO3-δ thin films. United States: N. p., 2020. Web. doi:10.1103/PhysRevMaterials.4.034403.
Chaturvedi, Vipul, Walter, Jeff, Paul, Arpita, Grutter, Alexander, Kirby, Brian, Jeong, Jong Seok, Zhou, Hua, Zhang, Zhan, Yu, Biqiong, Greven, Martin, Mkhoyan, K. Andre, Birol, Turan, & Leighton, Chris. Strain-induced majority carrier inversion in ferromagnetic epitaxial LaCoO3-δ thin films. United States. https://doi.org/10.1103/PhysRevMaterials.4.034403
Chaturvedi, Vipul, Walter, Jeff, Paul, Arpita, Grutter, Alexander, Kirby, Brian, Jeong, Jong Seok, Zhou, Hua, Zhang, Zhan, Yu, Biqiong, Greven, Martin, Mkhoyan, K. Andre, Birol, Turan, and Leighton, Chris. Wed . "Strain-induced majority carrier inversion in ferromagnetic epitaxial LaCoO3-δ thin films". United States. https://doi.org/10.1103/PhysRevMaterials.4.034403. https://www.osti.gov/servlets/purl/1614758.
@article{osti_1614758,
title = {Strain-induced majority carrier inversion in ferromagnetic epitaxial LaCoO3-δ thin films},
author = {Chaturvedi, Vipul and Walter, Jeff and Paul, Arpita and Grutter, Alexander and Kirby, Brian and Jeong, Jong Seok and Zhou, Hua and Zhang, Zhan and Yu, Biqiong and Greven, Martin and Mkhoyan, K. Andre and Birol, Turan and Leighton, Chris},
abstractNote = {Tensile-strained LaCoO3-δ thin films are ferromagnetic, in sharp contrast to the zero-spin bulk, although no clear consensus has emerged as to the origin of this phenomenon. While magnetism has been heavily studied, relatively little attention has been paid to electronic transport, due to the insulating nature of the strain-stabilized ferromagnetic state. Here, structure, magnetism, and transport are studied in epitaxial LaCoO3-δ films (10–22-nm thick) on various substrates (from 1.4% compressive to 2.5% tensile strain), using synchrotron x-ray diffraction, scanning probe and transmission electron microscopy, magnetometry, polarized neutron reflectometry, resistivity, and Hall effect. High quality, smooth films are obtained, exhibiting superstructures associated with both oxygen vacancy ordering and periodic in-plane ferroelastic domains. Consistent with prior work, ferromagnetism with an approximately 80–85 K Curie temperature is observed under tension; polarized neutron reflectometry confirms a relatively uniform magnetization depth profile, albeit with interfacial dead layer formation. Electrical transport is found to have similar semiconducting nature to bulk, but with reduced resistivity and activation energy. Hall effect measurements, however, reveal a striking inversion of the majority carrier type, from p-type in the bulk and under compression to n-type under tension. While thus far overlooked, ferromagnetism in epitaxial LaCoO3-δ films is thus directly correlated with n-type behavior, providing important insight into the ferromagnetic state in this system. Here, aided by density functional theory calculations, these results are interpreted in terms of tensile-strain-induced orbital occupation and band structure changes, including a rapid decrease in effective mass at the eg-derived conduction band minimum, and corresponding increase at the valence band maximum.},
doi = {10.1103/PhysRevMaterials.4.034403},
journal = {Physical Review Materials},
number = 3,
volume = 4,
place = {United States},
year = {Wed Mar 04 00:00:00 EST 2020},
month = {Wed Mar 04 00:00:00 EST 2020}
}

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