Abstract
We present a procedure for generating the parameters of the Hartmann-Tran profile (HTP) from purely first principles calculations. Starting from an absorber-perturber interaction potential, we calculate S-matrices describing the effect of collisions on the absorbing molecule. We then use the generalized Hess method to calculate speed-dependent pressure shift and broadening parameters, and the complex Dicke parameter, νopt, which accounts for such effects as the Dicke effect and correlations between dephasing and velocity-changing collisions. Based on these ab initio results, we derive the Hartmann-Tran profile parameters and evaluate the validity of the quadratic approximation of speed dependence and the hard-collision model of velocity-changing collisions adopted in the Hartmann-Tran profile. We also discuss the interpretation and speed dependence of νopt. Finally, we evaluate the approximation scheme for temperature dependence of HTP line-shape parameters adopted in the 2016 edition of the HITRAN database.
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