As light propagates through a medium, absorption caused by electronic or rovibrational transitions is evident in the transmitted spectrum. The incident electromagnetic field polarizes the medium and the absorption is due to the imaginary part of the linear susceptibility. In the time domain, the field establishes a coherence in the medium that radiates out of phase with the initial field. This coherence can persist for tens of picoseconds in atmospheric molecules such as ${\mathrm{H}}_2\mathrm{O}$. We propagate a few-cycle laser pulse centered at $1.8\mu \mathrm{m}$ through the atmosphere and measure the long-lasting molecular coherence in the time domain by high-order harmonic cross correlation. The measured optical free-induction decay of the pulse is compared with a calculation based on the calculated rovibrational spectrum of ${\mathrm{H}}_2\mathrm{O}$ absorption.

• Received 30 September 2016

DOI:https://doi.org/10.1103/PhysRevA.94.063410