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Origin of the multi-exponential decay dynamics in light-emitting silicon nanocrystals

Published online by Cambridge University Press:  01 February 2011

Cécile Reynaud ,
Olivier Guillois ,
Nathalie Herlin-Boime ,
Gilles Ledoux  and
Friedrich Huisken
Cécile Reynaud
Affiliation:
LFP (CEA-CNRS URA 2453), Service des Photons Atomes et Molécules, DSM, CEA-Saclay, France
Olivier Guillois
Affiliation:
LFP (CEA-CNRS URA 2453), Service des Photons Atomes et Molécules, DSM, CEA-Saclay, France
Nathalie Herlin-Boime
Affiliation:
LFP (CEA-CNRS URA 2453), Service des Photons Atomes et Molécules, DSM, CEA-Saclay, France
Gilles Ledoux
Affiliation:
LPCML, UMR CNRS 5620, Université Claude Bernard Lyon I, Villeurbanne, France Institute of Solid State Physics, University of Jena, and MPI for Astronomy, Heidelberg, Germany
Friedrich Huisken
Affiliation:
Institute of Solid State Physics, University of Jena, and MPI for Astronomy, Heidelberg, Germany
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Abstract

Light-emitting silicon nanocrystals (nc-Si) have attracted much interest due to their importance for optoelectronic devices. Electron hole recombination in a quantum confined system is generally considered as the theoretical frame explaining the photoluminescence (PL) origin. However, there is still a living debate, in particular regarding the PL decay dynamics. The decay is not single exponential and decay curves described by a stretched exponential law were systematically reported for all types of nanocrystalline silicon. The origin of this multi-exponential decay is often attributed to migration effects of the excitons between nanocrystals. In contrast to these approaches, the absence of carrier hopping has been demonstrated experimentally in porous silicon. In order to elucidate this question, specific samples were prepared, consisting in deposits made from gas phase grown silicon nanocrystals with different particle density. The nanoparticles were synthesized by laser pyrolysis of silane in a gas flow reactor, extracted as a supersonic beam, size-selected, and deposited downstream as films of variable densities by changing the deposition time. The nanoparticle number densities were determined by atomic force microscopy. Time-resolved photoluminescence measurements on these films were carried out as a function of the film density and at different PL wavelengths. The reported results showed photoluminescence properties independent of the film density. Even in the very low density film (∼4*109 particles/cm2) where nanoparticles are completely isolated from each other, the decay kinetics corresponds to a multi-exponential law. This means that exciton migration alone cannot explain the stretched exponential decay. Its origin must be linked to an intrinsic characteristic of the nc-Si particle. In this paper, the experimental results are described in more details and compared to the theoretical predictions available in the frame of the quantum confinement model. Then, the possible origins of the multi-exponential character of the decay dynamics is discussed, and the particular properties of the PL in indirect band-gap semiconductors emphasized.

Type
Research Article
Information
MRS Online Proceedings Library (OPL) , Volume 832: Symposium F – Group IV Semiconductor Nanostructures , 2004 , F6.2
Copyright
Copyright © Materials Research Society 2005

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