Carrier dynamics in metal oxide absorbers for solar fuel production
Dennis Friedrich a, Mario Borgwardt a, Sönke Müller a, Hannes Hempel b, Roel van de Krol a, Rainer Eichberger a
a Helmholtz-Zentrum Berlin für Materialien und Energie GmbH, Germany, Berlin, Germany
b Helmholtz-Zentrum Berlin für Materialien und Energie GmbH, Germany, Berlin, Germany
Materials for Sustainable Development Conference (MATSUS)
Proceedings of nanoGe September Meeting 2017 (NFM17)
SF1: Material and Device Innovations for the Practical Implementation of Solar Fuels (SolarFuel17)
Barcelona, Spain, 2017 September 4th - 9th
Organizers: Wilson Smith and Ki Tae Nam
Poster, Dennis Friedrich, 165
Publication date: 20th June 2016

The efficiency of photoelectrochemical (PEC) hydrogen production depends critically on the charge carrier dynamics in the bulk and near the surface of the semiconducting absorber material. Since charge separation and recombination typically takes place on fs – ns time scales, whereas the electrochemical reactions occur on μs – s time scales, understanding and controlling of reaction kinetics is crucially important. For the evaluation and optimization of newly developed materials based on metal oxide semiconductors we have gained knowledge on fundamental bulk properties such as diffusion lengths, trapping dynamics and lifetimes of charge carriers using time-resolved conductivity measurements on sub-picosecond (terahertz spectroscopy, TRTC) to microsecond (microwave spectroscopy, TRMC) timescales. 

Charge carrier dynamics near the surface of a semiconductor reflect, in the most basic picture, the competition between carrier recombination and carrier injection into the electrolyte We have employed femtosecond-resolved two-photon photoemission spectroscopy (fs-2PPE) as an explicitly surface-sensitive method to study the dynamics of surface electrons in Cu2O single crystals for different crystal facets and surface reconstructions. We have for the first time observed the transport of electrons to the surface and found a dramatic change in surface lifetime upon reconstruction or by deposition of a passivation layer. Analysis of the simultaneously measured kinetic energy spectra of the photoemitted electrons reveals how interfacial charge transfer mechanisms and surface electronic structure affects photochemical reactions at the surface.

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