Abrupt Size Partitioning of Multimodal Photoluminescence Relaxation in Monodisperse Silicon Nanocrystals

Samuel L. Brown, Joseph B. Miller, Rebecca J. Anthony, Uwe R. Kortshagen, Andrei Kryjevski, Erik K. Hobbie

Research output: Research - peer-reviewArticle

  • 6 Citations

Abstract

Intrinsic constraints on efficient photoluminescence (PL) from smaller alkene-capped silicon nanocrystals (SiNCs) put limits on potential applications, but the root cause of such effects remains elusive. Here, plasma-synthesized colloidal SiNCs separated into monodisperse fractions reveal an abrupt size-dependent partitioning of multilevel PL relaxation, which we study as a function of temperature. Guided by theory and simulation, we explore the potential role of resonant phonon interactions with "minigaps" that emerge in the electronic density of states (DOS) under strong quantum confinement. Such higher-order structures can be very sensitive to SiNC surface chemistry, which we suggest might explain the common implication of surface effects in both the emergence of multimodal PL relaxation and the loss of quantum yield with decreasing nanocrystal size. Our results have potentially profound implications for optimizing the radiative recombination kinetics and quantum yield of smaller ligand-passivated SiNCs.

LanguageEnglish (US)
Pages1597-1603
Number of pages7
JournalACS Nano
Volume11
Issue number2
DOIs
StatePublished - Feb 28 2017
Externally publishedYes

Profile

nanocrystals
photoluminescence
silicon
Silicon
Nanocrystals
Photoluminescence
Quantum yield
radiative recombination
alkenes
chemistry
ligands
causes
kinetics
electronics
simulation
interactions
temperature
Electronic density of states
Quantum confinement
Alkenes

Keywords

  • photoluminescence
  • quantum confinement
  • silicon nanocrystals
  • surface effects

ASJC Scopus subject areas

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

Cite this

Brown, S. L., Miller, J. B., Anthony, R. J., Kortshagen, U. R., Kryjevski, A., & Hobbie, E. K. (2017). Abrupt Size Partitioning of Multimodal Photoluminescence Relaxation in Monodisperse Silicon Nanocrystals. ACS Nano, 11(2), 1597-1603. DOI: 10.1021/acsnano.6b07285

Abrupt Size Partitioning of Multimodal Photoluminescence Relaxation in Monodisperse Silicon Nanocrystals. / Brown, Samuel L.; Miller, Joseph B.; Anthony, Rebecca J.; Kortshagen, Uwe R.; Kryjevski, Andrei; Hobbie, Erik K.

In: ACS Nano, Vol. 11, No. 2, 28.02.2017, p. 1597-1603.

Research output: Research - peer-reviewArticle

Brown, SL, Miller, JB, Anthony, RJ, Kortshagen, UR, Kryjevski, A & Hobbie, EK 2017, 'Abrupt Size Partitioning of Multimodal Photoluminescence Relaxation in Monodisperse Silicon Nanocrystals' ACS Nano, vol 11, no. 2, pp. 1597-1603. DOI: 10.1021/acsnano.6b07285
Brown SL, Miller JB, Anthony RJ, Kortshagen UR, Kryjevski A, Hobbie EK. Abrupt Size Partitioning of Multimodal Photoluminescence Relaxation in Monodisperse Silicon Nanocrystals. ACS Nano. 2017 Feb 28;11(2):1597-1603. Available from, DOI: 10.1021/acsnano.6b07285
Brown, Samuel L. ; Miller, Joseph B. ; Anthony, Rebecca J. ; Kortshagen, Uwe R. ; Kryjevski, Andrei ; Hobbie, Erik K./ Abrupt Size Partitioning of Multimodal Photoluminescence Relaxation in Monodisperse Silicon Nanocrystals. In: ACS Nano. 2017 ; Vol. 11, No. 2. pp. 1597-1603
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