Electrostatic potential and valence modulation in La0.7Sr0.3MnO3 thin films

Trappen, Robbyn; Garcia-Castro, A. C.; Tra, Vu Thanh; Huang, Chih-Yeh; Ibarra-Hernandez, Wilfredo; Fitch, James; Singh, Sobhit; Zhou, Jinling; Cabrera, Guerau; Chu, Ying-Hao; LeBeau, James M.; Romero, Aldo H.; Holcomb, Mikel B.

doi:10.1038/s41598-018-32701-x

Title: Electrostatic potential and valence modulation in La_0.7Sr_0.3MnO₃ thin films

Abstract

The Mn valence in thin film La_0.7Sr_0.3MnO₃ was studied as a function of film thickness in the range of 1–16 unit cells with a combination of non-destructive bulk and surface sensitive X-ray absorption spectroscopy techniques. Using a layer-by-layer valence model, it was found that while the bulk averaged valence hovers around its expected value of 3.3, a significant deviation occurs within several unit cells of the surface and interface. These results were supported by first principles calculations. The surface valence increases to up to Mn^3.7+, whereas the interface valence reduces down to Mn^2.5+. The change in valence from the expected bulk value is consistent with charge redistribution due to the polar discontinuity at the film-substrate interface. The comparison with theory employed here illustrates how this layer-by-layer valence evolves with film thickness and allows for a deeper understanding of the microscopic mechanisms at play in this effect. These results offer insight on how the two-dimensional electron gas is created in thin film oxide alloys and how the magnetic ordering is reduced with dimensionality.

Authors:

^[1]; Garcia-Castro, A. C. ^[2]; Tra, Vu Thanh ^[3]; Huang, Chih-Yeh ^[4]; Ibarra-Hernandez, Wilfredo ^[5]; Fitch, James ^[6];

^[1]; Zhou, Jinling ^[1]; Cabrera, Guerau ^[1]; Chu, Ying-Hao ^[3]; LeBeau, James M. ^[6];

^[5];

^[1]

West Virginia Univ., Morgantown, WV (United States). Dept. of Physics and Astronomy
West Virginia Univ., Morgantown, WV (United States). Dept. of Physics and Astronomy; Univ. of Liège (Belgium). Theoretical Physics of Materials; Industrial Univ. of Santander, Bucaramanga (Colombia). Dept. of Physics
National Chiao Tung Univ., Hsinchu (Taiwan). Inst. of Physics
West Virginia Univ., Morgantown, WV (United States). Dept. of Mechanical & Aerospace Engineering
West Virginia Univ., Morgantown, WV (United States). Dept. of Physics and Astronomy; Meritorious Autonomous Univ. of Puebla (BUAP) (Mexico). Faculty of Engineering
North Carolina State Univ., Raleigh, NC (United States). Dept. of Materials Science and Engineering

Publication Date:: Tue Sep 25 00:00:00 EDT 2018

Research Org.:: West Virginia Univ., Morgantown, WV (United States)

Sponsoring Org.:: USDOE Office of Science (SC), Basic Energy Sciences (BES); National Science Foundation (NSF)

OSTI Identifier:: 1499989

Grant/Contract Number:: SC0016176; AC02-05CH11231; DMR-1608656; ACI-1053575; DMREF-NSF 1434897

Resource Type:: Accepted Manuscript

Journal Name:: Scientific Reports

Additional Journal Information:: Journal Volume: 8; Journal ID: ISSN 2045-2322

Publisher:: Nature Publishing Group

Country of Publication:: United States

Language:: English

Subject:: 36 MATERIALS SCIENCE; electronic properties and materials; surfaces; interfaces and thin films

Citation Formats


                    Trappen, Robbyn, Garcia-Castro, A. C., Tra, Vu Thanh, Huang, Chih-Yeh, Ibarra-Hernandez, Wilfredo, Fitch, James, Singh, Sobhit, Zhou, Jinling, Cabrera, Guerau, Chu, Ying-Hao, LeBeau, James M., Romero, Aldo H., and Holcomb, Mikel B. Electrostatic potential and valence modulation in La0.7Sr0.3MnO3 thin films.  United States: N. p., 2018. 
Web.  doi:10.1038/s41598-018-32701-x.

