Journal Article PUBDB-2022-06265

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Unravelling the Origin of Ultra‐Low Conductivity in SrTiO$_3$ Thin Films: Sr Vacancies and Ti on A‐Sites Cause Fermi Level Pinning

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2022
Wiley-VCH Weinheim

Advanced functional materials 32(38), 2202226 () [10.1002/adfm.202202226]
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Abstract: Different SrTiO$_3$ thin films are investigated to unravel the nature of ultra-low conductivities recently found in SrTiO$_3$ films prepared by pulsed laser deposition. Impedance spectroscopy reveals electronically pseudo-intrinsic conductivities for a broad range of different dopants (Fe, Al, Ni) and partly high dopant concentrations up to several percent. Using inductively-coupled plasma optical emission spectroscopy and reciprocal space mapping, a severe Sr deficiency is found and positron annihilation lifetime spectroscopy revealed Sr vacancies as predominant point defects. From synchrotron-based X-ray standing wave and X-ray absorption spectroscopy measurements, a change in site occupation is deduced for Fe-doped SrTiO$_3$ films, accompanied by a change in the dopant type. Based on these experiments, a model is deduced, which explains the almost ubiquitous pseudo-intrinsic conductivity of these films. Sr deficiency is suggested as key driver by introducing Sr vacancies and causing site changes (Fe$_{Sr}$ and Ti$_{Sr}$) to accommodate nonstoichiometry. Sr vacancies act as mid-gap acceptor states, pinning the Fermi level, provided that additional donor states (most probably Ti$_{Sr}^{\bullet\bullet}$) are present. Defect chemical modeling revealed that such a Fermi level pinning also causes a self-limitation of the Ti site change and leads to a very robust pseudo-intrinsic situation, irrespective of Sr/Ti ratios and doping.

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Contributing Institute(s):
  1. DOOR-User (DOOR ; HAS-User)
  2. PETRA-D (FS-PETRA-D)
  3. Nanolab (FS-NL)
Research Program(s):
  1. 632 - Materials – Quantum, Complex and Functional Materials (POF4-632) (POF4-632)
  2. 6G3 - PETRA III (DESY) (POF4-6G3) (POF4-6G3)
Experiment(s):
  1. PETRA Beamline P24 (PETRA III)

Appears in the scientific report 2022
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 Record created 2022-11-01, last modified 2025-07-15


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