Surface brightens up Si quantum dots: direct bandgap-like size-tunable emission

K. Dohnalova, A.N. Poddubny, A.A. Prokofiev, W.D.A.M. Boer, C. Umesh, J.M.J. Paulusse, H. Zuilhof, T. Gregorkiewicz

Research output: Contribution to journalArticleAcademicpeer-review

198 Citations (Scopus)

Abstract

Colloidal semiconductor quantum dots (QDs) constitute a perfect material for ink-jet printable large area displays, photovoltaics, light-emitting diode, bio-imaging luminescent markers and many other applications. For this purpose, efficient light emission/absorption and spectral tunability are necessary conditions. These are currently fulfilled by the direct bandgap materials. Si-QDs could offer the solution to major hurdles posed by these materials, namely, toxicity (e.g., Cd-, Pb- or As-based QDs), scarcity (e.g., QD with In, Se, Te) and/or instability. Here we show that by combining quantum confinement with dedicated surface engineering, the biggest drawback of Si—the indirect bandgap nature—can be overcome, and a ‘direct bandgap’ variety of Si-QDs is created. We demonstrate this transformation on chemically synthesized Si-QDs using state-of-the-art optical spectroscopy and theoretical modelling. The carbon surface termination gives rise to drastic modification in electron and hole wavefunctions and radiative transitions between the lowest excited states of electron and hole attain ‘direct bandgap-like’ (phonon-less) character. This results in efficient fast emission, tunable within the visible spectral range by QD size. These findings are fully justified within a tight-binding theoretical model. When the C surface termination is replaced by oxygen, the emission is converted into the well-known red luminescence, with microsecond decay and limited spectral tunability. In that way, the ‘direct bandgap’ Si-QDs convert into the ‘traditional’ indirect bandgap form, thoroughly investigated in the past.
Original languageEnglish
Article numbere47
JournalLight : science & Application
Volume2
DOIs
Publication statusPublished - 2013

Keywords

  • silicon nanocrystals
  • dependent photoluminescence
  • optical-properties
  • nanoparticles
  • luminescence
  • alkyl
  • functionalization
  • nanoclusters
  • confinement
  • origin

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