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. APPLIED PHYSICS LETTERS, OCT 2, 2017. doi abstract bibtex 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. 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. Published by AIP Publishing.
@article{ ISI:000412645100009,
Author = {Ryu, S. and Zhou, H. and Paudel, T. R. and Irwin, J. and Podkaminer, J.
P. and Bark, C. W. and Lee, D. and Kim, T. H. and Fong, D. D. and
Rzchowski, M. S. and Tsymbal, E. Y. and Eom, C. B.},
Title = {{In-situ probing of coupled atomic restructuring and metallicity of oxide
heterointerfaces induced by polar adsorbates}},
Journal = {{APPLIED PHYSICS LETTERS}},
Year = {{2017}},
Volume = {{111}},
Number = {{14}},
Month = {{OCT 2}},
Abstract = {{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. 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. Published by AIP Publishing.}},
DOI = {{10.1063/1.4991956}},
Article-Number = {{141604}},
ISSN = {{0003-6951}},
EISSN = {{1077-3118}},
ResearcherID-Numbers = {{Tsymbal, Evgeny/G-3493-2013
}},
ORCID-Numbers = {{Tsymbal, Evgeny/0000-0002-6728-5480
Irwin, Julian/0000-0002-4845-7558}},
Unique-ID = {{ISI:000412645100009}},
}
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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. 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