We have developed a method for calculating the cubic anharmonic couplings in molecular crystals for normal modes with the zero wave vector in the framework of classical mechanics, and have applied it, combined with perturbation theory, to obtain the linewidths of all infrared absorption lines of crystalline pentaerythritol tetranitrate in the terahertz region (<100 cm(-1)). Contributions of the up- and down-conversion processes to the total linewidth were calculated. The computed linewidths are in qualitative agreement with experimental data and the results of molecular dynamics simulations. Quantum corrections to the linewidths in the terahertz region are shown to be negligible.
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http://dx.doi.org/10.1063/1.4866896 | DOI Listing |
J Chem Phys
January 2025
Department of Chemistry, Columbia University, New York, New York 10027, USA.
In this work, we investigate anharmonic vibrational polaritons formed due to strong light-matter interactions in an optical cavity between radiation modes and anharmonic vibrations beyond the long-wavelength limit. We introduce a conceptually simple description of light-matter interactions, where spatially localized cavity radiation modes couple to localized vibrations. Within this theoretical framework, we employ self-consistent phonon theory and vibrational dynamical mean-field theory to efficiently simulate momentum-resolved vibrational-polariton spectra, including effects of anharmonicity.
View Article and Find Full Text PDFSpectrochim Acta A Mol Biomol Spectrosc
December 2024
Hubei Key Laboratory of Optical Information and Pattern Recognition, Wuhan Institute of Technology, Wuhan 430205, China. Electronic address:
Two-dimensional antiferromagnetic materials have attracted wide attention in both performance and application, which are of great significance for spin valves and next-generation magnetic random access memory devices. The spin-phonon coupling effect plays a crucial role in magnon dynamics. However, there is still a lack of research on the spin-phonon coupling effect of two-dimensional antiferromagnetic flakes.
View Article and Find Full Text PDFJ Chem Phys
December 2024
Department of Physics, Stockholm University, AlbaNova University Center, SE-10691 Stockholm, Sweden.
Vibrational polaritons are formed by strong coupling of molecular vibrations and photon modes in an optical cavity. Experiments have demonstrated that vibrational strong coupling can change molecular properties and even affect chemical reactivity. However, the interactions in a molecular ensemble are complex, and the exact mechanisms that lead to modifications are not fully understood yet.
View Article and Find Full Text PDFJ Phys Chem A
January 2025
Astrophysics Branch, NASA Ames Research Center, MS 245-6, Moffett Field, California 94035, United States.
Anharmonic computations reveal an intense, narrow (20 cm, 0.043 μm) absorption feature at approximately 2160 cm (4.63 μm) in the vibrational spectra of 14 prototypical singly isocyano-substituted polycyclic aromatic hydrocarbons (NC-PAHs) attributed to the NC stretching mode.
View Article and Find Full Text PDFJ Chem Phys
December 2024
Department of Chemistry, University of Graz, Heinrichstraße 28/IV, 8010 Graz, Austria.
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