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Title: Ensemble brightening and enhanced quantum yield in size-purified silicon nanocrystals

Abstract

Here, we report on the quantum yield, photoluminescence (PL) lifetime and ensemble photoluminescent stability of highly monodisperse plasma-synthesized silicon nanocrystals (SiNCs) prepared though density-gradient ultracentrifugation in mixed organic solvents. Improved size uniformity leads to a reduction in PL line width and the emergence of entropic order in dry nanocrystal films. We find excellent agreement with the anticipated trends of quantum confinement in nanocrystalline silicon, with a solution quantum yield that is independent of nanocrystal size for the larger fractions but decreases dramatically with size for the smaller fractions. We also find a significant PL enhancement in films assembled from the fractions, and we use a combination of measurement, simulation and modeling to link this ‘brightening’ to a temporally enhanced quantum yield arising from SiNC interactions in ordered ensembles of monodisperse nanocrystals. Using an appropriate excitation scheme, we exploit this enhancement to achieve photostable emission.

Authors:
 [1];  [1];  [2];  [1];  [1];  [1]
  1. North Dakota State Univ., Fargo, ND (United States)
  2. Univ. of Minnesota, Minneapolis, MN (United States)
Publication Date:
Research Org.:
North Dakota State Univ., Fargo, ND (United States)
Sponsoring Org.:
USDOE Office of Energy Efficiency and Renewable Energy (EERE)
OSTI Identifier:
1053187
Report Number(s):
DOE/GO/88160-46
Journal ID: ISSN 1936-0851
Grant/Contract Number:  
FG36-08GO88160
Resource Type:
Accepted Manuscript
Journal Name:
ACS Nano
Additional Journal Information:
Journal Volume: 6; Journal Issue: 8; Journal ID: ISSN 1936-0851
Publisher:
American Chemical Society
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; nanocrystalline silicon; polydispersity; photoluminescent stability; quantum yield

Citation Formats

Miller, Joseph B., Van Sickle, Austin R., Anthony, Rebecca J., Kroll, Daniel M., Kortshagen, Uwe R., and Hobbie, Erik K. Ensemble brightening and enhanced quantum yield in size-purified silicon nanocrystals. United States: N. p., 2012. Web. doi:10.1021/nn302524k.
Miller, Joseph B., Van Sickle, Austin R., Anthony, Rebecca J., Kroll, Daniel M., Kortshagen, Uwe R., & Hobbie, Erik K. Ensemble brightening and enhanced quantum yield in size-purified silicon nanocrystals. United States. doi:https://doi.org/10.1021/nn302524k
Miller, Joseph B., Van Sickle, Austin R., Anthony, Rebecca J., Kroll, Daniel M., Kortshagen, Uwe R., and Hobbie, Erik K. Wed . "Ensemble brightening and enhanced quantum yield in size-purified silicon nanocrystals". United States. doi:https://doi.org/10.1021/nn302524k. https://www.osti.gov/servlets/purl/1053187.
@article{osti_1053187,
title = {Ensemble brightening and enhanced quantum yield in size-purified silicon nanocrystals},
author = {Miller, Joseph B. and Van Sickle, Austin R. and Anthony, Rebecca J. and Kroll, Daniel M. and Kortshagen, Uwe R. and Hobbie, Erik K.},
abstractNote = {Here, we report on the quantum yield, photoluminescence (PL) lifetime and ensemble photoluminescent stability of highly monodisperse plasma-synthesized silicon nanocrystals (SiNCs) prepared though density-gradient ultracentrifugation in mixed organic solvents. Improved size uniformity leads to a reduction in PL line width and the emergence of entropic order in dry nanocrystal films. We find excellent agreement with the anticipated trends of quantum confinement in nanocrystalline silicon, with a solution quantum yield that is independent of nanocrystal size for the larger fractions but decreases dramatically with size for the smaller fractions. We also find a significant PL enhancement in films assembled from the fractions, and we use a combination of measurement, simulation and modeling to link this ‘brightening’ to a temporally enhanced quantum yield arising from SiNC interactions in ordered ensembles of monodisperse nanocrystals. Using an appropriate excitation scheme, we exploit this enhancement to achieve photostable emission.},
doi = {10.1021/nn302524k},
journal = {ACS Nano},
number = 8,
volume = 6,
place = {United States},
year = {2012},
month = {7}
}

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Works referencing / citing this record:

Nanoparticles as macromolecules
journal, June 2013

  • Miller, Joseph B.; Hobbie, Erik K.
  • Journal of Polymer Science Part B: Polymer Physics, Vol. 51, Issue 16
  • DOI: 10.1002/polb.23327

Silicon Quantum Dot Light Emitting Diode at 620 nm
journal, May 2019

  • Yamada, Hiroyuki; Shirahata, Naoto
  • Micromachines, Vol. 10, Issue 5
  • DOI: 10.3390/mi10050318

Nanoparticles as macromolecules
journal, June 2013

  • Miller, Joseph B.; Hobbie, Erik K.
  • Journal of Polymer Science Part B: Polymer Physics, Vol. 51, Issue 16
  • DOI: 10.1002/polb.23327

Si/SiO2 Core/Shell Luminescent Silicon Nanocrystals and Porous Silicon Powders With High Quantum Yield, Long Lifetime, and Good Stability
journal, April 2019

  • Gelloz, Bernard; Juangsa, Firman Bagja; Nozaki, Tomohiro
  • Frontiers in Physics, Vol. 7
  • DOI: 10.3389/fphy.2019.00047

Silicon Quantum Dot Light Emitting Diode at 620 nm
journal, May 2019

  • Yamada, Hiroyuki; Shirahata, Naoto
  • Micromachines, Vol. 10, Issue 5
  • DOI: 10.3390/mi10050318

Assembly and Electronic Applications of Colloidal Nanomaterials
journal, November 2016


Effects of inter-nanocrystal distance on luminescence quantum yield in ensembles of Si nanocrystals
journal, December 2014

  • Valenta, J.; Greben, M.; Gutsch, S.
  • Applied Physics Letters, Vol. 105, Issue 24
  • DOI: 10.1063/1.4904472

Photoluminescence performance limits of Si nanocrystals in silicon oxynitride matrices
journal, October 2017

  • Valenta, Jan; Greben, Michael; Gutsch, Sebastian
  • Journal of Applied Physics, Vol. 122, Issue 14
  • DOI: 10.1063/1.4999023

Luminescent, water-soluble silicon quantum dots via micro-plasma surface treatment
journal, January 2016

  • Wu, Jeslin J.; Siva Santosh Kumar Kondeti, Vighneswara; Bruggeman, Peter J.
  • Journal of Physics D: Applied Physics, Vol. 49, Issue 8
  • DOI: 10.1088/0022-3727/49/8/08lt02

Silicon quantum dots: surface matters
journal, April 2014