In-situ probing of coupled atomic restructuring and metallicity of oxide heterointerfaces induced by polar adsorbates

Ryu, S.; Zhou, H.; Paudel, T. R.; Irwin, J.; Podkaminer, J. P.; Bark, C. W.; Lee, D.; Kim, T. H.; Fong, D. D.; Rzchowski, M. S.; Tsymbal, E. Y.; Eom, C. B.

doi:10.1063/1.4991956

Title: In-situ probing of coupled atomic restructuring and metallicity of oxide heterointerfaces induced by polar adsorbates

Journal Article · 02 October 2017 · Applied Physics Letters

DOI: https://doi.org/10.1063/1.4991956 · OSTI ID:1418361

^[1]; Zhou, H. ^[2]; Paudel, T. R. ^[3];

^[1];

^[1]; Bark, C. W. ^[1]; Lee, D. ^[1]; Kim, T. H. ^[1]; Fong, D. D. ^[2]; Rzchowski, M. S. ^[1]; Tsymbal, E. Y. ^[3]; Eom, C. B. ^[1]

Univ. of Wisconsin-Madison, Madison, WI (United States)
Argonne National Lab. (ANL), Argonne, IL (United States)
Univ. of Nebraska, Lincoln, NE (United States)

Microscopic understanding of the surface-controlled conductivity of the two dimensional electron gas at complex oxide interfaces is crucial for developing functional interfaces. We observe conductivity and structural modification using in-situ synchrotron surface x-ray diffraction as the surface of a model LaAlO₃/SrTiO₃ (001) heterostructure is changed by polar adsorbates. We find that polar adsorbate-induced interfacial metallicity reduces polar distortions in the LaAlO₃ layer. First-principles density functional theory calculations show that surface dipoles introduced by polar adsorbates lead to additional charge transfer and the reduction of polar displacements in the LaAlO₃ layer, consistent with the experimental observations. Our study supports that internal structural deformations controlling functionalities can be driven without the application of direct electrical or thermal bias and offers a route to tuning interfacial properties. Furthermore, these results also highlight the important role of in-situ x-ray scattering with atomic resolution in capturing and exploring structural distortions and charge density changes caused by external perturbations such as chemical adsorption, redox reaction, and generation and/or annihilation of surface defects.

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Research Organization:: Argonne National Laboratory (ANL), Argonne, IL (United States)

Sponsoring Organization:: National Science Foundation (NSF); Air Force Research Laboratory (AFRL), Air Force Office of Scientific Research (AFOSR); USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Materials Sciences & Engineering Division; USDOE

Grant/Contract Number:: AC02-06CH11357; FG02-06ER46327

OSTI ID:: 1418361

Alternate ID(s):: OSTI ID: 1396065

Journal Information:: Applied Physics Letters, Vol. 111, Issue 14; ISSN 0003-6951

Publisher:: American Institute of Physics (AIP)Copyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 2 works

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References (44)

