The importance of the electric‐dipole—electric‐quadrupole polarizability contribution to the vibrational Raman optical activity (VROA) and dimensionless circular intensity difference spectra of (1
- NSF-PAR ID:
- 10444149
- Editor(s):
- Dean, Nicky
- Date Published:
- Journal Name:
- Nature energy
- Volume:
- 7
- ISSN:
- 2058-7546
- Page Range / eLocation ID:
- 1013-1014
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
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Abstract S )‐camphor is examined. The spectra are simulated with and without this tensor contribution using density functional theory calculations, and similarity is evaluated for each against the experimental spectra. Careful examination of the comparison between experimental and calculated spectra reveals multiple vibrational bands, in the ~1,130–950 cm−1region, originating from −C–H bending vibrations that are dominated by the electric‐dipole—electric‐quadrupole polarizability contributions. The similarity overlap analysis also reveals that the similarity overlap between experimental and predicted spectra in the measured spectral range increases, by up to 12%, when electric‐dipole—electric‐quadrupole polarizability contributions are included. The negative VROA band at 1,125 cm−1in the experimental spectrum of (1S)‐(‐)‐camphor can only be reproduced in the predicted spectra when electric‐dipole—electric‐quadrupole polarizability contribution is included. Investigations on additional molecules indicated that (a) two experimental VROA bands of (1S,4R)‐(+)‐fenchone at ~1,740 and 220 cm−1originate from dominating electric‐dipole—electric‐quadrupole polarizability contribution and (b) the symmetric and antisymmetric ring deformation modes of dimethyloxirane have dominating electric‐dipole—electric‐quadrupole polarizability contribution. These observations establish the importance of electric‐dipole—electric‐quadrupole polarizability contribution to VROA for the first time. -
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