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Title: Effect of oxygen stoichiometry on the magnetization profiles and negative magnetization in LSMO thin films

Abstract

The depth-dependent magnetization in thin film oxygen stoichiometric and oxygen-deficient La0.7Sr0.3MnO3 is investigated by using polarized neutron reflectivity and DC bulk magnetometry. The polarized neutron reflectivity results reveal that the stoichiometric sample shows enhanced interfacial magnetization relative to the rest of the film. The oxygen-deficient sample exhibits a reduced average magnetization from the optimized recipe. Both films show regions of suppressed magnetization at the surface regardless of the growth pressure. The oxygen stoichiometric film does not show an interfacial dead layer, whereas the oxygen-deficient film exhibits a dead layer whose thickness changes with temperature. At a low applied field, we observe striking differences in the depth dependence of the magnetic ordering, with the oxygen-deficient film exhibiting exchange spring behavior, while the stoichiometric film shows a constant magnetization direction across the film. Furthermore, these results suggest that the incorporation of oxygen vacancies during growth leads to an accumulation of vacancies at the interface, which is enhanced at higher temperature due to increased oxygen mobility, creating a region of reduced magnetism that couples to the rest of the film. These results offer insight into the complex behavior and role of oxygen vacancies in the magnetism of these systems. Additionally, the study revealsmore » further details of the negative magnetization in La0.7Sr0.3MnO3 reported in previous studies, which are discussed here.« less

Authors:
 [1]; ORCiD logo [2];  [1];  [3]; ORCiD logo [1]; ORCiD logo [1]; ORCiD logo [1];  [4];  [3]; ORCiD logo [2];  [1]
  1. West Virginia Univ., Morgantown, WV (United States)
  2. National Inst. of Standards and Technology, Gaithersburg, MD (United States)
  3. North Carolina State Univ., Raleigh, NC (United States)
  4. Pennsylvania State Univ., University Park, PA (United States)
Publication Date:
Research Org.:
West Virginia Univ., Morgantown, WV (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1594013
Grant/Contract Number:  
SC0016176; DMR-1608656
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Applied Physics
Additional Journal Information:
Journal Volume: 126; Journal Issue: 10; Journal ID: ISSN 0021-8979
Publisher:
American Institute of Physics (AIP)
Country of Publication:
United States
Language:
English
Subject:
75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITY; interface; segregation

Citation Formats

Trappen, Robbyn, Grutter, Alexander J., Huang, Chih-Yeh, Penn, Aubrey, Mottaghi, Navid, Yousefi, Saeed, Haertter, Allison, Kumari, Shalini, LeBeau, James, Kirby, Brian J., and Holcomb, Mikel B. Effect of oxygen stoichiometry on the magnetization profiles and negative magnetization in LSMO thin films. United States: N. p., 2019. Web. doi:10.1063/1.5111858.
Trappen, Robbyn, Grutter, Alexander J., Huang, Chih-Yeh, Penn, Aubrey, Mottaghi, Navid, Yousefi, Saeed, Haertter, Allison, Kumari, Shalini, LeBeau, James, Kirby, Brian J., & Holcomb, Mikel B. Effect of oxygen stoichiometry on the magnetization profiles and negative magnetization in LSMO thin films. United States. https://doi.org/10.1063/1.5111858
Trappen, Robbyn, Grutter, Alexander J., Huang, Chih-Yeh, Penn, Aubrey, Mottaghi, Navid, Yousefi, Saeed, Haertter, Allison, Kumari, Shalini, LeBeau, James, Kirby, Brian J., and Holcomb, Mikel B. Mon . "Effect of oxygen stoichiometry on the magnetization profiles and negative magnetization in LSMO thin films". United States. https://doi.org/10.1063/1.5111858. https://www.osti.gov/servlets/purl/1594013.
@article{osti_1594013,
title = {Effect of oxygen stoichiometry on the magnetization profiles and negative magnetization in LSMO thin films},
author = {Trappen, Robbyn and Grutter, Alexander J. and Huang, Chih-Yeh and Penn, Aubrey and Mottaghi, Navid and Yousefi, Saeed and Haertter, Allison and Kumari, Shalini and LeBeau, James and Kirby, Brian J. and Holcomb, Mikel B.},
abstractNote = {The depth-dependent magnetization in thin film oxygen stoichiometric and oxygen-deficient La0.7Sr0.3MnO3 is investigated by using polarized neutron reflectivity and DC bulk magnetometry. The polarized neutron reflectivity results reveal that the stoichiometric sample shows enhanced interfacial magnetization relative to the rest of the film. The oxygen-deficient sample exhibits a reduced average magnetization from the optimized recipe. Both films show regions of suppressed magnetization at the surface regardless of the growth pressure. The oxygen stoichiometric film does not show an interfacial dead layer, whereas the oxygen-deficient film exhibits a dead layer whose thickness changes with temperature. At a low applied field, we observe striking differences in the depth dependence of the magnetic ordering, with the oxygen-deficient film exhibiting exchange spring behavior, while the stoichiometric film shows a constant magnetization direction across the film. Furthermore, these results suggest that the incorporation of oxygen vacancies during growth leads to an accumulation of vacancies at the interface, which is enhanced at higher temperature due to increased oxygen mobility, creating a region of reduced magnetism that couples to the rest of the film. These results offer insight into the complex behavior and role of oxygen vacancies in the magnetism of these systems. Additionally, the study reveals further details of the negative magnetization in La0.7Sr0.3MnO3 reported in previous studies, which are discussed here.},
doi = {10.1063/1.5111858},
journal = {Journal of Applied Physics},
number = 10,
volume = 126,
place = {United States},
year = {Mon Sep 09 00:00:00 EDT 2019},
month = {Mon Sep 09 00:00:00 EDT 2019}
}

