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Proc Natl Acad Sci U S A. 2004 Sep 7;101(36):13216-20. Epub 2004 Aug 19.

Coherent vibrational climbing in carboxyhemoglobin.

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  • 1Centre National de la Recherche Scientifique Unité Mixte de Recherche 7645, Institut National de la Santé et de la Recherche Médicale, Ecole Polytechnique-Ecole Nationale Supérieure de Techniques Avancées, Palaiseau, France.


We demonstrate vibrational climbing in the CO stretch of carboxyhemoglobin pumped by midinfrared chirped ultrashort pulses. By use of spectrally resolved pump-probe measurements, we directly observed the induced absorption lines caused by excited vibrational populations up to v = 6. In some cases, we also observed stimulated emission, providing direct evidence of vibrational population inversion. This study provides important spectroscopic parameters on the CO stretch in the strong-field regime, such as transition frequencies and dephasing times up to the v = 6 to v = 7 vibrational transition. We measured equally spaced vibrational transitions, in agreement with the energy levels of a Morse potential up to v = 6. It is interesting that the integral of the differential absorption spectra was observed to deviate far from zero, in contrast to what one would expect from a simple one-dimensional Morse model assuming a linear dependence of dipole moment with bond length.

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