Coexistence of magnetic order and two-dimensional superconductivity at LaAlO₃/SrTiO₃ interfaces Li, Lu; Richter, C.; Mannhart, J. Nature Physics, Vol. 7, Issue 10, p. 762-766 https://doi.org/10.1038/nphys2080	journal	September 2011
Reversible Chemical Switching of a Ferroelectric Film Wang, R. V.; Fong, D. D.; Jiang, F. Physical Review Letters, Vol. 102, Issue 4 https://doi.org/10.1103/PhysRevLett.102.047601	journal	January 2009
Stoichiometry control of the electronic properties of the LaAlO3/SrTiO3 heterointerface Sato, H. K.; Bell, C.; Hikita, Y. Applied Physics Letters, Vol. 102, Issue 25 https://doi.org/10.1063/1.4812353	journal	June 2013
Titanium dx y ferromagnetism at the LaAlO3/SrTiO3 interface Lee, J. -S.; Xie, Y. W.; Sato, H. K. Nature Materials, Vol. 12, Issue 8 https://doi.org/10.1038/nmat3674	journal	June 2013
Rewritable nanoscale oxide photodetector Irvin, Patrick; Ma, Yanjun; Bogorin, Daniela F. Nature Photonics, Vol. 4, Issue 12 https://doi.org/10.1038/nphoton.2010.238	journal	November 2010
Electronically coupled complementary interfaces between perovskite band insulators Huijben, Mark; Rijnders, Guus; Blank, Dave H. A. Nature Materials, Vol. 5, Issue 7 https://doi.org/10.1038/nmat1675	journal	June 2006
Evidence for charge–vortex duality at the LaAlO3/SrTiO3 interface Mehta, M. M.; Dikin, D. A.; Bark, C. W. Nature Communications, Vol. 3, Issue 1 https://doi.org/10.1038/ncomms1959	journal	January 2012
Insights from the study of high-temperature interface superconductivity Pereiro, J.; Bollinger, A. T.; Logvenov, G. Philosophical Transactions of the Royal Society A: Mathematical, Physical and Engineering Sciences, Vol. 370, Issue 1977 https://doi.org/10.1098/rsta.2012.0219	journal	October 2012
Electrostriction at the LaAlO 3 / SrTiO 3 Interface Cancellieri, C.; Fontaine, D.; Gariglio, S. Physical Review Letters, Vol. 107, Issue 5 https://doi.org/10.1103/PhysRevLett.107.056102	journal	July 2011
Structural Basis for the Conducting Interface between LaAlO3 and SrTiO3 Willmott, P. R.; Pauli, S. A.; Herger, R. Physical Review Letters, Vol. 99, Issue 15, Article No. 155502 https://doi.org/10.1103/PhysRevLett.99.155502	journal	October 2007
Metallic and Insulating Oxide Interfaces Controlled by Electronic Correlations Jang, H. W.; Felker, D. A.; Bark, C. W. Science, Vol. 331, Issue 6019 https://doi.org/10.1126/science.1198781	journal	February 2011
Gate-Controlled Spin Injection at LaAlO 3 / SrTiO 3 Interfaces Reyren, N.; Bibes, M.; Lesne, E. Physical Review Letters, Vol. 108, Issue 18 https://doi.org/10.1103/PhysRevLett.108.186802	journal	April 2012
Critical thickness for ferromagnetism in LaAlO3/SrTiO3 heterostructures Kalisky, Beena; Bert, Julie A.; Klopfer, Brannon B. Nature Communications, Vol. 3, Issue 1 https://doi.org/10.1038/ncomms1931	journal	January 2012
Effects of surface defects on two-dimensional electron gas at NdAlO3/SrTiO3 interface Xiang, X.; Qiao, L.; Xiao, H. Y. Scientific Reports, Vol. 4, Issue 1 https://doi.org/10.1038/srep05477	journal	June 2014
Coexistence of Superconductivity and Ferromagnetism in Two Dimensions Dikin, D. A.; Mehta, M.; Bark, C. W. Physical Review Letters, Vol. 107, Issue 5, Article No. 056802 https://doi.org/10.1103/PhysRevLett.107.056802	journal	July 2011
Surface Chemistry of Acetone on Metal Oxides: IR Observation of Acetone Adsorption and Consequent Surface Reactions on Silica−Alumina versus Silica and Alumina Zaki, M. I.; Hasan, M. A.; Al-Sagheer, F. A. Langmuir, Vol. 16, Issue 2 https://doi.org/10.1021/la990739q	journal	January 2000
Modulation of electron carrier density at the n-type LaAlO ₃ /SrTiO ₃ interface by water adsorption Li, Yun; Yu, Jaejun Journal of Physics: Condensed Matter, Vol. 25, Issue 26 https://doi.org/10.1088/0953-8984/25/26/265004	journal	June 2013
Evolution of the Interfacial Structure of LaAlO 3 on SrTiO 3 Pauli, S. A.; Leake, S. J.; Delley, B. Physical Review Letters, Vol. 106, Issue 3 https://doi.org/10.1103/PhysRevLett.106.036101	journal	January 2011
“Water-cycle” mechanism for writing and erasing nanostructures at the LaAlO3/SrTiO3 interface Bi, Feng; Bogorin, Daniela F.; Cen, Cheng Applied Physics Letters, Vol. 97, Issue 17 https://doi.org/10.1063/1.3506509	journal	October 2010
Structural Comparison of n -Type and p -Type LaAlO 3 / SrTiO 3 Interfaces Yamamoto, Ryosuke; Bell, Christopher; Hikita, Yasuyuki Physical Review Letters, Vol. 107, Issue 3 https://doi.org/10.1103/PhysRevLett.107.036104	journal	July 2011
Exchange bias in LaNiO3–LaMnO3 superlattices Gibert, Marta; Zubko, Pavlo; Scherwitzl, Raoul Nature Materials, Vol. 11, Issue 3 https://doi.org/10.1038/nmat3224	journal	January 2012
Nanoscale control of an interfacial metal–insulator transition at room temperature Cen, C.; Thiel, S.; Hammerl, G. Nature Materials, Vol. 7, Issue 4 https://doi.org/10.1038/nmat2136	journal	March 2008
