Evidence for photogenerated intermediate hole polarons in ZnO

Hikmet Sezen, Honghui Shang, Fabian Bebensee, Chengwu Yang, Maria Buchholz, Alexei Nefedov, Stefan Heissler, Christian Carbogno, Matthias Scheffler, Patrick Rinke and Christof Wöll ()
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Hikmet Sezen: Karlsruhe Institute of Technology (KIT), Institute of Functional Interfaces (IFG)
Honghui Shang: Fritz Haber Institute of the Max Planck Society
Fabian Bebensee: Karlsruhe Institute of Technology (KIT), Institute of Functional Interfaces (IFG)
Chengwu Yang: Karlsruhe Institute of Technology (KIT), Institute of Functional Interfaces (IFG)
Maria Buchholz: Karlsruhe Institute of Technology (KIT), Institute of Functional Interfaces (IFG)
Alexei Nefedov: Karlsruhe Institute of Technology (KIT), Institute of Functional Interfaces (IFG)
Stefan Heissler: Karlsruhe Institute of Technology (KIT), Institute of Functional Interfaces (IFG)
Christian Carbogno: Fritz Haber Institute of the Max Planck Society
Matthias Scheffler: Fritz Haber Institute of the Max Planck Society
Patrick Rinke: Fritz Haber Institute of the Max Planck Society
Christof Wöll: Karlsruhe Institute of Technology (KIT), Institute of Functional Interfaces (IFG)

Nature Communications, 2015, vol. 6, issue 1, 1-5

Abstract: 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.

Date: 2015
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DOI: 10.1038/ncomms7901

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