Engineering surface dipoles on mixed conducting oxides with ultra-thin oxide decoration layers

Research output: Contribution to journalArticleResearchpeer-review

Authors

  • Matthäus Siebenhofer
  • Andreas Nenning
  • Peter Blaha
  • Jürgen Fleig
  • Markus Kubicek

Organisational units

External Organisational units

  • Institute of Materials Science and Technology
  • Department of Materials Science & EngineeringMassachusetts Institute of Technology

Abstract

Improving materials for energy conversion and storage devices is deeply connected with an optimization of their surfaces and surface modification is a promising strategy on the way to enhance modern energy technologies. This study shows that surface modification with ultra-thin oxide layers allows for a systematic tailoring of the surface dipole and the work function of mixed ionic and electronic conducting oxides, and it introduces the ionic potential of surface cations as a readily accessible descriptor for these effects. The combination of X-ray photoelectron spectroscopy (XPS) and density functional theory (DFT) illustrates that basic oxides with a lower ionic potential than the host material induce a positive surface charge and reduce the work function of the host material and vice versa. As a proof of concept that this strategy is widely applicable to tailor surface properties, we examined the effect of ultra-thin decoration layers on the oxygen exchange kinetics of pristine mixed conducting oxide thin films in very clean conditions by means of in-situ impedance spectroscopy during pulsed laser deposition (i-PLD). The study shows that basic decorations with a reduced surface work function lead to a substantial acceleration of the oxygen exchange on the surfaces of diverse materials.

Details

Original languageEnglish
Article number1730
Number of pages10
JournalNature Communications
Volume15.2024
Issue number1
DOIs
Publication statusPublished - Feb 2024