A high-mobility electron gas at the LaAlO3/SrTiO3 heterointerface Ohtomo, A.; Hwang, H. Y. Nature, Vol. 427, Issue 6973 https://doi.org/10.1038/nature02308	journal	January 2004
Origin of insulating behavior of the p -type LaAlO 3 / SrTiO 3 interface: Polarization-induced asymmetric distribution of oxygen vacancies Zhang, Lixin; Zhou, Xiang-Feng; Wang, Hui-Tian Physical Review B, Vol. 82, Issue 12 https://doi.org/10.1103/PhysRevB.82.125412	journal	September 2010
Oxygen vacancies at titanate interfaces: Two-dimensional magnetism and orbital reconstruction Pavlenko, N.; Kopp, T.; Tsymbal, E. Y. Physical Review B, Vol. 86, Issue 6 https://doi.org/10.1103/PhysRevB.86.064431	journal	August 2012
Anomalous expansion of the copper-apical-oxygen distance in superconducting cuprate bilayers Zhou, H.; Yacoby, Y.; Butko, V. Y. Proceedings of the National Academy of Sciences, Vol. 107, Issue 18 https://doi.org/10.1073/pnas.0914702107	journal	April 2010
Control of electronic conduction at an oxide heterointerface using surface polar adsorbates Xie, Yanwu; Hikita, Yasuyuki; Bell, Christopher Nature Communications, Vol. 2, Issue 1 https://doi.org/10.1038/ncomms1501	journal	September 2011
Interface engineering of quantum Hall effects in digital transition metal oxide heterostructures Xiao, Di; Zhu, Wenguang; Ran, Ying Nature Communications, Vol. 2, Issue 1 https://doi.org/10.1038/ncomms1602	journal	September 2011
Acetone Chemistry on Oxidized and Reduced TiO ₂ (110) Henderson, Michael A. The Journal of Physical Chemistry B, Vol. 108, Issue 49 https://doi.org/10.1021/jp046357x	journal	December 2004
Surface defects and conduction in polar oxide heterostructures Bristowe, N. C.; Littlewood, P. B.; Artacho, Emilio Physical Review B, Vol. 83, Issue 20 https://doi.org/10.1103/PhysRevB.83.205405	journal	May 2011
Room-temperature electronically-controlled ferromagnetism at the LaAlO3/SrTiO3 interface Bi, Feng; Huang, Mengchen; Ryu, Sangwoo Nature Communications, Vol. 5, Issue 1 https://doi.org/10.1038/ncomms6019	journal	September 2014
A polarity-induced defect mechanism for conductivity and magnetism at polar–nonpolar oxide interfaces Yu, Liping; Zunger, Alex Nature Communications, Vol. 5, Issue 1 https://doi.org/10.1038/ncomms6118	journal	October 2014
Formation of oxygen vacancies and charge carriers induced in the n -type interface of a LaAlO 3 overlayer on SrTiO 3 (001) Li, Yun; Phattalung, Sutassana Na; Limpijumnong, Sukit Physical Review B, Vol. 84, Issue 24 https://doi.org/10.1103/PhysRevB.84.245307	journal	December 2011
Electronic reconstruction at an interface between a Mott insulator and a band insulator Okamoto, Satoshi; Millis, Andrew J. Nature, Vol. 428, Issue 6983 https://doi.org/10.1038/nature02450	journal	April 2004
Enhancement of superconductivity by a parallel magnetic field in two-dimensional superconductors Jeffrey Gardner, H.; Kumar, Ashwani; Yu, Liuqi Nature Physics, Vol. 7, Issue 11 https://doi.org/10.1038/nphys2075	journal	August 2011
Surface defects and conduction in polar oxide heterostructures Bristowe, N. C.; Littlewood, P. B.; Artacho, Emilio arXiv https://doi.org/10.48550/arxiv.1008.1951	text	January 2010
"Water-cycle" mechanism for writing and erasing nanostructures at the LaAlO3/SrTiO3 interface Bi, Feng; Bogorin, Daniela F.; Cen, Cheng arXiv https://doi.org/10.48550/arxiv.1009.3303	text	January 2010
Coexistence of superconductivity and ferromagnetism in two dimensions Dikin, D. A.; Mehta, M.; Bark, C. W. arXiv https://doi.org/10.48550/arxiv.1103.4006	text	January 2011
Interface engineering of quantum Hall effects in digital transition metal oxide heterostructures Xiao, Di; Zhu, Wenguang; Ran, Ying arXiv https://doi.org/10.48550/arxiv.1106.4296	text	January 2011
Oxygen vacancies at titanate interfaces: two-dimensional magnetism and orbital reconstruction Pavlenko, N.; Kopp, T.; Tsymbal, E. Y. arXiv https://doi.org/10.48550/arxiv.1204.4711	text	January 2012
Modulation of electron carrier density at the n-type LaAlO3/SrTiO3 interface by water adsorption Li, Yun; Yu, Jaejun arXiv https://doi.org/10.48550/arxiv.1303.4156	text	January 2013
Room-Temperature Electronically-Controlled Ferromagnetism at the LaAlO3/SrTiO3 Interface Bi, Feng; Huang, Mengchen; Bark, Chung-Wung arXiv https://doi.org/10.48550/arxiv.1307.5557	text	January 2013
A polarity-induced defect mechanism for conductivity and magnetism at polar-nonpolar oxide interfaces Yu, Liping; Zunger, Alex arXiv https://doi.org/10.48550/arxiv.1402.0895	text	January 2014
Electronically coupled complementary interfaces between perovskite band insulators Huijben, M.; Rijnders, G.; Blank, D. H. A. arXiv https://doi.org/10.48550/arxiv.cond-mat/0603088	text	January 2006

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Title: In-situ probing of coupled atomic restructuring and metallicity of oxide heterointerfaces induced by polar adsorbates

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