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@ARTICLE{Zurhelle:886051,
author = {Zurhelle, A. F. and Christensen, D. V. and Menzel, S. and
Gunkel, F.},
title = {{D}ynamics of the spatial separation of electrons and
mobile oxygen vacancies in oxide heterostructures},
journal = {Physical review materials},
volume = {4},
number = {10},
issn = {2475-9953},
address = {College Park, MD},
publisher = {APS},
reportid = {FZJ-2020-04238},
pages = {104604},
year = {2020},
abstract = {In the search for an oxide-based 2D electron system with a
large concentration of highly mobile electrons, a promising
strategy is to introduce electrons through donor doping
while spatially separating electrons and donors to prevent
scattering. In SrTiO3, this can be achieved by tailoring the
oxygen vacancy profile through reduction, e.g., by creating
an interface with an oxygen scavenging layer. Through
reduction, oxygen atoms are removed close to the interface,
leaving behind oxygen vacancies in the SrTiO3 lattice and
mobile electrons in the SrTiO3 conduction band. The commonly
assumed picture is that the oxygen vacancies then remain
confined close to the interface while the electrons leak a
few nanometers into the bulk, resulting in an
electron-defect separation and a highly mobile, oxide-based
2D electron system. So far it has remained unclear how the
confinement and electron-defect separation develop over
time. Here, we present transient finite element simulations
that consider three driving forces acting on the oxygen
vacancy distribution: diffusion due to the concentration
gradient, drift due to the intrinsic electric field, and an
oxygen vacancy trapping energy that holds oxygen vacancies
at the interface. Our simulations show that at room
temperature, three distinct regions are formed in SrTiO3
within days: (1) Oxygen vacancies are partially held at the
interface due to the oxygen vacancy trapping energy. (2) The
accompanying positive space charge causes an oxygen vacancy
depletion layer with large electron concentration and high
mobility just below the interface. This electron-defect
separation, indeed, leads to a highly conductive region. (3)
While we are able to describe measured conductivity data
with an oxygen vacancy trapping energy of −0.2 eV, this
value does not prevent oxygen vacancy diffusion into the
bulk: A diffusion front progresses into the bulk and leads
to significant conductivity arising over the first
micrometer within a couple of months. An enhanced oxygen
vacancy trapping energy of −0.5 eV or below would suppress
this loss of confinement, leading to a static and pronounced
electron-defect separation. Consequently, our results
highlight the importance of oxygen vacancy redistribution
and suggest the trapping energy of oxygen vacancies at the
interface as an important design parameter for
oxygen-vacancy-based 2D electron systems.},
cin = {PGI-7 / JARA-FIT},
ddc = {530},
cid = {I:(DE-Juel1)PGI-7-20110106 / $I:(DE-82)080009_20140620$},
pnm = {521 - Controlling Electron Charge-Based Phenomena
(POF3-521)},
pid = {G:(DE-HGF)POF3-521},
typ = {PUB:(DE-HGF)16},
UT = {WOS:000582800500001},
doi = {10.1103/PhysRevMaterials.4.104604},
url = {https://juser.fz-juelich.de/record/886051},
}