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Works referenced in this record:

Orientation Control of Interfacial Magnetism at La 0.67 Sr 0.33 MnO 3 /SrTiO 3 Interfaces
journal, May 2017

  • Guo, Er-Jia; Charlton, Timothy; Ambaye, Haile
  • ACS Applied Materials & Interfaces, Vol. 9, Issue 22
  • DOI: 10.1021/acsami.7b03252

Unconventional switching behavior in La 0.7 Sr 0.3 MnO 3 /La 0.7 Sr 0.3 CoO 3 exchange-spring bilayers
journal, November 2014

  • Li, Binzhi; Chopdekar, Rajesh V.; Arenholz, Elke
  • Applied Physics Letters, Vol. 105, Issue 20
  • DOI: 10.1063/1.4902115

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

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

Polarized neutron reflection as a probe of magnetic films and multilayers
journal, August 1992


Magnetoelasticity of Co25Fe75 thin films
journal, September 2019

  • Schwienbacher, Daniel; Pernpeintner, Matthias; Liensberger, Lukas
  • Journal of Applied Physics, Vol. 126, Issue 10
  • DOI: 10.1063/1.5116314

Spatial Evolution of the Ferromagnetic Phase Transition in an Exchange Graded Film
journal, January 2016


Accelerating Markov Chain Monte Carlo Simulation by Differential Evolution with Self-Adaptive Randomized Subspace Sampling
journal, January 2009

  • Vrugt, J. A.; ter Braak, C. J. F.; Diks, C. G. H.
  • International Journal of Nonlinear Sciences and Numerical Simulation, Vol. 10, Issue 3
  • DOI: 10.1515/IJNSNS.2009.10.3.273

Structural phases driven by oxygen vacancies at the La 0.7 Sr 0.3 MnO 3 /SrTiO 3 hetero-interface
journal, January 2015

  • Nord, M.; Vullum, P. E.; Moreau, M.
  • Applied Physics Letters, Vol. 106, Issue 4
  • DOI: 10.1063/1.4906920

Reversible control of magnetism in La 0.67 Sr 0.33 MnO 3 through chemically-induced oxygen migration
journal, February 2016

  • Grutter, A. J.; Gilbert, D. A.; Alaan, U. S.
  • Applied Physics Letters, Vol. 108, Issue 8
  • DOI: 10.1063/1.4942645

Symmetry-Driven Atomic Rearrangement at a Brownmillerite-Perovskite Interface
journal, December 2015

  • Meyer, Tricia L.; Jeen, Hyoungjeen; Gao, Xiang
  • Advanced Electronic Materials, Vol. 2, Issue 1
  • DOI: 10.1002/aelm.201500201

Nanoscale magnetic localization in exchange strength modulated ferromagnets
journal, August 2018


Preparation of atomically flat SrTiO 3 surfaces using a deionized-water leaching and thermal annealing procedure
journal, December 2012

  • Connell, J. G.; Isaac, B. J.; Ekanayake, G. B.
  • Applied Physics Letters, Vol. 101, Issue 25
  • DOI: 10.1063/1.4773052

CMR manganites: physics, thin films and devices
journal, April 2003


Reversed remanent magnetic configuration in epitaxial La 1− x Sr x MnO 3 films
journal, June 2011


