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Title: Surface control of epitaxial manganite films via oxygen pressure

Abstract

The trend to reduce device dimensions demands increasing attention to atomic-scale details of structure of thin films as well as to pathways to control it. We found that this is of special importance in the systems with multiple competing interactions. We have used in situ scanning tunneling microscopy to image surfaces of La5/8Ca3/8MnO3 films grown by pulsed laser deposition. The atomically resolved imaging was combined with in situ angle-resolved X-ray photoelectron spectroscopy. We find a strong effect of the background oxygen pressure during deposition on structural and chemical features of the film surface. Deposition at 50 mTorr of O2 leads to mixed-terminated film surfaces, with B-site (MnO2) termination being structurally imperfect at the atomic scale. Moreover, a relatively small reduction of the oxygen pressure to 20 mTorr results in a dramatic change of the surface structure leading to a nearly perfectly ordered B-site terminated surface with only a small fraction of A-site (La,Ca)O termination. This is accompanied, however, by surface roughening at a mesoscopic length scale. The results suggest that oxygen has a strong link to the adatom mobility during growth. The effect of the oxygen pressure on dopant surface segregation is also pronounced: Ca surface segregation is decreased withmore » oxygen pressure reduction.« less

Authors:
 [1];  [1];  [1];  [1];  [1];  [1];  [1];  [1];  [1];  [1]
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  1. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Publication Date:
Research Org.:
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)
Sponsoring Org.:
USDOE Office of Science (SC)
OSTI Identifier:
1190748
Grant/Contract Number:  
AC05-00OR22725
Resource Type:
Accepted Manuscript
Journal Name:
ACS Nano
Additional Journal Information:
Journal Volume: 9; Journal Issue: 4; Journal ID: ISSN 1936-0851
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
42 ENGINEERING; perovskite manganite; pulsed laser deposition; scanning tunneling microscopy; x-ray photoelectron spectroscopy; surface structure

Citation Formats

Tselev, Alexander, Vasudevan, Rama K., Gianfrancesco, Anthony G., Qiao, Liang, Ganesh, Panchapakesan, Meyer, Tricia L., Lee, Ho Nyung, Biegalski, Michael D., Baddorf, Arthur P., and Kalinin, Sergei. Surface control of epitaxial manganite films via oxygen pressure. United States: N. p., 2015. Web. doi:10.1021/acsnano.5b00743.
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Tselev, Alexander, Vasudevan, Rama K., Gianfrancesco, Anthony G., Qiao, Liang, Ganesh, Panchapakesan, Meyer, Tricia L., Lee, Ho Nyung, Biegalski, Michael D., Baddorf, Arthur P., & Kalinin, Sergei. Surface control of epitaxial manganite films via oxygen pressure. United States. https://doi.org/10.1021/acsnano.5b00743
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Tselev, Alexander, Vasudevan, Rama K., Gianfrancesco, Anthony G., Qiao, Liang, Ganesh, Panchapakesan, Meyer, Tricia L., Lee, Ho Nyung, Biegalski, Michael D., Baddorf, Arthur P., and Kalinin, Sergei. Wed . "Surface control of epitaxial manganite films via oxygen pressure". United States. https://doi.org/10.1021/acsnano.5b00743. https://www.osti.gov/servlets/purl/1190748.
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@article{osti_1190748,
title = {Surface control of epitaxial manganite films via oxygen pressure},
author = {Tselev, Alexander and Vasudevan, Rama K. and Gianfrancesco, Anthony G. and Qiao, Liang and Ganesh, Panchapakesan and Meyer, Tricia L. and Lee, Ho Nyung and Biegalski, Michael D. and Baddorf, Arthur P. and Kalinin, Sergei},
abstractNote = {The trend to reduce device dimensions demands increasing attention to atomic-scale details of structure of thin films as well as to pathways to control it. We found that this is of special importance in the systems with multiple competing interactions. We have used in situ scanning tunneling microscopy to image surfaces of La5/8Ca3/8MnO3 films grown by pulsed laser deposition. The atomically resolved imaging was combined with in situ angle-resolved X-ray photoelectron spectroscopy. We find a strong effect of the background oxygen pressure during deposition on structural and chemical features of the film surface. Deposition at 50 mTorr of O2 leads to mixed-terminated film surfaces, with B-site (MnO2) termination being structurally imperfect at the atomic scale. Moreover, a relatively small reduction of the oxygen pressure to 20 mTorr results in a dramatic change of the surface structure leading to a nearly perfectly ordered B-site terminated surface with only a small fraction of A-site (La,Ca)O termination. This is accompanied, however, by surface roughening at a mesoscopic length scale. The results suggest that oxygen has a strong link to the adatom mobility during growth. The effect of the oxygen pressure on dopant surface segregation is also pronounced: Ca surface segregation is decreased with oxygen pressure reduction.},
doi = {10.1021/acsnano.5b00743},
journal = {ACS Nano},
number = 4,
volume = 9,
place = {United States},
year = {Wed Mar 11 00:00:00 EDT 2015},
month = {Wed Mar 11 00:00:00 EDT 2015}
}
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https://doi.org/10.1021/acsnano.5b00743
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Works referenced in this record:

