Ultrafast mid-infrared spectrochronography of dispersion near molecular absorption bands

Quantitative characterization of dispersion near molecular resonances is difficult both conceptually and technically, as it requires systematic measurements of rapidly varying dispersion profiles across the edges of molecular absorption bands. Here, we show that this challenge can be confronted with an ultrafast spectrochronography technique that combines time-resolved four-wave mixing and cross-correlation frequency-resolved optical gating. We demonstrate that, with the spectrum of an ultrashort mid-infrared laser probe stretching across the edge of a molecular absorption band, the Wigner chronocyclic maps of such a probe reveal universal signatures of anomalous dispersion and help quantify such dispersion anomalies.