Understanding the Parameters Affecting the Photoluminescence of Silicon Nanoparticles

Silicon nanoparticles of 1–5 nm size (SiNPs) were synthesized by a bottom-up (BU) approach involving a chemical wet method. The contribution of different emitters to the overall excitation–emission matrix was analyzed on the assumption that pure substances existing in a unique form show an excitatio...

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Bibliographic Details
Published in:Journal of physical chemistry. C 2012-05, Vol.116 (20), p.11315-11325
Main Authors: Llansola Portolés, Manuel J, Pis Diez, Reinaldo, Dell’Arciprete, María L, Caregnato, Paula, Romero, Juan José, Mártire, Daniel O, Azzaroni, Omar, Ceolín, Marcelo, Gonzalez, Mónica C
Format: Article
Language:English
Subjects:
Condensed matter: electronic structure, electrical, magnetic, and optical properties
Condensed matter: structure, mechanical and thermal properties
Cross-disciplinary physics: materials science
rheology
Exact sciences and technology
Low-dimensional structures (superlattices, quantum well structures, multilayers): structure, and nonelectronic properties
Materials science
Nanocrystalline materials
Nanoscale materials and structures: fabrication and characterization
Optical properties and condensed-matter spectroscopy and other interactions of matter with particles and radiation
Optical properties of low-dimensional, mesoscopic, and nanoscale materials and structures
Physics
Structure of solids and liquids
crystallography
Surfaces and interfaces
thin films and whiskers (structure and nonelectronic properties)
X-ray diffraction and scattering
X-ray scattering (including small-angle scattering)
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Summary:Silicon nanoparticles of 1–5 nm size (SiNPs) were synthesized by a bottom-up (BU) approach involving a chemical wet method. The contribution of different emitters to the overall excitation–emission matrix was analyzed on the assumption that pure substances existing in a unique form show an excitation wavelength-invariant emission spectrum. The occurrence of emitters differing in size and aggregation was supported by transmission electron microscopy (TEM), small-angle X-ray scattering (SAXS), time-resolved single photon counting, and time-resolved anisotropy experiments. The effect on photoluminescence (PL) of the particle surface oxidation as a result of aging is studied and compared to that of surface oxidized particles obtained by a top-down (TD) approach following an electrochemical method with HF etching. Surface oxidation to SiO x seems to introduce two different effects on the SiNP PL. An emission originated in surface states associated to SiO x was identified and observed for SiNPs synthesized by both BU and TD approaches. Blue-shifted excitation–emission spectra associated to a silicon core in embedded SiO x nanostructures were also identified. Theoretical studies were carried out to help understand the observed results.
ISSN:1932-7447
1932-7455
DOI:10.1021/jp2117938