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@PHDTHESIS{Bumer:838034,
author = {Bäumer, Christoph},
title = {{S}pectroscopic characterization of localvalence change
processes in resistivelyswitching complex oxides},
volume = {150},
school = {RWTH Aachen},
type = {Dr.},
address = {Jülich},
publisher = {Forschungszentrum Jülich GmbH Zentralbibliothek, Verlag},
reportid = {FZJ-2017-06777},
isbn = {978-3-95806-246-7},
series = {Schriften des Forschungszentrums Jülich. Reihe
Schlüsseltechnologien / Key Technologies},
pages = {X, 206 S.},
year = {2017},
note = {RWTH Aachen, Diss., 2016},
abstract = {An increasingly interconnected world creates a high demand
for high-density and lowcost data storage. Redox-based
memristive devices, which allow switching between high and
low electrical resistances through the application of
voltages, are highly attractive candidates for
next-generation non-volatile memory. But their control and
rational design is complicated by poorly understood
switching and failure mechanisms. The complex nanoscale
redox processes that are suspected to drive so-called
resistive switching in these devices remain in adequately
characterized. Especially, quantitative information about
these processes, which is essential for further advances in
the educated design, has been experimentally in accessible
so far. Therefore, spectroscopic tools with high spatial
resolution are employed in this work to elucidate both
switching and failure mechanism of memristive devices based
on the model material SrTiO$_{3}$. After thorough electrical
characterization, two alternative photoelectron emission
microscopy approaches are used. As photoemission is a
surface sensitive process, the top electrodes of the devices
are removed before investigation in the first approach. In
the second step, thin graphene electrodes are employed,
enabling $\textit{in operando}$ characterization. In
combination with cross sectional, $\textit{in operando}$
transmission electron microscopy and spectroscopy, a clear
evidence of a reversible, localized redox reaction is
identied. In the low resistance state, a nanoscale lamentin
the SrTiO$_{3}$ is oxygen-decient, while it is nearly
stoichiometric in the high resistance state, resulting in a
valence change between Ti$^{3+}$ and Ti$^{4+}$. The carrier
concentration modulation resulting from this valence change
is quantied through comparison with calibration spectra. A
carrier concentration change by a factor of two causes two
orders of magnitude change in device resistance through a
modulation of the effective Schottky barrier at the
electrode/oxide interface. The microscopic origin of the
polarity of the resistance hysteresis in these devices has
long been debated, as it cannot be explained by the
typically involved purely internal redistribution of oxygen
vacancies. The spectroscopic results of this work reveal
that instead, oxygen evolution and reincorporation reactions
at the electrode/oxide interface are responsible for the
valence change in the SrTiO$_{3}$. Regarding the failure
mechanism, it is found that fast reoxidation frequently
results in retention failure in SrTiO$_{3}$ devices, which
can be inhibited by incidental, local phase separations.
Mimicking this phase separation by intentionally introducing
retention-stabilization layers with slow oxygen transport is
therefore derived as a design rule for
retention-failure-resistant devices.},
cin = {PGI-7},
cid = {I:(DE-Juel1)PGI-7-20110106},
pnm = {899 - ohne Topic (POF3-899)},
pid = {G:(DE-HGF)POF3-899},
typ = {PUB:(DE-HGF)3 / PUB:(DE-HGF)11},
url = {https://juser.fz-juelich.de/record/838034},
}