Critical features of colossal magnetoresistive manganites
journal, February 2006

Mixed-valence manganites
journal, November 2009

Colossal magnetoresistant materials: the key role of phase separation
journal, April 2001

Electric field effect in correlated oxide systems
journal, August 2003

  • Ahn, C. H.; Triscone, J. -M.; Mannhart, J.
  • Nature, Vol. 424, Issue 6952
  • DOI: 10.1038/nature01878

Strain-induced metal–insulator phase coexistence in perovskite manganites
journal, March 2004

Transient photoinduced ‘hidden’ phase in a manganite
journal, January 2011

  • Ichikawa, Hirohiko; Nozawa, Shunsuke; Sato, Tokushi
  • Nature Materials, Vol. 10, Issue 2
  • DOI: 10.1038/nmat2929

Giant magnetoresistance in organic spin-valves
journal, February 2004

Engineered Interface of Magnetic Oxides
journal, July 2004

Ferromagnetic manganites: spin-polarized conduction versus competing interactions
journal, March 2006

Unravelling the role of the interface for spin injection into organic semiconductors
journal, June 2010

  • Barraud, Clément; Seneor, Pierre; Mattana, Richard
  • Nature Physics, Vol. 6, Issue 8
  • DOI: 10.1038/nphys1688

Ferroelectric Control of Spin Polarization
journal, January 2010

Spin-Filter Tunnel Junction with Matched Fermi Surfaces
journal, August 2012

Tuning the Competition between Ferromagnetism and Antiferromagnetism in a Half-Doped Manganite through Magnetoelectric Coupling
journal, September 2013

Biskyrmion states and their current-driven motion in a layered manganite
journal, January 2014

  • Yu, X. Z.; Tokunaga, Y.; Kaneko, Y.
  • Nature Communications, Vol. 5, Issue 1
  • DOI: 10.1038/ncomms4198

Reversible Resistive Switching and Multilevel Recording in La 0.7 Sr 0.3 MnO 3 Thin Films for Low Cost Nonvolatile Memories
journal, October 2010

  • Moreno, César; Munuera, Carmen; Valencia, Sergio
  • Nano Letters, Vol. 10, Issue 10
  • DOI: 10.1021/nl1008162

Cathode materials for solid oxide fuel cells: a review
journal, October 2009

  • Sun, Chunwen; Hui, Rob; Roller, Justin
  • Journal of Solid State Electrochemistry, Vol. 14, Issue 7
  • DOI: 10.1007/s10008-009-0932-0

Microscopic origins for stabilizing room-temperature ferromagnetism in ultrathin manganite layers
journal, June 2010

