Buffer-gas pressure influence on multiphoton absorption in SF6–N2 mixtures

Abstract

In this article the results of pulsed IR photoacoustic spectroscopy measurements of multiphoton absorption and relaxation processes in SF6–N2 mixtures are presented. The total average number of absorbed photons per one absorbing molecule (basic physical quantity which characterized multiphoton processes) during the laser pulse 〈n〉total is used and analyzed with a generalized coupled two-level model. This type of analysis is based on buffer-gas pressure (pbuff) functional behavior of 〈n〉total and calculation of its partial values depending on collisions, 〈n〉coll, and laser fluence, 〈n〉Φ, influence. Using different methods of photoacoustic spectroscopy, collisionaly induced rotational and vibrational to translational relaxation process parameters (τrot and τV-T, respectively) are quantitatively obtained and used to determine partial values of 〈n〉coll, 〈n〉rot, and 〈n〉V-T. It will be shown that a method based on ∂〈n〉total/∂p functional dependence on pbuff and laser fluence Φ can be used to confirm or predict the existence of some processes during the laser pulse, such as dissociation or strong vibrational to vibrational energy transfer, which can contribute to the total amount of energy absorbed into the investigated sample. This could allow one to apply this method and control laser field–molecule interaction in different gas mixtures, and help one to understand multiphoton absorption processes in detail.