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                    Trappen, Robbyn, Garcia-Castro, A. C., Tra, Vu Thanh, Huang, Chih-Yeh, Ibarra-Hernandez, Wilfredo, Fitch, James, Singh, Sobhit, Zhou, Jinling, Cabrera, Guerau, Chu, Ying-Hao, LeBeau, James M., Romero, Aldo H., & Holcomb, Mikel B. Electrostatic potential and valence modulation in La0.7Sr0.3MnO3 thin films.  United States.  https://doi.org/10.1038/s41598-018-32701-x

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                    Trappen, Robbyn, Garcia-Castro, A. C., Tra, Vu Thanh, Huang, Chih-Yeh, Ibarra-Hernandez, Wilfredo, Fitch, James, Singh, Sobhit, Zhou, Jinling, Cabrera, Guerau, Chu, Ying-Hao, LeBeau, James M., Romero, Aldo H., and Holcomb, Mikel B. Tue .  
"Electrostatic potential and valence modulation in La0.7Sr0.3MnO3 thin films".  United States.  https://doi.org/10.1038/s41598-018-32701-x.  https://www.osti.gov/servlets/purl/1499989.

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@article{osti_1499989,

  title        = {Electrostatic potential and valence modulation in La0.7Sr0.3MnO3 thin films},

  author       = {Trappen, Robbyn and Garcia-Castro, A. C. and Tra, Vu Thanh and Huang, Chih-Yeh and Ibarra-Hernandez, Wilfredo and Fitch, James and Singh, Sobhit and Zhou, Jinling and Cabrera, Guerau and Chu, Ying-Hao and LeBeau, James M. and Romero, Aldo H. and Holcomb, Mikel B.},

  abstractNote = {The Mn valence in thin film La0.7Sr0.3MnO3 was studied as a function of film thickness in the range of 1–16 unit cells with a combination of non-destructive bulk and surface sensitive X-ray absorption spectroscopy techniques. Using a layer-by-layer valence model, it was found that while the bulk averaged valence hovers around its expected value of 3.3, a significant deviation occurs within several unit cells of the surface and interface. These results were supported by first principles calculations. The surface valence increases to up to Mn3.7+, whereas the interface valence reduces down to Mn2.5+. The change in valence from the expected bulk value is consistent with charge redistribution due to the polar discontinuity at the film-substrate interface. The comparison with theory employed here illustrates how this layer-by-layer valence evolves with film thickness and allows for a deeper understanding of the microscopic mechanisms at play in this effect. These results offer insight on how the two-dimensional electron gas is created in thin film oxide alloys and how the magnetic ordering is reduced with dimensionality.},

  doi          = {10.1038/s41598-018-32701-x},

  journal      = {Scientific Reports},

  number       = ,

  volume       = 8,

  place        = {United States},

  year         = {Tue Sep 25 00:00:00 EDT 2018},

  month        = {Tue Sep 25 00:00:00 EDT 2018}

}

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https://doi.org/10.1038/s41598-018-32701-x

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Cited by: 7 works

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Figures / Tables:

Figure 1: (a) TEM image of the film-substrate interface. (b) Results of the linear combination fits for the Mn K and L-edges. (c) Valence obtained from the linear combination fits (solid points) and experimental fit using the layer dependent valence model (solid lines). The dashed line indicates the expected bulkmore »

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Works referencing / citing this record:

Effect of oxygen stoichiometry on the magnetization profiles and negative magnetization in LSMO thin films
journal, September 2019

Trappen, Robbyn; Grutter, Alexander J.; Huang, Chih-Yeh
Journal of Applied Physics, Vol. 126, Issue 10
DOI: 10.1063/1.5111858

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Title: Electrostatic potential and valence modulation in La0.7Sr0.3MnO3 thin films

Abstract

Citation Formats

Figures / Tables:

Origin of the metal-insulator transition in ultrathin films of L a 2 / 3 S r 2 / 3 Mn O 3 journal, September 2015

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

Structural, magnetic, and electrical properties of single-crystalline La 1 − x Sr x MnO 3 ( 0.4 < x < 0.85 ) journal, September 2002

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

Mn Valency at La 0.7 Sr 0.3 MnO 3 /SrTiO 3 (0 0 1) Thin Film Interfaces journal, May 2009