Creation and Ordering of Oxygen Vacancies at WO 3−δ and Perovskite Interfaces
journal, April 2018

  • Zhang, Kelvin H. L.; Li, Guoqiang; Spurgeon, Steven R.
  • ACS Applied Materials & Interfaces, Vol. 10, Issue 20
  • DOI: 10.1021/acsami.8b03278

Melting of Oxygen Vacancy Order at Oxide–Heterostructure Interface
journal, August 2017

  • Hirai, Kei; Aso, Ryotaro; Ozaki, Yusuke
  • ACS Applied Materials & Interfaces, Vol. 9, Issue 35
  • DOI: 10.1021/acsami.7b08134

Structural and magnetic depth profiles of magneto-ionic heterostructures beyond the interface limit
journal, July 2016

  • Gilbert, Dustin A.; Grutter, Alexander J.; Arenholz, Elke
  • Nature Communications, Vol. 7, Issue 1
  • DOI: 10.1038/ncomms12264

Manipulation by exchange coupling in layered magnetic structures
journal, February 2014

  • Moskalenko, M. A.; Uzdin, V. M.; Zabel, H.
  • Journal of Applied Physics, Vol. 115, Issue 5
  • DOI: 10.1063/1.4864429

The equation of state of TaC0.99 by X-ray diffraction in radial scattering geometry to 32 GPa and 1073 K
journal, September 2019

  • Speziale, S.; Immoor, J.; Ermakov, A.
  • Journal of Applied Physics, Vol. 126, Issue 10
  • DOI: 10.1063/1.5115350

Suppression of the metal-insulator transition temperature in thin La0.7Sr0.3MnO3 films
journal, December 2004

  • Angeloni, M.; Balestrino, G.; Boggio, N. G.
  • Journal of Applied Physics, Vol. 96, Issue 11
  • DOI: 10.1063/1.1812599

Observation of the Strain Induced Magnetic Phase Segregation in Manganite Thin Films
journal, December 2014

  • Marín, Lorena; Rodríguez, Luis A.; Magén, César
  • Nano Letters, Vol. 15, Issue 1
  • DOI: 10.1021/nl503834b

Impact of Dzyaloshinskii-Moriya interactions on the thermal stability factor of heavy metal/magnetic metal/oxide based nano-pillars
journal, September 2019

  • Gastaldo, Daniele; Strelkov, Nikita; Buda-Prejbeanu, Liliana D.
  • Journal of Applied Physics, Vol. 126, Issue 10
  • DOI: 10.1063/1.5109484

Unconventional Transport through Graphene on SrTiO3: A Plausible Effect of SrTiO3 Phase-Transitions
journal, August 2014

  • Saha, Surajit; Kahya, Orhan; Jaiswal, Manu
  • Scientific Reports, Vol. 4, Issue 1
  • DOI: 10.1038/srep06173

Interface magnetism of La0.7Sr0.3MnO3 thin films studied by neutron reflectometry
journal, March 2000


The Origin of Oxygen Vacancies Controlling La 2/3 Sr 1/3 MnO 3 Electronic and Magnetic Properties
journal, January 2016

  • Guo, Haizhong; Wang, Jia-ou; He, Xu
  • Advanced Materials Interfaces, Vol. 3, Issue 5
  • DOI: 10.1002/admi.201500753

Growth of GaP 1   −   x   −   y As y N x on Si substrates by chemical beam epitaxy
journal, September 2019

  • Ben Saddik, K.; Braña, A. F.; López, N.
  • Journal of Applied Physics, Vol. 126, Issue 10
  • DOI: 10.1063/1.5111090

Electrostatic potential and valence modulation in La0.7Sr0.3MnO3 thin films
journal, September 2018


Effect of Interfacial Octahedral Behavior in Ultrathin Manganite Films
journal, April 2014

  • Moon, E. J.; Balachandran, P. V.; Kirby, B. J.
  • Nano Letters, Vol. 14, Issue 5
  • DOI: 10.1021/nl500235f

Surface Recombination in Ultra-Fast Carrier Dynamics of Perovskite Oxide La 0.7 Sr 0.3 MnO 3 Thin Films
journal, February 2019

  • Yousefi Sarraf, Saeed; Singh, Sobhit; Garcia-Castro, Andrés Camilo
  • ACS Nano, Vol. 13, Issue 3
  • DOI: 10.1021/acsnano.8b09595

Physical Justification for Negative Remanent Magnetization in Homogeneous Nanoparticles
journal, September 2014

