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Raman Spectroscopy: Overview

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The underlying principle of Raman spectroscopy is based on the interaction between light and matter, specifically molecules' inelastic scattering of photons. When a monochromatic beam of light, typically from a laser source, interacts with a sample, most scattered light has the same frequency as the incident light. This is known as Rayleigh scattering.
However, a small fraction of the scattered light exhibits a frequency shift due to the exchange of energy between the incident photons and...

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Characterization of Nanocrystal Size Distribution using Raman Spectroscopy with a Multi-particle Phonon Confinement Model

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Published on: August 22, 2015

Raman Spectroscopy of Oxide-Embedded and Ligand-Stabilized Silicon Nanocrystals.

Colin M Hessel, Junwei Wei, Dariya Reid

¹§Department of Electrical Engineering and Information Systems, School of Engineering, The University of Tokyo, Tokyo, Japan.

The Journal of Physical Chemistry Letters

|August 20, 2015

Summary

Raman spectroscopy reveals that silicon (Si) nanocrystal size significantly impacts their optical properties. Oxide-free Si nanocrystals show a more pronounced Raman shift with decreasing size than predicted, unlike oxide-embedded ones affected by matrix stress.

Keywords:

BP model HSQ RWL model Raman spectroscopy SAXS TEM X-ray diffraction XRD amorphous silicon hydrogen silsesquioxane modeling oxide-embedded phonon confinement silicon nanocrystals size determination small-angle X-ray scattering transmission electron microscopy

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Area of Science:

Materials Science
Nanotechnology
Solid State Physics

Background:

Silicon (Si) nanocrystals exhibit size-dependent optical and electronic properties.
Raman spectroscopy is a key technique for probing vibrational modes and material properties.
Existing models (e.g., Richter, Wang, and Ley) predict the size dependence of Raman shifts in Si nanocrystals.

Purpose of the Study:

To investigate the size-dependent Raman spectroscopy of oxide-embedded and oxide-free silicon (Si) nanocrystals.
To compare experimental Raman peak shifts with theoretical predictions.
To understand the influence of surface passivation and embedding matrix on Si nanocrystal properties.

Main Methods:

Synthesis of silicon (Si) nanocrystals with varying diameters (3 nm to >10 nm).
Characterization using Raman spectroscopy.
Analysis of Raman peak position (frequency) and line shape (broadening).

Main Results:

For ligand-passivated (oxide-free) Si nanocrystals, the Raman-active mode shifted to lower frequencies with decreasing size, showing asymmetric broadening.
The observed size dependence of Raman shifts in oxide-free Si nanocrystals was more significant than predicted by established models.
Oxide-embedded Si nanocrystals exhibited less pronounced Raman peak shifts due to stress induced by the surrounding matrix.

Conclusions:

The study highlights discrepancies between experimental Raman shifts and theoretical models for oxide-free Si nanocrystals, suggesting limitations in current models.
Matrix-induced stress significantly modifies the vibrational properties of embedded Si nanocrystals.
Surface passivation and the surrounding environment play crucial roles in determining the observable properties of Si nanocrystals.