Bright Silicon Nanocrystals from a Liquid Precursor: Quasi-Direct Recombination with High Quantum Yield

Todd A. Pringle, Katharine I. Hunter, Alexandra Brumberg, Kenneth J. Anderson, Jeffrey A. Fagan, Salim A. Thomas, Reed J. Petersen, Mahmud Sefannaser, Yulun Han, Samuel L. Brown, Dmitri S. Kilin, Richard D. Schaller, Uwe R. Kortshagen, Philip Raymond Boudjouk, Erik K. Hobbie

Research output: Contribution to journalArticle

Abstract

Silicon nanocrystals (SiNCs) with bright bandgap photoluminescence (PL) are of current interest for a range of potential applications, from solar windows to biomedical contrast agents. Here, we use the liquid precursor cyclohexasilane (Si6H12) for the plasma synthesis of colloidal SiNCs with exemplary core emission. Through size separation executed in an oxygen-shielded environment, we achieve PL quantum yields (QYs) approaching 70% while exposing intrinsic constraints on efficient core emission from smaller SiNCs. Time-resolved PL spectra of these fractions in response to femtosecond pulsed excitation reveal a zero-phonon radiative channel that anticorrelates with QY, which we model using advanced computational methods applied to a 2 nm SiNC. Our results offer additional insight into the photophysical interplay of the nanocrystal surface, quasi-direct recombination, and efficient SiNC core PL.

Original languageEnglish (US)
Pages (from-to)3858-3867
Number of pages10
JournalACS nano
Volume14
Issue number4
DOIs
StatePublished - Apr 28 2020

Keywords

  • liquid silane
  • photoluminescence quantum yield
  • quantum confinement
  • silicon nanocrystals
  • surface effects

ASJC Scopus subject areas

  • Materials Science(all)
  • Engineering(all)
  • Physics and Astronomy(all)

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  • Cite this

    Pringle, T. A., Hunter, K. I., Brumberg, A., Anderson, K. J., Fagan, J. A., Thomas, S. A., Petersen, R. J., Sefannaser, M., Han, Y., Brown, S. L., Kilin, D. S., Schaller, R. D., Kortshagen, U. R., Boudjouk, P. R., & Hobbie, E. K. (2020). Bright Silicon Nanocrystals from a Liquid Precursor: Quasi-Direct Recombination with High Quantum Yield. ACS nano, 14(4), 3858-3867. https://doi.org/10.1021/acsnano.9b09614