Photophysics of organically-capped silicon nanocrystals – A closer look into silicon nanocrystal luminescence using low temperature transient spectroscopy
In this paper a systematic and detailed study on the photophysical behavior of silicon nanocrystals (alkyl-capped, surface oxidized, oxide-encapsulated) is presented in order to elucidate the influence of local environment and surface species on the luminescence properties. Experiments at different temperatures – ranging from room temperature (RT) to 7 K – confirmed the important influence of the silicon nanocrystal (ncSi) surface on the photoluminescence (PL). Our comparative study of ncSi embedded in different matrices shows a strong increase of the exciton lifetimes at low temperature and the dominant widening of the bandgap for small ncSi after deactivation of traps below 100-150K. The present findings have significant implications for the use of ncSi in optoelectronic and biomedical applications, since they show that surface oxidation can occur in ligand-capped ncSi which limits the accessible emission wavelength for these applications to the orange/red spectral region when current passivation strategies are used.
Graphical abstract
Graphical abstract Highlights
► We present a systematic study on the photophysics of silicon nanocrystals. ► We study 3 local environments - alkyl-capped, surface oxidized, oxide-encapsulate. ► Even alkyl-capped ncSi are strongly affected by oxide surface species. ► Lifetimes significantly increase and bandgap widens drastically at low temperature. ► Turn-on of defect-free luminescence occurs at temperatures below 100-150K.
Authors:
Florian Maier-Flaig, Eric J. Henderson, Sebastian Valouch, Sönke Klinkhammer, Christian Kübel, Geoffrey A. Ozin, Uli Lemmer
Publication date:
Available online 29 May 2013
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