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Title: Real-space pseudopotential study of vibrational properties and Raman spectra in Si–Ge core-shell nanocrystals

Abstract

We examine the vibrational properties and Raman spectra of Si–Ge core-shell nanostructures using real-space pseudopotentials constructed within density functional theory. Our method uses no empirical parameters, unlike many popular methods for predicting Raman spectra for nanocrystals. Here, we find the dominant features of the Raman spectrum for the Si–Ge core-shell structure to be a superposition of the Raman spectra of the Ge and Si nanocrystals with optical peaks around 300 and 500 cm -1, respectively. We also find a Si–Ge “interface” peak at 400 cm -1. The Ge shell causes the Si core to expand from the equilibrium structure. This strain induces significant redshift in the Si contribution to the vibrational and Raman spectra, while the Ge shell is largely unstrained and does not exhibit this shift. We find that the ratio of peak heights is strongly related to the relative size of the core and shell regions. This finding suggests that Raman spectroscopy may be used to characterize the size of the core and shell in these structures.

Authors:
 [1];  [2]
  1. Univ. of Texas, Austin, TX (United States). Dept. of Chemical Engineering
  2. Univ. of Texas, Austin, TX (United States). Dept. of Physics and Chemical Engineering, Center for Computational Materials, Inst. for Computational Engineering and Sciences
Publication Date:
Research Org.:
Univ. of Texas, Austin, TX (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Advanced Scientific Computing Research (ASCR) (SC-21). Scientific Discovery through Advanced Computing (SciDAC); USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1468776
Alternate Identifier(s):
OSTI ID: 1243362
Grant/Contract Number:  
SC0008877; FG02-06ER46286
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Chemical Physics
Additional Journal Information:
Journal Volume: 144; Journal Issue: 12; Journal ID: ISSN 0021-9606
Publisher:
American Institute of Physics (AIP)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 36 MATERIALS SCIENCE

Citation Formats

Bobbitt, N. Scott, and Chelikowsky, James R. Real-space pseudopotential study of vibrational properties and Raman spectra in Si–Ge core-shell nanocrystals. United States: N. p., 2016. Web. doi:10.1063/1.4943970.
Bobbitt, N. Scott, & Chelikowsky, James R. Real-space pseudopotential study of vibrational properties and Raman spectra in Si–Ge core-shell nanocrystals. United States. doi:10.1063/1.4943970.
Bobbitt, N. Scott, and Chelikowsky, James R. Fri . "Real-space pseudopotential study of vibrational properties and Raman spectra in Si–Ge core-shell nanocrystals". United States. doi:10.1063/1.4943970. https://www.osti.gov/servlets/purl/1468776.
@article{osti_1468776,
title = {Real-space pseudopotential study of vibrational properties and Raman spectra in Si–Ge core-shell nanocrystals},
author = {Bobbitt, N. Scott and Chelikowsky, James R.},
abstractNote = {We examine the vibrational properties and Raman spectra of Si–Ge core-shell nanostructures using real-space pseudopotentials constructed within density functional theory. Our method uses no empirical parameters, unlike many popular methods for predicting Raman spectra for nanocrystals. Here, we find the dominant features of the Raman spectrum for the Si–Ge core-shell structure to be a superposition of the Raman spectra of the Ge and Si nanocrystals with optical peaks around 300 and 500 cm-1, respectively. We also find a Si–Ge “interface” peak at 400 cm-1. The Ge shell causes the Si core to expand from the equilibrium structure. This strain induces significant redshift in the Si contribution to the vibrational and Raman spectra, while the Ge shell is largely unstrained and does not exhibit this shift. We find that the ratio of peak heights is strongly related to the relative size of the core and shell regions. This finding suggests that Raman spectroscopy may be used to characterize the size of the core and shell in these structures.},
doi = {10.1063/1.4943970},
journal = {Journal of Chemical Physics},
number = 12,
volume = 144,
place = {United States},
year = {2016},
month = {3}
}

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