Valence state fossils in Proterozoic stromatolites by L-edge X-ray absorption spectroscopy: VALENCE STATE FOSSILS IN STROMATOLITE journal, July 2007

Charge Transfer to LaAlO 3 /SrTiO 3 Interfaces Controlled by Surface Water Adsorption and Proton Hopping journal, May 2016

The origin of two-dimensional electron gases at oxide interfaces: insights from theory journal, March 2014

Impedance of Solid Oxide Fuel Cell LSM/YSZ Composite Cathodes journal, January 2001

Evidence for Mn 2 + ions at surfaces of La 0.7 Sr 0.3 Mn O 3 thin films journal, January 2005

Soft X-ray magnetic circular dichroism study of the colossal magnetoresistance compound La1−xSrxMnO3 journal, August 1997

Thickness-dependent ferromagnetic metal to paramagnetic insulator transition in La 0.6 Sr 0.4 MnO 3 thin films studied by x-ray magnetic circular dichroism journal, June 2014

Quantitative charge state analysis of manganese biominerals in aqueous suspension using scanning transmission X-ray microscopy (STXM) journal, March 2003

Magnetic and electric “dead” layers in (La 0.7 Sr 0.3 )MnO 3 thin films journal, April 2001

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

Visualizing the interfacial evolution from charge compensation to metallic screening across the manganite metal–insulator transition journal, March 2014

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

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

Correlation between Mn and Ru valence states and magnetic phases in SrMn 1 − x Ru x O 3 journal, February 2015

Magnetic dead layers in Fe films induced by a lattice mismatch at an interface journal, September 2004

Multiple Scattering Calculations of Bonding and X-ray Absorption Spectroscopy of Manganese Oxides journal, April 2003

Effect of oxygen stoichiometry on the electrical properties of La0.5Sr0.5CoO3 electrodes journal, April 1997

Preventing the Reconstruction of the Polar Discontinuity at Oxide Heterointerfaces journal, March 2012

The dependence of oxygen vacancy distributions in BiFeO3 films on oxygen pressure and substrate journal, July 2009

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

Electronic correlation and strain effects at the interfaces between polar and nonpolar complex oxides journal, August 2012

Interfacial effects in manganite thin films with different capping layers of interest for spintronic applications journal, July 2011

Thickness dependence of La 0.7 Sr 0.3 MnO 3 /PbZr 0.2 Ti 0.8 O 3 magnetoelectric interfaces journal, October 2015

Magnetic dead layers in sputtered Co40Fe40B20 films journal, April 2008

Why some interfaces cannot be sharp journal, January 2006

Influence of the Synthetic Pathway on the Properties of Oxygen-Deficient Manganese-Related Perovskites journal, July 2007

Tailoring LaAlO 3 /SrTiO 3 Interface Metallicity by Oxygen Surface Adsorbates journal, March 2016

Electrostatic carrier doping of GdTiO 3 /SrTiO 3 interfaces journal, December 2011

Determination of Mn valence states in mixed-valent manganates by XANES spectroscopy journal, May 2012

The origin of two-dimensional electron gases at oxide interfaces: insights from theory. text, January 2014

Soft X-Ray Magnetic Circular Dichroism Study of the Colossal Magnetoresistance Compound La 1-x Sr x MnO 3 journal, April 1997

Electrostatic carrier doping of GdTiO3/SrTiO3 interfaces text, January 2011

Preventing the reconstruction of the polar discontinuity at oxide heterointerfaces text, January 2012

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Why Some Interfaces Cannot be Sharp text, January 2005

Effect of oxygen stoichiometry on the magnetization profiles and negative magnetization in LSMO thin films journal, September 2019

Title: Electrostatic potential and valence modulation in La_0.7Sr_0.3MnO₃ thin films

Origin of the metal-insulator transition in ultrathin films of $L a_{2 / 3} S r_{2 / 3} Mn O_{3}$
journal, September 2015

Orientation Control of Interfacial Magnetism at La _0.67 Sr _0.33 MnO ₃ /SrTiO ₃ Interfaces
journal, May 2017

Structural, magnetic, and electrical properties of single-crystalline ${La}_{1 - x} {Sr}_{x} {MnO}_{3}$ $(0.4 < x < 0.85)$
journal, September 2002

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

Mn Valency at La _0.7 Sr _0.3 MnO ₃ /SrTiO ₃ (0 0 1) Thin Film Interfaces
journal, May 2009