  • Gu, Shuo; He, Weidong; Zhang, Ming
  • Scientific Reports, Vol. 4, Issue 1
  • DOI: 10.1038/srep06267

Observation and interpretation of negative remanent magnetization and inverted hysteresis loops in a thin film of La 0.7 Sr 0.3 MnO 3
journal, September 2018

  • Mottaghi, Navid; Trappen, Robbyn B.; Kumari, Shalini
  • Journal of Physics: Condensed Matter, Vol. 30, Issue 40
  • DOI: 10.1088/1361-648X/aade14

Physical interpretation of hysteresis loops: Micromagnetic modeling of fine particle magnetite: PHYSICAL INTERPRETATION OF HYSTERESIS LOOPS
journal, October 2002

  • Tauxe, Lisa; Bertram, H. Neal; Seberino, Christian
  • Geochemistry, Geophysics, Geosystems, Vol. 3, Issue 10
  • DOI: 10.1029/2001GC000241

The effect of the in-plane demagnetizing field on films with weak perpendicular magnetic anisotropy
journal, September 2006

  • de Abril, Oscar; Sánchez, María del Carmen; Aroca, Claudio
  • Journal of Applied Physics, Vol. 100, Issue 6
  • DOI: 10.1063/1.2349359

Strain-induced phase separation in La 0.7 Sr 0.3 Mn O 3 thin films
journal, December 2006


Thermochemical characterization of Zr/Fe 2 O 3 pyrotechnic mixture under natural aging conditions
journal, September 2019

  • Han, Byung Heon; Kim, Yoocheon; Jang, Seung-gyo
  • Journal of Applied Physics, Vol. 126, Issue 10
  • DOI: 10.1063/1.5096803

Size effects in the formation of an uncompensated ferromagnetic moment in NiO nanoparticles
journal, September 2019

  • Popkov, S. I.; Krasikov, A. A.; Dubrovskiy, A. A.
  • Journal of Applied Physics, Vol. 126, Issue 10
  • DOI: 10.1063/1.5109054

Oxygen content of La1−xSrxMnO3−y thin films and its relation to electric-magnetic properties
journal, April 2006

  • Sakai, Joe; Ito, Nobuaki; Imai, Syozo
  • Journal of Applied Physics, Vol. 99, Issue 8
  • DOI: 10.1063/1.2176323

Achieving excellent metallic magnet-based absorbents by regulating the eddy current effect
journal, September 2019

  • Shi, Yupeng; Zhang, Miaomiao; Zhang, Xuefeng
  • Journal of Applied Physics, Vol. 126, Issue 10
  • DOI: 10.1063/1.5109538

Step-induced uniaxial magnetic anisotropy of La0:67Sr0:33MnO3 thin films
journal, December 2005

  • Mathews, Mercy; Postma, Ferry M.; Lodder, J. Cock
  • Applied Physics Letters, Vol. 87, Issue 24
  • DOI: 10.1063/1.2143136

The exchange-spring magnet: a new material principle for permanent magnets
journal, July 1991

  • Kneller, E. F.; Hawig, R.
  • IEEE Transactions on Magnetics, Vol. 27, Issue 4, p. 3588-3560
  • DOI: 10.1109/20.102931

Developments in rock magnetism
journal, June 1990


Tuning the entanglement between orbital reconstruction and charge transfer at a film surface
journal, February 2014

  • Cui, B.; Song, C.; Li, F.
  • Scientific Reports, Vol. 4, Issue 1
  • DOI: 10.1038/srep04206

Correlation between surface rumpling and structural phase transformation in SrTiO 3
journal, March 2012


Magnetic dead layers in sputtered Co40Fe40B20 films
journal, April 2008

  • Oguz, K.; Jivrajka, P.; Venkatesan, M.
  • Journal of Applied Physics, Vol. 103, Issue 7
  • DOI: 10.1063/1.2838851

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

Optimized fabrication of high-quality La 0.67 Sr 0.33 MnO 3 thin films considering all essential characteristics
journal, April 2011


Mid-wavelength infrared photo response and band alignment for sensitized PbSe thin films
journal, September 2019

  • Jang, Moon-Hyung; Litwin, Peter M.; Yoo, Sung-Shik
  • Journal of Applied Physics, Vol. 126, Issue 10
  • DOI: 10.1063/1.5114923

Magnetic properties of epitaxial CoCr films with depth-dependent exchange-coupling profiles
journal, April 2017


Correlation between surface rumpling and structural phase transformation of SrTiO3
text, January 2011


Spatial evolution of the ferromagnetic phase transition in an exchange graded film
text, January 2015