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

Journal Article · · ACS Nano
DOI:https://doi.org/10.1021/nn302524k· OSTI ID:1053187
 [1];  [1];  [2];  [1];  [1];  [1]
  1. North Dakota State Univ., Fargo, ND (United States)
  2. Univ. of Minnesota, Minneapolis, MN (United States)

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.

Research Organization:
North Dakota State Univ., Fargo, ND (United States)
Sponsoring Organization:
USDOE Office of Energy Efficiency and Renewable Energy (EERE)
Grant/Contract Number:
FG36-08GO88160
OSTI ID:
1053187
Report Number(s):
DOE/GO/88160-46
Journal Information:
ACS Nano, Vol. 6, Issue 8; ISSN 1936-0851
Publisher:
American Chemical SocietyCopyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 91 works
Citation information provided by
Web of Science

References (60)

Quantum dot heterostructures: Fabrication, properties, lasers (Review) journal April 1998
Quantum dot bioconjugates for imaging, labelling and sensing journal June 2005
Quantum Dot Bioconjugates for Ultrasensitive Nonisotopic Detection journal September 1998
Cytotoxicity of Colloidal CdSe and CdSe/ZnS Nanoparticles journal February 2005
Probing the Cytotoxicity of Semiconductor Quantum Dots journal January 2004
Silicon nanocrystals with ensemble quantum yields exceeding 60% journal June 2006
Enhanced Photoluminescence from Si Nano-organosols by Functionalization with Alkenes and Their Size Evolution journal January 2006
Size and Spectroscopy of Silicon Nanoparticles Prepared via Reduction of SiCl4 journal November 2006
Oxide and hydrogen capped ultrasmall blue luminescent Si nanoparticles journal August 2000
Preparation of Monodisperse Silicon Nanocrystals Using Density Gradient Ultracentrifugation journal August 2011
Size-Dependent Absolute Quantum Yields for Size-Separated Colloidally-Stable Silicon Nanocrystals journal December 2011
Synthesis of Ligand-Stabilized Silicon Nanocrystals with Size-Dependent Photoluminescence Spanning Visible to Near-Infrared Wavelengths journal December 2011
Silicon quantum wire array fabrication by electrochemical and chemical dissolution of wafers journal September 1990
Porous silicon formation: A quantum wire effect journal February 1991
Biocompatible Luminescent Silicon Quantum Dots for Imaging of Cancer Cells journal May 2008
Luminescent passive-oxidized silicon quantum dots as biological staining labels and their cytotoxicity effects at high concentration journal September 2008
Electrochemistry and Electrogenerated Chemiluminescence from Silicon Nanocrystal Quantum Dots journal May 2002
Water-Soluble Photoluminescent Silicon Quantum Dots journal July 2005
Biodegradable luminescent porous silicon nanoparticles for in vivo applications journal February 2009
Hybrid Solar Cells from P3HT and Silicon Nanocrystals journal January 2009
Plasma-Assisted Synthesis of Silicon Nanocrystal Inks journal September 2007
High efficiency photoluminescence from silicon nanocrystals prepared by plasma synthesis and organic surface passivation journal December 2006
Air-stable full-visible-spectrum emission from silicon nanocrystals synthesized by an all-gas-phase plasma approach journal May 2008
Routes to Achieving High Quantum Yield Luminescence from Gas-Phase-Produced Silicon Nanocrystals journal August 2011
Surface Functionalization of Silicon Nanoparticles Produced by Laser-Driven Pyrolysis of Silane followed by HF−HNO 3 Etching journal May 2004
Rapid Separation and Purification of Nanoparticles in Organic Density Gradients journal February 2010
Emission intermittency in silicon nanocrystals journal September 2004
Brightening, Blinking, Bluing and Bleaching in the Life of a Quantum Dot: Friend or Foe? journal September 2009
Electron−Phonon Coupling and Localization of Excitons in Single Silicon Nanocrystals journal February 2008
Resonant Coupling between Surface Vibrations and Electronic States in Silicon Nanocrystals at the Strong Confinement Regime journal December 2005
Photoluminescence properties of silicon nanocrystals as a function of their size journal December 2000
Photoluminescence of size-separated silicon nanocrystals: Confirmation of quantum confinement journal June 2002
Effect of passivation and aging on the photoluminescence of silicon nanocrystals journal December 2001
Size-Dependent Intrinsic Radiative Decay Rates of Silicon Nanocrystals at Large Confinement Energies journal February 2008
Photoluminescence quantum yields of amorphous and crystalline silicon nanoparticles journal September 2009
Theoretical aspects of the luminescence of porous silicon journal October 1993
Light-Emitting Silicon Nanocrystals from Laser Pyrolysis journal December 2002
Silicon nanocrystals dispersed in water: Photosensitizers for molecular oxygen journal May 2010
Size Tunable Visible Luminescence from Individual Organic Monolayer Stabilized Silicon Nanocrystal Quantum Dots journal July 2002
Self-Organization of CdSe Nanocrystallites into Three-Dimensional Quantum Dot Superlattices journal November 1995
Suppression of crystal nucleation in polydisperse colloids due to increase of the surface free energy journal October 2001
Wide Varieties of Cationic Nanoparticles Induce Defects in Supported Lipid Bilayers journal January 2008
Enhanced Fluorescence Intermittency of CdSe-ZnS Quantum-Dot Clusters journal December 2006
Photoinduced Fluorescence Enhancement in Mono- and Multilayer Films of CdSe/ZnS Quantum Dots:  Dependence on Intensity and Wavelength of Excitation Light journal May 2005
Monte-Carlo simulations of photoinduced fluorescence enhancement in semiconductor quantum dot arrays journal March 2005
Intensified blinking, continuous memory loss, and fluorescence enhancement of interacting light-emission quantum dots journal November 2009
Collective fluorescence enhancement in nanoparticle clusters journal June 2011
Electron Migration Limits the Rate of Photobrightening in Thin Films of CdSe Quantum Dots in a Dry N 2 (g) Atmosphere journal February 2011
Photoenhancement of Luminescence in Colloidal CdSe Quantum Dot Solutions journal October 2003
Photobrightening and photodarkening in PbS quantum dots journal January 2006
Photoluminescence enhancement in thin films of PbSe nanocrystals journal September 2008
Surface Transformation and Photoinduced Recovery in CdSe Nanocrystals journal April 2001
Surface State Analysis of Photobrightening in CdSe Nanocrystal Thin Films journal November 2003
Enhancement of the Photoluminescence of CdSe Nanocrystals Dispersed in CHCl 3 by Oxygen Passivation of Surface States journal June 2003
Quantum Dot Photoluminescence Activation and Decay: Dark, Bright, and Reversible Populations in ZnS-Capped CdSe Nanocrystals journal September 2011
Ellipsometric determination of optical constants for silicon and thermally grown silicon dioxide via a multi-sample, multi-wavelength, multi-angle investigation journal March 1998
Blinking and nonradiant dark fraction of water-soluble quantum dots in aqueous solution journal September 2005
Colloidal Quantum Dots: Think Outside the (Particle-in-a-)Box journal December 2011
Efficient Exciton Transport between Strongly Quantum-Confined Silicon Quantum Dots journal April 2012
Energy transfer between semiconductor nanocrystals: Validity of Förster’s theory journal May 2007

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Spectral dependencies of the stretched exponential dispersion factor and photoluminescence quantum yield as a common feature of nanocrystalline Si text January 2019
Cationic Silicon Nanocrystals with Colloidal Stability, pH‐Independent Positive Surface Charge and Size Tunable Photoluminescence in the Near‐Infrared to Red Spectral Range journal January 2016
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