Valence state fossils in Proterozoic stromatolites by L-edge X-ray absorption spectroscopy: VALENCE STATE FOSSILS IN STROMATOLITE
journal, July 2007

Charge Transfer to LaAlO ₃ /SrTiO ₃ Interfaces Controlled by Surface Water Adsorption and Proton Hopping
journal, May 2016

The origin of two-dimensional electron gases at oxide interfaces: insights from theory
journal, March 2014

Impedance of Solid Oxide Fuel Cell LSM/YSZ Composite Cathodes
journal, January 2001

Evidence for ${Mn}^{2 +}$ ions at surfaces of ${La}_{0.7} {Sr}_{0.3} Mn O_{3}$ thin films
journal, January 2005

Soft X-ray magnetic circular dichroism study of the colossal magnetoresistance compound La1−xSrxMnO3
journal, August 1997

Thickness-dependent ferromagnetic metal to paramagnetic insulator transition in ${La}_{0.6}$ ${Sr}_{0.4}$ ${MnO}_{3}$ thin films studied by x-ray magnetic circular dichroism
journal, June 2014

Quantitative charge state analysis of manganese biominerals in aqueous suspension using scanning transmission X-ray microscopy (STXM)
journal, March 2003

Magnetic and electric “dead” layers in (La _0.7 Sr _0.3 )MnO ₃ thin films
journal, April 2001

Strain-induced phase separation in ${La}_{0.7} {Sr}_{0.3} Mn O_{3}$ thin films
journal, December 2006

Visualizing the interfacial evolution from charge compensation to metallic screening across the manganite metal–insulator transition
journal, March 2014

Structural phases driven by oxygen vacancies at the La _0.7 Sr _0.3 MnO ₃ /SrTiO ₃ hetero-interface
journal, January 2015

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

Correlation between Mn and Ru valence states and magnetic phases in ${SrMn}_{1 - x} {Ru}_{x} O_{3}$
journal, February 2015

Magnetic dead layers in Fe films induced by a lattice mismatch at an interface
journal, September 2004

Multiple Scattering Calculations of Bonding and X-ray Absorption Spectroscopy of Manganese Oxides
journal, April 2003

Effect of oxygen stoichiometry on the electrical properties of La0.5Sr0.5CoO3 electrodes
journal, April 1997

Preventing the Reconstruction of the Polar Discontinuity at Oxide Heterointerfaces
journal, March 2012

The dependence of oxygen vacancy distributions in BiFeO3 films on oxygen pressure and substrate
journal, July 2009

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

Electronic correlation and strain effects at the interfaces between polar and nonpolar complex oxides
journal, August 2012

Interfacial effects in manganite thin films with different capping layers of interest for spintronic applications
journal, July 2011

Thickness dependence of La _0.7 Sr _0.3 MnO ₃ /PbZr _0.2 Ti _0.8 O ₃ magnetoelectric interfaces
journal, October 2015

Magnetic dead layers in sputtered Co40Fe40B20 films
journal, April 2008

Why some interfaces cannot be sharp
journal, January 2006

Influence of the Synthetic Pathway on the Properties of Oxygen-Deficient Manganese-Related Perovskites
journal, July 2007

Tailoring LaAlO ₃ /SrTiO ₃ Interface Metallicity by Oxygen Surface Adsorbates
journal, March 2016

Electrostatic carrier doping of GdTiO ₃ /SrTiO ₃ interfaces
journal, December 2011

Determination of Mn valence states in mixed-valent manganates by XANES spectroscopy
journal, May 2012

The origin of two-dimensional electron gases at oxide interfaces: insights from theory.
text, January 2014

Soft X-Ray Magnetic Circular Dichroism Study of the Colossal Magnetoresistance Compound La _1-x Sr _x MnO ₃
journal, April 1997

Electrostatic carrier doping of GdTiO3/SrTiO3 interfaces
text, January 2011

Preventing the reconstruction of the polar discontinuity at oxide heterointerfaces
text, January 2012

Origin of two-dimensional electron gases at oxide interfaces: insights from theory
text, January 2013

Why Some Interfaces Cannot be Sharp
text, January 2005

Effect of oxygen stoichiometry on the magnetization profiles and negative magnetization in LSMO thin films
journal, September 2019