Density-functional-based predictions of Raman and IR spectra for small Si clusters

Jackson, Koblar and Pederson, Mark R. and Porezag, Dirk and Hajnal, Zoltán and Frauenheim, Thomas (1997) Density-functional-based predictions of Raman and IR spectra for small Si clusters. Physical Review B (Condensed Matter), 55 (4). pp. 2549-2555. ISSN 0163-1829

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Abstract

We have used a density-functional-based approach to study the response of silicon clusters to applied electric fields. For the dynamical response, we have calculated the Raman activities and infrared (IR) intensities for all of the vibrational modes of several clusters (SiN with N=3-8, 10, 13, 20, and 21) using the local density approximation (LDA). For the smaller clusters (N=3-8) our results are in good agreement with previous quantum-chemical calculations and experimental measurements, establishing that LDA-based IR and Raman data can be used in conjunction with measured spectra to determine the structure of clusters observed in experiment. To illustrate the potential of the method for larger clusters, we present calculated IR and Raman data for two low-energy isomers of Si10 and for the lowest-energy structure of Si13 found to date. For the static response, we compare our calculated polarizabilities for N=10, 13, 20, and 21 to recent experimental measurements. The calculated results are in rough agreement with experiment, but show less variation with cluster size than the measurements. Taken together, our results show that LDA calculations can offer a powerful means for establishing the structures of experimentally fabricated clusters and nanoscale systems.

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