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

Bobbitt, N. Scott; Chelikowsky, James R.

doi:10.1063/1.4943970

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

Journal Article · Fri Mar 25 00:00:00 EDT 2016 · Journal of Chemical Physics

DOI:https://doi.org/10.1063/1.4943970· OSTI ID:1468776

Bobbitt, N. Scott ^[1]; Chelikowsky, James R. ^[2]

Univ. of Texas, Austin, TX (United States). Dept. of Chemical Engineering; University of Texas at Austin
Univ. of Texas, Austin, TX (United States). Dept. of Physics and Chemical Engineering, Center for Computational Materials, Inst. for Computational Engineering and Sciences

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.

View Accepted Manuscript (DOE)

Research Organization:: Univ. of Texas, Austin, TX (United States)

Sponsoring Organization:: USDOE; 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)

Grant/Contract Number:: FG02-06ER46286; SC0008877

OSTI ID:: 1468776

Alternate ID(s):: OSTI ID: 1243362

Journal Information:: Journal of Chemical Physics, Journal Name: Journal of Chemical Physics Journal Issue: 12 Vol. 144; ISSN JCPSA6; ISSN 0021-9606

Publisher:: American Institute of Physics (AIP)Copyright Statement

Country of Publication:: United States

Language:: English

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