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Ab initio modeling of molecular IR spectra of astrophysical interest: application to CH4

Journal Article · · Astronomy and Astrophysics

Aims. We describe an ab initio-based numerical method of obtaining infrared spectroscopic data (line list) of polyatomic molecules that allows calculation of complete sets of lines for temperatures up to several thousand Kelvin.While the main focus is on completeness and consistency, not spectroscopic accuracy, the approach is in principle “exact” for line positions and, although not exact for line strengths, of sufficient accuracy to be of value, especially in wavelength regions where there are gaps in reliable experimental data. Methods. Global potential energy and dipole moment hypersurfaces are fitted to the results of ab initio electronic structure calculations. The MULTIMODE software is then used to obtain rovibrational energy levels and dipole transition matrix elements. This information is used to calculate a complete set of Einstein coefficients of spontaneous emission Ai j. Results. The method is applied to obtain a spectroscopic database for methane containing over 1.4 million lines up to an upper state energy of 6200 cm-1 (~9000 K). The emission spectrum of CH4 at 1000 K is calculated with the complete set of Einstein coefficients and compared with the one obtained from the HITRAN database. Gaps in the database are realistically filled in by the calculated spectrum. Conclusions. Consistent and complete databases are important for astrophysical applications. Databases obtained by the method described here fulfill this requirement and are sufficiently accurate for astrophysical applications such as model atmosphere calculations and the corresponding synthetic spectra.

Research Organization:
Emory Univ., Atlanta, GA (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Fusion Energy Sciences (FES) (SC-24)
DOE Contract Number:
FG02-07ER54914
OSTI ID:
1124178
Report Number(s):
DOE-Emory-DE-FG02-07ER54914-02; 5-22145
Journal Information:
Astronomy and Astrophysics, Journal Name: Astronomy and Astrophysics Journal Issue: 2 Vol. 495; ISSN 0004-6361
Publisher:
EDP Sciences
Country of Publication:
United States
Language:
English

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  • Carter, Stuart; Bowman, Joel M.; Handy, Nicholas C.
  • Theoretical Chemistry Accounts: Theory, Computation, and Modeling (Theoretica Chimica Acta), Vol. 100, Issue 1-4 https://doi.org/10.1007/s002140050379
journal November 1998