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

文献信息

发布日期 2016-10-05
DOI 10.1039/C6CP05683K
影响因子 3.676
作者

A. Jolene Mork, Elizabeth M. Y. Lee, William A. Tisdale


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摘要

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 = 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 = 0 mode, which we identify as a higher spherical harmonic—the n = 2, = 0 eigenmode—rather than a two-phonon scattering event.

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来源期刊

Physical Chemistry Chemical Physics

Physical Chemistry Chemical Physics
CiteScore: 5.5
自引率: 10.3%
年发文量: 3036

Physical Chemistry Chemical Physics (PCCP) is an international journal co-owned by 19 physical chemistry and physics societies from around the world. This journal publishes original, cutting-edge research in physical chemistry, chemical physics and biophysical chemistry. To be suitable for publication in PCCP, articles must include significant innovation and/or insight into physical chemistry; this is the most important criterion that reviewers and Editors will judge against when evaluating submissions. The journal has a broad scope and welcomes contributions spanning experiment, theory, computation and data science. Topical coverage includes spectroscopy, dynamics, kinetics, statistical mechanics, thermodynamics, electrochemistry, catalysis, surface science, quantum mechanics, quantum computing and machine learning. Interdisciplinary research areas such as polymers and soft matter, materials, nanoscience, energy, surfaces/interfaces, and biophysical chemistry are welcomed if they demonstrate significant innovation and/or insight into physical chemistry. Joined experimental/theoretical studies are particularly appreciated when complementary and based on up-to-date approaches.

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