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Nat Commun. 2015 Apr 22;6:6901. doi: 10.1038/ncomms7901.

Evidence for photogenerated intermediate hole polarons in ZnO.

Nature communications

Hikmet Sezen, Honghui Shang, Fabian Bebensee, Chengwu Yang, Maria Buchholz, Alexei Nefedov, Stefan Heissler, Christian Carbogno, Matthias Scheffler, Patrick Rinke, Christof Wöll

Affiliations

  1. Karlsruhe Institute of Technology (KIT), Institute of Functional Interfaces (IFG), 76021 Karlsruhe, Germany.
  2. Fritz Haber Institute of the Max Planck Society, Faradayweg 4-6, 14195 Berlin, Germany.
  3. 1] Fritz Haber Institute of the Max Planck Society, Faradayweg 4-6, 14195 Berlin, Germany [2] COMP/Department of Applied Physics, Aalto University School of Science, P.O. Box 11100, FI-00076 Aalto, Finland.

PMID: 25902307 DOI: 10.1038/ncomms7901

Abstract

Despite their pronounced importance for oxide-based photochemistry, optoelectronics and photovoltaics, only fairly little is known about the polaron lifetimes and binding energies. Polarons represent a crucial intermediate step populated immediately after dissociation of the excitons formed in the primary photoabsorption process. Here we present a novel approach to studying photoexcited polarons in an important photoactive oxide, ZnO, using infrared (IR) reflection-absorption spectroscopy (IRRAS) with a time resolution of 100 ms. For well-defined (10-10) oriented ZnO single-crystal substrates, we observe intense IR absorption bands at around 200 meV exhibiting a pronounced temperature dependence. On the basis of first-principles-based electronic structure calculations, we assign these features to hole polarons of intermediate coupling strength.

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