Few-cycle mid-infrared pulse generation, characterization, and coherent propagation in optically dense media

The generation of four- to five-cycle mid-infrared pulses using a single-stage potassium niobate optical parametric amplifier (OPA) is demonstrated. The OPA is pumped by a gain-switched Ti:Sapphire regenerative amplifier and is seeded with the near-infrared portion of a white light continuum. The OPA is continuously tunable from 2700 to 4700 nm, and maintains sub-65 fs pulses that are fully characterized using cross-correlation frequency-resolved optical gating (XFROG). These are the shortest near-transform-limited pulses reported over this large infrared spectral range. This apparatus is used to measure ultrafast vibrational responses, specifically, pulse profiles modified by the free-induction decay (FID) of O–H oscillators. Both the intensity and instantaneous phase of these pulses are determined after traversing samples of isotopically diluted water (HDO in D2O) using XFROG, representing a new application of the XFROG technique to the study of (dipolar) molecular responses. Pronounced beating of the t...

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