  • Kourkoutis, L. F.; Song, J. H.; Hwang, H. Y.
  • Proceedings of the National Academy of Sciences, Vol. 107, Issue 26
  • DOI: 10.1073/pnas.1005693107

Thickness-dependent magnetotransport in ultrathin manganite films
journal, May 1999

  • Sun, J. Z.; Abraham, D. W.; Rao, R. A.
  • Applied Physics Letters, Vol. 74, Issue 20
  • DOI: 10.1063/1.124050

Surface electronic structure and magnetic properties of doped manganites
journal, September 1999

Full bulk spin polarization and intrinsic tunnel barriers at the surface of layered manganites
journal, December 2004

  • Freeland, J. W.; Gray, K. E.; Ozyuzer, L.
  • Nature Materials, Vol. 4, Issue 1
  • DOI: 10.1038/nmat1280

Surface polaron formation in the Holstein model
journal, October 2009

Competition between reduced delocalization and charge transfer effects for a two-band Hubbard model
journal, August 2011

Interface Effects in Perovskite Thin Films
journal, February 2012

Nanoscale Multiphase Separation at La 2 / 3 Ca 1 / 3 MnO 3 / SrTiO 3 Interfaces
journal, July 2001

Establishing the LaMnO 3 Surface Phase Diagram in an Oxygen Environment: An ab Initio Kinetic Monte Carlo Simulation Study
journal, December 2012

  • Pilania, G.; Gao, P. -X.; Ramprasad, R.
  • The Journal of Physical Chemistry C, Vol. 116, Issue 50
  • DOI: 10.1021/jp3083985

Atomically Resolved Surface Structure of SrTiO 3 (001) Thin Films Grown in Step-Flow Mode by Pulsed Laser Deposition
journal, June 2010

  • Iwaya, Katsuya; Ohsawa, Takeo; Shimizu, Ryota
  • Applied Physics Express, Vol. 3, Issue 7
  • DOI: 10.1143/APEX.3.075701

Thickness-dependent local surface electronic structures of homoepitaxial SrTiO3 thin films
journal, October 2010

  • Ohsawa, T.; Iwaya, K.; Shimizu, R.
  • Journal of Applied Physics, Vol. 108, Issue 7
  • DOI: 10.1063/1.3485826

Oxygen-Induced Surface Reconstruction of SrRuO 3 and Its Effect on the BaTiO 3 Interface
journal, June 2010

  • Shin, Junsoo; Borisevich, Albina Y.; Meunier, Vincent
  • ACS Nano, Vol. 4, Issue 7
  • DOI: 10.1021/nn1008337

Oxygen Control of Atomic Structure and Physical Properties of SrRuO 3 Surfaces
journal, April 2013

  • Tselev, Alexander; Ganesh, P.; Qiao, Liang
  • ACS Nano, Vol. 7, Issue 5
  • DOI: 10.1021/nn400923n

Visualizing Atomistic Formation Process of SrO x Thin Films on SrTiO 3
journal, March 2014

  • Ohsawa, Takeo; Shimizu, Ryota; Iwaya, Katsuya
  • ACS Nano, Vol. 8, Issue 3
  • DOI: 10.1021/nn405359u

Epitaxial Growth Process of La 0.7 Ca 0.3 MnO 3 Thin Films on SrTiO 3 (001): Thickness-Dependent Inhomogeneity Caused by Excess Ti Atoms
journal, March 2014

  • Shimizu, Ryota; Ohsawa, Takeo; Iwaya, Katsuya
  • Crystal Growth & Design, Vol. 14, Issue 4
  • DOI: 10.1021/cg4013119

Atomic-scale images of charge ordering in a mixed-valence manganite
journal, April 2002

  • Renner, Ch.; Aeppli, G.; Kim, B. -G.
  • Nature, Vol. 416, Issue 6880
  • DOI: 10.1038/416518a

Atomically resolved scanning tunneling microscopy on perovskite manganite single crystals
journal, May 2010

