Previous infrared pump-probe experiments have utilized pulses generated by typical optical parametric amplifiers, limiting the observable spectral bandwidth to a few hundred wavenumbers.  This requires greater frequency ranges to be measured in parts, as the OPA must be tuned to multiple wavelengths. We have overcome this barrier by focusing the fundamental, second harmonic and third harmonic of 1 mJ, 25 fs, 800 nm pulses in air, generating ultrafast broadband pulses.  The resulting mid-IR continnum spans frequencies from less than 700 cm-1 to more than 5000 cm-1 with a pulse duration of approximately 150 fs.  This source has been utilized in IR pump-continuum IR probe studies on a variety of systems, ranging from the narrow and long-lived dicarbonylacetonato rhodium(I) in hexane to the very broad, fast, and highly-coupled 7-azaindole�acetic acid heterodimer in carbon tetrachloride.

Ultrafast continuum mid-infrared source for probing the entire vibrational spectrum

244th National Meeting (2012)

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