Simulation of collision-induced absorption spectra based on classical trajectories and ab initio potential and induced dipole surfaces. II. CO2–Ar rototranslational band including true dimer contribution

Chistikov, D.N.; Finenko, A.A.; Kalugina, Y.N.; Lokshtanov, S.E.; Petrov, S.V.; Vigasin, A.A.

Авторы: Chistikov Daniil N., Finenko Artem A., Kalugina Yulia N., Lokshtanov Sergei E., Petrov Sergey V., Vigasin Andrey A.
Журнал: Journal of Chemical Physics
Том: 155
Номер: 6
Год издания: 2021
Издательство: AIP Publishing
Местоположение издательства: United States
Первая страница: 064301-1
Последняя страница: 064301-17
DOI: 10.1063/5.0060779
Аннотация: This paper presents further development of the new semi-classical trajectory-based formalism described in Paper I [Chistikov et al., J. Chem. Phys. 151, 194106 (2019)]. We report the results of simulation and analysis of the low-frequency collision-induced absorption (CIA) in CO2–Ar, including its true dimer component. Our consideration relies on the use of ab initio intermolecular potential energy and induced dipole surfaces for CO2–Ar calculated in an assumption of a rigid CO2 structure using the CCSD(T) method. The theory, the details of which are reported in Paper I [Chistikov et al., J. Chem. Phys. 151, 194106 (2019)], permits taking into account the effect of unbound and quasi-bound classical trajectories on the CIA in the range of a rototranslational band. This theory is largely extended by trajectory-based simulation of the true bound dimer absorption in the present paper. The spectra are obtained from a statistical average over a vast ensembleof classical trajectories restricted by properly chosen domains in the phase space. Rigorous classical theory is developed for two low-order spectral moments interpreted as the Boltzmann-weighted average of the respective dipole functions. These spectral moments were then used to check the accuracy of our trajectory-based spectra, for which both spectral moments can be evaluated independently in terms of specificintegrals over the trajectory-based calculated spectral profiles. Good agreement between the spectral moments calculated as integrals overthe frequency domain or the phase space largely supports the reliability of our simulated CIA spectra, which conform with the available microwave and far-infrared observations.
Добавил в систему: Финенко Артём Андреевич

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Simulation of collision-induced absorption spectra based on classical trajectories and ab initio potential and induced dipole surfaces. II. CO2–Ar rototranslational band including true dimer contributionстатья