  • Rößler, Sahana; Padmanabhan, B.; Elizabeth, Suja
  • Applied Physics Letters, Vol. 96, Issue 20
  • DOI: 10.1063/1.3432753

Polarons and confinement of electronic motion to two dimensions in a layered manganite
journal, April 2006

  • Rønnow, H. M.; Renner, Ch.; Aeppli, G.
  • Nature, Vol. 440, Issue 7087
  • DOI: 10.1038/nature04650

Imaging oxygen defects and their motion at a manganite surface
journal, March 2011

  • Bryant, B.; Renner, Ch.; Tokunaga, Y.
  • Nature Communications, Vol. 2, Issue 1
  • DOI: 10.1038/ncomms1219

Mesoscopic Texture in Manganites
journal, January 2003

  • Mathur, Neil; Littlewood, Peter
  • Physics Today, Vol. 56, Issue 1
  • DOI: 10.1063/1.1554133

Cation Size Mismatch and Charge Interactions Drive Dopant Segregation at the Surfaces of Manganite Perovskites
journal, May 2013

  • Lee, Wonyoung; Han, Jeong Woo; Chen, Yan
  • Journal of the American Chemical Society, Vol. 135, Issue 21
  • DOI: 10.1021/ja3125349

Tunable Metallicity of the La 5 / 8 Ca 3 / 8 MnO 3 ( 001 ) Surface by an Oxygen Overlayer
journal, February 2009

Enhanced Thermodynamic Stability of Epitaxial Oxide Thin Films
journal, July 2008

  • Song, Jong Hyun; Susaki, Tomofumi; Hwang, Harold Y.
  • Advanced Materials, Vol. 20, Issue 13
  • DOI: 10.1002/adma.200701919

Critical thickness and orbital ordering in ultrathin La 0.7 Sr 0.3 MnO 3 films
journal, September 2008

Interface and Surface Cation Stoichiometry Modified by Oxygen Vacancies in Epitaxial Manganite Films
journal, June 2012

  • Li, Zhipeng; Bosman, Michel; Yang, Zhen
  • Advanced Functional Materials, Vol. 22, Issue 20
  • DOI: 10.1002/adfm.201200143

Consequences of High Adatom Energy during Pulsed Laser Deposition of La 0.7 Sr 0.3 MnO 3
journal, January 2012

  • Boschker, Jos E.; Folven, Erik; Monsen, Åsmund F.
  • Crystal Growth & Design, Vol. 12, Issue 2
  • DOI: 10.1021/cg201461a

Atomic Layer Engineering of Perovskite Oxides for Chemically Sharp Heterointerfaces
journal, October 2012

  • Choi, Woo Seok; Rouleau, Christopher M.; Seo, Sung Seok A.
  • Advanced Materials, Vol. 24, Issue 48
  • DOI: 10.1002/adma.201202691

Surfaces of the perovskite manganites La 1 − x Ca x MnO 3
journal, May 1999

In situ photoemission characterization of terminating-layer-controlled La0.6Sr0.4MnO3 thin films
journal, May 2003

  • Kumigashira, H.; Horiba, K.; Ohguchi, H.
  • Applied Physics Letters, Vol. 82, Issue 20
  • DOI: 10.1063/1.1575932

The surface layer of cleaved bilayer manganites
journal, December 2006

X-ray photoelectron diffraction study of dopant effects in La 0.7 X 0.3 MnO 3 (X = La, Sr, Ca, Ce) thin films
journal, February 2013

  • Raisch, C.; Langheinrich, C.; Werner, R.
  • Journal of Applied Physics, Vol. 113, Issue 6
  • DOI: 10.1063/1.4789988

Mn 3 s exchange splitting in mixed-valence manganites
journal, February 2002

XPS investigation of Mn valence in lanthanum manganite thin films under variation of oxygen content
journal, April 2006

Surface characterization of colossal magnetoresistive manganites La1−xSrxMnO3 using photoelectron spectroscopy
journal, August 2006

