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Temperature dependence of acoustic vibrations of CdSe and CdSe–CdS core–shell nanocrystals measured by low-frequency Raman spectroscopy

Author(s)
Mork, Anna Jolene; Lee, Elizabeth M.; Tisdale, William
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Abstract
We measure the temperature dependence of breathing-mode acoustic vibrations of semiconductor nanocrystals using low-frequency Raman spectroscopy. In CdSe core-only nanocrystals, the lowest-energy l = 0 mode red-shifts with increasing temperature by ∼5% between 77–300 K. Changes to the interatomic bond distances in the inorganic crystal lattice, with corresponding changes to the bulk modulus and density of the material, contribute to the observed energy shift but do not fully explain its magnitude across all nanocrystal sizes. Invariance of the Raman linewidth over the same temperature range suggests that the acoustic breathing mode is inhomogeneously broadened. The acoustic phonons of CdSe/CdS core–shell composite nanocrystals display similar qualitative behavior. However, for large core–shell nanocrystals, we observe a higher-order Raman peak at approximately twice the energy of the l = 0 mode, which we identify as a higher spherical harmonic—the n = 2, l = 0 eigenmode—rather than a two-phonon scattering event.
Date issued
2016-10
URI
http://hdl.handle.net/1721.1/107952
Department
Massachusetts Institute of Technology. Department of Chemical Engineering
Journal
Physical Chemistry Chemical Physics
Publisher
Royal Society of Chemistry
Citation
Mork, A. Jolene, Elizabeth M. Y. Lee, and William A. Tisdale. “Temperature Dependence of Acoustic Vibrations of CdSe and CdSe–CdS Core–shell Nanocrystals Measured by Low-Frequency Raman Spectroscopy.” Phys. Chem. Chem. Phys. 18.41 (2016): 28797–28801. © 2017 Royal Society of Chemistry
Version: Final published version
ISSN
1463-9076
1463-9084

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