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Title: Identifying Ionic and Electronic Charge Transfer at Oxide Heterointerfaces

Abstract

The ability to tailor oxide heterointerfaces has led to novel properties in low-dimensional oxide systems. A fundamental understanding of these properties is based on the concept of electronic charge transfer. However, the electronic properties of oxide heterointerfaces crucially depend on their ionic constitution and defect structure: ionic charges contribute to charge transfer and screening at oxide interfaces, triggering a thermodynamic balance of ionic and electronic structures. Quantitative understanding of the electronic and ionic roles regarding charge-transfer phenomena poses a central challenge. Here, the electronic and ionic structure is simultaneously investigated at the prototypical charge-transfer heterointerface, LaAlO3/SrTiO3. Applying in situ photoemission spectroscopy under oxygen ambient, ionic and electronic charge transfer is deconvoluted in response to the oxygen atmosphere at elevated temperatures. In this way, both the rich and variable chemistry of complex oxides and the associated electronic properties are equally embraced. The interfacial electron gas is depleted through an ionic rearrangement in the strontium cation sublattice when oxygen is applied, resulting in an inverse and reversible balance between cation vacancies and electrons, while the mobility of ionic species is found to be considerably enhanced as compared to the bulk. Triggered by these ionic phenomena, the electronic transport and magnetic signature ofmore » the heterointerface are significantly altered.« less

Authors:
ORCiD logo [1];  [2];  [2];  [3];  [4];  [5];  [6];  [3];  [7];  [4];  [8];  [1]
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  1. Institute for Electronic Materials (IWE 2), and Juelich‐Aachen Research Alliance for Fundamentals on Future Information Technology (JARA‐FIT) RWTH Aachen University 52074 Aachen Germany, Peter Grünberg Institute 7 Forschungszentrum Jülich GmbH, and JARA‐FIT 52425 Jülich Germany
  2. Department of Surface and Plasma Science Faculty of Mathematics and Physics Charles University Prague 180 00 Czech Republic
  3. Peter Grünberg Institute 1 and Institute for Advanced Simulation Forschungszentrum Jülich GmbH and JARA‐FIT 52425 Jülich Germany
  4. Peter Grünberg Institute 7 Forschungszentrum Jülich GmbH, and JARA‐FIT 52425 Jülich Germany
  5. Chemical Sciences Division Lawrence Berkeley National Lab. Berkeley CA 94720 USA, Department of Inorganic Chemistry Fritz Haber Institute of the Max Planck Society 14195 Berlin Germany
  6. Peter Grünberg Institute 6, and JARA‐FIT Forschungszentrum Jülich GmbH 52425 Jülich Germany
  7. Physical and Computational Sciences Directorate Pacific Northwest National Laboratory Richland WA 99354 USA
  8. Peter Grünberg Institute 7 Forschungszentrum Jülich GmbH, and JARA‐FIT 52425 Jülich Germany, Peter Grünberg Institute 6, and JARA‐FIT Forschungszentrum Jülich GmbH 52425 Jülich Germany
Publication Date:
Research Org.:
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States); Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES); German Research Foundation (DFG)
OSTI Identifier:
1762525
Alternate Identifier(s):
OSTI ID: 1763699; OSTI ID: 1777107; OSTI ID: 1785863
Report Number(s):
PNNL-SA-152968
Journal ID: ISSN 0935-9648
Grant/Contract Number:  
AC02-05CH11231; 10122; 315025796; AC05-76RL01830; DE‐AC02‐05CH11231
Resource Type:
Published Article
Journal Name:
Advanced Materials
Additional Journal Information:
Journal Name: Advanced Materials Journal Volume: 33 Journal Issue: 4; Journal ID: ISSN 0935-9648
Publisher:
Wiley
Country of Publication:
Germany
Language:
English
Subject:
36 MATERIALS SCIENCE

Citation Formats

Rose, Marc‐André, Šmíd, Břetislav, Vorokhta, Mykhailo, Slipukhina, Ivetta, Andrä, Michael, Bluhm, Hendrik, Duchoň, Tomáš, Ležaić, Marjana, Chambers, Scott A., Dittmann, Regina, Mueller, David N., and Gunkel, Felix. Identifying Ionic and Electronic Charge Transfer at Oxide Heterointerfaces. Germany: N. p., 2020. Web. https://doi.org/10.1002/adma.202004132.
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Rose, Marc‐André, Šmíd, Břetislav, Vorokhta, Mykhailo, Slipukhina, Ivetta, Andrä, Michael, Bluhm, Hendrik, Duchoň, Tomáš, Ležaić, Marjana, Chambers, Scott A., Dittmann, Regina, Mueller, David N., & Gunkel, Felix. Identifying Ionic and Electronic Charge Transfer at Oxide Heterointerfaces. Germany. https://doi.org/10.1002/adma.202004132
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Rose, Marc‐André, Šmíd, Břetislav, Vorokhta, Mykhailo, Slipukhina, Ivetta, Andrä, Michael, Bluhm, Hendrik, Duchoň, Tomáš, Ležaić, Marjana, Chambers, Scott A., Dittmann, Regina, Mueller, David N., and Gunkel, Felix. Wed . "Identifying Ionic and Electronic Charge Transfer at Oxide Heterointerfaces". Germany. https://doi.org/10.1002/adma.202004132.
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@article{osti_1762525,
title = {Identifying Ionic and Electronic Charge Transfer at Oxide Heterointerfaces},
author = {Rose, Marc‐André and Šmíd, Břetislav and Vorokhta, Mykhailo and Slipukhina, Ivetta and Andrä, Michael and Bluhm, Hendrik and Duchoň, Tomáš and Ležaić, Marjana and Chambers, Scott A. and Dittmann, Regina and Mueller, David N. and Gunkel, Felix},
abstractNote = {The ability to tailor oxide heterointerfaces has led to novel properties in low-dimensional oxide systems. A fundamental understanding of these properties is based on the concept of electronic charge transfer. However, the electronic properties of oxide heterointerfaces crucially depend on their ionic constitution and defect structure: ionic charges contribute to charge transfer and screening at oxide interfaces, triggering a thermodynamic balance of ionic and electronic structures. Quantitative understanding of the electronic and ionic roles regarding charge-transfer phenomena poses a central challenge. Here, the electronic and ionic structure is simultaneously investigated at the prototypical charge-transfer heterointerface, LaAlO3/SrTiO3. Applying in situ photoemission spectroscopy under oxygen ambient, ionic and electronic charge transfer is deconvoluted in response to the oxygen atmosphere at elevated temperatures. In this way, both the rich and variable chemistry of complex oxides and the associated electronic properties are equally embraced. The interfacial electron gas is depleted through an ionic rearrangement in the strontium cation sublattice when oxygen is applied, resulting in an inverse and reversible balance between cation vacancies and electrons, while the mobility of ionic species is found to be considerably enhanced as compared to the bulk. Triggered by these ionic phenomena, the electronic transport and magnetic signature of the heterointerface are significantly altered.},
doi = {10.1002/adma.202004132},
journal = {Advanced Materials},
number = 4,
volume = 33,
place = {Germany},
year = {2020},
month = {12}
}
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