  • Mannella, N.; Rosenhahn, A.; Nambu, A.
  • Journal of Electron Spectroscopy and Related Phenomena, Vol. 153, Issue 1-2
  • DOI: 10.1016/j.elspec.2006.06.003

X-ray photoelectron spectroscopy study of (Ca1−xLax)MnO2.97 (0.1 ≦ x ≦ 0.4)
journal, March 1987

A Combined Ion Scattering, Photoemission, and DFT Investigation on the Termination Layer of a La 0.7 Sr 0.3 MnO 3 Spin Injecting Electrode
journal, June 2014

  • Poggini, L.; Ninova, S.; Graziosi, P.
  • The Journal of Physical Chemistry C, Vol. 118, Issue 25
  • DOI: 10.1021/jp5026619

Contribution of oxygen partial pressures investigated over a wide range to SrRuO3 thin-film properties in laser deposition processing
journal, May 2005

  • Yoo, Y. Z.; Chmaissem, O.; Kolesnik, S.
  • Journal of Applied Physics, Vol. 97, Issue 10
  • DOI: 10.1063/1.1909284

Crystallinity, surface morphology, and magnetic properties of La0.7Sr0.3MnO3 thin films: An approach based on the laser ablation plume range models
journal, May 2003

  • Koubaa, M.; Haghiri-Gosnet, A. M.; Desfeux, R.
  • Journal of Applied Physics, Vol. 93, Issue 9
  • DOI: 10.1063/1.1566093

Physics and diagnostics of laser ablation plume propagation for high-Tc superconductor film growth
journal, November 1992

Pulsed laser deposition of oxides: Why the optimum rate is about 1 Å per pulse
journal, September 1998

  • Strikovski, Mikhail; Miller, John H.
  • Applied Physics Letters, Vol. 73, Issue 12
  • DOI: 10.1063/1.122260

The microstructure of sputter‐deposited coatings
journal, November 1986

  • Thornton, John A.
  • Journal of Vacuum Science & Technology A: Vacuum, Surfaces, and Films, Vol. 4, Issue 6
  • DOI: 10.1116/1.573628

In situ characterization of strontium surface segregation in epitaxial La0.7Sr0.3MnO3 thin films as a function of oxygen partial pressure
journal, October 2008

  • Fister, Tim T.; Fong, Dillon D.; Eastman, Jeffrey A.
  • Applied Physics Letters, Vol. 93, Issue 15
  • DOI: 10.1063/1.2987731

Nearly total spin polarization in La2/3Sr1/3MnO3 from tunneling experiments
journal, January 2003

  • Bowen, M.; Bibes, M.; Barthélémy, A.
  • Applied Physics Letters, Vol. 82, Issue 2
  • DOI: 10.1063/1.1534619

Elastic and orbital effects on thickness-dependent properties of manganite thin films
journal, December 2007

Diffusion and segregation effects in doped manganite/titanate heterostructures
journal, May 2004

  • Simon, J.; Walther, T.; Mader, W.
  • Applied Physics Letters, Vol. 84, Issue 19
  • DOI: 10.1063/1.1738930

Dynamic layer rearrangement during growth of layered oxide films by molecular beam epitaxy
journal, August 2014

  • Lee, J. H.; Luo, G.; Tung, I. C.
  • Nature Materials, Vol. 13, Issue 9
  • DOI: 10.1038/nmat4039

Effect of silver doping on the surface of La 5/8 Ca 3/8 MnO 3 epitaxial films
journal, September 2014

  • Tselev, A.; Vasudevan, R. K.; Kalinin, S. V.
  • Applied Physics Letters, Vol. 105, Issue 10
  • DOI: 10.1063/1.4895026
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    journal, January 2017

    • Li, Yifeng; Zhang, Wenqiang; Zheng, Yun
    • Chemical Society Reviews, Vol. 46, Issue 20
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    Growth of In 2 O 3 (111) thin films with optimized surfaces
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