We study and describe the reshaping of ultrashort and broadband mid-IR optical pulses in an ambient atmosphere. While all pulse propagation undergoes dispersion and absorption, which causes pulse reshaping, the effects are strongly pronounced for broadband radiation in the mid-IR due to the orders of magnitude greater oscillator strengths of molecular constituents of our atmosphere. A noticeable macroscopic impact is a transition of the measured autocorrelation function from squared hyperbolic secant to Lorentzian, which we fully explain based on pulse propagation, including molecular free induction decay. Electro-optical sampling directly reveals the light wave response to atmospheric molecular free induction decay, and a Kramers–Kronig-based propagation model thoroughly explains the observation. The findings are essential for applications in sensing, standoff detection, high-energy pulse propagation, and energy delivery.
