Use of Ab Initio Methods for the Interpretation of the Experimental IR Reflectance Spectra of Crystalline Compounds

It is shown that ab initio simulation can be used as a powerful complementary tool in the interpretation of the experimental reflectance spectra R(v) of crystalline compounds. Experimental frequencies and intensities are obtained from a best fit of R(v) with a set of damped harmonic oscillators, who...

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Main Authors: De La Pierre, Marco, Orlando, R., Dovesi, R.
Format: Journal Article
Published: Wiley 2014
Online Access:http://hdl.handle.net/20.500.11937/18954
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author De La Pierre, Marco
Orlando, R.
Dovesi, R.
author_facet De La Pierre, Marco
Orlando, R.
Dovesi, R.
author_sort De La Pierre, Marco
building Curtin Institutional Repository
collection Online Access
description It is shown that ab initio simulation can be used as a powerful complementary tool in the interpretation of the experimental reflectance spectra R(v) of crystalline compounds. Experimental frequencies and intensities are obtained from a best fit of R(v) with a set of damped harmonic oscillators, whose number and initial position in frequency can dramatically influence the final results, as the parameters are strongly correlated. Computed ab initio values for frequencies and intensities are accurate enough to represent an excellent starting point for the best fit process. Moreover, at variance with respect to experiment, simulation permits to identify all the symmetry allowed modes, also when characterized by low intensity or when close to a very intense peak. Overall, simulation-aided analysis of experimental spectra prevents from classifying combination modes as fundamental modes and permits to discard artifacts due to superposition of bands, background, and noise. Finally, it allows to (almost) completely characterize the set of fundamental modes.
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spelling curtin-20.500.11937-189542019-02-19T05:35:28Z Use of Ab Initio Methods for the Interpretation of the Experimental IR Reflectance Spectra of Crystalline Compounds De La Pierre, Marco Orlando, R. Dovesi, R. It is shown that ab initio simulation can be used as a powerful complementary tool in the interpretation of the experimental reflectance spectra R(v) of crystalline compounds. Experimental frequencies and intensities are obtained from a best fit of R(v) with a set of damped harmonic oscillators, whose number and initial position in frequency can dramatically influence the final results, as the parameters are strongly correlated. Computed ab initio values for frequencies and intensities are accurate enough to represent an excellent starting point for the best fit process. Moreover, at variance with respect to experiment, simulation permits to identify all the symmetry allowed modes, also when characterized by low intensity or when close to a very intense peak. Overall, simulation-aided analysis of experimental spectra prevents from classifying combination modes as fundamental modes and permits to discard artifacts due to superposition of bands, background, and noise. Finally, it allows to (almost) completely characterize the set of fundamental modes. 2014 Journal Article http://hdl.handle.net/20.500.11937/18954 10.1002/jcc.23283 Wiley fulltext
spellingShingle De La Pierre, Marco
Orlando, R.
Dovesi, R.
Use of Ab Initio Methods for the Interpretation of the Experimental IR Reflectance Spectra of Crystalline Compounds
title Use of Ab Initio Methods for the Interpretation of the Experimental IR Reflectance Spectra of Crystalline Compounds
title_full Use of Ab Initio Methods for the Interpretation of the Experimental IR Reflectance Spectra of Crystalline Compounds
title_fullStr Use of Ab Initio Methods for the Interpretation of the Experimental IR Reflectance Spectra of Crystalline Compounds
title_full_unstemmed Use of Ab Initio Methods for the Interpretation of the Experimental IR Reflectance Spectra of Crystalline Compounds
title_short Use of Ab Initio Methods for the Interpretation of the Experimental IR Reflectance Spectra of Crystalline Compounds
title_sort use of ab initio methods for the interpretation of the experimental ir reflectance spectra of crystalline compounds
url http://hdl.handle.net/20.500.11937/18954