http://arxiv.org/abs/2102.06582
Aromatic Infrared Bands (AIBs) are a set of bright and ubiquitous emission bands, observed in regions illuminated by stellar ultraviolet photons, from our galaxy all the way out to cosmological distances. The forthcoming James Webb Space Telescope will unveil unprecedented spatial and spectral details in the AIB spectrum; significant advancement is thus necessary now to model the infrared emission of polycyclic aromatic hydrocarbons, their presumed carriers, with enough detail to exploit the information content of the AIBs. This requires including anharmonicity in such models, and to do so systematically for all species included, requiring a difficult compromise between accuracy and efficiency. We propose a new recipe using minimal assumptions on the general behaviour of band positions and widths with temperature, which can be defined by a small number of empirical parameters. We explore here the performances of a full quantum method, AnharmoniCaOs, relying on an ab initio potential, and Molecular Dynamics simulations using a Density Functional based Tight Binding potential to determine these parameters for the case of pyrene, for which high temperature gas-phase data are available. The first one is very accurate and detailed, but it becomes computationally very expensive for increasing T; the second trades some accuracy for speed, making it suitable to provide approximate, general trends at high temperatures. We propose to use, for each species and band, the best available empirical parameters for a fast, yet sufficiently accurate spectral model of PAH emission properly including anharmonicity. Modelling accuracy will depend critically on these empirical parameters, allowing for an incremental improvement in model results, as better estimates become gradually available.
S. Chakraborty, G. Mulas, M. Rapacioli, et. al.
Mon, 15 Feb 21
28/53
Comments: submitted to the Journal of Molecular Spectroscopy