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Ultrafast continuum mid-infrared spectroscopy: probing the entire vibrational spectrum in a single laser shot with femtosecond time resolution

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Abstract

Until now, ultrafast IR spectroscopy has been limited by the bandwidth of optical parametric amplifiers, typically 100400cm1. Here we present the first example of transient IR spectroscopy using a continuum laser source to probe the entire mid-IR region with ultrafast time resolution. The continuum source is based on focusing the fundamental, second harmonic, and third harmonic of 1 mJ, 25 fs, 800 nm pulses in air, generating 150fs continuum mid-IR pulses that span the frequency range of <400 to >5000cm-1 or, conversely, <2 to >25μm. We characterize the spectral and temporal properties of dicarbonylacetonato rhodium(I) in hexane. We further demonstrate the versatility of the method by measuring the very fast and broad (>1500cm-1) spectral changes following IR excitation associated with the 7-azaindole–acetic acid heterodimer in carbon tetrachloride.

©2012 Optical Society of America

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